From 676991d4dfb76b22ea0513d2eae04f7fcad992eb Mon Sep 17 00:00:00 2001 From: =?UTF-8?q?Alo=C3=AFs=20Castellano?= Date: Thu, 6 Feb 2025 16:41:25 +0100 Subject: [PATCH 01/28] First draft of reshaped anharmonic_free_energy --- src/anharmonic_free_energy/Makefile | 13 +- src/anharmonic_free_energy/energy.f90 | 632 --------------------- src/anharmonic_free_energy/epot.f90 | 337 +---------- src/anharmonic_free_energy/fourthorder.f90 | 434 ++++++++++++++ src/anharmonic_free_energy/main.f90 | 402 +++++++++---- src/anharmonic_free_energy/old.main.f90 | 253 +++++++++ src/anharmonic_free_energy/options.f90 | 44 +- src/anharmonic_free_energy/thermo.f90 | 31 + src/anharmonic_free_energy/thirdorder.f90 | 292 ++++++++++ src/libolle/gottochblandat.f90 | 6 + src/libolle/gottochblandat_physics.f90 | 21 + src/libolle/type_phonon_dispersions.f90 | 98 +++- 12 files changed, 1467 insertions(+), 1096 deletions(-) create mode 100644 src/anharmonic_free_energy/fourthorder.f90 create mode 100644 src/anharmonic_free_energy/old.main.f90 create mode 100644 src/anharmonic_free_energy/thermo.f90 create mode 100644 src/anharmonic_free_energy/thirdorder.f90 diff --git a/src/anharmonic_free_energy/Makefile b/src/anharmonic_free_energy/Makefile index 2eeeeee8..a93d2d11 100644 --- a/src/anharmonic_free_energy/Makefile +++ b/src/anharmonic_free_energy/Makefile @@ -3,7 +3,7 @@ CODE=anharmonic_free_energy PROG=../../build/$(CODE)/$(CODE) OBJECT_PATH=../../build/$(CODE)/ -OBJS = $(OBJECT_PATH)main.o $(OBJECT_PATH)options.o $(OBJECT_PATH)energy.o $(OBJECT_PATH)epot.o +OBJS = $(OBJECT_PATH)main.o $(OBJECT_PATH)options.o $(OBJECT_PATH)thirdorder.o $(OBJECT_PATH)fourthorder.o $(OBJECT_PATH)epot.o LPATH = -L../../lib $(blaslapackLPATH) $(incLPATHhdf) $(incLPATHmpi) IPATH = -I../../inc/libolle -I../../inc/libflap $(blaslapackIPATH) $(incIPATHhdf) $(incIPATHmpi) @@ -24,12 +24,15 @@ clean: .f90.o: $(F90) $(F90FLAGS) -c $< $(LIBS) -$(OBJECT_PATH)main.o: main.f90 $(OBJECT_PATH)options.o $(OBJECT_PATH)energy.o $(OBJECT_PATH)epot.o +$(OBJECT_PATH)main.o: main.f90 $(OBJECT_PATH)options.o $(OBJECT_PATH)thirdorder.o $(OBJECT_PATH)fourthorder.o $(OBJECT_PATH)epot.o $(OBJECT_PATH)thermo.o $(F90) $(F90FLAGS) -c main.f90 $(LIBS) -o $@ -$(OBJECT_PATH)energy.o: $(OBJECT_PATH)options.o - $(F90) $(F90FLAGS) -c energy.f90 $(LIBS) -o $@ +$(OBJECT_PATH)thirdorder.o: $(OBJECT_PATH)options.o + $(F90) $(F90FLAGS) -c thirdorder.f90 $(LIBS) -o $@ +$(OBJECT_PATH)fourthorder.o: $(OBJECT_PATH)options.o + $(F90) $(F90FLAGS) -c fourthorder.f90 $(LIBS) -o $@ $(OBJECT_PATH)options.o: $(F90) $(F90FLAGS) -c options.f90 $(LIBS) -o $@ $(OBJECT_PATH)epot.o: epot.f90 $(F90) $(F90FLAGS) -c epot.f90 $(LIBS) -o $@ - +$(OBJECT_PATH)thermo.o: thermo.f90 + $(F90) $(F90FLAGS) -c thermo.f90 $(LIBS) -o $@ diff --git a/src/anharmonic_free_energy/energy.f90 b/src/anharmonic_free_energy/energy.f90 index c3b502d2..eaa52a9c 100644 --- a/src/anharmonic_free_energy/energy.f90 +++ b/src/anharmonic_free_energy/energy.f90 @@ -358,115 +358,6 @@ subroutine perturbative_anharmonic_free_energy(p, fct, fcf, qp, dr, temperature, write (*, *) '... got anharmonic free energy (', tochar(t1 - timer), 's)' end if - ! !> and the fourth order things - ! fourth: block - ! real(r8), parameter :: fourphonon_prefactor=1.0_r8/32.0_r8 - ! complex(r8) :: c0 - ! !real(r8), dimension(:,:,:), allocatable :: psibuf - ! real(r8), dimension(4) :: omega - ! real(r8), dimension(3) :: qv1,qv2,qv3,qv4 - ! real(r8) :: psi,prefactor,n1,n2,f1 - ! integer :: q1,q2,b1,b2,b3,i,j,l - ! ! buffers for speed - ! complex(r8), dimension(:,:), allocatable :: egv,flat_cwrk - ! real(r8), dimension(:,:), allocatable :: flat_m,flat_r2,flat_r3,flat_r4 - ! real(r8), dimension(dr%n_mode) :: dumom1,dumom3,dump1,dump3 - ! real(r8) :: omthres - ! integer(i8) :: ctrlong - ! integer, dimension(:,:), allocatable :: flat_ai - ! integer :: nquartet - ! - ! - ! allocate(en4(dr%n_mode,qp%n_irr_point)) - ! en4=0.0_r8 - ! - ! omthres=dr%omega_min*0.5_r8 - ! ! create some buffers - ! nquartet=0 - ! do i=1,fcf%na - ! nquartet=nquartet+fcf%atom(i)%n - ! enddo - ! allocate(flat_m(81,nquartet)) - ! allocate(flat_r2(3,nquartet)) - ! allocate(flat_r3(3,nquartet)) - ! allocate(flat_r4(3,nquartet)) - ! allocate(flat_cwrk(81,fcf%na**4)) - ! allocate(flat_ai(4,nquartet)) - ! l=0 - ! do i=1,fcf%na - ! do j=1,fcf%atom(i)%n - ! l=l+1 - ! flat_r2(:,l)=fcf%atom(i)%quartet(j)%lv2 - ! flat_r3(:,l)=fcf%atom(i)%quartet(j)%lv3 - ! flat_r4(:,l)=fcf%atom(i)%quartet(j)%lv4 - ! flat_m(:,l)=lo_flattentensor( fcf%atom(i)%quartet(j)%mwm ) - ! flat_ai(:,l)=[fcf%atom(i)%quartet(j)%i1,fcf%atom(i)%quartet(j)%i2,fcf%atom(i)%quartet(j)%i3,fcf%atom(i)%quartet(j)%i4] - ! enddo - ! enddo - ! allocate(egv(dr%n_mode,4)) - ! egv=0.0_r8 - ! ! the unit - ! !prefactor=1.0_r8/32.0_r8 - ! - ! ! start integrating - ! ctrlong=0 - ! do q1=1,qp%n_irr_point - ! do q2=1,qp%n_full_point - ! ! q-vectors - ! qv1= qp%ip(q1)%r*lo_twopi - ! qv2=-qp%ip(q1)%r*lo_twopi - ! qv3= qp%ap(q2)%r*lo_twopi - ! qv4=-qp%ap(q2)%r*lo_twopi - ! ! store omega and planck-factors in a buffer - ! do b1=1,dr%n_mode - ! dumom1(b1)=dr%iq(q1)%omega(b1) - ! dumom3(b1)=dr%aq(q2)%omega(b1) - ! dump1(b1)=lo_planck(temperature,dumom1(b1)) - ! dump3(b1)=lo_planck(temperature,dumom3(b1)) - ! enddo - ! - ! prefactor=fourphonon_prefactor*qp%ap(q2)%integration_weight - ! - ! ! technically four band-loops, but b1=b2 and b3=b4 - ! do b1=1,dr%n_mode - ! ctrlong=ctrlong+1; if ( mod(ctrlong,int(mw%n,r8)) .ne. mw%r ) cycle - ! do b3=1,dr%n_mode - ! omega=[dumom1(b1),dumom1(b1),dumom3(b3),dumom3(b3)] - ! if ( minval(omega) .lt. omthres ) cycle - ! egv(:,1)=dr%iq(q1)%egv(:,b1) - ! egv(:,2)=conjg(dr%iq(q1)%egv(:,b1)) - ! egv(:,3)=dr%aq(q2)%egv(:,b3) - ! egv(:,4)=conjg(dr%aq(q2)%egv(:,b3)) - ! call loc_4phpsi(fcf%na,nquartet,flat_r2,flat_r3,flat_r4,flat_m,flat_cwrk,flat_ai,omega,egv,qv2,qv3,qv4,c0) - ! psi=real(c0,r8) - ! - ! n1=dump1(b1) - ! n2=dump3(b3) - ! f1=(2*n1+1)*(2*n2+1)*psi*prefactor - ! - ! - ! en4(b1,q1)=en4(b1,q1)+f1 - ! enddo - ! enddo - ! enddo - ! if ( mw%talk ) write(*,*) 'did',q1,qp%n_irr_point - ! enddo - ! - ! if ( mw%talk ) then - ! write(*,*) 'fourth new:',free_energy_fourthorder - ! endif - ! - ! call mw%allreduce('sum',en4) - ! free_energy_fourthorder=0.0_r8 - ! do q1=1,qp%n_irr_point - ! free_energy_fourthorder=free_energy_fourthorder+sum(en4(:,q1))*qp%ip(q1)%integration_weight - ! enddo - ! free_energy_fourthorder=free_energy_fourthorder/p%na - ! - ! if ( mw%talk ) then - ! write(*,*) 'fourth old:',free_energy_fourthorder - ! endif - ! end block fourth end subroutine !> pre-transform to get half of the third order matrix element @@ -628,527 +519,4 @@ pure function triplet_to_singlet(gi, ny, nz) result(l) end function end function -! subroutine loc_4phpsi(na,nquartet,flv2,flv3,flv4,fm,fcw,fai,omega,egv,q2,q3,q4,psi) -! !> temporary work arrays, that actually is the force constant -! integer, intent(in) :: na,nquartet -! real(r8), dimension(3,nquartet), intent(in) :: flv2,flv3,flv4 -! real(r8), dimension(81,nquartet), intent(in) :: fm -! complex(r8), dimension(81,na*na*na*na), intent(inout) :: fcw -! integer, dimension(4,nquartet), intent(in) :: fai -! !> four frequencies -! real(r8), dimension(4), intent(in) :: omega -! !> four eigenvectors -! complex(r8), dimension(na*3,4), intent(in) :: egv -! !> three q-points -! real(r8), dimension(3), intent(in) :: q2,q3,q4 -! !> the matrix element -! complex(r8), intent(out) :: psi -! -! complex(r8) :: expiqr,c0 -! real(r8), dimension(3) :: rv2,rv3,rv4 -! real(r8) :: iqr,omegaprod -! real(r8), parameter :: enhet=1.0_r8 !5.8104841317859603E074_r8 -! integer :: atom1,atom2,atom3,atom4,i,j,k,l,k1,k2,k3,k4,ii,jj -! integer :: na3,na2 -! -! na3=na*na*na -! na2=na*na -! ! Eigenvector product, again -! do atom1=1,na -! do atom2=1,na -! do atom3=1,na -! do atom4=1,na -! ii=(atom1-1)*na3+(atom2-1)*na2+(atom3-1)*na+atom4 -! do i=1,3 -! do j=1,3 -! do k=1,3 -! do l=1,3 -! jj=(i-1)*27+(j-1)*9+(k-1)*3+l -! k1=(atom1-1)*3+i -! k2=(atom2-1)*3+j -! k3=(atom3-1)*3+k -! k4=(atom4-1)*3+l -! fcw(jj,ii)=egv(k1,1)*egv(k2,2)*egv(k3,3)*egv(k4,4) -! enddo -! enddo -! enddo -! enddo -! enddo -! enddo -! enddo -! enddo -! -! ! Frequency product -! omegaprod=omega(1)*omega(2)*omega(3)*omega(4) -! omegaprod=sqrt(omegaprod) -! ! The actual matrix element -! c0=0.0_r8 -! do i=1,nquartet -! atom1=fai(1,i) -! atom2=fai(2,i) -! atom3=fai(3,i) -! atom4=fai(4,i) -! ii=(atom1-1)*na3+(atom2-1)*na2+(atom3-1)*na+atom4 -! rv2=flv2(:,i) -! rv3=flv3(:,i) -! rv4=flv4(:,i) -! iqr=dot_product(q2,rv2)+dot_product(q3,rv3)+dot_product(q4,rv4) -! expiqr=cmplx(cos(iqr),sin(iqr),r8) -! c0=c0+sum(fcw(:,ii)*fm(:,i))*expiqr -! enddo -! psi=enhet*c0/omegaprod -! end subroutine - -! !> impossibly convoluted way of calculating the anharmonic free energy. Really parallel though! -! subroutine impossible_free_energy(uc,fc,fct,fcf,qp,dr,temperature,free_energy_thirdorder,free_energy_fourthorder,mw) -! !> crystal structure -! type(lo_crystalstructure), intent(in) :: uc -! !> second order force constant -! type(lo_forceconstant_secondorder), intent(inout) :: fc -! !> third order force constant -! type(lo_forceconstant_thirdorder), intent(in) :: fct -! !> fourth order force constant -! type(lo_forceconstant_fourthorder), intent(in) :: fcf -! !> q-point mesh -! type(lo_fft_mesh), intent(in) :: qp -! !> dispersions -! type(lo_phonon_dispersions), intent(in) :: dr -! !> temperature -! real(r8) :: temperature -! !> free energies -! real(r8), intent(out) :: free_energy_thirdorder,free_energy_fourthorder -! !> mpi helper -! type(lo_mpi_helper) :: mw -! -! real(r8), dimension(:,:), allocatable :: en3,en4 -! real(r8) :: omthres,sigma -! integer :: index_gamma -! real(r8) :: t0,t1 -! -! t0=walltime() -! t1=t0 -! -! init: block -! integer :: i -! sigma=lo_mean(dr%default_smearing) -! omthres=dr%omega_min*0.5_r8 -! index_gamma=-1 -! do i=1,qp%n_irr_point -! if ( lo_sqnorm(qp%ip(i)%r) .lt. lo_sqtol ) then -! index_gamma=i -! exit -! endif -! enddo -! lo_allocate(en3(dr%n_mode,qp%n_irr_point)) -! lo_allocate(en4(dr%n_mode,qp%n_irr_point)) -! en3=0.0_r8 -! en4=0.0_r8 -! -! if ( mw%talk ) then -! t1=walltime() -! write(*,*) 'init:',t1-t0 -! t0=t1 -! endif -! end block init -! -! ! Start with the third order -! third: block -! complex(r8) :: c0 -! real(r8), dimension(3) :: v0,qv1,qv2,qv3,omega -! real(r8) :: psisquare,doublepsi,prefactor -! real(r8) :: n1,n2,n3,f0,f1,f2,f3 -! integer, dimension(3) :: gi -! integer :: q1,q2,q3,iq2,b1,b2,b3,ctr -! ! buffers for speed -! complex(r8), dimension(:,:,:,:,:,:), allocatable :: cwrk,cdwrk -! real(r8), dimension(dr%n_mode) :: pbuf1,pbuf2,pbuf3,ombuf1,ombuf2,ombuf3 -! real(r8), parameter :: onethird=1.0_r8/3.0_r8 -! -! ! work-array for the scattering amplitude -! allocate(cwrk(3,3,3,fct%na,fct%na,fct%na)) ! work-array for scattering amplitude -! allocate(cdwrk(3,3,3,fct%na,fct%na,fct%na)) ! work-array for scattering amplitude -! -! ctr=0 -! prefactor=-1.0_r8/48.0_r8 -! do q1=1,qp%n_irr_point -! do q2=1,qp%n_full_point -! ! locate the third q-vector -! v0=uc%cartesian_to_fractional(-qp%ip(q1)%r-qp%ap(q2)%r,reciprocal=.true.) -! gi=qp%index_from_coordinate(v0) -! q3=qp%gridind2ind(gi(1),gi(2),gi(3)) -! ! buffer things -! do b1=1,dr%n_mode -! ombuf1(b1)=dr%iq(q1)%omega(b1) -! ombuf2(b1)=dr%aq(q2)%omega(b1) -! ombuf3(b1)=dr%aq(q3)%omega(b1) -! pbuf1(b1)=lo_planck(temperature,ombuf1(b1)) -! pbuf2(b1)=lo_planck(temperature,ombuf2(b1)) -! pbuf3(b1)=lo_planck(temperature,ombuf3(b1)) -! enddo -! ! get the vectors, and add 2*pi -! qv1=-qp%ip(q1)%r*lo_twopi -! qv2=-qp%ap(q2)%r*lo_twopi -! qv3=-qp%ap(q3)%r*lo_twopi -! ! do the MPI-division here. Should make it really parallel. -! ! should also mean minimal overhead. -! do b1=1,dr%n_mode -! ctr=ctr+1; if ( mod(ctr,mw%n) .ne. mw%r ) cycle -! do b2=1,dr%n_mode -! do b3=1,dr%n_mode -! omega(1)=ombuf1(b1) -! omega(2)=ombuf2(b2) -! omega(3)=ombuf3(b3) -! if ( minval(omega) .gt. omthres ) then -! ! normal three-phonon thing, matrix element -! call loc_3phpsi(fct,omega,dr%iq(q1)%egv(:,b1),dr%aq(q2)%egv(:,b2),dr%aq(q3)%egv(:,b3),qv2,qv3,cwrk,c0) -! psisquare=abs(conjg(c0)*c0) -! n1=pbuf1(b1) -! n2=pbuf2(b2) -! n3=pbuf3(b3) -! ! prefactors for the other stuff -! f1=n1*n2+n1+onethird -! f1=3*f1*real(1.0_r8/( omega(1)+omega(2)+omega(3)+lo_imag*sigma )) -! f2=2*n1*n3-n1*n2+n3 -! f2=3*f2*real(1.0_r8/( omega(1)+omega(2)-omega(3)+lo_imag*sigma )) -! else -! f1=0.0_r8 -! f2=0.0_r8 -! psisquare=0.0_r8 -! endif -! ! get the double-psi term -! !omega(3)=dr%iq(index_gamma)%omega(b3) -! !if ( minval(omega) .gt. omthres ) then -! ! call loc_3phdbl(fct,omega,dr%iq(q1)%egv(:,b1),dr%aq(q2)%egv(:,b2),dr%aq(index_gamma)%egv(:,b3),qv1,qv2,cwrk,cdwrk,c0) -! ! doublepsi=real(c0) -! ! f3=6*(n1*(n2+1)+0.25_r8) -! ! f3=f3*real(1.0_r8/( omega(3)+lo_imag*sigma )) -! !else -! ! doublepsi=0.0_r8 -! ! f3=0.0_r8 -! !endif -! doublepsi=0.0_r8 -! f3=0.0_r8 -! ! Add it up -! !psisquare=1.0_r8 -! f0=( (f1+f2)*psisquare+f3*doublepsi )*prefactor -! en3(b1,q1)=en3(b1,q1)+f0 -! enddo -! enddo -! enddo -! enddo -! enddo -! -! if ( mw%talk ) then -! t1=walltime() -! write(*,*) 'third:',t1-t0 -! t0=t1 -! endif -! -! end block third -! -! !> and the fourth order things -! fourth: block -! complex(r8) :: c0 -! real(r8), dimension(:,:,:), allocatable :: psibuf -! real(r8), dimension(4) :: omega -! real(r8), dimension(3) :: qv1,qv2,qv3,qv4 -! real(r8) :: psi,prefactor,n1,n2,f1 -! integer :: q1,q2,b1,b2,b3,b4,i,j,l -! ! buffers for speed -! complex(r8), dimension(:,:), allocatable :: egv,flat_cwrk -! real(r8), dimension(:,:), allocatable :: flat_m,flat_r2,flat_r3,flat_r4 -! real(r8), dimension(dr%n_mode) :: dumom1,dumom3,dump1,dump3 -! integer(i8) :: ctrlong -! integer, dimension(:,:), allocatable :: flat_ai -! integer :: nquartet -! -! ! create some buffers -! nquartet=0 -! do i=1,fcf%na -! nquartet=nquartet+fcf%atom(i)%n -! enddo -! allocate(flat_m(81,nquartet)) -! allocate(flat_r2(3,nquartet)) -! allocate(flat_r3(3,nquartet)) -! allocate(flat_r4(3,nquartet)) -! allocate(flat_cwrk(81,fcf%na**4)) -! allocate(flat_ai(4,nquartet)) -! l=0 -! do i=1,fcf%na -! do j=1,fcf%atom(i)%n -! l=l+1 -! flat_r2(:,l)=fcf%atom(i)%quartet(j)%lv2 -! flat_r3(:,l)=fcf%atom(i)%quartet(j)%lv3 -! flat_r4(:,l)=fcf%atom(i)%quartet(j)%lv4 -! flat_m(:,l)=lo_flattentensor( fcf%atom(i)%quartet(j)%mwm ) -! flat_ai(:,l)=[fcf%atom(i)%quartet(j)%i1,fcf%atom(i)%quartet(j)%i2,fcf%atom(i)%quartet(j)%i3,fcf%atom(i)%quartet(j)%i4] -! enddo -! enddo -! lo_allocate(egv(dr%n_mode,4)) -! egv=0.0_r8 -! ! the unit -! prefactor=1.0_r8/32.0_r8 -! -! ! start integrating -! ctrlong=0 -! do q1=1,qp%n_irr_point -! do q2=1,qp%n_full_point -! ! q-vectors -! qv1= qp%ip(q1)%r*lo_twopi -! qv2=-qp%ip(q1)%r*lo_twopi -! qv3= qp%ap(q2)%r*lo_twopi -! qv4=-qp%ap(q2)%r*lo_twopi -! ! store omega and planck-factors in a buffer -! do b1=1,dr%n_mode -! dumom1(b1)=dr%iq(q1)%omega(b1) -! dumom3(b1)=dr%aq(q2)%omega(b1) -! dump1(b1)=lo_planck(temperature,dumom1(b1)) -! dump3(b1)=lo_planck(temperature,dumom3(b1)) -! enddo -! ! technically four band-loops, but b1=b2 and b3=b4 -! do b1=1,dr%n_mode -! ctrlong=ctrlong+1; if ( mod(ctrlong,int(mw%n,r8)) .ne. mw%r ) cycle -! do b3=1,dr%n_mode -! omega=[dumom1(b1),dumom1(b1),dumom3(b3),dumom3(b3)] -! if ( minval(omega) .lt. omthres ) cycle -! egv(:,1)=dr%iq(q1)%egv(:,b1) -! egv(:,2)=conjg(dr%iq(q1)%egv(:,b1)) -! egv(:,3)=dr%aq(q2)%egv(:,b3) -! egv(:,4)=conjg(dr%aq(q2)%egv(:,b3)) -! call loc_4phpsi(fcf%na,nquartet,flat_r2,flat_r3,flat_r4,flat_m,flat_cwrk,flat_ai,omega,egv,qv2,qv3,qv4,c0) -! psi=real(c0) -! n1=dump1(b1) -! n2=dump3(b3) -! f1=(2*n1+1)*(2*n2+1)*psi*prefactor -! en4(b1,q1)=en4(b1,q1)+f1 -! enddo -! enddo -! enddo -! enddo -! -! if ( mw%talk ) then -! t1=walltime() -! write(*,*) 'fourth:',t1-t0 -! t0=t1 -! endif -! -! end block fourth -! -! !> add things up -! finalize: block -! integer :: i,j -! call mpi_allreduce(MPI_IN_PLACE,en3,dr%n_mode*qp%n_irr_point,MPI_DOUBLE_PRECISION,MPI_SUM,mw%comm,mw%error ) -! call mpi_allreduce(MPI_IN_PLACE,en4,dr%n_mode*qp%n_irr_point,MPI_DOUBLE_PRECISION,MPI_SUM,mw%comm,mw%error ) -! en3=en3/real(qp%n_full_point,r8)/real(fc%na,r8) -! en4=en4/real(qp%n_full_point,r8)/real(fc%na,r8) -! free_energy_thirdorder=0.0_r8 -! free_energy_fourthorder=0.0_r8 -! do i=1,qp%n_irr_point -! free_energy_thirdorder=free_energy_thirdorder+sum(en3(:,i))*qp%ip(i)%integration_weight -! free_energy_fourthorder=free_energy_fourthorder+sum(en4(:,i))*qp%ip(i)%integration_weight -! enddo -! end block finalize -! -! contains -! ! specialized four-phonon matrix element, where q2=-q1, q4=-q3 -! subroutine loc_4phpsi(na,nquartet,flv2,flv3,flv4,fm,fcw,fai,omega,egv,q2,q3,q4,psi) -! !> temporary work arrays, that actually is the force constant -! integer, intent(in) :: na,nquartet -! real(r8), dimension(3,nquartet), intent(in) :: flv2,flv3,flv4 -! real(r8), dimension(81,nquartet), intent(in) :: fm -! complex(r8), dimension(81,na*na*na*na), intent(inout) :: fcw -! integer, dimension(4,nquartet), intent(in) :: fai -! !> four frequencies -! real(r8), dimension(4), intent(in) :: omega -! !> four eigenvectors -! complex(r8), dimension(na*3,4), intent(in) :: egv -! !> three q-points -! real(r8), dimension(3), intent(in) :: q2,q3,q4 -! !> the matrix element -! complex(r8), intent(out) :: psi -! -! complex(r8) :: expiqr,c0 -! real(r8), dimension(3) :: rv2,rv3,rv4 -! real(r8) :: iqr,omegaprod -! real(r8), parameter :: enhet=1.0_r8 !5.8104841317859603E074_r8 -! integer :: atom1,atom2,atom3,atom4,i,j,k,l,k1,k2,k3,k4,ii,jj -! integer :: na3,na2 -! -! na3=na*na*na -! na2=na*na -! ! Eigenvector product, again -! do atom1=1,na -! do atom2=1,na -! do atom3=1,na -! do atom4=1,na -! ii=(atom1-1)*na3+(atom2-1)*na2+(atom3-1)*na+atom4 -! do i=1,3 -! do j=1,3 -! do k=1,3 -! do l=1,3 -! jj=(i-1)*27+(j-1)*9+(k-1)*3+l -! k1=(atom1-1)*3+i -! k2=(atom2-1)*3+j -! k3=(atom3-1)*3+k -! k4=(atom4-1)*3+l -! fcw(jj,ii)=egv(k1,1)*egv(k2,2)*egv(k3,3)*egv(k4,4) -! enddo -! enddo -! enddo -! enddo -! enddo -! enddo -! enddo -! enddo -! -! ! Frequency product -! omegaprod=omega(1)*omega(2)*omega(3)*omega(4) -! omegaprod=sqrt(omegaprod) -! ! The actual matrix element -! c0=0.0_r8 -! do i=1,nquartet -! atom1=fai(1,i) -! atom2=fai(2,i) -! atom3=fai(3,i) -! atom4=fai(4,i) -! ii=(atom1-1)*na3+(atom2-1)*na2+(atom3-1)*na+atom4 -! rv2=flv2(:,i) -! rv3=flv3(:,i) -! rv4=flv4(:,i) -! iqr=dot_product(q2,rv2)+dot_product(q3,rv3)+dot_product(q4,rv4) -! expiqr=cmplx(cos(iqr),sin(iqr),r8) -! c0=c0+sum(fcw(:,ii)*fm(:,i))*expiqr -! enddo -! psi=enhet*c0/omegaprod -! end subroutine -! !> The three-phonon matrix element -! pure subroutine loc_3phpsi(fc,omega,egv1,egv2,egv3,q2,q3,egvprod,psi) -! !> the third order force constant -! class(lo_forceconstant_thirdorder), intent(in) :: fc -! !> the frequencies in question -! real(r8), dimension(3), intent(in) :: omega -! !> the eigenvectors -! complex(r8), dimension(fc%na*3), intent(in) :: egv1,egv2,egv3 -! !> the two q-vectors that matter -! real(r8), dimension(3), intent(in) :: q2,q3 -! !> work array -! complex(r8), dimension(3,3,3,fc%na,fc%na,fc%na), intent(inout) :: egvprod -! ! Matrix element -! complex(r8), intent(out) :: psi -! -! complex(r8) :: expiqr,c0 -! real(r8), dimension(3) :: rv2,rv3 -! real(r8) :: iqr,omegaprod -! real(r8), parameter :: enhet=1.0_r8 !2.367755374064161E51_r8 -! integer :: atom1,atom2,atom3,i,j,k,k1,k2,k3,t -! -! ! Eigenvector product -! do atom3=1,fc%na -! do atom2=1,fc%na -! do atom1=1,fc%na -! do k=1,3 -! do j=1,3 -! do i=1,3 -! k1=(atom1-1)*3+i -! k2=(atom2-1)*3+j -! k3=(atom3-1)*3+k -! egvprod(i,j,k,atom1,atom2,atom3)=egv1(k1)*egv2(k2)*egv3(k3) -! enddo -! enddo -! enddo -! enddo -! enddo -! enddo -! ! Frequency product -! omegaprod=omega(1)*omega(2)*omega(3) -! omegaprod=sqrt(omegaprod) -! ! The actual matrix element -! c0=0.0_r8 -! do atom1=1,fc%na -! do t=1,fc%atom(atom1)%n -! atom2=fc%atom(atom1)%triplet(t)%i2 -! atom3=fc%atom(atom1)%triplet(t)%i3 -! -! rv2=fc%atom(atom1)%triplet(t)%lv2 -! rv3=fc%atom(atom1)%triplet(t)%lv3 -! -! iqr=dot_product(q2,rv2)+dot_product(q3,rv3) -! expiqr=cmplx(cos(iqr),sin(iqr),r8) -! ! Note that the masses are premultiplied into the forceconstants, much faster. -! c0=c0+sum(fc%atom(atom1)%triplet(t)%mwm*egvprod(:,:,:,atom1,atom2,atom3))*expiqr -! enddo -! enddo -! psi=enhet*c0/omegaprod -! end subroutine -! !> The three-phonon matrix element, but product of two complex thingies -! subroutine loc_3phdbl(fc,omega,egv1,egv2,egv3,q1,q2,egvprod1,egvprod2,doublepsi) -! !> the third order force constant -! class(lo_forceconstant_thirdorder), intent(in) :: fc -! !> the frequencies in question -! real(r8), dimension(3), intent(in) :: omega -! !> the eigenvectors -! complex(r8), dimension(fc%na*3), intent(in) :: egv1,egv2,egv3 -! !> the two q-vectors that matter -! real(r8), dimension(3), intent(in) :: q1,q2 -! !> work arrays -! complex(r8), dimension(3,3,3,fc%na,fc%na,fc%na), intent(inout) :: egvprod1,egvprod2 -! !> double psi -! complex(r8), intent(out) :: doublepsi -! ! -! integer :: atom1,atom2,atom3,i,j,k,k1,k2,k3,t -! complex(r8) :: expiqr,c0,c1 -! real(r8), dimension(3) :: rv2,rv3 -! real(r8), parameter :: enhet=2.367755374064161E51_r8 -! real(r8) :: iqr,omegaprod1,omegaprod2 -! -! ! Not enough room on the stack for large unitcells, have to allocate space -! do atom3=1,fc%na -! do atom2=1,fc%na -! do atom1=1,fc%na -! do k=1,3 -! do j=1,3 -! do i=1,3 -! k1=(atom1-1)*3+i -! k2=(atom2-1)*3+j -! k3=(atom3-1)*3+k -! egvprod1(i,j,k,atom1,atom2,atom3)=egv1(k1)*conjg(egv1(k2))*egv3(k3) -! egvprod2(i,j,k,atom1,atom2,atom3)=egv2(k1)*conjg(egv2(k2))*conjg(egv3(k3)) -! enddo -! enddo -! enddo -! enddo -! enddo -! enddo -! -! ! Frequency product -! omegaprod1=omega(1)*omega(1)*omega(3) -! omegaprod2=omega(2)*omega(2)*omega(3) -! omegaprod1=sqrt(omegaprod1) -! omegaprod2=sqrt(omegaprod2) -! ! The actual matrix element -! c0=0.0_r8 -! c1=0.0_r8 -! do atom1=1,fc%na -! do t=1,fc%atom(atom1)%n -! atom2=fc%atom(atom1)%triplet(t)%i2 -! atom3=fc%atom(atom1)%triplet(t)%i3 -! rv2=fc%atom(atom1)%triplet(t)%lv2 -! rv3=fc%atom(atom1)%triplet(t)%lv3 -! ! -! iqr=dot_product(-q1,rv2) -! expiqr=cmplx(cos(iqr),sin(iqr),r8) -! c0=c0+sum(fc%atom(atom1)%triplet(t)%mwm*egvprod1(:,:,:,atom1,atom2,atom3))*expiqr -! ! -! iqr=dot_product(-q2,rv2) -! expiqr=cmplx(cos(iqr),sin(iqr),r8) -! c1=c1+sum(fc%atom(atom1)%triplet(t)%mwm*egvprod2(:,:,:,atom1,atom2,atom3))*expiqr -! enddo -! enddo -! ! I predid the multiplication -! c0=enhet*c0/omegaprod1 -! c1=enhet*c1/omegaprod2 -! doublepsi=c0*c1 -! end subroutine -! end subroutine - end module diff --git a/src/anharmonic_free_energy/epot.f90 b/src/anharmonic_free_energy/epot.f90 index 9085ea65..1e1264c9 100644 --- a/src/anharmonic_free_energy/epot.f90 +++ b/src/anharmonic_free_energy/epot.f90 @@ -27,127 +27,19 @@ module epot contains procedure :: setup => setup_potential_energy_differences - procedure :: statistical_sampling procedure :: energies_and_forces end type contains -!> statistically sample -subroutine statistical_sampling(pot, uc, ss, fc, temperature, mw, mem, verbosity) - !> container for potential energy differences - class(lo_energy_differences), intent(inout) :: pot - !> unitcell - type(lo_crystalstructure), intent(in) :: uc - !> supercell - type(lo_crystalstructure), intent(in) :: ss - !> second order forceconstant - type(lo_forceconstant_secondorder), intent(in) :: fc - !> temperature - real(r8), intent(in) :: temperature - !> MPI helper - type(lo_mpi_helper), intent(inout) :: mw - !> memory tracker - type(lo_mem_helper), intent(inout) :: mem - !> talk a lot? - integer, intent(in) :: verbosity - - type(lo_crystalstructure) :: p - integer, parameter :: ninner = 20, nouter = 40 - integer :: initer, outiter, nstep, ctr, i - real(r8), dimension(:, :), allocatable :: ebuf, rbuf - real(r8), dimension(:, :), allocatable :: f2, f3, f4, fp - real(r8) :: e2, e3, e4, ep, deltaE, expdeltaE, ikbt, tomev, emean - - ! Copy of structure to work with - p = ss - - ! Total number of steps we are doing? - nstep = ninner*nouter - - ! Some helper space - call mem%allocate(ebuf, [nstep, 3], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%allocate(rbuf, [3, mw%n], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - ebuf = 0.0_r8 - rbuf = 0.0_r8 - - ! Dummy space for force - call mem%allocate(f2, [3, ss%na], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%allocate(f3, [3, ss%na], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%allocate(f4, [3, ss%na], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%allocate(fp, [3, ss%na], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - f2 = 0.0_r8 - f3 = 0.0_r8 - f4 = 0.0_r8 - fp = 0.0_r8 - - ! Thermal factor? - ikbt = 1.0_r8/(temperature*lo_kb_hartree) - tomev = lo_Hartree_to_eV*1000 - - ctr = 0 - outloop: do outiter = 1, nouter - inloop: do initer = 1, ninner - ctr = ctr + 1 - - ! Reset structure - p%u = 0.0_r8 - p%v = 0.0_r8 - p%r = ss%r - ! Get new structure - call pot%fc2%initialize_cell(p, uc, fc, temperature, .true., .false., -1.0_r8, mw, nosync=.true.) - ! Calculate the energy - call pot%energies_and_forces(p%u, e2, e3, e4, ep, f2, f3, f4, fp) - e2 = e2 !/ss%na - e3 = e3 !/ss%na - e4 = e4 !/ss%na - ep = ep !/ss%na - - ! H1-H0 difference - deltaE = e3 + e4 - expdeltaE = exp(-deltaE*ikbt) - ebuf(ctr, 1) = deltaE - ebuf(ctr, 2) = expdeltaE - end do inloop - - ! Get new mean energy - emean = lo_mean(ebuf(1:ctr, 1))/mw%n - call mw%allreduce('sum', emean) - do i = 1, ctr - ebuf(i, 3) = ebuf(i, 1) - emean - ebuf(i, 3) = exp(-ebuf(i, 3)*ikbt) - end do - - ! Print a little summary - rbuf = 0.0_r8 - rbuf(1, mw%r + 1) = lo_mean(ebuf(1:ctr, 1))/ss%na - rbuf(2, mw%r + 1) = -log(lo_mean(ebuf(1:ctr, 2)))/ikbt/ss%na - rbuf(3, mw%r + 1) = -log(lo_mean(ebuf(1:ctr, 3)))/ikbt/ss%na + emean/ss%na - call mw%allreduce('sum', rbuf) - - if (verbosity .gt. 0) then - write (*, *) ctr, lo_mean(rbuf(3, :))*tomev, lo_mean(rbuf(2, :))*tomev, lo_stddev(rbuf(1, :))*tomev, lo_stddev(rbuf(2, :))*tomev - end if - end do outloop - - call mem%deallocate(ebuf, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%deallocate(rbuf, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%deallocate(f2, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%deallocate(f3, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%deallocate(f4, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%deallocate(fp, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) -end subroutine - ! !> calculate energies and forces for a given configuration -subroutine energies_and_forces(pot, u, e2, e3, e4, ep, f2, f3, f4, fp) +subroutine energies_and_forces(pot, u, e2, e3, e4, ep) !> container for potential energy differences class(lo_energy_differences), intent(in) :: pot !> displacements real(r8), dimension(:, :), intent(in) :: u !> energies real(r8), intent(out) :: e2, e3, e4, ep - !> forces - real(r8), dimension(:, :), intent(out) :: f2, f3, f4, fp real(r8), dimension(3, 3, 3, 3) :: m4 real(r8), dimension(3, 3, 3) :: m3 @@ -159,10 +51,6 @@ subroutine energies_and_forces(pot, u, e2, e3, e4, ep, f2, f3, f4, fp) e3 = 0.0_r8 e4 = 0.0_r8 ep = 0.0_r8 - f2 = 0.0_r8 - f3 = 0.0_r8 - f4 = 0.0_r8 - fp = 0.0_r8 ! pair term do a1 = 1, size(u, 2) @@ -173,7 +61,6 @@ subroutine energies_and_forces(pot, u, e2, e3, e4, ep, f2, f3, f4, fp) v0 = v0 - matmul(m2, u(:, a2)) end do e2 = e2 - dot_product(u(:, a1), v0)*0.5_r8 - f2(:, a1) = v0 end do ! polar term @@ -185,7 +72,6 @@ subroutine energies_and_forces(pot, u, e2, e3, e4, ep, f2, f3, f4, fp) v0 = v0 - matmul(pot%fcp(:, :, a1, a2), u(:, a2)) end do ep = ep - dot_product(u(:, a1), v0)*0.5_r8 - fp(:, a1) = v0 end do end if @@ -208,7 +94,6 @@ subroutine energies_and_forces(pot, u, e2, e3, e4, ep, f2, f3, f4, fp) end do end do v0 = v0*0.5_r8 - f3(:, a1) = v0 e3 = e3 - dot_product(v0, u(:, a1))/3.0_r8 end do end if @@ -236,7 +121,6 @@ subroutine energies_and_forces(pot, u, e2, e3, e4, ep, f2, f3, f4, fp) end do end do v0 = v0/6.0_r8 - f4(:, a1) = v0 e4 = e4 - dot_product(v0, u(:, a1))/4.0_r8 end do end if @@ -312,223 +196,4 @@ subroutine setup_potential_energy_differences(pot, uc, ss, fc2, fc3, fc4, mw, ve end if end subroutine -! !> remove longrange interactions -! subroutine potential_energy_difference(sim,uc,ss,fc,fct,fcf,Uref,mw,verbosity) -! !> force-displacement data -! type(lo_mdsim), intent(inout) :: sim -! !> unitcell -! type(lo_crystalstructure), intent(inout) :: uc -! !> supercell -! type(lo_crystalstructure), intent(inout) :: ss -! !> second order forceconstant -! type(lo_forceconstant_secondorder), intent(in) :: fc -! !> third order forceconstant -! type(lo_forceconstant_thirdorder), intent(in) :: fct -! !> fourth order forceconstant -! type(lo_forceconstant_fourthorder), intent(in) :: fcf -! !> reference energy -! real(flyt), intent(in) :: Uref -! !> mpi things -! type(lo_mpi_helper), intent(inout) :: mw -! !> how much to talk -! integer, intent(in) :: verbosity -! -! type(lo_forceconstant_secondorder) :: fcss -! type(lo_forceconstant_thirdorder) :: fctss -! type(lo_forceconstant_fourthorder) :: fcfss -! real(flyt), dimension(:,:,:,:), allocatable :: forceconstant -! real(flyt), dimension(:,:), allocatable :: fp,f2,f3,f4,de -! ! real(flyt), dimension(:,:), allocatable :: f,de -! ! real(flyt), dimension(3,3) :: m0,m1 -! ! real(flyt), dimension(3) :: v0 -! ! real(flyt) :: epot,epot_2,epot_3,epot_4,epot_dd -! ! integer :: a1,a2,t,u -! -! init: block -! real(flyt), dimension(3,3) :: m0,m1 -! real(flyt) :: t0,f0 -! integer :: a1,a2 -! if ( mw%talk ) then -! write(*,*) '' -! write(*,*) 'CALCULATING POTENTIAL ENERGY DIFFERENCES' -! endif -! ! Remap the forceconstants to the supercell -! call ss%classify('supercell',uc) -! call fc%remap(uc,ss,fcss) -! call fct%remap(uc,ss,fctss) -! call fcf%remap(uc,ss,fcfss) -! if ( mw%talk ) write(*,*) '... remapped forceconstants' -! ! Get the dipole-dipole forceconstant -! if ( fc%polar ) then -! lo_allocate(forceconstant(3,3,ss%na,ss%na)) -! call fc%supercell_longrange_dynamical_matrix_at_gamma(ss,forceconstant,1E-15_flyt) -! ! small sanity-check, just in case -! f0=0.0_flyt -! do a1=1,ss%na -! do a2=a1,ss%na -! m0=forceconstant(:,:,a1,a2) -! m1=transpose(forceconstant(:,:,a2,a1)) -! f0=f0+lo_frobnorm(m0-m1) -! enddo -! enddo -! f0=f0/(ss%na**2) -! if ( f0 .gt. lo_tol ) then -! write(*,*) 'ERROR, non-Hermitian electrostatic forceconstant: ',f0 -! write(*,*) 'If this keeps happening I should not hard-code the Ewald tolerance.' -! stop -! endif -! endif -! -! ! some space for energies and forces -! lo_allocate(de(sim%nt,5)) -! lo_allocate(fp(3,ss%na)) -! lo_allocate(f2(3,ss%na)) -! lo_allocate(f3(3,ss%na)) -! lo_allocate(f4(3,ss%na)) -! de=0.0_flyt -! fp=0.0_flyt -! f2=0.0_flyt -! f3=0.0_flyt -! f4=0.0_flyt -! end block init -! -! forceenergy: block -! real(flyt), dimension(3,3,3,3) :: m4 -! real(flyt), dimension(3,3,3) :: m3 -! real(flyt), dimension(3,3) :: m2 -! real(flyt), dimension(3) :: u1,u2,u3,u4,v0 -! real(flyt) :: energy -! integer :: a1,a2,a3,a4,i1,i2,i3,i4,i,j,k,l,t -! -! do t=1,sim%nt -! ! get the raw energy -! de(t,1)=sim%stat%potential_energy(t) -! -! ! secondorder energy, first the polar term (if applicable) -! energy=0.0_flyt -! if ( fc%polar ) then -! do a1=1,ss%na -! v0=0.0_flyt -! do a2=1,ss%na -! v0=v0+matmul(forceconstant(:,:,a2,a1),u(:,a2,t)) -! enddo -! energy=energy+dot_product(u(:,a1,t),v0)*0.5_flyt -! enddo -! endif -! ! then the pair term, always there -! do a1=1,ss%na -! v0=0.0_flyt -! do i1=1,fcss%atom(a1)%n -! a2=fcss%atom(a1)%pair(i1)%i2 -! m2=fcss%atom(a1)%pair(i1)%m -! v0=v0+matmul(m2,u(:,a2,t)) -! enddo -! energy=energy+dot_product(u(:,a1,t),v0)*0.5_flyt -! enddo -! de(t,2)=energy -! -! ! triplet term -! f3=0.0_flyt -! energy=0.0_flyt -! do a1=1,fcss%na -! v0=0.0_flyt -! do i=1,fctss%atom(a1)%n -! m3=fctss%atom(a1)%triplet(i)%m -! a2=fctss%atom(a1)%triplet(i)%i2 -! a3=fctss%atom(a1)%triplet(i)%i3 -! u2=u(:,a2,t) -! u3=u(:,a3,t) -! do i1=1,3 -! do i2=1,3 -! do i3=1,3 -! v0(i1)=v0(i1)-m3(i1,i2,i3)*u2(i2)*u3(i3) -! enddo -! enddo -! enddo -! enddo -! f3(:,a1)=v0*0.5_flyt -! energy=energy-dot_product(f3(:,a1),u(:,a1,t))/3.0_flyt -! enddo -! de(t,3)=energy -! -! ! quartet term -! f4=0.0_flyt -! energy=0.0_flyt -! do a1=1,fcfss%na -! v0=0.0_flyt -! do i=1,fcfss%atom(a1)%n -! m4=fcfss%atom(a1)%quartet(i)%m -! a2=fcfss%atom(a1)%quartet(i)%i2 -! a3=fcfss%atom(a1)%quartet(i)%i3 -! a4=fcfss%atom(a1)%quartet(i)%i4 -! u2=u(:,a2,t) -! u3=u(:,a3,t) -! u4=u(:,a4,t) -! do i1=1,3 -! do i2=1,3 -! do i3=1,3 -! do i4=1,3 -! v0(i1)=v0(i1)-m4(i1,i2,i3,i4)*u2(i2)*u3(i3)*u4(i4) -! enddo -! enddo -! enddo -! enddo -! enddo -! f4(:,a1)=v0/6.0_flyt -! energy=energy-dot_product(f4(:,a1),u(:,a1,t))/4.0_flyt -! enddo -! de(t,4)=energy -! enddo -! end block forceenergy -! -! if ( mw%talk ) then -! write(*,*) ' raw avg potential energy:',lo_mean(de(:,1)) -! write(*,*) ' E-E2:',lo_mean(de(:,1)-de(:,2)) -! write(*,*) ' E-E2-E3:',lo_mean(de(:,1)-de(:,2)-de(:,3)) -! write(*,*) ' E-E2-E3-E4:',lo_mean(de(:,1)-de(:,2)-de(:,3)-de(:,4)) -! endif -! -! -! !! Energy per atom -! !de=1000*de/sim%na -! ! -! !if ( mw%talk ) then -! !write(*,*) 'RAW:',lo_mean(de(:,1)),lo_stddev(de(:,1)) -! !write(*,*) 'RAW:',lo_mean(de(:,1)-de(:,3)),lo_stddev(de(:,1)-de(:,3)) -! !write(*,*) 'RAW:',lo_mean(de(:,1)-de(:,2)-de(:,3)),lo_stddev(de(:,1)-de(:,2)-de(:,3)) -! !write(*,*) 'RAW:',lo_mean(de(:,1)-de(:,2)-de(:,3)-de(:,4)),lo_stddev(de(:,1)-de(:,2)-de(:,3)-de(:,4)) -! !write(*,*) 'RAW:',lo_mean(de(:,1)-de(:,2)-de(:,3)-de(:,4)-de(:,5)),lo_stddev(de(:,1)-de(:,2)-de(:,3)-de(:,4)-de(:,5)) -! !u=open_file('out','outfile.U0') -! ! do t=1,sim%nt -! ! write(u,"(6(1X,E18.12))") de(t,:)/1000*sim%na,(de(t,1)-de(t,2)-de(t,3)-de(t,4)-de(t,5))/1000*sim%na -! ! enddo -! !close(u) -! !endif -! -! ! t0=walltime() -! ! call lo_progressbar_init() -! ! ! Subtract forces -! ! lo_allocate(f(3,ss%na)) -! ! do t=1,sim%nt -! ! ! calculate the long-range forces -! ! f=0.0_flyt -! ! do a1=1,ss%na -! ! do a2=1,ss%na -! ! v0=matmul(forceconstant(:,:,a1,a2),u(:,a2,t)) -! ! f(:,a1)=f(:,a1)-v0 -! ! enddo -! ! enddo -! ! ! sanity check that they add up to zero -! ! if ( abs(sum(f)) .gt. lo_sqtol ) then -! ! write(*,*) '' -! ! write(*,*) 'ERROR: dipole-dipole forces do not add up to zero!' -! ! stop -! ! endif -! ! ! subtract them -! ! sim%f(:,:,t)=sim%f(:,:,t)-f -! ! if( lo_trueNtimes(t,50,sim%nt) ) call lo_progressbar(' ... subtracting dipole-dipole forces',t,sim%nt) -! ! enddo -! ! call lo_progressbar(' ... subtracting dipole-dipole forces',sim%nt,sim%nt,walltime()-t0) -! end subroutine - end module diff --git a/src/anharmonic_free_energy/fourthorder.f90 b/src/anharmonic_free_energy/fourthorder.f90 new file mode 100644 index 00000000..7fa710a1 --- /dev/null +++ b/src/anharmonic_free_energy/fourthorder.f90 @@ -0,0 +1,434 @@ +module fourthorder +!! Compute the fourth order contribution to the anharmonic free energy +use konstanter, only: r8, lo_freqtol, lo_twopi, lo_imag, lo_kb_Hartree, lo_exitcode_param +use gottochblandat, only: walltime, lo_trueNtimes, lo_progressbar_init, lo_progressbar, lo_planck, & + lo_planck_deriv, lo_planck_secondderiv +use mpi_wrappers, only: lo_mpi_helper, lo_stop_gracefully +use lo_memtracker, only: lo_mem_helper +use type_qpointmesh, only: lo_qpoint_mesh, lo_fft_mesh +use type_crystalstructure, only: lo_crystalstructure +use type_forceconstant_fourthorder, only: lo_forceconstant_fourthorder +use type_phonon_dispersions, only: lo_phonon_dispersions +use lo_timetracker, only: lo_timer +use lo_fftgrid_helper, only: fft_fourth_grid_index + +implicit none +private + +public :: free_energy_fourthorder +public :: free_energy_fourthorder_secondorder + +contains +!> Calculate the fourth order free energy +subroutine free_energy_fourthorder(uc, fcf, qp, dr, temperature, df4, s4, cv4, quantum, mw, mem) + !> crystal structure + type(lo_crystalstructure), intent(in) :: uc + !> fourth order force constant + type(lo_forceconstant_fourthorder), intent(in) :: fcf + !> q-point mesh + class(lo_qpoint_mesh), intent(in) :: qp + !> dispersions + type(lo_phonon_dispersions), intent(in) :: dr + !> temperature + real(r8) :: temperature + !> free energies, entropy and heat capacity + real(r8), intent(out) :: df4, s4, cv4 + !> what to compute + logical, intent(in) :: quantum + !> mpi helper + type(lo_mpi_helper), intent(inout) :: mw + !> memory tracker + type(lo_mem_helper), intent(inout) :: mem + + !> Frequency scaled eigenvectors + complex(r8), dimension(:), allocatable :: egv1, egv2, egv3, egv4 + !> Helper for Fourier transform of psi3 + complex(r8), dimension(:), allocatable :: ptf, evp1, evp2, evp3 + !> Frequencies, bose-einstein occupation and scattering strength and some other buffer + real(r8) :: sig, om1, om2, om3, om4, n1, n2, n3, n4, psisq, f0, f1, f2, t0, prefactor + !> + real(r8) :: s1, s2, s3, mult, dn1, dn2, ddn1, ddn2, df0, ddf0 + !> The complex threephonon matrix element + complex(r8) :: c0 + !> Integers for do loops and counting + integer :: qi, q1, q2, q3, q4, b1, b2, b3, b4, i, ctr + + ! We start by allocating everything + call mem%allocate(ptf, dr%n_mode**4, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%allocate(evp1, dr%n_mode**2, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%allocate(evp2, dr%n_mode**3, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%allocate(evp3, dr%n_mode**4, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%allocate(egv1, dr%n_mode, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%allocate(egv2, dr%n_mode, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + + t0 = walltime() + + df4 = 0.0_r8 + cv4 = 0.0_r8 + + do q1=1, qp%n_irr_point + do q2=1, qp%n_full_point + ctr = ctr + 1 + if (mod(ctr, mw%n) .ne. mw%r) cycle + + prefactor = qp%ip(q1)%integration_weight*qp%ap(q2)%integration_weight/uc%na + ! pre-transform the matrix element + call pretransform_phi4_first(fcf, qp%ap(q1)%r, qp%ap(q2)%r, ptf) + + do b1=1, dr%n_mode + om1 = dr%iq(q1)%omega(b1) + if (om1 .lt. lo_freqtol) cycle + egv1 = dr%iq(q1)%egv(:, b1)/sqrt(om1) + do b2=1, dr%n_mode + om2 = dr%aq(q2)%omega(b2) + if (om2 .lt. lo_freqtol) cycle + + egv2 = dr%aq(q2)%egv(:, b2)/sqrt(om2) + evp1 = 0.0_r8 + evp2 = 0.0_r8 + evp3 = 0.0_r8 + call zgerc(dr%n_mode, dr%n_mode, (1.0_r8, 0.0_r8), egv1, 1, egv1, 1, evp1, dr%n_mode) + call zgerc(dr%n_mode, dr%n_mode, (1.0_r8, 0.0_r8), egv2, 1, egv2, 1, evp2, dr%n_mode) + call zgeru(dr%n_mode**2, dr%n_mode**2, (1.0_r8, 0.0_r8), evp2, 1, evp1, 1, evp3, dr%n_mode**2) + evp3 = conjg(evp3) + psisq = real(dot_product(evp3, ptf), r8) + + if (quantum) then + n1 = lo_planck(temperature, om1) + n2 = lo_planck(temperature, om2) + dn1 = lo_planck_deriv(temperature, om1) + dn2 = lo_planck_deriv(temperature, om2) + ddn1 = lo_planck_secondderiv(temperature, om1) + ddn2 = lo_planck_secondderiv(temperature, om2) + f0 = (2.0_r8 * n1 + 1.0_r8) * (2.0_r8 * n2 + 1.0_r8) * psisq * prefactor / 32.0_r8 + + df0 = 2.0_r8 * dn1 * (2.0_r8 * n2 + 1.0_r8) + (2.0_r8 * n1 + 1.0_r8) * 2.0_r8 * dn2 + df0 = df0 * psisq * prefactor / 32.0_r8 + + f1 = 2.0_r8 * ddn1 * (2.0_r8 * n2 + 1.0_r8) + 2.0_r8 * ddn2 * (2.0_r8 * n1 + 1.0_r8) + & + 8.0_r8 * dn1 * dn2 + ddf0 = ddf0 * temperature * psisq * prefactor / 32.0_r8 + else + f0 = (lo_kb_Hartree*temperature)**2 / (om1*om2) / 8.0_r8 + df0 = lo_kb_Hartree**2 * temperature / (om1*om2) / 4.0_r8 + ddf0 = lo_kb_Hartree**2 * temperature / (om1*om2) / 4.0_r8 + end if + df4 = df4 + f0 * psisq * prefactor + s4 = s4 - df0 * psisq * prefactor + cv4 = cv4 - df0 * psisq * prefactor + end do + end do + end do + if (mw%talk .and. lo_trueNtimes(q1, 127, qp%n_irr_point)) then + call lo_progressbar(' ... fourth order', q1, qp%n_irr_point, walltime() - t0) + end if + end do + ! For a nice progressbar + if (mw%talk) then + call lo_progressbar(' ... fourth order', qp%n_irr_point, qp%n_irr_point, walltime() - t0) + end if + call mw%allreduce('sum', df4) + call mw%allreduce('sum', s4) + call mw%allreduce('sum', cv4) + + call mem%deallocate(ptf, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%deallocate(evp1, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%deallocate(evp2, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%deallocate(evp3, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%deallocate(egv1, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%deallocate(egv2, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + +end subroutine + +!> Calculate the fourth order free energy +subroutine free_energy_fourthorder_secondorder(uc, fcf, qp, dr, temperature, fe4, s4, cv4, quantum, mw, mem) + !> crystal structure + type(lo_crystalstructure), intent(in) :: uc + !> fourth order force constant + type(lo_forceconstant_fourthorder), intent(in) :: fcf + !> q-point mesh + class(lo_qpoint_mesh), intent(in) :: qp + !> dispersions + type(lo_phonon_dispersions), intent(in) :: dr + !> temperature + real(r8) :: temperature + !> free energies, entropy and heat capacity + real(r8), intent(out) :: fe4, s4, cv4 + !> what to compute + logical, intent(in) :: quantum + !> mpi helper + type(lo_mpi_helper), intent(inout) :: mw + !> memory tracker + type(lo_mem_helper), intent(inout) :: mem + + !> Frequency scaled eigenvectors + complex(r8), dimension(:), allocatable :: egv1, egv2, egv3, egv4 + !> Helper for Fourier transform of psi3 + complex(r8), dimension(:), allocatable :: ptf, evp1, evp2, evp3 + !> Frequencies, bose-einstein occupation and scattering strength and some other buffer + real(r8) :: sigma, om1, om2, om3, om4, n1, n2, n3, n4, psisq, f0, f1, f2, f3, t0, prefactor + !> + real(r8) :: s1, s2, s3, mult, dn1, dn2, ddn1, ddn2, df0, ddf0, np1, np2, np3, np4, sig, sig1, sig2, sig3, sig4 + !> The multiplicities + real(r8) :: m0, m1, m2, m3 + !> The complex threephonon matrix element + complex(r8) :: c0 + !> Integers for do loops and counting + integer :: qi, q1, q2, q3, q4, b1, b2, b3, b4, i, ctr + !> The dimension of the q-grid + integer, dimension(3) :: dims + + ! We start by allocating everything + call mem%allocate(ptf, dr%n_mode**4, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%allocate(evp1, dr%n_mode**2, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%allocate(evp2, dr%n_mode**3, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%allocate(evp3, dr%n_mode**4, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%allocate(egv1, dr%n_mode, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%allocate(egv2, dr%n_mode, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%allocate(egv3, dr%n_mode, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%allocate(egv4, dr%n_mode, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + + t0 = walltime() + + fe4 = 0.0_r8 + s4 = 0.0_r8 + cv4 = 0.0_r8 + + select type (qp) + class is (lo_fft_mesh) + dims = qp%griddensity + class default + call lo_stop_gracefully(['This routine only works with FFT meshes'], lo_exitcode_param, __FILE__, __LINE__) + end select + + do q1=1, qp%n_irr_point + do q2=1, qp%n_full_point + do q3=1, qp%n_full_point + ctr = ctr + 1 + if (mod(ctr, mw%n) .ne. mw%r) cycle + q4 = fft_fourth_grid_index(qp%ip(q1)%full_index, q2, q3, dims) + + if (q3 .lt. q2) cycle + if (q4 .lt. q3) cycle + + if (q2 .eq. q3 .and. q3 .eq. q4) then + m0 = 1.0_r8 + m1 = 1.0_r8 + m2 = 1.0_r8 + m3 = 1.0_r8 + else if ((q2 .ne. q3 .and. q3 .eq. q4) .or. & + (q3 .ne. q2 .and. q2 .eq. q4) .or. & + (q4 .ne. q2 .and. q2 .eq. q3)) then + m0 = 3.0_r8 + m1 = 1.0_r8 + m2 = 1.0_r8 + m3 = 1.0_r8 + else + m0 = 6.0_r8 + m1 = 2.0_r8 + m2 = 2.0_r8 + m3 = 2.0_r8 + end if + + prefactor = qp%ip(q1)%integration_weight*qp%ap(q2)%integration_weight*qp%ap(q2)%integration_weight/uc%na + ! pre-transform the matrix element + call pretransform_phi4(fcf, qp%ap(q2)%r, qp%ap(q3)%r, qp%ap(q4)%r, ptf) + + do b1=1, dr%n_mode + om1 = dr%iq(q1)%omega(b1) + if (om1 .lt. lo_freqtol) cycle + egv1 = dr%iq(q1)%egv(:, b1)/sqrt(om1) + do b2=1, dr%n_mode + om2 = dr%aq(q2)%omega(b2) + if (om2 .lt. lo_freqtol) cycle + + egv2 = dr%aq(q2)%egv(:, b2)/sqrt(om2) + evp1 = 0.0_r8 + call zgeru(dr%n_mode, dr%n_mode, (1.0_r8, 0.0_r8), egv2, 1, egv1, 1, evp1, dr%n_mode) + do b3=1, dr%n_mode + om3 = dr%aq(q3)%omega(b3) + if (om3 .lt. lo_freqtol) cycle + + egv3 = dr%aq(q3)%egv(:, b3)/sqrt(om3) + evp2 = 0.0_r8 + call zgeru(dr%n_mode, dr%n_mode**2, (1.0_r8, 0.0_r8), egv3, 1, evp1, 1, evp2, dr%n_mode) + do b4=1, dr%n_mode + om4 = dr%aq(q4)%omega(b4) + if (om4 .lt. lo_freqtol) cycle + + egv4 = dr%aq(q4)%egv(:, b4)/sqrt(om4) + evp3 = 0.0_r8 + call zgeru(dr%n_mode, dr%n_mode**3, (1.0_r8, 0.0_r8), egv4, 1, evp2, 1, evp3, dr%n_mode) + evp3 = conjg(evp3) + c0 = dot_product(evp3, ptf) + psisq = abs(c0*conjg(c0))*prefactor + + if (om4 .lt. lo_freqtol) cycle + + if (quantum) then + n1 = lo_planck(temperature, om1) + n2 = lo_planck(temperature, om2) + n3 = lo_planck(temperature, om3) + n4 = lo_planck(temperature, om4) + np1 = n1 + 1.0_r8 + np2 = n2 + 1.0_r8 + np3 = n3 + 1.0_r8 + np4 = n4 + 1.0_r8 + + f1 = np1*np2*np3*np4 - n1*n2*n3*n4 / (om1+om2+om3+om4) + if (abs(-om1+om2+om3+om4) .lt. lo_freqtol) then + sig1 = dr%default_smearing(b1) + sig2 = dr%default_smearing(b2) + sig3 = dr%default_smearing(b3) + sig = sqrt(sig1**2 + sig2**2 + sig3**2 + sig4**2) + f2 = 4.0_r8*(n1*np2*np3*np4 - np1*n2*n3*n4) * real(1.0/(-om1+om2+om3+om4 + lo_imag*sig)) + else + f2 = 4.0_r8*(n1*np2*np3*np4 - np1*n2*n3*n4) / (-om1+om2+om3+om4) + end if + if (abs(om1+om2-om3-om4) .lt. lo_freqtol) then + sig1 = dr%default_smearing(b1) + sig2 = dr%default_smearing(b2) + sig3 = dr%default_smearing(b3) + sig = sqrt(sig1**2 + sig2**2 + sig3**2 + sig4**2) + f3 = 3.0_r8*(n1*n2*(n3+n4+1.0_r8) - n3*n4*(n1+n2+1.0_r8))*real(1.0/(om1+om2-om3-om4 + lo_imag*sig)) + else + f3 = 3.0_r8*(n1*n2*(n3+n4+1.0_r8) - n3*n4*(n1+n2+1.0_r8)) / (om1+om2-om3-om4) + end if + + f0 = (f1 + f2 + f3) / 768.0_r8 + else + f0 = (lo_kb_Hartree*temperature)**3 / (om1*om2*om3*om4) / 48.0_r8 + df0 = lo_kb_Hartree**3*temperature**2 / (om1*om2*om3*om4) / 16.0_r8 + ddf0 = lo_kb_Hartree**3*temperature**2 / (om1*om2*om3*om4) / 8.0_r8 + end if + fe4 = fe4 - f0 * psisq + s4 = s4 + df0 * psisq + cv4 = cv4 + ddf0 * psisq + end do + end do + end do + end do + end do + end do + if (mw%talk .and. lo_trueNtimes(q1, 127, qp%n_irr_point)) then + call lo_progressbar(' ... fourth order', q1, qp%n_irr_point, walltime() - t0) + end if + end do + ! For a nice progressbar + if (mw%talk) then + call lo_progressbar(' ... fourth order', qp%n_irr_point, qp%n_irr_point, walltime() - t0) + end if + call mw%allreduce('sum', fe4) + call mw%allreduce('sum', s4) + call mw%allreduce('sum', cv4) + + call mem%deallocate(ptf, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%deallocate(evp1, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%deallocate(evp2, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%deallocate(evp3, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%deallocate(egv1, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%deallocate(egv2, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%deallocate(egv3, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%deallocate(egv4, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) +end subroutine + +!> Get the Fourier transform of the fourth order matrix element +subroutine pretransform_phi4_first(fcf, q1, q2, ptf) + !> fourth order forceconstant + type(lo_forceconstant_fourthorder), intent(in) :: fcf + !> q-vectors + real(r8), dimension(3), intent(in) :: q1, q2 + !> flattened, pretransformed matrix element + complex(r8), dimension(:), intent(out) :: ptf + + integer :: i, j, k, l, m + + complex(r8) :: expiqr + real(r8), dimension(3) :: rv2, rv3, rv4 + real(r8) :: iqr + integer :: a1, a2, a3, a4, ia, ib, ic, id, q, nb + + nb = fcf%na*3 + ptf = 0.0_r8 + do a1 = 1, fcf%na + do q = 1, fcf%atom(a1)%n + a2 = fcf%atom(a1)%quartet(q)%i2 + a3 = fcf%atom(a1)%quartet(q)%i3 + a4 = fcf%atom(a1)%quartet(q)%i4 + + rv2 = fcf%atom(a1)%quartet(q)%lv2 + rv3 = fcf%atom(a1)%quartet(q)%lv3 + rv4 = fcf%atom(a1)%quartet(q)%lv4 + + iqr = -dot_product(q1, rv2) + dot_product(q2, rv3) - dot_product(q2, rv4) + iqr = -iqr*lo_twopi + expiqr = cmplx(cos(iqr), sin(iqr), r8) + do l = 1, 3 + do k = 1, 3 + do j = 1, 3 + do i = 1, 3 + ia = (a1 - 1)*3 + i + ib = (a2 - 1)*3 + j + ic = (a3 - 1)*3 + k + id = (a4 - 1)*3 + l + ! Now for the grand flattening scheme, consistent with the zgeru operations above. + m = (ia - 1)*nb*nb*nb + (ib - 1)*nb*nb + (ic - 1)*nb + id + ptf(m) = ptf(m) + fcf%atom(a1)%quartet(q)%mwm(i, j, k, l)*expiqr + end do + end do + end do + end do + end do + end do +end subroutine + +!> Do half the transform to q-space +pure subroutine pretransform_phi4(fcf, q2, q3, q4, ptf) + !> Fourth order forceconstant + class(lo_forceconstant_fourthorder), intent(in) :: fcf + !> The q-vectors, without the 2pi + real(r8), dimension(3), intent(in) :: q2, q3, q4 + !> Flattened, pre-transformed matrix element + complex(r8), dimension(:), intent(out) :: ptf + + integer :: i, j, k, l, m + + complex(r8) :: expiqr + real(r8), dimension(3) :: rv2, rv3, rv4 + real(r8) :: iqr + integer :: a1, a2, a3, a4, ia, ib, ic, id, q, nb + + nb = fcf%na*3 + ptf = 0.0_r8 + do a1 = 1, fcf%na + do q = 1, fcf%atom(a1)%n + a2 = fcf%atom(a1)%quartet(q)%i2 + a3 = fcf%atom(a1)%quartet(q)%i3 + a4 = fcf%atom(a1)%quartet(q)%i4 + + rv2 = fcf%atom(a1)%quartet(q)%lv2 + rv3 = fcf%atom(a1)%quartet(q)%lv3 + rv4 = fcf%atom(a1)%quartet(q)%lv4 + + iqr = dot_product(q2, rv2) + dot_product(q3, rv3) + dot_product(q4, rv4) + iqr = -iqr*lo_twopi + expiqr = cmplx(cos(iqr), sin(iqr), r8) + do l = 1, 3 + do k = 1, 3 + do j = 1, 3 + do i = 1, 3 + ia = (a1 - 1)*3 + i + ib = (a2 - 1)*3 + j + ic = (a3 - 1)*3 + k + id = (a4 - 1)*3 + l + ! Now for the grand flattening scheme, consistent with the zgeru operations. + m = (ia - 1)*nb*nb*nb + (ib - 1)*nb*nb + (ic - 1)*nb + id + ptf(m) = ptf(m) + fcf%atom(a1)%quartet(q)%mwm(i, j, k, l)*expiqr + end do + end do + end do + end do + end do + end do +end subroutine +end module diff --git a/src/anharmonic_free_energy/main.f90 b/src/anharmonic_free_energy/main.f90 index f815e238..14258208 100644 --- a/src/anharmonic_free_energy/main.f90 +++ b/src/anharmonic_free_energy/main.f90 @@ -1,6 +1,6 @@ program anharmonic_free_energy !!{!src/anharmonic_free_energy/manual.md!} -use konstanter, only: r8, lo_Hartree_to_eV, lo_kb_Hartree, lo_pressure_HartreeBohr_to_GPa +use konstanter, only: r8, lo_Hartree_to_eV, lo_kb_Hartree, lo_pressure_HartreeBohr_to_GPa, lo_tol, lo_status use gottochblandat, only: open_file, walltime, lo_linspace, lo_progressbar_init, lo_progressbar, tochar, & lo_does_file_exist, lo_mean, lo_stddev use mpi_wrappers, only: lo_mpi_helper @@ -17,8 +17,10 @@ program anharmonic_free_energy use type_phonon_dos, only: lo_phonon_dos use options, only: lo_opts -use energy, only: perturbative_anharmonic_free_energy +use thirdorder, only: free_energy_thirdorder +use fourthorder, only: free_energy_fourthorder, free_energy_fourthorder_secondorder use epot, only: lo_energy_differences +use thermo, only: lo_thermodynamics implicit none @@ -26,15 +28,14 @@ program anharmonic_free_energy type(lo_forceconstant_secondorder) :: fc type(lo_forceconstant_thirdorder) :: fct type(lo_forceconstant_fourthorder) :: fcf -type(lo_phonon_dispersions) :: dr type(lo_crystalstructure) :: uc -class(lo_qpoint_mesh), allocatable :: qp type(lo_mpi_helper) :: mw type(lo_mem_helper) :: mem type(lo_timer) :: tmr -type(lo_mdsim) :: sim -real(r8), dimension(3, 5) :: cumulant +type(lo_thermodynamics) :: thermo +real(r8), dimension(3, 5) :: cumulant, cumulant_var +real(r8), dimension(3, 3, 5) :: stress_pot, stress_potvar real(r8) :: timer_init, timer_total real(r8) :: U0, U1, energy_unit_factor logical :: havehighorder @@ -46,12 +47,16 @@ program anharmonic_free_energy call opts%parse() call tmr%start() -! set up all possible meshes and get all dispersions init: block - integer :: t, u - + call mw%init() ! only be verbose on the first rank if (.not. mw%talk) opts%verbosity = -10 + call tmr%start() + + if (mw%talk) then + write(*, *) 'Recap of the parameters governing the calculation' + write(*, *) '' + end if ! Read structure call uc%readfromfile('infile.ucposcar', verbosity=opts%verbosity) @@ -69,16 +74,32 @@ program anharmonic_free_energy call tmr%tock('reading input') - ! Get a q-mesh for the integrations. Always an FFT mesh. - if (mw%talk) write (*, *) '... generating q-mesh' - call lo_generate_qmesh(qp, uc, opts%qgrid, 'fft', timereversal=.true., headrankonly=.false., mw=mw, mem=mem, verbosity=opts%verbosity) + timer_init = walltime() - timer_init + + thermo%temperature = opts%temperature +end block init - ! Dispersions for everyone! +latdyn: block + !> The phonon dispersion relation + type(lo_phonon_dispersions) :: dr + !> The qpoint mesh + class(lo_qpoint_mesh), allocatable :: qp + !> Some stuffs + real(r8) :: temperature + !> Some integers for do loops + integer :: i + + if (mw%talk) then + write(*, *) '' + write(*, *) 'HARMONIC CONTRIBUTION' + end if + + if (mw%talk) write(*, *) '... generating q-mesh' + call lo_generate_qmesh(qp, uc, opts%qgrid, 'fft', timereversal=.true., headrankonly=.false., mw=mw, mem=mem, verbosity=opts%verbosity) + if (mw%talk) write(*, *) '... generating harmonic dispersion' call dr%generate(qp, fc, uc, mw=mw, mem=mem, verbosity=opts%verbosity) - if (mw%talk) write (*, *) '... got the full dispersion relations' - call tmr%tock('harmonic properties') - ! Check for imaginary modes right away + ! Little sanity check if (dr%omega_min .lt. 0.0_r8) then ! Dump the free energies if (mw%talk) then @@ -87,71 +108,165 @@ program anharmonic_free_energy call mw%destroy() stop end if - timer_init = walltime() - timer_init -end block init + temperature = opts%temperature -! We start with the potential energy terms since those are much faster -epotthings: block + ! We start by computing everything we can from the harmonic phonons + if (opts%quantum) then + thermo%f0 = dr%phonon_free_energy(temperature) + thermo%s0 = dr%phonon_entropy(temperature) + thermo%u0 = thermo%f0 + temperature * thermo%s0 + thermo%cv0 = dr%phonon_cv(temperature) + call dr%phonon_kinetic_stress(qp, uc, temperature, thermo%stress_kin) + else + thermo%f0 = dr%phonon_free_energy_classical(temperature) + thermo%u0 = 3.0_r8 * lo_kb_Hartree * temperature + thermo%s0 = (thermo%u0 - thermo%f0) / temperature + thermo%cv0 = 3.0_r8 * lo_kb_Hartree + thermo%stress_kin = 0.0_r8 + do i=1, 3 + thermo%stress_kin(i, i) = -lo_kb_Hartree * temperature * uc%na / uc%volume + end do + end if + write(*, *) 'Free energy' + write(*, *) thermo%f0 + write(*, *) 'Entropy' + write(*, *) thermo%s0 + write(*, *) 'Internal energy' + write(*, *) thermo%u0 + write(*, *) '' + + write(*, *) 'Potential stress' + do i=1, 3 + write(*, '(1X,F24.12,1X,F24.12,1X,F24.12)') thermo%stress_pot(i, :) * lo_pressure_HartreeBohr_to_GPa + end do + write(*, *) 'Kinetic stress' + do i=1, 3 + write(*, '(1X,F24.12,1X,F24.12,1X,F24.12)') thermo%stress_kin(i, :) * lo_pressure_HartreeBohr_to_GPa + end do + call tmr%tock('harmonic properties') + +end block latdyn + +calcepot: block + type(lo_mdsim) :: sim type(lo_energy_differences) :: pot type(lo_crystalstructure) :: ss - real(r8), dimension(:, :), allocatable :: f2, f3, f4, fp + real(r8), dimension(:, :, :, :), allocatable :: sdiff + real(r8), dimension(:, :, :), allocatable :: buf_stress + real(r8), dimension(:, :), allocatable :: buf real(r8), dimension(:, :), allocatable :: ediff + real(r8), dimension(3, 3) :: s2, s3, s4, sp - real(r8) :: e2, e3, e4, ep, inverse_kbt - integer :: i + real(r8) :: e2, e3, e4, ep, inverse_kbt, f0 + integer :: i, j, a, b, blocksize + + if (mw%talk) then + write(*, *) '' + write(*, *) 'Computing energy differences' + end if call ss%readfromfile('infile.ssposcar') call ss%classify('supercell', uc) - call pot%setup(uc, ss, fc, fct, fcf, mw, opts%verbosity + 1) + call pot%setup(uc, ss, fc, fct, fcf, mw, opts%verbosity+1) - ! Fetch simulation data from file + ! We fetch the simulation data if (lo_does_file_exist('infile.sim.hdf5')) then call sim%read_from_hdf5('infile.sim.hdf5', verbosity=opts%verbosity + 2, stride=-1) else call sim%read_from_file(verbosity=opts%verbosity + 2, stride=1, magnetic=.false., dielectric=.false., nrand=-1, mw=mw) end if - allocate (f2(3, ss%na)) - allocate (f3(3, ss%na)) - allocate (f4(3, ss%na)) - allocate (fp(3, ss%na)) + if (abs(opts%temperature - sim%temperature_thermostat) .gt. lo_tol) then + write(*, *) + write(*, *) 'WARNING: input and simulation temperatures do not match' + write(*, '(1X,A24,F24.12)') 'Input temperature', opts%temperature + write(*, '(1X,A24,F24.12)') 'Simulation temperature', sim%temperature_thermostat + write(*, *) 'Results might be garbage !' + write(*, *) + end if + + thermo%temperature = sim%temperature_thermostat + if (thermo%temperature .gt. 1E-5_r8) then + inverse_kbt = 1.0_r8/lo_kb_Hartree/thermo%temperature + else + inverse_kbt = 0.0_r8 + end if + + if (mw%talk) write(*, *) '... computing energy differences' ! Calculate the baseline energy allocate (ediff(sim%nt, 5)) + allocate (sdiff(sim%nt, 3, 3, 5)) ediff = 0.0_r8 + sdiff = 0.0_r8 + ! First, we compute the energy differences do i = 1, sim%nt if (mod(i, mw%n) .ne. mw%r) cycle - call pot%energies_and_forces(sim%u(:, :, i), e2, e3, e4, ep, f2, f3, f4, fp) + call pot%energies_and_forces(sim%u(:, :, i), e2, e3, e4, ep) + ! We store the energy differences ediff(i, 1) = sim%stat%potential_energy(i) ediff(i, 2) = sim%stat%potential_energy(i) - e2 ediff(i, 3) = sim%stat%potential_energy(i) - e2 - ep ediff(i, 4) = sim%stat%potential_energy(i) - e2 - ep - e3 ediff(i, 5) = sim%stat%potential_energy(i) - e2 - ep - e3 - e4 + + ! But also the stress + sdiff(i, :, :, 1) = sim%stat%stress(:, :, i) +! sdiff(i, :, :, 2) = sim%stat%stress(:, :, i) - s2 +! sdiff(i, :, :, 2) = sim%stat%stress(:, :, i) - s2 - sp +! sdiff(i, :, :, 2) = sim%stat%stress(:, :, i) - s2 - sp - s3 +! sdiff(i, :, :, 2) = sim%stat%stress(:, :, i) - s2 - sp - s3 - s4 end do call mw%allreduce('sum', ediff) - - if (sim%temperature_thermostat .gt. 1E-5_r8) then - inverse_kbt = 1.0_r8/lo_kb_Hartree/sim%temperature_thermostat - else - inverse_kbt = 0.0_r8 - end if - - ! Compute the first and second order cumulants - do i = 1, 5 - cumulant(1, i) = lo_mean(ediff(:, i)) - cumulant(2, i) = lo_mean((ediff(:, i) - cumulant(1, i))**2) - cumulant(2, i) = cumulant(2, i)*inverse_kbt*0.5_r8 - cumulant(3, i) = lo_mean((ediff(:, i) - cumulant(1, i))**3) - cumulant(3, i) = cumulant(3, i)*inverse_kbt**2/6.0_r8 + call mw%allreduce('sum', sdiff) + + ! We can now compute all properties, including their errors using block averaging + cumulant = 0.0_r8 + cumulant_var = 0.0_r8 + blocksize = floor(real(sim%nt, r8) / real(opts%nblocks)) + allocate(buf(3, opts%nblocks)) + allocate(buf_stress(3, 3, opts%nblocks)) + do i=1, 5 + ! Here we compute all properties for each blocks + do j=1, opts%nblocks + f0 = lo_mean(ediff(blocksize*j:min(blocksize*j+1, sim%nt), i)) + buf(1, j) = lo_mean(ediff(blocksize*j:min(blocksize*j+1, sim%nt), i)) + buf(2, j) = lo_mean((ediff(blocksize*j:min(blocksize*j+1, sim%nt), i) - f0)**2) + buf(3, j) = lo_mean((ediff(blocksize*j:min(blocksize*j+1, sim%nt), i) - f0)**3) + + do a=1, 3 + do b=1, 3 + buf_stress(a, b, j) = lo_mean(sdiff(i, a, b, blocksize*j:min(blocksize*j+1, sim%nt))) + end do + end do + end do + ! First order cumulant + cumulant(1, i) = lo_mean(buf(1, :)) + cumulant_var(1, i) = lo_mean((buf(1, :) - cumulant(1, i))**2) + ! Second order cumulant + cumulant(2, i) = lo_mean(buf(2, :)) + cumulant_var(2, i) = lo_mean((buf(2, :) - cumulant(2, i))**2) + ! Third order cumulant + cumulant(3, i) = lo_mean(buf(3, :)) + cumulant_var(3, i) = lo_mean((buf(3, :) - cumulant(3, i))**2) + + do a=1, 3 + do b=1, 3 + stress_pot(a, b, i) = lo_mean(buf_stress(a, b, :)) + stress_potvar(a, b, i) = lo_mean((buf_stress(a, b, :) - thermo%stress_pot(a, b))**2) + end do + end do end do - - ! And normalize it to be per atom cumulant = cumulant/real(ss%na, r8) + cumulant(2, :) = 0.5_r8 * cumulant(2, :) * inverse_kbt + cumulant_var(2, :) = 0.5_r8 * cumulant_var(2, :) * inverse_kbt + cumulant_var(3, :) = cumulant_var(3, :) * inverse_kbt**2 / 6.0_r8 if (mw%talk) then + write (*, *) '' write (*, *) 'Temperature (K) (from infile.meta): ', sim%temperature_thermostat write (*, *) 'Potential energy:' write (*, "(1X,A,E21.14,1X,A,F21.14)") ' input: ', cumulant(1, 1)*lo_Hartree_to_eV, ' upper bound:', cumulant(2, 1)*lo_Hartree_to_eV @@ -164,86 +279,139 @@ program anharmonic_free_energy write (*, "(1X,A,E21.14,1X,A,F21.14)") ' E-fc2-polar-fc3-fc4: ', cumulant(1, 5)*lo_Hartree_to_eV, ' upper bound:', cumulant(2, 5)*lo_Hartree_to_eV end if end if -end block epotthings + call tmr%tock('cumulants') +end block calcepot -! Calculate the actual free energy -getenergy: block - real(r8) :: f_ph, ah3, ah4, fe2_1, fe2_2, fe3_1, fe3_2, fe4_1, fe4_2, pref - integer :: u - character(len=1000) :: opf +latdyn3ph: block + !> The phonon dispersion relation + type(lo_phonon_dispersions) :: dr + !> The qpoint mesh + class(lo_qpoint_mesh), allocatable :: qp + !> The third order contribution + real(r8) :: fe3, s3, cv3 - ! Some heuristics to figure out what the temperature is. - if (opts%quantum) then - f_ph = dr%phonon_free_energy(sim%temperature_thermostat) - else - f_ph = dr%phonon_free_energy_classical(sim%temperature_thermostat) - end if - if (havehighorder) then - select type (qp); type is (lo_fft_mesh) - call perturbative_anharmonic_free_energy(uc, fct, fcf, qp, dr, sim%temperature_thermostat, ah3, ah4, & - opts%fourthorder, opts%quantum, mw, mem, opts%verbosity + 1) - end select - else - ah3 = 0.0_r8 - ah4 = 0.0_r8 + if (opts%thirdorder) then + if (mw%talk) then + write(*, *) '' + write(*, *) 'THREE PHONONS CONTRIBUTION' + end if + + if (mw%talk) write(*, *) '... generating q-mesh' + call lo_generate_qmesh(qp, uc, opts%qg3ph, 'fft', timereversal=.true., headrankonly=.false., mw=mw, mem=mem, verbosity=opts%verbosity) + if (mw%talk) write(*, *) '... generating harmonic dispersion' + call dr%generate(qp, fc, uc, mw=mw, mem=mem, verbosity=opts%verbosity) + + call free_energy_thirdorder(uc, fct, qp, dr, opts%temperature, fe3, s3, cv3, opts%quantum, mw, mem) + thermo%f3 = fe3 + thermo%s3 = s3 + thermo%u3 = (fe3 + opts%temperature * s3) + thermo%cv3 = cv3 + + if (mw%talk) write(*, *) fe3 * lo_Hartree_to_eV + if (mw%talk) write(*, *) thermo%u3 * lo_Hartree_to_eV + if (mw%talk) write(*, *) s3 / lo_kb_Hartree + if (mw%talk) write(*, *) cv3 / lo_kb_Hartree end if + call tmr%tock('three-phonon') - if (opts%stochastic) then - pref = -1.0_r8 - else - pref = 1.0_r8 +end block latdyn3ph + +latdyn4ph: block + !> The phonon dispersion relation + type(lo_phonon_dispersions) :: dr + !> The qpoint mesh + class(lo_qpoint_mesh), allocatable :: qp + !> The third order contribution + real(r8) :: fe4, s4, cv4 + + if (opts%fourthorder) then + if (mw%talk) then + write(*, *) '' + write(*, *) 'FOUR PHONONS CONTRIBUTION' + end if + + if (mw%talk) write(*, *) '... generating q-mesh' + call lo_generate_qmesh(qp, uc, opts%qg4ph, 'fft', timereversal=.true., headrankonly=.false., mw=mw, mem=mem, verbosity=opts%verbosity) + if (mw%talk) write(*, *) '... generating harmonic dispersion' + call dr%generate(qp, fc, uc, mw=mw, mem=mem, verbosity=opts%verbosity) + + call free_energy_fourthorder(uc, fcf, qp, dr, opts%temperature, fe4, s4, cv4, opts%quantum, mw, mem) + thermo%f4 = fe4 + thermo%s4 = s4 + thermo%u4 = (fe4 + opts%temperature * s4) + thermo%cv4 = cv4 + + if (mw%talk) write(*, *) fe4 * lo_Hartree_to_eV + if (mw%talk) write(*, *) thermo%u4 * lo_Hartree_to_eV + if (mw%talk) write(*, *) s4 / lo_kb_Hartree + if (mw%talk) write(*, *) cv4 / lo_kb_Hartree + + call free_energy_fourthorder_secondorder(uc, fcf, qp, dr, opts%temperature, fe4, s4, cv4, opts%quantum, mw, mem) + thermo%f4 = thermo%f4 + fe4 + thermo%s4 = thermo%s4 + s4 + thermo%u4 = thermo%u4 + (fe4 + opts%temperature * s4) + thermo%cv4 = thermo%cv4 + cv4 + + if (mw%talk) write(*, *) fe4 * lo_Hartree_to_eV + if (mw%talk) write(*, *) (fe4 + opts%temperature * s4) * lo_Hartree_to_eV + if (mw%talk) write(*, *) s4 / lo_kb_Hartree + if (mw%talk) write(*, *) cv4 / lo_kb_Hartree end if + call tmr%tock('four-phonon') + +end block latdyn4ph + +summary: block + real(r8) :: f0, f1, f2 + character(len=1000) :: opf1, opf2 + if (mw%talk) then - opf = '(1X,A23,1X,F20.7)' - ! Write on a file - u = open_file('out', 'outfile.anharmonic_free_energy') - fe2_1 = (cumulant(1, 3) + f_ph)*lo_Hartree_to_eV - fe2_2 = (cumulant(1, 3) + f_ph + pref*cumulant(2, 3))*lo_Hartree_to_eV - write (u, "(1X, A17, F8.2, 1X, A17)") '# Free energy at ', sim%temperature_thermostat, 'K, unit : eV/atom' - write (u, *) '# Lowest order (1st order cumulant, 2nd order cumulant)' - write (u, "(1X, 2(F25.10,' '))") fe2_1, fe2_2 + write(*, *) '' + write(*, *) 'SUMMARY OF RESULTS' + write(*, *) '' + opf1 = '(1X,3(A20))' + opf2 = '(1X,3(F20.12))' + f0 = (cumulant(1, 2) + thermo%f0) * lo_Hartree_to_eV + f1 = (cumulant(1, 2) + thermo%f0 + thermo%f3) * lo_Hartree_to_eV + f2 = (cumulant(1, 2) + thermo%f0 + thermo%f3 + thermo%f4) * lo_Hartree_to_eV + write(*, *) 'Free energy [eV/at]' + write(*, opf1) 'zeroth order', 'first order', 'second order' + write(*, opf2) f0, f1, f2 + + f0 = (cumulant(1, 2) + thermo%u0) * lo_Hartree_to_eV + f1 = (cumulant(1, 2) + thermo%u0 + thermo%u3) * lo_Hartree_to_eV + f2 = (cumulant(1, 2) + thermo%u0 + thermo%u3 + thermo%u4) * lo_Hartree_to_eV + write(*, *) 'Internal energy [eV/at]' + write(*, opf1) 'zeroth order', 'first order', 'second order' + write(*, opf2) f0, f1, f2 + + f0 = (thermo%s0) / lo_kb_Hartree + f1 = (thermo%s0 + thermo%s3) / lo_kb_Hartree + f2 = (thermo%s0 + thermo%s3 + thermo%s4) / lo_kb_Hartree + write(*, *) 'Entropy [eV/at/K]' + write(*, opf1) 'zeroth order', 'first order', 'second order' + write(*, opf2) f0, f1, f2 + + f0 = (thermo%cv0) / lo_kb_Hartree + f1 = (thermo%cv0 + thermo%cv3) / lo_kb_Hartree + f2 = (thermo%cv0 + thermo%cv3 + thermo%cv4) / lo_kb_Hartree + write(*, *) 'Heat capacity [kb]' + write(*, opf1) 'zeroth order', 'first order', 'second order' + write(*, opf2) f0, f1, f2 + write (*, *) '' - write (*, *) 'Lowest order approximation to the free energy (eV/atom):' - write (*, *) 'Calculated as + F_phonon' - write (*, opf) 'F =', fe2_1 - write (*, opf) 'F_phonon =', f_ph*lo_Hartree_to_eV - write (*, opf) 'Second order cumulant =', cumulant(2, 3)*lo_Hartree_to_eV - write (*, opf) 'Third order cumulant =', cumulant(3, 3)*lo_Hartree_to_eV - if (opts%thirdorder .or. opts%fourthorder) then - fe3_1 = (cumulant(1, 4) + f_ph + ah3)*lo_Hartree_to_eV - fe3_2 = (cumulant(1, 4) + f_ph + ah3 + pref*cumulant(2, 4))*lo_Hartree_to_eV - write (u, *) '# Third order anharmonic corrections (1st order cumulant, 2nd order cumulant)' - write (u, "(1X, 2(F25.10,' '))") fe3_1, fe3_2 - write (*, *) '' - write (*, *) 'Free energy with third order anharmonic corrections (eV/atom):' - write (*, *) 'Calculated as + F_phonon + F_3' - write (*, opf) 'F =', fe3_1 - write (*, opf) 'F_phonon =', f_ph*lo_Hartree_to_eV - write (*, opf) 'F_3 =', ah3*lo_Hartree_to_eV - write (*, opf) 'Second order cumulant =', cumulant(2, 4)*lo_Hartree_to_eV - write (*, opf) 'Third order cumulant =', cumulant(3, 4)*lo_Hartree_to_eV - end if - if (opts%fourthorder) then - fe4_1 = (cumulant(1, 5) + f_ph + ah3 + ah4)*lo_Hartree_to_eV - fe4_2 = (cumulant(1, 5) + f_ph + ah3 + ah4 + pref*cumulant(2, 5))*lo_Hartree_to_eV - write (u, *) '# Fourth order anharmonic corrections (1st order cumulant, 2nd order cumulant)' - write (u, "(1X, 2(F25.10,' '))") fe4_1, fe4_2 - write (*, *) '' - write (*, *) 'Free energy with fourth order anharmonic corrections (eV/atom):' - write (*, *) 'Calculated as + F_phonon + F_3 + F_4' - write (*, opf) 'F =', fe4_1 - write (*, opf) 'F_phonon =', f_ph*lo_Hartree_to_eV - write (*, opf) 'F_3 =', ah3*lo_Hartree_to_eV - write (*, opf) 'F_4 =', ah4*lo_Hartree_to_eV - write (*, opf) 'Second order cumulant =', cumulant(2, 5)*lo_Hartree_to_eV - write (*, opf) 'Third order cumulant =', cumulant(3, 5)*lo_Hartree_to_eV - end if - end if + write (*, '(1X,A)') 'SUGGESTED CITATIONS:' + write (*, '(1X,A41,A)') 'Software: ', 'F. Knoop et al., J. Open Source Softw 9(94), 6150 (2024)' -end block getenergy + end if + call tmr%stop() + if (mw%talk) write(*, *) '' + call tmr%dump(mw, 'Timings:') -! Kill MPI -call mw%destroy() +end block summary +! And we are done! +call mpi_barrier(mw%comm, mw%error) +call mpi_finalize(lo_status) end program diff --git a/src/anharmonic_free_energy/old.main.f90 b/src/anharmonic_free_energy/old.main.f90 new file mode 100644 index 00000000..29509e94 --- /dev/null +++ b/src/anharmonic_free_energy/old.main.f90 @@ -0,0 +1,253 @@ +program anharmonic_free_energy +!!{!src/anharmonic_free_energy/manual.md!} +use konstanter, only: r8, lo_Hartree_to_eV, lo_kb_Hartree, lo_pressure_HartreeBohr_to_GPa +use gottochblandat, only: open_file, walltime, lo_linspace, lo_progressbar_init, lo_progressbar, tochar, & + lo_does_file_exist, lo_mean, lo_stddev +use mpi_wrappers, only: lo_mpi_helper +use lo_memtracker, only: lo_mem_helper +use lo_timetracker, only: lo_timer +use type_crystalstructure, only: lo_crystalstructure +use type_forceconstant_secondorder, only: lo_forceconstant_secondorder +use type_forceconstant_thirdorder, only: lo_forceconstant_thirdorder +use type_forceconstant_fourthorder, only: lo_forceconstant_fourthorder +use type_mdsim, only: lo_mdsim +use type_qpointmesh, only: lo_qpoint_mesh, lo_generate_qmesh, lo_read_qmesh_from_file, lo_fft_mesh +use type_phonon_dispersions, only: lo_phonon_dispersions +use lo_phonon_bandstructure_on_path, only: lo_phonon_bandstructure +use type_phonon_dos, only: lo_phonon_dos + +use options, only: lo_opts +use energy, only: perturbative_anharmonic_free_energy +use epot, only: lo_energy_differences +use type_thermodynamics, only: lo_thermodynamics + +implicit none + +type(lo_opts) :: opts +type(lo_forceconstant_secondorder) :: fc +type(lo_forceconstant_thirdorder) :: fct +type(lo_forceconstant_fourthorder) :: fcf +type(lo_phonon_dispersions) :: dr +type(lo_crystalstructure) :: uc +class(lo_qpoint_mesh), allocatable :: qp +type(lo_mpi_helper) :: mw +type(lo_mem_helper) :: mem +type(lo_timer) :: tmr +type(lo_mdsim) :: sim + +type(lo_thermodynamics) :: thermo +real(r8), dimension(3, 5) :: cumulant +real(r8) :: timer_init, timer_total +real(r8) :: U0, U1, energy_unit_factor +logical :: havehighorder + +! Init MPI, timers and options +call mw%init() +timer_total = walltime() +timer_init = walltime() +call opts%parse() +call tmr%start() + +! set up all possible meshes and get all dispersions +init: block + integer :: t, u + + ! only be verbose on the first rank + if (.not. mw%talk) opts%verbosity = -10 + + ! Read structure + call uc%readfromfile('infile.ucposcar', verbosity=opts%verbosity) + call uc%classify('wedge', timereversal=.true.) + if (mw%talk) write (*, *) '... read unitcell' + + ! Read forceconstants + call fc%readfromfile(uc, 'infile.forceconstant', mem, verbosity=-1) + if (mw%talk) write (*, *) '... read second order forceconstant' + + if (opts%thirdorder) call fct%readfromfile(uc, 'infile.forceconstant_thirdorder') + if (opts%fourthorder) call fcf%readfromfile(uc, 'infile.forceconstant_fourthorder') + havehighorder = .false. + if (opts%thirdorder .or. opts%fourthorder) havehighorder = .true. + + call tmr%tock('reading input') + + ! Get a q-mesh for the integrations. Always an FFT mesh. + if (mw%talk) write (*, *) '... generating q-mesh' + call lo_generate_qmesh(qp, uc, opts%qgrid, 'fft', timereversal=.true., headrankonly=.false., mw=mw, mem=mem, verbosity=opts%verbosity) + + ! Dispersions for everyone! + call dr%generate(qp, fc, uc, mw=mw, mem=mem, verbosity=opts%verbosity) + if (mw%talk) write (*, *) '... got the full dispersion relations' + call tmr%tock('harmonic properties') + + ! Check for imaginary modes right away + if (dr%omega_min .lt. 0.0_r8) then + ! Dump the free energies + if (mw%talk) then + write (*, *) 'Found negative eigenvalues. Stopping prematurely since no free energy can be defined.' + end if + call mw%destroy() + stop + end if + timer_init = walltime() - timer_init + +end block init + +! We start with the potential energy terms since those are much faster +epotthings: block + type(lo_energy_differences) :: pot + type(lo_crystalstructure) :: ss + + real(r8), dimension(:, :), allocatable :: f2, f3, f4, fp + real(r8), dimension(:, :), allocatable :: ediff + + real(r8) :: e2, e3, e4, ep, inverse_kbt + integer :: i + + call ss%readfromfile('infile.ssposcar') + call ss%classify('supercell', uc) + call pot%setup(uc, ss, fc, fct, fcf, mw, opts%verbosity + 1) + + thermo%volume = uc%volume + + ! Fetch simulation data from file + if (lo_does_file_exist('infile.sim.hdf5')) then + call sim%read_from_hdf5('infile.sim.hdf5', verbosity=opts%verbosity + 2, stride=-1) + else + call sim%read_from_file(verbosity=opts%verbosity + 2, stride=1, magnetic=.false., dielectric=.false., nrand=-1, mw=mw) + end if + + allocate (f2(3, ss%na)) + allocate (f3(3, ss%na)) + allocate (f4(3, ss%na)) + allocate (fp(3, ss%na)) + + ! Calculate the baseline energy + allocate (ediff(sim%nt, 5)) + ediff = 0.0_r8 + + do i = 1, sim%nt + if (mod(i, mw%n) .ne. mw%r) cycle + call pot%energies_and_forces(sim%u(:, :, i), e2, e3, e4, ep, f2, f3, f4, fp) + ediff(i, 1) = sim%stat%potential_energy(i) + ediff(i, 2) = sim%stat%potential_energy(i) - e2 + ediff(i, 3) = sim%stat%potential_energy(i) - e2 - ep + ediff(i, 4) = sim%stat%potential_energy(i) - e2 - ep - e3 + ediff(i, 5) = sim%stat%potential_energy(i) - e2 - ep - e3 - e4 + end do + call mw%allreduce('sum', ediff) + + if (sim%temperature_thermostat .gt. 1E-5_r8) then + inverse_kbt = 1.0_r8/lo_kb_Hartree/sim%temperature_thermostat + else + inverse_kbt = 0.0_r8 + end if + + ! Compute the first and second order cumulants + do i = 1, 5 + cumulant(1, i) = lo_mean(ediff(:, i)) + cumulant(2, i) = lo_mean((ediff(:, i) - cumulant(1, i))**2) + cumulant(2, i) = cumulant(2, i)*inverse_kbt*0.5_r8 + cumulant(3, i) = lo_mean((ediff(:, i) - cumulant(1, i))**3) + cumulant(3, i) = cumulant(3, i)*inverse_kbt**2/6.0_r8 + end do + + ! And normalize it to be per atom + cumulant = cumulant/real(ss%na, r8) + + if (mw%talk) then + write (*, *) 'Temperature (K) (from infile.meta): ', sim%temperature_thermostat + write (*, *) 'Potential energy:' + write (*, "(1X,A,E21.14,1X,A,F21.14)") ' input: ', cumulant(1, 1)*lo_Hartree_to_eV, ' upper bound:', cumulant(2, 1)*lo_Hartree_to_eV + write (*, "(1X,A,E21.14,1X,A,F21.14)") ' E-fc2: ', cumulant(1, 2)*lo_Hartree_to_eV, ' upper bound:', cumulant(2, 2)*lo_Hartree_to_eV + write (*, "(1X,A,E21.14,1X,A,F21.14)") ' E-fc2-polar: ', cumulant(1, 3)*lo_Hartree_to_eV, ' upper bound:', cumulant(2, 3)*lo_Hartree_to_eV + if (opts%thirdorder) then + write (*, "(1X,A,E21.14,1X,A,F21.14)") ' E-fc2-polar-fc3: ', cumulant(1, 4)*lo_Hartree_to_eV, ' upper bound:', cumulant(2, 4)*lo_Hartree_to_eV + end if + if (opts%fourthorder) then + write (*, "(1X,A,E21.14,1X,A,F21.14)") ' E-fc2-polar-fc3-fc4: ', cumulant(1, 5)*lo_Hartree_to_eV, ' upper bound:', cumulant(2, 5)*lo_Hartree_to_eV + end if + end if +end block epotthings + +! Calculate the actual free energy +getenergy: block + real(r8) :: f_ph, ah3, ah4, fe2_1, fe2_2, fe3_1, fe3_2, fe4_1, fe4_2, pref + integer :: u + character(len=1000) :: opf + + ! Some heuristics to figure out what the temperature is. + if (opts%quantum) then + f_ph = dr%phonon_free_energy(sim%temperature_thermostat) + else + f_ph = dr%phonon_free_energy_classical(sim%temperature_thermostat) + end if + + if (havehighorder) then + select type (qp); type is (lo_fft_mesh) + call perturbative_anharmonic_free_energy(uc, fct, fcf, qp, dr, sim%temperature_thermostat, ah3, ah4, & + opts%fourthorder, opts%quantum, mw, mem, opts%verbosity + 1) + end select + else + ah3 = 0.0_r8 + ah4 = 0.0_r8 + end if + + if (opts%stochastic) then + pref = -1.0_r8 + else + pref = 1.0_r8 + end if + if (mw%talk) then + opf = '(1X,A23,1X,F20.7)' + ! Write on a file + u = open_file('out', 'outfile.anharmonic_free_energy') + fe2_1 = (cumulant(1, 3) + f_ph)*lo_Hartree_to_eV + fe2_2 = (cumulant(1, 3) + f_ph + pref*cumulant(2, 3))*lo_Hartree_to_eV + write (u, "(1X, A17, F8.2, 1X, A17)") '# Free energy at ', sim%temperature_thermostat, 'K, unit : eV/atom' + write (u, *) '# Lowest order (1st order cumulant, 2nd order cumulant)' + write (u, "(1X, 2(F25.10,' '))") fe2_1, fe2_2 + write (*, *) '' + write (*, *) 'Lowest order approximation to the free energy (eV/atom):' + write (*, *) 'Calculated as + F_phonon' + write (*, opf) 'F =', fe2_1 + write (*, opf) 'F_phonon =', f_ph*lo_Hartree_to_eV + write (*, opf) 'Second order cumulant =', cumulant(2, 3)*lo_Hartree_to_eV + write (*, opf) 'Third order cumulant =', cumulant(3, 3)*lo_Hartree_to_eV + if (opts%thirdorder .or. opts%fourthorder) then + fe3_1 = (cumulant(1, 4) + f_ph + ah3)*lo_Hartree_to_eV + fe3_2 = (cumulant(1, 4) + f_ph + ah3 + pref*cumulant(2, 4))*lo_Hartree_to_eV + write (u, *) '# Third order anharmonic corrections (1st order cumulant, 2nd order cumulant)' + write (u, "(1X, 2(F25.10,' '))") fe3_1, fe3_2 + write (*, *) '' + write (*, *) 'Free energy with third order anharmonic corrections (eV/atom):' + write (*, *) 'Calculated as + F_phonon + F_3' + write (*, opf) 'F =', fe3_1 + write (*, opf) 'F_phonon =', f_ph*lo_Hartree_to_eV + write (*, opf) 'F_3 =', ah3*lo_Hartree_to_eV + write (*, opf) 'Second order cumulant =', cumulant(2, 4)*lo_Hartree_to_eV + write (*, opf) 'Third order cumulant =', cumulant(3, 4)*lo_Hartree_to_eV + end if + if (opts%fourthorder) then + fe4_1 = (cumulant(1, 5) + f_ph + ah3 + ah4)*lo_Hartree_to_eV + fe4_2 = (cumulant(1, 5) + f_ph + ah3 + ah4 + pref*cumulant(2, 5))*lo_Hartree_to_eV + write (u, *) '# Fourth order anharmonic corrections (1st order cumulant, 2nd order cumulant)' + write (u, "(1X, 2(F25.10,' '))") fe4_1, fe4_2 + write (*, *) '' + write (*, *) 'Free energy with fourth order anharmonic corrections (eV/atom):' + write (*, *) 'Calculated as + F_phonon + F_3 + F_4' + write (*, opf) 'F =', fe4_1 + write (*, opf) 'F_phonon =', f_ph*lo_Hartree_to_eV + write (*, opf) 'F_3 =', ah3*lo_Hartree_to_eV + write (*, opf) 'F_4 =', ah4*lo_Hartree_to_eV + write (*, opf) 'Second order cumulant =', cumulant(2, 5)*lo_Hartree_to_eV + write (*, opf) 'Third order cumulant =', cumulant(3, 5)*lo_Hartree_to_eV + end if + end if + +end block getenergy + +! Kill MPI +call mw%destroy() + +end program diff --git a/src/anharmonic_free_energy/options.f90 b/src/anharmonic_free_energy/options.f90 index e7c1f3f8..af8f1f8a 100644 --- a/src/anharmonic_free_energy/options.f90 +++ b/src/anharmonic_free_energy/options.f90 @@ -9,9 +9,11 @@ module options public :: lo_opts type lo_opts - integer, dimension(3) :: qgrid + real(r8) :: temperature + integer, dimension(3) :: qgrid, qg3ph, qg4ph integer :: integrationtype integer :: verbosity + integer :: nblocks logical :: quantum = .false. logical :: stochastic = .false. logical :: thirdorder = .false. @@ -44,6 +46,18 @@ subroutine parse(opts) ! Specify some options cli_qpoint_grid + call cli%add(switch='--qpoint_grid3ph', switch_ab='-qg3ph', & + help='Dimension of the q-grid for three phonon contribution', & + nargs='3', required=.false., act='store', def='-1 -1 -1', error=lo_status) + if (lo_status .ne. 0) stop + call cli%add(switch='--qpoint_grid4ph', switch_ab='-qg4ph', & + help='Dimension of the q-grid for four phonon contribution', & + nargs='3', required=.false., act='store', def='-1 -1 -1', error=lo_status) + if (lo_status .ne. 0) stop + call cli%add(switch='--temperature', & + help='The temperature at which the thermodynamic properties are computed', & + required=.false., act='store', def='300', error=lo_status) + if (lo_status .ne. 0) stop call cli%add(switch='--quantum', & help='Use Bose-Einstein occupations to compute the free energy', & required=.false., act='store_true', def='.false.', error=lo_status) @@ -60,6 +74,10 @@ subroutine parse(opts) help='Compute fourth order anharmonic correction to the free energy', & required=.false., act='store_true', def='.false.', error=lo_status) if (lo_status .ne. 0) stop + call cli%add(switch='--nblocks', & + help='Number of blocks used to compute uncertainty', & + required=.false., act='store', def='10', error=lo_status) + if (lo_status .ne. 0) stop cli_manpage cli_verbose @@ -79,17 +97,39 @@ subroutine parse(opts) call cli%get(switch='--verbose', val=dumlog, error=lo_status); errctr = errctr + lo_status; if (dumlog) opts%verbosity = 2 ! get real options + call cli%get(switch='--temperature', val=opts%temperature, error=lo_status); errctr = errctr + lo_status call cli%get(switch='--qpoint_grid', val=opts%qgrid, error=lo_status); errctr = errctr + lo_status call cli%get(switch='--quantum', val=opts%quantum, error=lo_status); errctr = errctr + lo_status call cli%get(switch='--stochastic', val=opts%stochastic, error=lo_status); errctr = errctr + lo_status call cli%get(switch='--thirdorder', val=opts%thirdorder, error=lo_status); errctr = errctr + lo_status call cli%get(switch='--fourthorder', val=opts%fourthorder, error=lo_status); errctr = errctr + lo_status + call cli%get(switch='--nblocks', val=opts%nblocks, error=lo_status); errctr = errctr + lo_status + call cli%get(switch='--qpoint_grid3ph', val=opts%qg3ph, error=lo_status); errctr = errctr + lo_status + call cli%get(switch='--qpoint_grid4ph', val=opts%qg4ph, error=lo_status); errctr = errctr + lo_status + call cli%get(switch='--nblocks', val=opts%nblocks, error=lo_status); errctr = errctr + lo_status ! If we have fourthorder we should also have thirdorder - if (opts%fourthorder) opts%thirdorder = .true. +! if (opts%fourthorder) opts%thirdorder = .true. if (errctr .ne. 0) call lo_stop_gracefully(['Failed parsing the command line options'], lo_exitcode_baddim) + if (maxval(opts%qg3ph) .gt. 0 .and. .not. opts%thirdorder) then + write(*, *) 'You have to enable thirdorder to use a three-phonon q-grid, stopping calculation.' + stop + end if + if (minval(opts%qg3ph) .le. 0 .and. opts%thirdorder) then + opts%qg3ph = opts%qgrid + end if + + if (maxval(opts%qg4ph) .gt. 0 .and. .not. opts%fourthorder) then + write(*, *) 'You have to enable fourthorder to use a four-phonon q-grid, stopping calculation.' + stop + end if + if (minval(opts%qg4ph) .le. 0 .and. opts%fourthorder) then + write(*, *) opts%qg4ph + opts%qg4ph = opts%qgrid + end if + end subroutine end module diff --git a/src/anharmonic_free_energy/thermo.f90 b/src/anharmonic_free_energy/thermo.f90 new file mode 100644 index 00000000..7bb5493f --- /dev/null +++ b/src/anharmonic_free_energy/thermo.f90 @@ -0,0 +1,31 @@ +#include "precompilerdefinitions" +module thermo +use konstanter, only: r8, lo_huge + +implicit none +private +public :: lo_thermodynamics + +type lo_thermodynamics + !> The temperature at which everything is evaluated + real(r8) :: temperature=-lo_huge + !> The volume + real(r8) :: volume=-lo_huge + !> The free energies + real(r8) :: f0, f3, f4 + !> The internal energy + real(r8) :: u0, u3, u4 + !> The entropy + real(r8) :: s0, s3, s4 + !> The heat capacity at constant volume + real(r8) :: cv0, cv3, cv4 + !> The heat capacity at constant pressure + real(r8) :: cp0, cp3, cp4 + !> The pressure + real(r8) :: p=-lo_huge + !> The stress tensor + real(r8), dimension(3, 3) :: stress_pot, stress_kin, stress_potvar + !> The thermal expansion + real(r8) :: alpha +end type +end module diff --git a/src/anharmonic_free_energy/thirdorder.f90 b/src/anharmonic_free_energy/thirdorder.f90 new file mode 100644 index 00000000..55419201 --- /dev/null +++ b/src/anharmonic_free_energy/thirdorder.f90 @@ -0,0 +1,292 @@ +module thirdorder +!! Compute the third order contribution to the anharmonic free energy +use konstanter, only: r8, lo_freqtol, lo_twopi, lo_imag, lo_kb_Hartree, lo_exitcode_param +use gottochblandat, only: walltime, lo_trueNtimes, lo_progressbar_init, lo_progressbar, lo_planck, & + lo_planck_deriv, lo_planck_secondderiv +use mpi_wrappers, only: lo_mpi_helper, lo_stop_gracefully +use lo_memtracker, only: lo_mem_helper +use type_qpointmesh, only: lo_qpoint_mesh, lo_fft_mesh +use type_crystalstructure, only: lo_crystalstructure +use type_forceconstant_thirdorder, only: lo_forceconstant_thirdorder +use type_phonon_dispersions, only: lo_phonon_dispersions +use lo_timetracker, only: lo_timer + +implicit none +private + +public :: free_energy_thirdorder + +contains +!> Calculate the third order free energy +subroutine free_energy_thirdorder(uc, fct, qp, dr, temperature, fe3, s3, cv3, quantum, mw, mem) + !> crystal structure + type(lo_crystalstructure), intent(in) :: uc + !> third order force constant + type(lo_forceconstant_thirdorder), intent(in) :: fct + !> q-point mesh + class(lo_qpoint_mesh), intent(in) :: qp + !> dispersions + type(lo_phonon_dispersions), intent(in) :: dr + !> temperature + real(r8) :: temperature + !> free energies and heat capacity + real(r8), intent(out) :: fe3, s3, cv3 + !> what to compute + logical, intent(in) :: quantum + !> mpi helper + type(lo_mpi_helper), intent(inout) :: mw + !> memory tracker + type(lo_mem_helper), intent(inout) :: mem + + !> Frequency scaled eigenvectors + complex(r8), dimension(:), allocatable :: egv1, egv2, egv3 + !> Helper for Fourier transform of psi3 + complex(r8), dimension(:), allocatable :: ptf, evp1, evp2 + !> Frequencies, bose-einstein occupation and scattering strength and some other buffer + real(r8) :: sigma, om1, om2, om3, n2, n3, psisq, f0, f1, plf0, plf1, perm, f2, n1, pref, t0, prefactor + !> + real(r8) :: sig1, sig2, sig3, mult, dn1, dn2, dn3, ddn1, ddn2, ddn3, df1, df2, ddf1, ddf2, df0, ddf0 + !> The complex threephonon matrix element + complex(r8) :: c0 + !> Integers for do loops and counting + integer :: qi, q1, q2, q3, q2p, q3p, b1, b2, b3, i, ctr + !> The dimension of the q-grid + integer, dimension(3) :: dims + + ! We start by allocating everything + call mem%allocate(ptf, dr%n_mode**3, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%allocate(evp1, dr%n_mode**2, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%allocate(evp2, dr%n_mode**3, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%allocate(egv1, dr%n_mode, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%allocate(egv2, dr%n_mode, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%allocate(egv3, dr%n_mode, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + + t0 = walltime() + + select type (qp) + class is (lo_fft_mesh) + dims = qp%griddensity + class default + call lo_stop_gracefully(['This routine only works with FFT meshes'], lo_exitcode_param, __FILE__, __LINE__) + end select + + fe3 = 0.0_r8 + cv3 = 0.0_r8 + + do q1=1, qp%n_irr_point + do q2=1, qp%n_full_point + ctr = ctr + 1 + if (mod(ctr, mw%n) .ne. mw%r) cycle + q3 = fft_third_grid_index(qp%ip(q1)%full_index, q2, dims) + if (q3 .lt. q2) cycle + + ! The prefactor to take into account what we are skipping + if (q2 .eq. q3) then + mult = 1.0_r8 + else + mult = 2.0_r8 + end if + + prefactor = qp%ip(q1)%integration_weight*qp%ap(q2)%integration_weight*mult/uc%na + ! pre-transform the matrix element + call pretransform_phi3(fct, qp%ap(q2)%r, qp%ap(q3)%r, ptf) + + do b1=1, dr%n_mode + om1 = dr%iq(q1)%omega(b1) + if (om1 .lt. lo_freqtol) cycle + egv1 = dr%iq(q1)%egv(:, b1)/sqrt(om1) + do b2=1, dr%n_mode + om2 = dr%aq(q2)%omega(b2) + if (om2 .lt. lo_freqtol) cycle + + egv2 = dr%aq(q2)%egv(:, b2)/sqrt(om2) + evp1 = 0.0_r8 + call zgeru(dr%n_mode, dr%n_mode, (1.0_r8, 0.0_r8), egv2, 1, egv1, 1, evp1, dr%n_mode) + do b3=1, dr%n_mode + om3 = dr%aq(q3)%omega(b3) + if (om3 .lt. lo_freqtol) cycle + egv3 = dr%aq(q3)%egv(:, b3)/sqrt(om3) + + evp2 = 0.0_r8 + call zgeru(dr%n_mode, dr%n_mode**2, (1.0_r8, 0.0_r8), egv3, 1, evp1, 1, evp2, dr%n_mode) + evp2 = conjg(evp2) + c0 = dot_product(evp2, ptf) + psisq = real(conjg(c0)*c0, r8) * prefactor + + if (quantum) then + n1 = lo_planck(temperature, om1) + n2 = lo_planck(temperature, om2) + n3 = lo_planck(temperature, om3) + + dn1 = lo_planck_deriv(temperature, om1) + dn2 = lo_planck_deriv(temperature, om1) + dn3 = lo_planck_deriv(temperature, om1) + + ddn1 = lo_planck_secondderiv(temperature, om1) + ddn2 = lo_planck_secondderiv(temperature, om1) + ddn3 = lo_planck_secondderiv(temperature, om1) + + f1 = (n1 + 1.0_r8)*(n2 + n3 + 1.0_r8) + n2*n3 + f2 = n1*n2 + n1*n3 - n2*n3 + 1.0_r8 + + df1 = dn1 * (n2 + n3 + 1.0_r8) + (n1 + 1.0_r8) * (dn2 + dn3) + dn2 * n3 + n2 * dn3 + df2 = dn1 * n2 + n1 * dn2 + dn1 * n3 + n1 * dn3 - dn2 * n3 - n2 * dn3 + + ddf1 = ddn1 * (n2 + n3 + 1.0_r8) + 2.0_r8 * dn1 * (dn2 + dn3) + (n1 + 1.0_r8) * (ddn2 + ddn3) + & + ddn2 * n3 + n2 * ddn3 + 2.0_r8 * dn2 * dn3 + ddf2 = ddn1 * n2 + n1 * ddn2 + 2.0_r8 * dn1 * dn2 + ddn1 * n3 + n1 * ddn3 + 2.0_r8 * dn1 * dn3 - & + ddn2 * n3 - n2 * ddn3 - 2.0_r8 * dn2 * dn3 + + f1 = f1/(om1 + om2 + om3) + df1 = df1/(om1 + om2 + om3) + ddf1 = ddf1/(om1 + om2 + om3) + if (abs(om1 + om2 - om3) .lt. lo_freqtol) then + ! Get a smearing parameter + sig1 = dr%default_smearing(b1) + sig2 = dr%default_smearing(b2) + sig3 = dr%default_smearing(b3) + sigma = sqrt(sig1**2 + sig2**2 + sig3**2) + f2 = 3*f2*real(1.0/(om1 + om2 - om3 + lo_imag*sigma), r8) + df2 = 3.0_r8 * df2 * real(1.0/(om1 + om2 - om3 + lo_imag*sigma), r8) + ddf2 = 3.0_r8 * ddf2 * real(1.0/(om1 + om2 - om3 + lo_imag*sigma), r8) + else + f2 = 3.0_r8 * f2 / (om1 + om2 - om3) + df2 = 3.0_r8 * df2 / (om1 + om2 - om3) + ddf2 = 3.0_r8 * ddf2 / (om1 + om2 - om3) + end if + f0 = (f1 + f2) / 48.0_r8 + df0 = (df1 + df2) / 48.0_r8 + ddf0 = (ddf1 + ddf2) * temperature / 48.0_r8 + else + f0 = (lo_kb_Hartree*temperature)**2 / (om1*om2*om3) / 12.0_r8 + df0 = lo_kb_Hartree**2 * temperature / (om1*om2*om3) / 6.0_r8 + ddf0 = lo_kb_Hartree**2 * temperature / (om1*om2*om3) / 6.0_r8 + end if + fe3 = fe3 - f0 * psisq + s3 = s3 + df0 * psisq + cv3 = cv3 + ddf0 * psisq + end do + end do + end do + end do + if (mw%talk .and. lo_trueNtimes(q1, 127, qp%n_irr_point)) then + call lo_progressbar(' ... third order', q1, qp%n_irr_point, walltime() - t0) + end if + end do + if (mw%talk) then + call lo_progressbar(' ... third order', qp%n_irr_point, qp%n_irr_point, walltime() - t0) + end if + + call mw%allreduce('sum', fe3) + call mw%allreduce('sum', cv3) +end subroutine + +!> Get the Fourier transform of the third order matrix element +subroutine pretransform_phi3(fct, q2, q3, ptf) + !> third order forceconstant + type(lo_forceconstant_thirdorder), intent(in) :: fct + !> q-vectors + real(r8), dimension(3), intent(in) :: q2, q3 + !> flattened, pretransformed matrix element + complex(r8), dimension(:), intent(out) :: ptf + + integer :: i, j, k, l + + complex(r8) :: expiqr + real(r8), dimension(3) :: rv2, rv3 + real(r8) :: iqr + integer :: a1, a2, a3, ia, ib, ic, t, nb + + nb = fct%na*3 + ptf = 0.0_r8 + do a1 = 1, fct%na + do t = 1, fct%atom(a1)%n + a2 = fct%atom(a1)%triplet(t)%i2 + a3 = fct%atom(a1)%triplet(t)%i3 + + rv2 = fct%atom(a1)%triplet(t)%lv2 + rv3 = fct%atom(a1)%triplet(t)%lv3 + + iqr = dot_product(q2, rv2) + dot_product(q3, rv3) + iqr = -iqr*lo_twopi + expiqr = cmplx(cos(iqr), sin(iqr), r8) + do i = 1, 3 + do j = 1, 3 + do k = 1, 3 + ia = (a1 - 1)*3 + i + ib = (a2 - 1)*3 + j + ic = (a3 - 1)*3 + k + ! Now for the grand flattening scheme, consistent with the zgeru operations above. + l = (ia - 1)*nb*nb + (ib - 1)*nb + ic + ptf(l) = ptf(l) + fct%atom(a1)%triplet(t)%mwm(i, j, k)*expiqr + end do + end do + end do + end do + end do +end subroutine + +!> returns the index on the grid that gives q3=-q1-q2 +pure function fft_third_grid_index(i1, i2, dims) result(i3) + !> index to q1 + integer, intent(in) :: i1 + !> index to q2 + integer, intent(in) :: i2 + !> dimensions of the grid + integer, dimension(3), intent(in) :: dims + !> index to q3 + integer :: i3 + + integer, dimension(3) :: gi1, gi2, gi3 + integer :: l, k + + ! Convert triplet to singlet + gi1 = singlet_to_triplet(i1, dims(2), dims(3)) + gi2 = singlet_to_triplet(i2, dims(2), dims(3)) + do l = 1, 3 + gi3(l) = 3 - gi1(l) - gi2(l) + end do + do k = 1, 3 + do l = 1, 3 + if (gi3(l) .lt. 1) gi3(l) = gi3(l) + dims(l) + if (gi3(l) .gt. dims(l)) gi3(l) = gi3(l) - dims(l) + end do + end do + ! convert it back to a singlet + i3 = triplet_to_singlet(gi3, dims(2), dims(3)) + +contains + !> convert a linear index to a triplet + pure function singlet_to_triplet(l, ny, nz) result(gi) + !> linear index + integer, intent(in) :: l + !> second dimension + integer, intent(in) :: ny + !> third dimension + integer, intent(in) :: nz + !> grid-index + integer, dimension(3) :: gi + + integer :: i, j, k + + k = mod(l, nz) + if (k .eq. 0) k = nz + j = mod((l - k)/nz, ny) + 1 + i = (l - k - (j - 1)*nz)/(nz*ny) + 1 + gi = [i, j, k] + end function + !> convert a triplet index to a singlet + pure function triplet_to_singlet(gi, ny, nz) result(l) + !> grid-index + integer, dimension(3), intent(in) :: gi + !> second dimension + integer, intent(in) :: ny + !> third dimension + integer, intent(in) :: nz + !> linear index + integer :: l + + l = (gi(1) - 1)*ny*nz + (gi(2) - 1)*nz + gi(3) + end function +end function +end module diff --git a/src/libolle/gottochblandat.f90 b/src/libolle/gottochblandat.f90 index ce75b0da..dc834127 100644 --- a/src/libolle/gottochblandat.f90 +++ b/src/libolle/gottochblandat.f90 @@ -73,6 +73,7 @@ module gottochblandat public :: lo_harmonic_oscillator_entropy public :: lo_harmonic_oscillator_free_energy public :: lo_harmonic_oscillator_internal_energy +public :: lo_classical_harmonic_oscillator_entropy public :: lo_index_in_periodic_array public :: lo_invert3x3matrix public :: lo_sqrt3x3matrix @@ -678,6 +679,11 @@ module elemental function lo_harmonic_oscillator_cv(temp,omega) result(cv) real(flyt), intent(in) :: omega real(flyt) :: cv end function + module elemental function lo_classical_harmonic_oscillator_entropy(temp,omega) result(s) + real(flyt), intent(in) :: temp + real(flyt), intent(in) :: omega + real(flyt) :: s + end function module subroutine lo_untangle_one_tetrahedron(corner,energy,groupvelocity,degentol,permutation,success,error_interp_energy,error_interp_gradient) real(r8), dimension(3,4), intent(in) :: corner real(r8), dimension(:,:), intent(in) :: energy diff --git a/src/libolle/gottochblandat_physics.f90 b/src/libolle/gottochblandat_physics.f90 index a5801e64..f9676c08 100644 --- a/src/libolle/gottochblandat_physics.f90 +++ b/src/libolle/gottochblandat_physics.f90 @@ -327,6 +327,27 @@ module elemental function lo_harmonic_oscillator_entropy(temp,omega) result(s) endif end function +module elemental function lo_classical_harmonic_oscillator_entropy(temp, omega) result(s) + !> Temperature in K + real(flyt), intent(in) :: temp + !> Angular frequency in hartree + real(flyt), intent(in) :: omega + !> The entropy in Hartreee/K + real(flyt) :: s + + if ( omega .lt. lo_freqtol ) then + s=0.0_flyt + return + endif + + if ( temp .lt. lo_temperaturetol ) then + s=0.0_flyt + return + endif + + s=lo_kb_Hartree*(1.0_r8 - log(omega/lo_kb_Hartree/temp)) +end function + !> Heat capacity (Cv) for a single harmonic oscillator in eV/K module elemental function lo_harmonic_oscillator_cv(temp,omega) result(cv) !> Temperature in K diff --git a/src/libolle/type_phonon_dispersions.f90 b/src/libolle/type_phonon_dispersions.f90 index e9877bc0..0bf5e957 100644 --- a/src/libolle/type_phonon_dispersions.f90 +++ b/src/libolle/type_phonon_dispersions.f90 @@ -9,10 +9,10 @@ module type_phonon_dispersions lo_Hartree_to_Joule, lo_exitcode_physical, lo_imag, lo_time_s_to_au use gottochblandat, only: open_file, walltime, tochar, lo_trueNtimes, lo_classical_harmonic_oscillator_free_energy, & lo_harmonic_oscillator_cv, lo_harmonic_oscillator_entropy, lo_harmonic_oscillator_free_energy, & - lo_planck, lo_sqnorm, lo_progressbar_init, lo_progressbar, qsort, lo_outerproduct, lo_chop, & - lo_symmetric_eigensystem_3x3matrix, lo_flattentensor, lo_unflatten_2tensor, & - lo_linear_least_squares, lo_nullspace_coefficient_matrix, lo_identitymatrix, & - lo_real_pseudoinverse, lo_determ + lo_classical_harmonic_oscillator_entropy, lo_planck, lo_sqnorm, lo_progressbar_init, & + lo_progressbar, qsort, lo_outerproduct, lo_chop, lo_symmetric_eigensystem_3x3matrix, & + lo_flattentensor, lo_unflatten_2tensor, lo_linear_least_squares, lo_nullspace_coefficient_matrix, & + lo_identitymatrix, lo_real_pseudoinverse, lo_determ use mpi_wrappers, only: lo_mpi_helper, lo_stop_gracefully use lo_memtracker, only: lo_mem_helper use type_blas_lapack_wrappers, only: lo_gemm, lo_gemv @@ -138,6 +138,8 @@ module type_phonon_dispersions procedure :: phonon_angular_momentum_matrix !> thermal displacement covariance matrix procedure :: thermal_displacement_matrix + !> kinetic contribution to the stress tensor + procedure :: phonon_kinetic_stress !> store the full grid in a hdf file procedure :: write_to_hdf5 !> store the irreducible grid in a hdf5 file @@ -864,6 +866,58 @@ pure function phonon_entropy(dr, temperature, modenum, sitenum) result(s) s = s/dr%n_full_qpoint/(dr%n_mode/3) end function +!> calculate the phonon entropy as a direct sum +pure function phonon_entropy_classical(dr, temperature, modenum, sitenum) result(s) + !> the phonon dispersions + class(lo_phonon_dispersions), intent(in) :: dr + !> the temperature + real(r8), intent(in) :: temperature + !> the entropy in eV/K/atom (entropy for the modenum-th mode if modenum is specified) + real(r8) :: s + !> calculate vibrational entropy for a specific mode + integer, intent(in), optional :: modenum + !> project entropy onto a specific site + integer, intent(in), optional :: sitenum + + complex(r8), dimension(3) :: cv0 + real(r8) :: w + integer :: i, j + + ! Calculate the entropy of only one mode if modenum is specified + if (present(modenum)) then + j = modenum + s = 0.0_r8 + do i = 1, dr%n_full_qpoint + s = s + lo_classical_harmonic_oscillator_entropy(temperature, dr%aq(i)%omega(j)) + end do + s = s/dr%n_full_qpoint/(dr%n_mode/3) + return + end if + + ! If modenum or sitenum was not specified, calculate the total entropy + if (present(sitenum)) then + s = 0.0_r8 + do i = 1, dr%n_full_qpoint + do j = 1, dr%n_mode + cv0 = dr%aq(i)%egv((sitenum - 1)*3 + 1:sitenum*3, j) + w = abs(dot_product(cv0, cv0)) + s = s + w*lo_classical_harmonic_oscillator_entropy(temperature, dr%aq(i)%omega(j)) + end do + end do + s = s/dr%n_full_qpoint/(dr%n_mode/3) + return + end if + + ! If modenum or sitenum was not specified, calculate the total entropy + s = 0.0_r8 + do i = 1, dr%n_full_qpoint + do j = 1, dr%n_mode + s = s + lo_classical_harmonic_oscillator_entropy(temperature, dr%aq(i)%omega(j)) + end do + end do + s = s/dr%n_full_qpoint/(dr%n_mode/3) +end function + !> calculate phonon angular momentum matrix subroutine phonon_angular_momentum_matrix(dr, qp, uc, temperature, alpha, mw) !> dispersion relations @@ -1079,6 +1133,42 @@ subroutine thermal_displacement_matrix(dr, qp, uc, temperature, sigma, mw, mem) call mem%deallocate(vX, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) end subroutine +!> Calculate the kinetic contribution to the stress tensor +subroutine phonon_kinetic_stress(dr, qp, uc, temperature, kinsigma) + !> dispersion relations + class(lo_phonon_dispersions), intent(in) :: dr + !> qpoint mesh + class(lo_qpoint_mesh), intent(in) :: qp + !> crystal structure + type(lo_crystalstructure), intent(in) :: uc + !> temperature + real(r8), intent(in) :: temperature + !> displacement covariance matrix + real(r8), dimension(3, 3), intent(out) :: kinsigma + + !> The eigenvector for a given mode + complex(r8), dimension(3) :: egv + !> Some buffers + real(r8) :: pref, om, f0 + !> Integers for do loop + integer :: aq, im, a + + kinsigma = 0.0_r8 + pref = 1.0_r8 / uc%volume / qp%n_full_point + do aq=1, qp%n_full_point + do im=1, dr%n_mode + om = dr%aq(aq)%omega(im) + if (om .lt. lo_freqtol) cycle + f0 = om * (lo_planck(temperature, om) + 0.5_r8) * pref + do a=1, uc%na + egv = dr%aq(aq)%egv((a - 1)*3 + 1:a*3, im) + kinsigma(:, :) = kinsigma(:, :) - real(lo_outerproduct(egv, egv)) * f0 + end do + end do + end do + kinsigma(:, :) = lo_chop(kinsigma(:, :), 1e-12_r8) +end subroutine + !> Calculate all the harmonic things for a q-point subroutine harmonic_things_for_single_point(ompoint, fc, p, mem, qpoint, qvec, qdirection) !> point in the dispersions From 62f0086f77413f8043ee7d45d8dc30becfdce487 Mon Sep 17 00:00:00 2001 From: =?UTF-8?q?Alo=C3=AFs=20Castellano?= Date: Thu, 13 Feb 2025 22:58:11 +0100 Subject: [PATCH 02/28] First draft for cleaner anharmonic free energy and other thermodynamic properties --- src/anharmonic_free_energy/Makefile | 12 +- src/anharmonic_free_energy/epot.f90 | 142 ++++++++++- .../lo_thermodynamic_helpers.f90 | 78 ++++++ src/anharmonic_free_energy/main.f90 | 230 +++++------------- src/anharmonic_free_energy/thermo.f90 | 31 --- src/anharmonic_free_energy/thirdorder.f90 | 121 ++++++++- src/libolle/type_phonon_dispersions.f90 | 2 +- 7 files changed, 406 insertions(+), 210 deletions(-) create mode 100644 src/anharmonic_free_energy/lo_thermodynamic_helpers.f90 delete mode 100644 src/anharmonic_free_energy/thermo.f90 diff --git a/src/anharmonic_free_energy/Makefile b/src/anharmonic_free_energy/Makefile index a93d2d11..f1877a4b 100644 --- a/src/anharmonic_free_energy/Makefile +++ b/src/anharmonic_free_energy/Makefile @@ -3,7 +3,7 @@ CODE=anharmonic_free_energy PROG=../../build/$(CODE)/$(CODE) OBJECT_PATH=../../build/$(CODE)/ -OBJS = $(OBJECT_PATH)main.o $(OBJECT_PATH)options.o $(OBJECT_PATH)thirdorder.o $(OBJECT_PATH)fourthorder.o $(OBJECT_PATH)epot.o +OBJS = $(OBJECT_PATH)main.o $(OBJECT_PATH)lo_thermodynamic_helpers.o $(OBJECT_PATH)options.o $(OBJECT_PATH)thirdorder.o $(OBJECT_PATH)fourthorder.o $(OBJECT_PATH)epot.o LPATH = -L../../lib $(blaslapackLPATH) $(incLPATHhdf) $(incLPATHmpi) IPATH = -I../../inc/libolle -I../../inc/libflap $(blaslapackIPATH) $(incIPATHhdf) $(incIPATHmpi) @@ -24,15 +24,15 @@ clean: .f90.o: $(F90) $(F90FLAGS) -c $< $(LIBS) -$(OBJECT_PATH)main.o: main.f90 $(OBJECT_PATH)options.o $(OBJECT_PATH)thirdorder.o $(OBJECT_PATH)fourthorder.o $(OBJECT_PATH)epot.o $(OBJECT_PATH)thermo.o +$(OBJECT_PATH)main.o: main.f90 $(OBJECT_PATH)options.o $(OBJECT_PATH)lo_thermodynamic_helpers.o $(OBJECT_PATH)thirdorder.o $(OBJECT_PATH)fourthorder.o $(OBJECT_PATH)epot.o $(F90) $(F90FLAGS) -c main.f90 $(LIBS) -o $@ -$(OBJECT_PATH)thirdorder.o: $(OBJECT_PATH)options.o +$(OBJECT_PATH)thirdorder.o: $(OBJECT_PATH)options.o $(OBJECT_PATH)lo_thermodynamic_helpers.o $(F90) $(F90FLAGS) -c thirdorder.f90 $(LIBS) -o $@ $(OBJECT_PATH)fourthorder.o: $(OBJECT_PATH)options.o $(F90) $(F90FLAGS) -c fourthorder.f90 $(LIBS) -o $@ $(OBJECT_PATH)options.o: $(F90) $(F90FLAGS) -c options.f90 $(LIBS) -o $@ -$(OBJECT_PATH)epot.o: epot.f90 +$(OBJECT_PATH)epot.o: epot.f90 $(OBJECT_PATH)lo_thermodynamic_helpers.o $(F90) $(F90FLAGS) -c epot.f90 $(LIBS) -o $@ -$(OBJECT_PATH)thermo.o: thermo.f90 - $(F90) $(F90FLAGS) -c thermo.f90 $(LIBS) -o $@ +$(OBJECT_PATH)lo_thermodynamic_helpers.o: lo_thermodynamic_helpers.f90 + $(F90) $(F90FLAGS) -c lo_thermodynamic_helpers.f90 $(LIBS) -o $@ diff --git a/src/anharmonic_free_energy/epot.f90 b/src/anharmonic_free_energy/epot.f90 index 1e1264c9..7de7706a 100644 --- a/src/anharmonic_free_energy/epot.f90 +++ b/src/anharmonic_free_energy/epot.f90 @@ -12,6 +12,7 @@ module epot use type_forceconstant_thirdorder, only: lo_forceconstant_thirdorder use type_forceconstant_fourthorder, only: lo_forceconstant_fourthorder use type_mdsim, only: lo_mdsim +use lo_thermodynamic_helpers, only: lo_thermodynamics, lo_symmetrize_stress implicit none private @@ -28,29 +29,35 @@ module epot contains procedure :: setup => setup_potential_energy_differences procedure :: energies_and_forces + procedure :: compute_realspace_thermo end type contains ! !> calculate energies and forces for a given configuration -subroutine energies_and_forces(pot, u, e2, e3, e4, ep) +subroutine energies_and_forces(pot, ss, u, e2, e3, e4, ep, s3) + !> The unitcell + type(lo_crystalstructure), intent(in) :: ss !> container for potential energy differences class(lo_energy_differences), intent(in) :: pot !> displacements real(r8), dimension(:, :), intent(in) :: u !> energies real(r8), intent(out) :: e2, e3, e4, ep + !> stress + real(r8), dimension(3, 3), intent(out) :: s3 real(r8), dimension(3, 3, 3, 3) :: m4 real(r8), dimension(3, 3, 3) :: m3 real(r8), dimension(3, 3) :: m2 - real(r8), dimension(3) :: v0, u2, u3, u4 - integer :: a1, a2, a3, a4, i1, i2, i3, i4, i + real(r8), dimension(3) :: v0, u1, u2, u3, u4 + integer :: a1, a2, a3, a4, i1, i2, i3, i4, i5, i e2 = 0.0_r8 e3 = 0.0_r8 e4 = 0.0_r8 ep = 0.0_r8 + s3 = 0.0_r8 ! pair term do a1 = 1, size(u, 2) @@ -83,12 +90,16 @@ subroutine energies_and_forces(pot, u, e2, e3, e4, ep) m3 = pot%fc3%atom(a1)%triplet(i)%m a2 = pot%fc3%atom(a1)%triplet(i)%i2 a3 = pot%fc3%atom(a1)%triplet(i)%i3 + u1 = u(:, a1) u2 = u(:, a2) u3 = u(:, a3) do i1 = 1, 3 do i2 = 1, 3 do i3 = 1, 3 v0(i1) = v0(i1) - m3(i1, i2, i3)*u2(i2)*u3(i3) + do i4 = 1, 3 + s3(i3, i4) = s3(i3, i4) + m3(i1, i2, i3)*u1(i1)*u2(i2)*pot%fc3%atom(a1)%triplet(i)%rv3(i4) / ss%volume / 6.0_r8 + end do end do end do end do @@ -196,4 +207,129 @@ subroutine setup_potential_energy_differences(pot, uc, ss, fc2, fc3, fc4, mw, ve end if end subroutine +subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, mw) + !> container for potential energy differences + class(lo_energy_differences), intent(in) :: pot + !> The supercell + type(lo_crystalstructure), intent(in) :: ss + !> The simulation + type(lo_mdsim), intent(in) :: sim + !> The thermodynamic helper + type(lo_thermodynamics), intent(inout) :: thermo + !> Number of blocks + integer, intent(in) :: nblocks + !> MPI + type(lo_mpi_helper), intent(inout) :: mw + + real(r8), dimension(3, 5) :: cumulant, cumulant_var + real(r8), dimension(3, 3, 5) :: stress_pot, stress_potvar + real(r8), dimension(:, :, :, :), allocatable :: sdiff + real(r8), dimension(:, :, :), allocatable :: buf_stress + real(r8), dimension(:, :), allocatable :: buf + real(r8), dimension(:, :), allocatable :: ediff + real(r8), dimension(3, 3) :: s3, sk2, sk3, sk4, skp + + real(r8) :: e2, e3, e4, ep, inverse_kbt, f0 + integer :: i, j, a, b, blocksize, istart, iend + + if (thermo%temperature .gt. 1E-5_r8) then + inverse_kbt = 1.0_r8/lo_kb_Hartree/thermo%temperature + else + inverse_kbt = 0.0_r8 + end if + + allocate(ediff(sim%nt, 5)) + allocate(sdiff(sim%nt, 3, 3, 2)) + ediff = 0.0_r8 + sdiff = 0.0_r8 + + ! Let's compute energies and stress differences + do i=1, sim%nt + if (mod(i, mw%n) .ne. mw%r) cycle + call pot%energies_and_forces(ss, sim%u(:, :, i), e2, e3, e4, ep, s3) + ! We store the energy differences + ediff(i, 1) = sim%stat%potential_energy(i) + ediff(i, 2) = sim%stat%potential_energy(i) - e2 + ediff(i, 3) = sim%stat%potential_energy(i) - e2 - ep + ediff(i, 4) = sim%stat%potential_energy(i) - e2 - ep - e3 + ediff(i, 5) = sim%stat%potential_energy(i) - e2 - ep - e3 - e4 + + ! But also the stress + sdiff(i, :, :, 1) = sim%stat%stress(:, :, i) + sdiff(i, :, :, 2) = sim%stat%stress(:, :, i) - s3 + end do + + allocate(buf(3, nblocks)) + allocate(buf_stress(3, 3, nblocks)) + + cumulant = 0.0_r8 + cumulant_var = 0.0_r8 + stress_pot = 0.0_r8 + stress_potvar = 0.0_r8 + blocksize = floor((real(sim%nt, r8)) / real(nblocks)) + buf = 0.0_r8 + buf_stress = 0.0_r8 + + do i=1, 5 + ! First, let's compute properties for each blocks + do j=1, nblocks + istart = blocksize*j + iend = min(blocksize*j + 1, sim%nt) + + f0 = lo_mean(ediff(istart:iend, i)) + buf(1, j) = lo_mean(ediff(istart:iend, i)) + buf(2, j) = lo_mean((ediff(istart:iend, i) - f0)**2) + buf(3, j) = lo_mean((ediff(istart:iend, i) - f0)**3) + + do a=1, 3 + do b=1, 3 + buf_stress(a, b, j) = lo_mean(sdiff(istart:iend, a, b, i)) + end do + end do + end do + ! First order cumulant + cumulant(1, i) = lo_mean(buf(1, :)) + cumulant_var(1, i) = lo_mean((buf(1, :) - cumulant(1, i))**2) + ! Second order cumulant + cumulant(2, i) = lo_mean(buf(2, :)) + cumulant_var(2, i) = lo_mean((buf(2, :) - cumulant(2, i))**2) + ! Third order cumulant + cumulant(3, i) = lo_mean(buf(3, :)) + cumulant_var(3, i) = lo_mean((buf(3, :) - cumulant(3, i))**2) + + ! Same for the stress + if (i .lt. 3) then + do a=1, 3 + do b=1, 3 + stress_pot(a, b, i) = lo_mean(buf_stress(a, b, :)) + stress_potvar(a, b, i) = lo_mean((buf_stress(a, b, :) - stress_pot(a, b, i))**2) + end do + end do + end if + end do + ! We add the prefactor for the cumulants + cumulant = cumulant/real(ss%na, r8) + cumulant(2, :) = 0.5_r8 * cumulant(2, :) * inverse_kbt + cumulant_var(2, :) = 0.5_r8 * cumulant_var(2, :) * inverse_kbt + cumulant_var(3, :) = cumulant_var(3, :) * inverse_kbt**2 / 6.0_r8 + ! And we can store everything + thermo%clt_ifc2_1(1) = cumulant(1, 3) + thermo%clt_ifc2_1(2) = cumulant_var(1, 3) + thermo%clt_ifc2_2(1) = cumulant(2, 3) + thermo%clt_ifc2_2(2) = cumulant_var(2, 3) + thermo%clt_ifc3_1(1) = cumulant(1, 4) + thermo%clt_ifc3_1(2) = cumulant_var(1, 4) + thermo%clt_ifc3_2(1) = cumulant(2, 4) + thermo%clt_ifc3_2(2) = cumulant_var(2, 4) + thermo%clt_ifc4_1(1) = cumulant(1, 5) + thermo%clt_ifc4_1(2) = cumulant_var(1, 5) + thermo%clt_ifc4_2(1) = cumulant(2, 5) + thermo%clt_ifc4_2(2) = cumulant_var(2, 5) + ! Stress included + thermo%stress_pot(:, :) = stress_pot(:, :, 1) + thermo%stress_potvar(:, :) = stress_potvar(:, :, 1) + thermo%stress_diff(:, :) = stress_pot(:, :, 2) + thermo%stress_potvar(:, :) = stress_potvar(:, :, 2) +end subroutine + end module diff --git a/src/anharmonic_free_energy/lo_thermodynamic_helpers.f90 b/src/anharmonic_free_energy/lo_thermodynamic_helpers.f90 new file mode 100644 index 00000000..f19249b3 --- /dev/null +++ b/src/anharmonic_free_energy/lo_thermodynamic_helpers.f90 @@ -0,0 +1,78 @@ +#include "precompilerdefinitions" +module lo_thermodynamic_helpers +use konstanter, only: r8, lo_huge +use type_crystalstructure, only: lo_crystalstructure +use type_symmetryoperation, only: lo_operate_on_secondorder_tensor + +implicit none +private +public :: lo_thermodynamics +public :: lo_symmetrize_stress +public :: lo_full_to_voigt + +!> A container for all thermodynamic results +type lo_thermodynamics + !> The temperature at which everything is evaluated + real(r8) :: temperature=-lo_huge + !> The volume + real(r8) :: volume=-lo_huge + !> The free energies + real(r8) :: f0, f3, f4 + !> The internal energy + real(r8) :: u0, u3, u4 + !> The entropy + real(r8) :: s0, s3, s4 + !> The heat capacity at constant volume + real(r8) :: cv0, cv3, cv4 + !> The heat capacity at constant pressure + real(r8) :: cp0, cp3, cp4 + !> The cumulant contributions + real(r8), dimension(2) :: clt_ifc2_1, clt_ifc2_2 + real(r8), dimension(2) :: clt_ifc3_1, clt_ifc3_2 + real(r8), dimension(2) :: clt_ifc4_1, clt_ifc4_2 + !> The pressure + real(r8) :: p=-lo_huge + !> The stress tensor + real(r8), dimension(3, 3) :: stress_pot, stress_kin, stress_potvar + real(r8), dimension(3, 3) :: stress_3ph, stress_diff, stress_diffvar + !> The thermal expansion + real(r8), dimension(3, 3) :: alpha +end type + +contains +subroutine lo_symmetrize_stress(m, uc) + !> The input matrix + real(r8), dimension(3, 3), intent(inout) :: m + !> The unitcell + type(lo_crystalstructure), intent(in) :: uc + + real(r8), dimension(3, 3) :: tmp + integer :: iop + + tmp = 0.0_r8 + do iop = 1, uc%sym%n + tmp = tmp + lo_operate_on_secondorder_tensor(uc%sym%op(iop), m) + end do + m = tmp / real(uc%sym%n, r8) +end subroutine + +function lo_full_to_voigt(i, j) result(k) + !> Inputs + integer, intent(in) :: i + integer, intent(in) :: j + + integer :: k + + integer, dimension(2) :: d + k = 0 + if (i < j) then + d = [i, j] + else + d = [j, i] + end if + if (d(1) .eq. d(2)) k = d(1) + if (d(1) .eq. 1 .and. d(2) .eq. 2) k = 6 + if (d(1) .eq. 1 .and. d(2) .eq. 3) k = 5 + if (d(1) .eq. 2 .and. d(2) .eq. 3) k = 4 +end function +end module diff --git a/src/anharmonic_free_energy/main.f90 b/src/anharmonic_free_energy/main.f90 index 14258208..f839ac2e 100644 --- a/src/anharmonic_free_energy/main.f90 +++ b/src/anharmonic_free_energy/main.f90 @@ -1,8 +1,9 @@ program anharmonic_free_energy !!{!src/anharmonic_free_energy/manual.md!} -use konstanter, only: r8, lo_Hartree_to_eV, lo_kb_Hartree, lo_pressure_HartreeBohr_to_GPa, lo_tol, lo_status +use konstanter, only: r8, lo_Hartree_to_eV, lo_kb_Hartree, lo_pressure_HartreeBohr_to_GPa, lo_tol, lo_status, lo_freqtol, lo_twopi use gottochblandat, only: open_file, walltime, lo_linspace, lo_progressbar_init, lo_progressbar, tochar, & - lo_does_file_exist, lo_mean, lo_stddev + lo_does_file_exist, lo_mean, lo_stddev, lo_harmonic_oscillator_internal_energy, lo_chop, & + lo_invert_real_matrix, lo_harmonic_oscillator_cv use mpi_wrappers, only: lo_mpi_helper use lo_memtracker, only: lo_mem_helper use lo_timetracker, only: lo_timer @@ -17,10 +18,10 @@ program anharmonic_free_energy use type_phonon_dos, only: lo_phonon_dos use options, only: lo_opts -use thirdorder, only: free_energy_thirdorder +use thirdorder, only: free_energy_thirdorder, elastic_thirdorder use fourthorder, only: free_energy_fourthorder, free_energy_fourthorder_secondorder use epot, only: lo_energy_differences -use thermo, only: lo_thermodynamics +use lo_thermodynamic_helpers, only: lo_thermodynamics, lo_symmetrize_stress, lo_full_to_voigt implicit none @@ -38,7 +39,7 @@ program anharmonic_free_energy real(r8), dimension(3, 3, 5) :: stress_pot, stress_potvar real(r8) :: timer_init, timer_total real(r8) :: U0, U1, energy_unit_factor -logical :: havehighorder +logical :: havehighorder, havesim ! Init MPI, timers and options call mw%init() @@ -56,8 +57,15 @@ program anharmonic_free_energy if (mw%talk) then write(*, *) 'Recap of the parameters governing the calculation' write(*, *) '' + write (*, '(1X,A40,F20.12)') 'Temperature ', opts%temperature + write (*, '(1X,A40,L3)') 'Classical limit ', opts%quantum + write (*, '(1X,A40,I4,I4,I4)') 'Q-point grid Harmonic ', opts%qgrid + write (*, '(1X,A40,I4,I4,I4)') 'Third order q-point grid ', opts%qg3ph + write (*, '(1X,A40,I4,I4,I4)') 'Fourth order q-point grid ', opts%qg4ph + write(*, *) '' end if + if (mw%talk) write(*, *) '... reading input files' ! Read structure call uc%readfromfile('infile.ucposcar', verbosity=opts%verbosity) call uc%classify('wedge', timereversal=.true.) @@ -67,8 +75,14 @@ program anharmonic_free_energy call fc%readfromfile(uc, 'infile.forceconstant', mem, verbosity=-1) if (mw%talk) write (*, *) '... read second order forceconstant' - if (opts%thirdorder) call fct%readfromfile(uc, 'infile.forceconstant_thirdorder') - if (opts%fourthorder) call fcf%readfromfile(uc, 'infile.forceconstant_fourthorder') + if (opts%thirdorder) then + call fct%readfromfile(uc, 'infile.forceconstant_thirdorder') + if (mw%talk) write (*, *) '... read third order forceconstant' + end if + if (opts%fourthorder) then + call fcf%readfromfile(uc, 'infile.forceconstant_fourthorder') + if (mw%talk) write (*, *) '... read fourth order forceconstant' + end if havehighorder = .false. if (opts%thirdorder .or. opts%fourthorder) havehighorder = .true. @@ -111,6 +125,7 @@ program anharmonic_free_energy temperature = opts%temperature + if (mw%talk) write(*, *) '... computing thermodynamic properties with harmonic dispersion' ! We start by computing everything we can from the harmonic phonons if (opts%quantum) then thermo%f0 = dr%phonon_free_energy(temperature) @@ -125,27 +140,25 @@ program anharmonic_free_energy thermo%cv0 = 3.0_r8 * lo_kb_Hartree thermo%stress_kin = 0.0_r8 do i=1, 3 - thermo%stress_kin(i, i) = -lo_kb_Hartree * temperature * uc%na / uc%volume + thermo%stress_kin(i, i) = lo_kb_Hartree * temperature * uc%na / uc%volume end do end if - write(*, *) 'Free energy' - write(*, *) thermo%f0 - write(*, *) 'Entropy' - write(*, *) thermo%s0 - write(*, *) 'Internal energy' - write(*, *) thermo%u0 - write(*, *) '' - - write(*, *) 'Potential stress' - do i=1, 3 - write(*, '(1X,F24.12,1X,F24.12,1X,F24.12)') thermo%stress_pot(i, :) * lo_pressure_HartreeBohr_to_GPa - end do - write(*, *) 'Kinetic stress' - do i=1, 3 - write(*, '(1X,F24.12,1X,F24.12,1X,F24.12)') thermo%stress_kin(i, :) * lo_pressure_HartreeBohr_to_GPa - end do - call tmr%tock('harmonic properties') + ! Usually not needed here, but always a good idea to clean + call lo_symmetrize_stress(thermo%stress_kin, uc) + thermo%stress_kin = lo_chop(thermo%stress_kin, sum(abs(thermo%stress_kin))*1e-6_r8) + ! If we have third order IFC, might as well compute elastic things + if (opts%thirdorder) then + if (mw%talk) write(*, *) '... computing third order contribution to elastic properties' + + call elastic_thirdorder(uc, fc, fct, qp, dr, opts%temperature, thermo%stress_3ph, thermo%alpha, opts%quantum, mw, mem) + ! Now we symmetrize and store everything + call lo_symmetrize_stress(thermo%stress_3ph, uc) + thermo%stress_3ph = lo_chop(thermo%stress_3ph, sum(abs(thermo%stress_3ph))*1e-6_r8) + call lo_symmetrize_stress(thermo%alpha, uc) + thermo%alpha = lo_chop(thermo%alpha, sum(abs(thermo%alpha))*1e-6_r8) + end if + call tmr%tock('harmonic properties') end block latdyn calcepot: block @@ -157,15 +170,17 @@ program anharmonic_free_energy real(r8), dimension(:, :, :), allocatable :: buf_stress real(r8), dimension(:, :), allocatable :: buf real(r8), dimension(:, :), allocatable :: ediff - real(r8), dimension(3, 3) :: s2, s3, s4, sp + real(r8), dimension(3, 3) :: s3, sk2, sk3, sk4, skp real(r8) :: e2, e3, e4, ep, inverse_kbt, f0 integer :: i, j, a, b, blocksize + real(r8) :: stol - if (mw%talk) then - write(*, *) '' - write(*, *) 'Computing energy differences' - end if + if (mw%talk) write(*, *) '' + if (lo_does_file_exist('infile.sim.hdf5') .or. lo_does_file_exist('infile.meta')) then + havesim = .true. + + if (mw%talk) write(*, *) 'Computing energy differences' call ss%readfromfile('infile.ssposcar') call ss%classify('supercell', uc) @@ -178,7 +193,7 @@ program anharmonic_free_energy call sim%read_from_file(verbosity=opts%verbosity + 2, stride=1, magnetic=.false., dielectric=.false., nrand=-1, mw=mw) end if - if (abs(opts%temperature - sim%temperature_thermostat) .gt. lo_tol) then + if (abs(opts%temperature - sim%temperature_thermostat) .gt. lo_tol .and. mw%talk) then write(*, *) write(*, *) 'WARNING: input and simulation temperatures do not match' write(*, '(1X,A24,F24.12)') 'Input temperature', opts%temperature @@ -187,7 +202,6 @@ program anharmonic_free_energy write(*, *) end if - thermo%temperature = sim%temperature_thermostat if (thermo%temperature .gt. 1E-5_r8) then inverse_kbt = 1.0_r8/lo_kb_Hartree/thermo%temperature else @@ -195,93 +209,27 @@ program anharmonic_free_energy end if if (mw%talk) write(*, *) '... computing energy differences' + call pot%compute_realspace_thermo(ss, sim, thermo, opts%nblocks, mw) + + stol = sum(abs(thermo%stress_pot)) * 1e-6_r8 + call lo_symmetrize_stress(thermo%stress_pot, uc) + thermo%stress_pot = lo_chop(thermo%stress_pot, stol) + call lo_symmetrize_stress(thermo%stress_potvar, uc) + thermo%stress_potvar = lo_chop(thermo%stress_potvar, stol) + call lo_symmetrize_stress(thermo%stress_diff, uc) + thermo%stress_diff = lo_chop(thermo%stress_diff, stol) + call lo_symmetrize_stress(thermo%stress_diffvar, uc) + thermo%stress_diffvar = lo_chop(thermo%stress_diffvar, stol) - ! Calculate the baseline energy - allocate (ediff(sim%nt, 5)) - allocate (sdiff(sim%nt, 3, 3, 5)) - ediff = 0.0_r8 - sdiff = 0.0_r8 - - ! First, we compute the energy differences - do i = 1, sim%nt - if (mod(i, mw%n) .ne. mw%r) cycle - call pot%energies_and_forces(sim%u(:, :, i), e2, e3, e4, ep) - ! We store the energy differences - ediff(i, 1) = sim%stat%potential_energy(i) - ediff(i, 2) = sim%stat%potential_energy(i) - e2 - ediff(i, 3) = sim%stat%potential_energy(i) - e2 - ep - ediff(i, 4) = sim%stat%potential_energy(i) - e2 - ep - e3 - ediff(i, 5) = sim%stat%potential_energy(i) - e2 - ep - e3 - e4 - - ! But also the stress - sdiff(i, :, :, 1) = sim%stat%stress(:, :, i) -! sdiff(i, :, :, 2) = sim%stat%stress(:, :, i) - s2 -! sdiff(i, :, :, 2) = sim%stat%stress(:, :, i) - s2 - sp -! sdiff(i, :, :, 2) = sim%stat%stress(:, :, i) - s2 - sp - s3 -! sdiff(i, :, :, 2) = sim%stat%stress(:, :, i) - s2 - sp - s3 - s4 - end do - call mw%allreduce('sum', ediff) - call mw%allreduce('sum', sdiff) - - ! We can now compute all properties, including their errors using block averaging - cumulant = 0.0_r8 - cumulant_var = 0.0_r8 - blocksize = floor(real(sim%nt, r8) / real(opts%nblocks)) - allocate(buf(3, opts%nblocks)) - allocate(buf_stress(3, 3, opts%nblocks)) - do i=1, 5 - ! Here we compute all properties for each blocks - do j=1, opts%nblocks - f0 = lo_mean(ediff(blocksize*j:min(blocksize*j+1, sim%nt), i)) - buf(1, j) = lo_mean(ediff(blocksize*j:min(blocksize*j+1, sim%nt), i)) - buf(2, j) = lo_mean((ediff(blocksize*j:min(blocksize*j+1, sim%nt), i) - f0)**2) - buf(3, j) = lo_mean((ediff(blocksize*j:min(blocksize*j+1, sim%nt), i) - f0)**3) - - do a=1, 3 - do b=1, 3 - buf_stress(a, b, j) = lo_mean(sdiff(i, a, b, blocksize*j:min(blocksize*j+1, sim%nt))) - end do - end do - end do - ! First order cumulant - cumulant(1, i) = lo_mean(buf(1, :)) - cumulant_var(1, i) = lo_mean((buf(1, :) - cumulant(1, i))**2) - ! Second order cumulant - cumulant(2, i) = lo_mean(buf(2, :)) - cumulant_var(2, i) = lo_mean((buf(2, :) - cumulant(2, i))**2) - ! Third order cumulant - cumulant(3, i) = lo_mean(buf(3, :)) - cumulant_var(3, i) = lo_mean((buf(3, :) - cumulant(3, i))**2) - - do a=1, 3 - do b=1, 3 - stress_pot(a, b, i) = lo_mean(buf_stress(a, b, :)) - stress_potvar(a, b, i) = lo_mean((buf_stress(a, b, :) - thermo%stress_pot(a, b))**2) - end do - end do - end do - cumulant = cumulant/real(ss%na, r8) - cumulant(2, :) = 0.5_r8 * cumulant(2, :) * inverse_kbt - cumulant_var(2, :) = 0.5_r8 * cumulant_var(2, :) * inverse_kbt - cumulant_var(3, :) = cumulant_var(3, :) * inverse_kbt**2 / 6.0_r8 - - if (mw%talk) then - write (*, *) '' - write (*, *) 'Temperature (K) (from infile.meta): ', sim%temperature_thermostat - write (*, *) 'Potential energy:' - write (*, "(1X,A,E21.14,1X,A,F21.14)") ' input: ', cumulant(1, 1)*lo_Hartree_to_eV, ' upper bound:', cumulant(2, 1)*lo_Hartree_to_eV - write (*, "(1X,A,E21.14,1X,A,F21.14)") ' E-fc2: ', cumulant(1, 2)*lo_Hartree_to_eV, ' upper bound:', cumulant(2, 2)*lo_Hartree_to_eV - write (*, "(1X,A,E21.14,1X,A,F21.14)") ' E-fc2-polar: ', cumulant(1, 3)*lo_Hartree_to_eV, ' upper bound:', cumulant(2, 3)*lo_Hartree_to_eV - if (opts%thirdorder) then - write (*, "(1X,A,E21.14,1X,A,F21.14)") ' E-fc2-polar-fc3: ', cumulant(1, 4)*lo_Hartree_to_eV, ' upper bound:', cumulant(2, 4)*lo_Hartree_to_eV - end if - if (opts%fourthorder) then - write (*, "(1X,A,E21.14,1X,A,F21.14)") ' E-fc2-polar-fc3-fc4: ', cumulant(1, 5)*lo_Hartree_to_eV, ' upper bound:', cumulant(2, 5)*lo_Hartree_to_eV + else + havesim = .false. + if (mw%talk) then + write(*, *) 'No simulation found, skipping computation of cumulant correction' end if end if - call tmr%tock('cumulants') end block calcepot + latdyn3ph: block !> The phonon dispersion relation type(lo_phonon_dispersions) :: dr @@ -307,11 +255,6 @@ program anharmonic_free_energy thermo%s3 = s3 thermo%u3 = (fe3 + opts%temperature * s3) thermo%cv3 = cv3 - - if (mw%talk) write(*, *) fe3 * lo_Hartree_to_eV - if (mw%talk) write(*, *) thermo%u3 * lo_Hartree_to_eV - if (mw%talk) write(*, *) s3 / lo_kb_Hartree - if (mw%talk) write(*, *) cv3 / lo_kb_Hartree end if call tmr%tock('three-phonon') @@ -342,21 +285,11 @@ program anharmonic_free_energy thermo%u4 = (fe4 + opts%temperature * s4) thermo%cv4 = cv4 - if (mw%talk) write(*, *) fe4 * lo_Hartree_to_eV - if (mw%talk) write(*, *) thermo%u4 * lo_Hartree_to_eV - if (mw%talk) write(*, *) s4 / lo_kb_Hartree - if (mw%talk) write(*, *) cv4 / lo_kb_Hartree - call free_energy_fourthorder_secondorder(uc, fcf, qp, dr, opts%temperature, fe4, s4, cv4, opts%quantum, mw, mem) thermo%f4 = thermo%f4 + fe4 thermo%s4 = thermo%s4 + s4 thermo%u4 = thermo%u4 + (fe4 + opts%temperature * s4) thermo%cv4 = thermo%cv4 + cv4 - - if (mw%talk) write(*, *) fe4 * lo_Hartree_to_eV - if (mw%talk) write(*, *) (fe4 + opts%temperature * s4) * lo_Hartree_to_eV - if (mw%talk) write(*, *) s4 / lo_kb_Hartree - if (mw%talk) write(*, *) cv4 / lo_kb_Hartree end if call tmr%tock('four-phonon') @@ -366,45 +299,6 @@ program anharmonic_free_energy real(r8) :: f0, f1, f2 character(len=1000) :: opf1, opf2 - if (mw%talk) then - write(*, *) '' - write(*, *) 'SUMMARY OF RESULTS' - write(*, *) '' - opf1 = '(1X,3(A20))' - opf2 = '(1X,3(F20.12))' - f0 = (cumulant(1, 2) + thermo%f0) * lo_Hartree_to_eV - f1 = (cumulant(1, 2) + thermo%f0 + thermo%f3) * lo_Hartree_to_eV - f2 = (cumulant(1, 2) + thermo%f0 + thermo%f3 + thermo%f4) * lo_Hartree_to_eV - write(*, *) 'Free energy [eV/at]' - write(*, opf1) 'zeroth order', 'first order', 'second order' - write(*, opf2) f0, f1, f2 - - f0 = (cumulant(1, 2) + thermo%u0) * lo_Hartree_to_eV - f1 = (cumulant(1, 2) + thermo%u0 + thermo%u3) * lo_Hartree_to_eV - f2 = (cumulant(1, 2) + thermo%u0 + thermo%u3 + thermo%u4) * lo_Hartree_to_eV - write(*, *) 'Internal energy [eV/at]' - write(*, opf1) 'zeroth order', 'first order', 'second order' - write(*, opf2) f0, f1, f2 - - f0 = (thermo%s0) / lo_kb_Hartree - f1 = (thermo%s0 + thermo%s3) / lo_kb_Hartree - f2 = (thermo%s0 + thermo%s3 + thermo%s4) / lo_kb_Hartree - write(*, *) 'Entropy [eV/at/K]' - write(*, opf1) 'zeroth order', 'first order', 'second order' - write(*, opf2) f0, f1, f2 - - f0 = (thermo%cv0) / lo_kb_Hartree - f1 = (thermo%cv0 + thermo%cv3) / lo_kb_Hartree - f2 = (thermo%cv0 + thermo%cv3 + thermo%cv4) / lo_kb_Hartree - write(*, *) 'Heat capacity [kb]' - write(*, opf1) 'zeroth order', 'first order', 'second order' - write(*, opf2) f0, f1, f2 - - write (*, *) '' - write (*, '(1X,A)') 'SUGGESTED CITATIONS:' - write (*, '(1X,A41,A)') 'Software: ', 'F. Knoop et al., J. Open Source Softw 9(94), 6150 (2024)' - - end if call tmr%stop() if (mw%talk) write(*, *) '' call tmr%dump(mw, 'Timings:') diff --git a/src/anharmonic_free_energy/thermo.f90 b/src/anharmonic_free_energy/thermo.f90 deleted file mode 100644 index 7bb5493f..00000000 --- a/src/anharmonic_free_energy/thermo.f90 +++ /dev/null @@ -1,31 +0,0 @@ -#include "precompilerdefinitions" -module thermo -use konstanter, only: r8, lo_huge - -implicit none -private -public :: lo_thermodynamics - -type lo_thermodynamics - !> The temperature at which everything is evaluated - real(r8) :: temperature=-lo_huge - !> The volume - real(r8) :: volume=-lo_huge - !> The free energies - real(r8) :: f0, f3, f4 - !> The internal energy - real(r8) :: u0, u3, u4 - !> The entropy - real(r8) :: s0, s3, s4 - !> The heat capacity at constant volume - real(r8) :: cv0, cv3, cv4 - !> The heat capacity at constant pressure - real(r8) :: cp0, cp3, cp4 - !> The pressure - real(r8) :: p=-lo_huge - !> The stress tensor - real(r8), dimension(3, 3) :: stress_pot, stress_kin, stress_potvar - !> The thermal expansion - real(r8) :: alpha -end type -end module diff --git a/src/anharmonic_free_energy/thirdorder.f90 b/src/anharmonic_free_energy/thirdorder.f90 index 55419201..e7fc65c5 100644 --- a/src/anharmonic_free_energy/thirdorder.f90 +++ b/src/anharmonic_free_energy/thirdorder.f90 @@ -2,21 +2,137 @@ module thirdorder !! Compute the third order contribution to the anharmonic free energy use konstanter, only: r8, lo_freqtol, lo_twopi, lo_imag, lo_kb_Hartree, lo_exitcode_param use gottochblandat, only: walltime, lo_trueNtimes, lo_progressbar_init, lo_progressbar, lo_planck, & - lo_planck_deriv, lo_planck_secondderiv + lo_planck_deriv, lo_planck_secondderiv, lo_invert_real_matrix, & + lo_harmonic_oscillator_cv, lo_harmonic_oscillator_internal_energy use mpi_wrappers, only: lo_mpi_helper, lo_stop_gracefully use lo_memtracker, only: lo_mem_helper use type_qpointmesh, only: lo_qpoint_mesh, lo_fft_mesh use type_crystalstructure, only: lo_crystalstructure +use type_forceconstant_secondorder, only: lo_forceconstant_secondorder use type_forceconstant_thirdorder, only: lo_forceconstant_thirdorder use type_phonon_dispersions, only: lo_phonon_dispersions use lo_timetracker, only: lo_timer +use lo_thermodynamic_helpers, only: lo_full_to_voigt + implicit none private +public :: elastic_thirdorder public :: free_energy_thirdorder contains +subroutine elastic_thirdorder(uc, fc, fct, qp, dr, temperature, p3ph, alpha, quantum, mw, mem) + !> crystal structure + type(lo_crystalstructure), intent(in) :: uc + !> second order force constants + type(lo_forceconstant_secondorder), intent(inout) :: fc + !> third order force constant + type(lo_forceconstant_thirdorder), intent(in) :: fct + !> q-point mesh + class(lo_qpoint_mesh), intent(in) :: qp + !> dispersions + type(lo_phonon_dispersions), intent(in) :: dr + !> temperature + real(r8), intent(in) :: temperature + !> free energies and heat capacity + real(r8), dimension(3, 3), intent(out) :: p3ph, alpha + !> what to compute + logical, intent(in) :: quantum + !> mpi helper + type(lo_mpi_helper), intent(inout) :: mw + !> memory tracker + type(lo_mem_helper), intent(inout) :: mem + + complex(r8), dimension(:), allocatable :: egv + complex(r8), dimension(3, 3) :: c0 + real(r8), dimension(6, 6) :: cij, sij + real(r8), dimension(3, 3) :: grun, buf + real(r8), dimension(3) :: qv, rv2, rv3 + real(r8), dimension(2) :: d + complex(r8) :: expiqr, evprod + real(r8) :: om, iqr, invsqrtmass, u0, cv0 + integer :: q1, b1, a1, t, a2, a3, i, j, k, l, ivoigt, jvoigt, ctr + + allocate(egv(dr%n_mode)) + + p3ph = 0.0_r8 + buf = 0.0_r8 + + ctr = 0 + do q1=1, qp%n_full_point + qv = qp%ap(q1)%r * lo_twopi + do b1=1, dr%n_mode + ctr = ctr + 1 + if (mod(ctr, mw%n) .ne. mw%r) cycle + om = dr%aq(q1)%omega(b1) + if (om .lt. lo_freqtol) cycle + c0 = 0.0_r8 + egv = dr%aq(q1)%egv(:, b1) + do a1=1, fct%na + do t=1, fct%atom(a1)%n + a2 = fct%atom(a1)%triplet(t)%i2 + a3 = fct%atom(a1)%triplet(t)%i3 + rv2 = fct%atom(a1)%triplet(t)%lv2 + rv3 = fct%atom(a1)%triplet(t)%rv3 + invsqrtmass = uc%invsqrtmass(a1) * uc%invsqrtmass(a2) + iqr = -dot_product(qv, rv2) + expiqr = cmplx(cos(iqr), sin(iqr), r8) + do i=1, 3 + do j=1, 3 + evprod = conjg(egv((a1-1) * 3 + i)) * egv((a2-1) * 3 + j) * expiqr + do k=1, 3 + do l=1, 3 + c0(k, l) = c0(k, l) + fct%atom(a1)%triplet(t)%m(i, j, k) * evprod * rv3(l) * invsqrtmass + end do + end do + end do + end do + end do + end do + grun = -real(c0, r8) / (6.0_r8 * om**2) + + ! Now we can accumulate things using the Gruneisen parameter + if (quantum) then + u0 = lo_harmonic_oscillator_internal_energy(temperature, om) + cv0 = lo_harmonic_oscillator_cv(temperature, om) + else + u0 = lo_kb_Hartree * temperature + cv0 = lo_kb_Hartree + end if + + p3ph(:, :) = p3ph(:, :) - grun(:, :) * u0 * qp%ap(q1)%integration_weight / uc%volume + do i=1, 3 + do j=1, 3 + buf(i, j) = buf(i, j) + cv0 * grun(i, j) * qp%ap(q1)%integration_weight + end do + end do + + end do + end do + call mw%allreduce('sum', p3ph) + call mw%allreduce('sum', buf) + + call fc%get_elastic_constants(uc, mw, -1) + cij = fc%elastic_constants_voigt + fc%elastic_constants_voigt_longrange + call lo_invert_real_matrix(cij, sij) + + alpha = 0.0_r8 + do i=1, 3 + do j=1, 3 + do k=1, 3 + do l=1, 3 + ivoigt = lo_full_to_voigt(i, j) + jvoigt = lo_full_to_voigt(k, l) + + alpha(i, j) = alpha(i, j) + sij(ivoigt, jvoigt) * buf(k, l) / uc%volume + end do + end do + end do + end do +end subroutine + + !> Calculate the third order free energy subroutine free_energy_thirdorder(uc, fct, qp, dr, temperature, fe3, s3, cv3, quantum, mw, mem) !> crystal structure @@ -126,12 +242,15 @@ subroutine free_energy_thirdorder(uc, fct, qp, dr, temperature, fe3, s3, cv3, qu ddn2 = lo_planck_secondderiv(temperature, om1) ddn3 = lo_planck_secondderiv(temperature, om1) + ! This are the formula to get the free energy f1 = (n1 + 1.0_r8)*(n2 + n3 + 1.0_r8) + n2*n3 f2 = n1*n2 + n1*n3 - n2*n3 + 1.0_r8 + ! Here is for the entropy df1 = dn1 * (n2 + n3 + 1.0_r8) + (n1 + 1.0_r8) * (dn2 + dn3) + dn2 * n3 + n2 * dn3 df2 = dn1 * n2 + n1 * dn2 + dn1 * n3 + n1 * dn3 - dn2 * n3 - n2 * dn3 + ! And the heat capacity ddf1 = ddn1 * (n2 + n3 + 1.0_r8) + 2.0_r8 * dn1 * (dn2 + dn3) + (n1 + 1.0_r8) * (ddn2 + ddn3) + & ddn2 * n3 + n2 * ddn3 + 2.0_r8 * dn2 * dn3 ddf2 = ddn1 * n2 + n1 * ddn2 + 2.0_r8 * dn1 * dn2 + ddn1 * n3 + n1 * ddn3 + 2.0_r8 * dn1 * dn3 - & diff --git a/src/libolle/type_phonon_dispersions.f90 b/src/libolle/type_phonon_dispersions.f90 index 0bf5e957..d22d99c8 100644 --- a/src/libolle/type_phonon_dispersions.f90 +++ b/src/libolle/type_phonon_dispersions.f90 @@ -1162,7 +1162,7 @@ subroutine phonon_kinetic_stress(dr, qp, uc, temperature, kinsigma) f0 = om * (lo_planck(temperature, om) + 0.5_r8) * pref do a=1, uc%na egv = dr%aq(aq)%egv((a - 1)*3 + 1:a*3, im) - kinsigma(:, :) = kinsigma(:, :) - real(lo_outerproduct(egv, egv)) * f0 + kinsigma(:, :) = kinsigma(:, :) + real(lo_outerproduct(egv, egv)) * f0 end do end do end do From ac42a62206798b3f23a0b1c6215679bb54670e20 Mon Sep 17 00:00:00 2001 From: =?UTF-8?q?Alo=C3=AFs=20Castellano?= Date: Fri, 14 Feb 2025 10:17:16 +0100 Subject: [PATCH 03/28] Small correction for cumulants and added some printing of results --- src/anharmonic_free_energy/energy_aux.f90 | 553 ---------------------- src/anharmonic_free_energy/energy_dos.f90 | 173 ------- src/anharmonic_free_energy/epot.f90 | 23 +- src/anharmonic_free_energy/main.f90 | 170 +++++-- 4 files changed, 151 insertions(+), 768 deletions(-) delete mode 100644 src/anharmonic_free_energy/energy_aux.f90 delete mode 100644 src/anharmonic_free_energy/energy_dos.f90 diff --git a/src/anharmonic_free_energy/energy_aux.f90 b/src/anharmonic_free_energy/energy_aux.f90 deleted file mode 100644 index 8cfc2ae7..00000000 --- a/src/anharmonic_free_energy/energy_aux.f90 +++ /dev/null @@ -1,553 +0,0 @@ - -! !> Get the spectral anharmonic free energy -! subroutine spectral_free_energy(qp,dr,uc,F3,F4,npts,unitfactor,mw) -! !> qpoint mesh -! class(lo_qpoint_mesh), intent(inout) :: qp -! !> phonon dispersions -! type(lo_phonon_dispersions), intent(in) :: dr -! !> crystal structure -! type(lo_crystalstructure), intent(in) :: uc -! !> anharmonic free energy -! real(r8), dimension(:,:), intent(in) :: F3,F4 -! !> number of points on the x-axis -! integer, intent(in) :: npts -! !> output units -! real(r8), intent(in) :: unitfactor -! !> MPI helper -! type(lo_mpi_helper), intent(in) :: mw -! -! ! -! complex(r8), dimension(3) :: v0 -! real(r8), dimension(:,:,:), allocatable :: tetvals,tetF3,tetF4,buf3,buf4,buf3b,buf4b,tetsiteproj -! real(r8), dimension(:,:), allocatable :: yp3,yp4 -! real(r8), dimension(:), allocatable :: x,yt3,yt4 -! real(r8), dimension(4) :: tete,tv3,tv4,w1,w2 -! real(r8), dimension(9) :: kernel -! real(r8), dimension(uc%na) :: tetpr -! real(r8) :: invf,sigma,deltae,t0,ftot3,ftot4,f0,f1,f2,nf3,nf4 -! integer :: q,t,i,j,k,l,ii,jj,li,u -! character(len=1000) :: opf -! -! ! Distribute q-points and tetrahedrons over MPI -! t0=walltime() -! !if ( qp%mpi%initialized .eqv. .false. ) call qp%divide_across_mpi(mw%comm) -! ! Prefetch things for tetrahedrons. -! lo_allocate(tetsiteproj(uc%na,dr%n_mode,qp%mpi%ntet)) -! lo_allocate(tetvals(4,dr%n_mode,qp%mpi%ntet)) -! lo_allocate(tetF3(4,dr%n_mode,qp%mpi%ntet)) -! lo_allocate(tetF4(4,dr%n_mode,qp%mpi%ntet)) -! tetvals=0.0_r8 -! tetsiteproj=0.0_r8 -! tetF3=0.0_r8 -! tetF4=0.0_r8 -! do li=1,qp%mpi%ntet -! i=qp%mpi%tet(li) -! do j=1,4 -! ! energies -! l=qp%tet(i)%irrind(j) -! do k=1,dr%n_mode -! tetvals(j,k,li)=dr%iq(l)%omega(k) -! tetF3(j,k,li)=F3(k,l) -! tetF4(j,k,li)=F4(k,l) -! enddo -! ! projections -! do ii=1,uc%na -! do jj=1,dr%n_mode -! v0=dr%iq(l)%egv((ii-1)*3+1:ii*3,jj) -! tetsiteproj(ii,jj,li)=tetsiteproj(ii,jj,li)+abs(dot_product(v0,v0))*0.25_r8 -! enddo -! enddo -! enddo -! enddo -! -! ! Calculate it by energy, mode, site. Make some space -! lo_allocate(buf3(uc%na,npts,dr%n_mode)) -! lo_allocate(buf4(uc%na,npts,dr%n_mode)) -! buf3=0.0_r8 -! buf4=0.0_r8 -! ! Get the x-axis -! lo_allocate(x(npts)) -! call lo_linspace(0.0_r8,dr%omega_max*1.1_r8,x) -! invf=npts/x(npts) -! sigma=dr%default_smearing() -! deltae=(x(2)-x(1))*0.25_r8 -! -! ! Now do the actual integration -! if ( mw%talk ) call lo_progressbar_init() -! do li=1,qp%mpi%ntet -! i=qp%mpi%tet(li) -! do k=1,dr%n_mode -! ! prefetch some stuff -! tete=tetvals(:,k,li) -! tv3=tetF3(:,k,li) -! tv4=tetF4(:,k,li) -! tetpr=tetsiteproj(:,k,li) -! ii=max(floor( (minval(tete)-2*deltae)*invf ),1) -! jj=min(ceiling( (maxval(tete)+2*deltae)*invf ),npts) -! ! Add it up -! do l=ii,jj -! call lo_integration_weights_for_one_tetrahedron(qp%tet(i),tete,x(l)-deltae,w1,sigma,blochlcorrections=.false.) -! call lo_integration_weights_for_one_tetrahedron(qp%tet(i),tete,x(l)+deltae,w2,sigma,blochlcorrections=.false.) -! buf3(:,l,k)=buf3(:,l,k)+tetpr*(sum( (w1+w2)*tv3 ))*0.5_r8 -! buf4(:,l,k)=buf4(:,l,k)+tetpr*(sum( (w1+w2)*tv4 ))*0.5_r8 -! enddo -! enddo -! if ( mw%talk ) then -! if ( lo_trueNtimes(li,60,qp%mpi%ntet) ) call lo_progressbar(' ... spectral free energy',li,qp%mpi%ntet) -! endif -! enddo -! ! Sum it ip -! lo_allocate(buf3b(uc%na,npts,dr%n_mode)) -! lo_allocate(buf4b(uc%na,npts,dr%n_mode)) -! buf3b=0.0_r8 -! buf4b=0.0_r8 -! call mpi_allreduce(buf3,buf3b,uc%na*dr%n_mode*npts,MPI_DOUBLE_PRECISION,MPI_SUM,mw%comm,mw%error) -! call mpi_allreduce(buf4,buf4b,uc%na*dr%n_mode*npts,MPI_DOUBLE_PRECISION,MPI_SUM,mw%comm,mw%error) -! -! if ( mw%talk ) then -! call lo_progressbar(' ... spectral free energy',li,qp%mpi%ntet,walltime()-t0) -! endif -! -! ! Scale to reasonable units -! x=x*unitfactor -! buf3b=buf3b/unitfactor -! buf4b=buf4b/unitfactor -! ! Normalize things properly. First calculate the total contribution. -! ftot3=0.0_r8 -! ftot4=0.0_r8 -! l=0 -! do i=1,qp%n_irr_point -! do j=1,dr%n_mode -! l=l+1 -! ftot3=ftot3+qp%ip(i)%weight*F3(j,i) -! ftot4=ftot4+F4(j,i)*qp%ip(i)%weight/uc%na -! enddo -! enddo -! ! Sum up the spectral to a total. -! lo_allocate(yt3(npts)) -! lo_allocate(yt4(npts)) -! yt3=0.0_r8 -! yt4=0.0_r8 -! do j=1,dr%n_mode -! do i=1,uc%na -! yt3=yt3+buf3b(i,:,j) -! yt4=yt4+buf4b(i,:,j) -! enddo -! enddo -! nf3=ftot3/lo_trapezoid_integration(x,yt3) -! nf4=ftot4/lo_trapezoid_integration(x,yt4) -! yt3=yt3*nf3 -! yt4=yt4*nf4 -! ! Now construct the site-projected -! lo_allocate(yp3(npts,uc%na)) -! lo_allocate(yp4(npts,uc%na)) -! yp3=0.0_r8 -! yp4=0.0_r8 -! do j=1,dr%n_mode -! do i=1,uc%na -! yp3(:,i)=yp3(:,i)+buf3b(i,:,j) -! yp4(:,i)=yp4(:,i)+buf4b(i,:,j) -! enddo -! enddo -! ! Make sure the site-projected add up to the total -! do i=1,npts -! f0=abs(sum(yp3(i,:))) -! if ( f0 .gt. 1E-30_r8 ) then -! yp3(i,:)=yp3(i,:)*abs(yt3(i))/f0 -! else -! yp3(i,:)=0.0_r8 -! endif -! f0=abs(sum(yp4(i,:))) -! if ( f0 .gt. 1E-30_r8 ) then -! yp4(i,:)=yp4(i,:)*yt4(i)/f0 -! else -! yp4(i,:)=0.0_r8 -! endif -! enddo -! -! ! Dump to file -! if ( mw%talk ) then -! ! output format -! u=open_file('out','dumspf') -! opf="("//tochar(uc%na*2+3)//"(2X,E18.12))" -! do i=1,npts -! write(u,opf) x(i),yt3(i),yt4(i),yp3(i,:),yp4(i,:) -! enddo -! close(u) -! endif -! -! end subroutine - -! !> Calculate all scattering rates, MPI-distributed -! subroutine getscatteringrates(sr,qpoint,ompoint,qp,dr,uc,fc,fct,fcf,verbosity,mw) -! !> scattering rates -! class(lo_listofscatteringrates), intent(out) :: sr -! !> q-point in question -! type(lo_qpoint) :: qpoint -! !> harmonic properties -! type(lo_phonon_dispersions_qpoint), intent(in) :: ompoint -! !> qpoint mesh -! class(lo_qpoint_mesh), intent(in) :: qp -! !> phonon dispersions -! type(lo_phonon_dispersions), intent(in) :: dr -! !> crystal structure -! type(lo_crystalstructure), intent(in) :: uc -! !> second order forceconstant -! type(lo_forceconstant_secondorder), intent(inout) :: fc -! !> third order force constant -! type(lo_forceconstant_thirdorder), intent(in) :: fct -! !> fourth order force constants -! type(lo_forceconstant_fourthorder), intent(in) :: fcf -! !> how much to talk -! integer, intent(in) :: verbosity -! !> MPI communicator -! type(lo_mpi_helper), intent(in) :: mw -! -! ! Just keep a list of q3, temporarily -! type(lo_qpoint) :: qpgamma -! type(lo_phonon_dispersions_qpoint) :: ompgamma -! real(r8), dimension(:,:), allocatable :: qvec3 -! complex(r8), dimension(:,:,:), allocatable :: egv3 -! -! ! First get the third frequency at all q-points -! thirdfreq: block -! type(lo_qpoint) :: dq3 -! type(lo_phonon_dispersions_qpoint) :: ompoint -! complex(r8), dimension(:,:,:), allocatable :: egv3buf -! complex(r8), dimension(:,:,:), allocatable :: Dq -! complex(r8), dimension(:,:), allocatable :: D -! real(r8), dimension(:,:), allocatable :: om3buf,qv3buf -! real(r8), dimension(:,:,:), allocatable :: vel3buf -! real(r8), dimension(3) :: qv1,qv2,qv3 -! real(r8) :: t0 -! integer :: lq,q,b1,b2,l -! -! ! Gamma-point things -! qpgamma%r=0.0_r8 -! qpgamma%r=0.0_r8 -! call lo_get_small_group_of_qpoint(qpgamma,uc) -! lo_allocate(ompgamma%omega(dr%n_mode)) -! lo_allocate(ompgamma%vel(3,dr%n_mode)) -! lo_allocate(ompgamma%egv(dr%n_mode,dr%n_mode)) -! lo_allocate(ompgamma%degeneracy(dr%n_mode)) -! lo_allocate(ompgamma%degenmode(dr%n_mode,dr%n_mode)) -! write(*,*) 'fixme generate thingy' -! !call ompgamma%generate(fc,uc,qpgamma) -! -! lo_allocate(sr%omega_gamma(dr%n_mode)) -! sr%omega_gamma=ompgamma%omega -! -! t0=walltime() -! lo_allocate(om3buf(dr%n_mode,qp%n_full_point)) -! lo_allocate(vel3buf(3,dr%n_mode,qp%n_full_point)) -! lo_allocate(egv3buf(dr%n_mode,dr%n_mode,qp%n_full_point)) -! lo_allocate(qv3buf(3,qp%n_full_point)) -! qv3buf=0.0_r8 -! om3buf=0.0_r8 -! vel3buf=0.0_r8 -! egv3buf=0.0_r8 -! lo_allocate(Dq(dr%n_mode,dr%n_mode,3)) -! lo_allocate(D(dr%n_mode,dr%n_mode)) -! ! Calculate all the frequencies and stuff for the third q-point -! write(*,*) 'FIXME MPI' -! ! do lq=1,qp%mpi%nqtot -! ! q=qp%mpi%qtot(lq) -! ! -! ! ! Get the q-vectors -! ! qv1=qpoint%r -! ! qv2=qp%ap(q)%r -! ! qv3=-qv1-qv2 -! ! ! Frequencies and stuff at the third point -! ! dq3%r=qv3 -! ! dq3%r=dq3%r-uc%bz%gshift(dq3%r) -! ! ! store third q-point for later -! ! qv3buf(:,q)=dq3%r -! ! ! get phonon frequencies -! ! call lo_get_small_group_of_qpoint(dq3,uc) -! ! call fc%dynamicalmatrix(uc,dq3,D,Dq) -! ! call fc%frequencies_eigenvectors_groupvelocities(uc,D,Dq,om3buf(:,q),egv3buf(:,:,q),vel3buf(:,:,q),dq3) -! ! enddo -! ! Communicate this to all ranks -! lo_allocate(sr%omega3(dr%n_mode,qp%n_full_point)) -! lo_allocate(sr%vel3(3,dr%n_mode,qp%n_full_point)) -! lo_allocate(egv3(dr%n_mode,dr%n_mode,qp%n_full_point)) -! lo_allocate(qvec3(3,qp%n_full_point)) -! sr%omega3=0.0_r8 -! sr%vel3=0.0_r8 -! egv3=0.0_r8 -! qvec3=0.0_r8 -! call mpi_allreduce(om3buf,sr%omega3,dr%n_mode*qp%n_full_point,MPI_DOUBLE_PRECISION,MPI_SUM,mw%comm,mw%error) -! call mpi_allreduce(vel3buf,sr%vel3,3*dr%n_mode*qp%n_full_point,MPI_DOUBLE_PRECISION,MPI_SUM,mw%comm,mw%error) -! call mpi_allreduce(egv3buf,egv3,dr%n_mode*dr%n_mode*qp%n_full_point,MPI_DOUBLE_COMPLEX,MPI_SUM,mw%comm,mw%error) -! call mpi_allreduce(qv3buf,qvec3,3*qp%n_full_point,MPI_DOUBLE_PRECISION,MPI_SUM,mw%comm,mw%error) -! if ( verbosity .gt. 0 ) then -! write(*,*) '' -! write(*,*) "... got q'' frequencies in ",tochar(walltime()-t0),'s' -! endif -! ! cleanup -! lo_deallocate(om3buf) -! lo_deallocate(vel3buf) -! lo_deallocate(egv3buf) -! lo_deallocate(qv3buf) -! lo_deallocate(Dq) -! lo_deallocate(D) -! end block thirdfreq -! -! !> get the threephonon matrix elements -! threephsc: block -! complex(r8), dimension(:,:), allocatable :: egv -! complex(r8) :: c0 -! real(r8), dimension(:,:,:,:), allocatable :: psibuf,dblbuf -! real(r8), dimension(3) :: qv1,qv2,qv3,omega -! real(r8) :: t0,f0 -! integer :: q,b1,b2,b3,l,k,ii,jj,kk,bb1,bb2,bb3,n1,n2,n3 -! logical, dimension(:,:,:), allocatable :: fixdeg -! -! lo_allocate(psibuf(dr%n_mode,dr%n_mode,dr%n_mode,qp%n_full_point)) -! lo_allocate(dblbuf(dr%n_mode,dr%n_mode,dr%n_mode,qp%n_full_point)) -! lo_allocate(egv(dr%n_mode,3)) -! psibuf=0.0_r8 -! dblbuf=0.0_r8 -! egv=0.0_r8 -! -! t0=walltime() -! if ( verbosity .gt. 0 ) call lo_progressbar_init() -! l=0 -! k=0 -! -! do q=1,qp%n_full_point -! qv1=-qpoint%r*lo_twopi -! qv2=-qp%ap(q)%r*lo_twopi -! qv3=-qvec3(:,q)*lo_twopi -! do b1=1,dr%n_mode -! do b2=1,dr%n_mode -! do b3=1,dr%n_mode -! ! MPI division -! l=l+1 -! if ( mod(l,mw%n) .ne. mw%r ) cycle -! omega(1)=ompoint%omega(b1) -! omega(2)=dr%aq(q)%omega(b2) -! omega(3)=sr%omega3(b3,q) -! ! prefetch eigenvectors -! egv(:,1)=ompoint%egv(:,b1) -! egv(:,2)=dr%aq(q)%egv(:,b2) -! egv(:,3)=egv3(:,b3,q) -! ! To finally get the scattering rates -! if ( minval(omega) .gt. dr%omega_min*0.5_r8 ) then -! c0=fct%scatteringamplitude(omega,egv,qv2,qv3) -! psibuf(b1,b2,b3,q)=abs(conjg(c0)*c0) -! else -! psibuf(b1,b2,b3,q)=0.0_r8 -! endif -! ! And perhaps the double scattering rate thingy -! if ( ompgamma%omega(b3) .gt. dr%omega_min*0.5_r8 ) then -! ! b3 needs to be an optical mode -! omega(3)=ompgamma%omega(b3) -! egv(:,3)=ompgamma%egv(:,b3) -! ! And the weird double scatteringrates -! dblbuf(b1,b2,b3,q)=0.0_r8 !real(double_scatteringamplitude(fct,omega,egv,qv1,qv2)) -! else -! dblbuf(b1,b2,b3,q)=0.0_r8 -! endif -! enddo -! enddo -! if ( verbosity .gt. 0 ) then -! k=k+1 -! if ( lo_trueNtimes(k,127,qp%n_full_point*dr%n_mode) ) call lo_progressbar(' ... threephonon matrixelements',k,qp%n_full_point*dr%n_mode) -! endif -! enddo -! enddo -! lo_allocate(sr%psi_3ph_sq(dr%n_mode,dr%n_mode,dr%n_mode,qp%n_full_point)) -! lo_allocate(sr%psi_3ph_db(dr%n_mode,dr%n_mode,dr%n_mode,qp%n_full_point)) -! sr%psi_3ph_sq=0.0_r8 -! sr%psi_3ph_db=0.0_r8 -! ! sum it up -! call mpi_allreduce(psibuf,sr%psi_3ph_sq,dr%n_mode*dr%n_mode*dr%n_mode*qp%n_full_point,MPI_DOUBLE_PRECISION,MPI_SUM,mw%comm,mw%error) -! call mpi_allreduce(dblbuf,sr%psi_3ph_db,dr%n_mode*dr%n_mode*dr%n_mode*qp%n_full_point,MPI_DOUBLE_PRECISION,MPI_SUM,mw%comm,mw%error) -! if ( verbosity .gt. 0 ) call lo_progressbar(' ... threephonon matrixelements',qp%n_full_point*dr%n_mode,qp%n_full_point*dr%n_mode,walltime()-t0) -! end block threephsc -! -! ! And the four-phonon scattering elements -! fourphsc: block -! complex(r8), dimension(:,:), allocatable :: dumegv1,dumegv2,dumegv3,dumegv4,egv -! complex(r8) :: c0 -! real(r8), dimension(:,:,:), allocatable :: psibuf -! real(r8), dimension(:), allocatable :: dumom1,dumom2,dumom3,dumom4 -! real(r8), dimension(4) :: omega -! real(r8), dimension(3) :: qv1,qv2,qv3,qv4 -! real(r8) :: omegathres,t0 -! integer :: b1,b2,b3,b4,q1,ctr -! -! t0=walltime() -! lo_allocate(psibuf(dr%n_mode,dr%n_mode,qp%n_full_point)) -! psibuf=0.0_r8 -! ! For the other q-points -! lo_allocate(dumom1(dr%n_mode)) -! lo_allocate(dumom2(dr%n_mode)) -! lo_allocate(dumom3(dr%n_mode)) -! lo_allocate(dumom4(dr%n_mode)) -! lo_allocate(dumegv1(dr%n_mode,dr%n_mode)) -! lo_allocate(dumegv2(dr%n_mode,dr%n_mode)) -! lo_allocate(dumegv3(dr%n_mode,dr%n_mode)) -! lo_allocate(dumegv4(dr%n_mode,dr%n_mode)) -! lo_allocate(egv(dr%n_mode,4)) -! dumom1=0.0_r8 -! dumom2=0.0_r8 -! dumom3=0.0_r8 -! dumom4=0.0_r8 -! dumegv1=0.0_r8 -! dumegv2=0.0_r8 -! dumegv3=0.0_r8 -! dumegv4=0.0_r8 -! omegathres=dr%omega_min*0.5_r8 -! ctr=0 -! if ( verbosity .gt. 0 ) call lo_progressbar_init() -! do q1=1,qp%n_full_point -! dumom1=ompoint%omega -! dumom2=ompoint%omega -! dumom3=dr%aq(q1)%omega -! dumom4=dr%aq(q1)%omega -! dumegv1=ompoint%egv -! dumegv2=conjg(ompoint%egv) -! dumegv3=dr%aq(q1)%egv -! dumegv4=conjg(dr%aq(q1)%egv) -! qv1=qpoint%r*lo_twopi -! qv2=-qpoint%r*lo_twopi -! qv3=qp%ap(q1)%r*lo_twopi -! qv4=-qp%ap(q1)%r*lo_twopi -! do b1=1,dr%n_mode -! b2=b1 -! ! mpit thingy -! ctr=ctr+1 -! if ( mod(ctr,mw%n) .ne. mw%r ) cycle -! do b3=1,dr%n_mode -! b4=b3 -! omega=[dumom1(b1),dumom2(b2),dumom3(b3),dumom4(b4)] -! egv(:,1)=dumegv1(:,b1) -! egv(:,2)=dumegv2(:,b2) -! egv(:,3)=dumegv3(:,b3) -! egv(:,4)=dumegv4(:,b4) -! if ( minval(omega) .gt. omegathres ) then -! c0=fcf%scatteringamplitude(omega,egv,qv2,qv3,qv4) -! else -! c0=0.0_r8 -! endif -! psibuf(b1,b3,q1)=real(c0) -! enddo -! ! -! if ( verbosity .gt. 0 ) then -! if ( lo_trueNtimes(ctr,127,qp%n_full_point*dr%n_mode) ) call lo_progressbar(' ... fourphonon matrixelements',ctr,qp%n_full_point*dr%n_mode) -! endif -! enddo -! enddo -! lo_allocate(sr%psi_4ph(dr%n_mode,dr%n_mode,qp%n_full_point)) -! sr%psi_4ph=0.0_r8 -! call mpi_allreduce(psibuf,sr%psi_4ph,dr%n_mode*dr%n_mode*qp%n_full_point,MPI_DOUBLE_PRECISION,MPI_SUM,mw%comm,mw%error) -! if ( verbosity .gt. 0 ) call lo_progressbar(' ... fourphonon matrixelements',qp%n_full_point*dr%n_mode,qp%n_full_point*dr%n_mode,walltime()-t0) -! end block fourphsc -! -! end subroutine - -! !> harmonic properties at specific q-vector -! subroutine harmonic_things_at_single_q(q,uc,fc,loto,ompoint) -! !> Cartesian coordinates of the q-point in question -! real(r8), dimension(3), intent(in) :: q -! !> crystal structure -! type(lo_crystalstructure), intent(in) :: uc -! !> second order force constant -! type(lo_forceconstant_secondorder), intent(in) :: fc -! !> electrostatic corrections -! type(lo_loto), intent(in) :: loto -! !> harmonic properties at this q-point -! type(lo_phonon_dispersions_qpoint), intent(out) :: ompoint -! -! type(lo_qpoint) :: qpoint -! complex(r8), dimension(:,:,:), allocatable :: Dq -! complex(r8), dimension(:,:), allocatable :: D -! integer :: nb -! ! -! nb=uc%na*3 -! qpoint%v=q -! qpoint%w=qpoint%v-uc%bz%gshift(q+lo_degenvector) -! call lo_get_small_group_of_qpoint(qpoint,uc) -! lo_allocate(ompoint%omega(nb)) -! lo_allocate(ompoint%vel(3,nb)) -! lo_allocate(ompoint%egv(nb,nb)) -! lo_allocate(D(nb,nb)) -! lo_allocate(Dq(3,nb,nb)) -! call lo_get_dynamical_matrix(fc,uc,qpoint,loto,D,Dq) -! call lo_get_omega_and_velocities(D,Dq,uc,ompoint%omega,ompoint%egv,ompoint%vel,qpoint=qpoint) -! lo_deallocate(D) -! lo_deallocate(Dq) -! end subroutine - -! !> The three-phonon matrix element, but product of two complex thingies -! pure complex(r8) function double_scatteringamplitude(fc,omega,egv,q1,q2) -! !> the third order force constant -! class(lo_forceconstant_thirdorder), intent(in) :: fc -! !> the frequencies in question -! real(r8), dimension(3), intent(in) :: omega -! !> the eigenvectors -! complex(r8), dimension(:,:), intent(in) :: egv -! !> the two q-vectors that matter -! real(r8), dimension(3), intent(in) :: q1,q2 -! ! -! integer :: atom1,atom2,atom3,i,j,k,k1,k2,k3,t -! complex(r8) :: expiqr,c0,c1 -! real(r8), dimension(3) :: rv2,rv3 -! real(r8) :: iqr,omegaprod1,omegaprod2,enhet -! ! -! complex(r8), dimension(:,:,:,:,:,:), allocatable :: egvprod1,egvprod2 -! ! -! ! Not enough room on the stack for large unitcells, have to allocate space -! allocate(egvprod1(3,3,3,fc%na,fc%na,fc%na)) -! allocate(egvprod2(3,3,3,fc%na,fc%na,fc%na)) -! ! Eigenvector product -! do atom3=1,fc%na -! do atom2=1,fc%na -! do atom1=1,fc%na -! do k=1,3 -! do j=1,3 -! do i=1,3 -! k1=(atom1-1)*3+i -! k2=(atom2-1)*3+j -! k3=(atom3-1)*3+k -! egvprod1(i,j,k,atom1,atom2,atom3)=egv(k1,1)*conjg(egv(k2,1))*egv(k3,3) -! egvprod2(i,j,k,atom1,atom2,atom3)=egv(k1,2)*conjg(egv(k2,2))*conjg(egv(k3,3)) -! enddo -! enddo -! enddo -! enddo -! enddo -! enddo -! ! Frequency product -! omegaprod1=omega(1)*omega(1)*omega(3) -! omegaprod2=omega(2)*omega(2)*omega(3) -! omegaprod1=sqrt(omegaprod1) -! omegaprod2=sqrt(omegaprod2) -! ! The actual matrix element -! c0=0.0_r8 -! c1=0.0_r8 -! do atom1=1,fc%na -! do t=1,fc%atom(atom1)%n -! atom2=fc%atom(atom1)%triplet(t)%i2 -! atom3=fc%atom(atom1)%triplet(t)%i3 -! rv2=fc%atom(atom1)%triplet(t)%lv2 -! rv3=fc%atom(atom1)%triplet(t)%lv3 -! ! -! iqr=dot_product(-q1,rv2) !+dot_product(q3,rv3) -! expiqr=cmplx(cos(iqr),sin(iqr),r8) -! c0=c0+sum(fc%atom(atom1)%triplet(t)%mwm*egvprod1(:,:,:,atom1,atom2,atom3))*expiqr -! ! -! iqr=dot_product(-q2,rv2) !+dot_product(-q3,rv3) -! expiqr=cmplx(cos(iqr),sin(iqr),r8) -! c1=c1+sum(fc%atom(atom1)%triplet(t)%mwm*egvprod2(:,:,:,atom1,atom2,atom3))*expiqr -! enddo -! enddo -! ! I predid the multiplication -! enhet=2.367755374064161E51_r8 -! c0=enhet*c0/omegaprod1 -! c1=enhet*c1/omegaprod2 -! ! -! double_scatteringamplitude=c0*c1 -! end function diff --git a/src/anharmonic_free_energy/energy_dos.f90 b/src/anharmonic_free_energy/energy_dos.f90 deleted file mode 100644 index 34f5e538..00000000 --- a/src/anharmonic_free_energy/energy_dos.f90 +++ /dev/null @@ -1,173 +0,0 @@ - -!!> calculate things as a density of states -!subroutine get_free_energy_on_grid(qpd,drd,uc,fc,fct,fcf,qp,dr,loto,opts,mw,lsmpi) -! !> q-point mesh -! type(lo_monkhorst_pack_mesh), intent(in) :: qpd -! !> harmonic properties on this mesh -! type(lo_phonon_dispersions), intent(in) :: drd -! !> crystal structure -! type(lo_crystalstructure), intent(inout) :: uc -! !> second order force constant -! type(lo_forceconstant_secondorder), intent(in) :: fc -! !> third order force constant -! type(lo_forceconstant_thirdorder), intent(in) :: fct -! !> fourth order force constant -! type(lo_forceconstant_fourthorder), intent(in) :: fcf -! !> q-point mesh -! type(lo_monkhorst_pack_mesh), intent(in) :: qp -! !> harmonic properties on this mesh -! type(lo_phonon_dispersions), intent(in) :: dr -! !> electrostatic corrections -! type(lo_loto), intent(in) :: loto -! !> all settings -! type(lo_opts), intent(in) :: opts -! !> mpi communicator -! type(lo_mpiinfo), intent(in) :: mw -! !> mpi helper -! type(lo_lsmpi), intent(in) :: lsmpi -! -! ! stuff for the DOS mesh -! type(lo_phonon_selfenergy) :: se -! type(lo_phonon_dos) :: pd -! complex(flyt), dimension(3) :: cv0 -! real(flyt), dimension(:,:,:), allocatable :: dumdos,dumdosbuf -! real(flyt), dimension(:,:), allocatable :: dum_site,dum_mode -! real(flyt), dimension(:), allocatable :: dum -! real(flyt) :: f0,f1,t0,sigma,weight -! integer :: q1,lqp,mode,i -! -! t0=mpi_wtime() -! ! switch off openMP -! call omp_set_num_threads(1) -! -! if ( mw%talk ) call lo_progressbar_init() -! lo_allocate(dumdos(opts%nf,dr%nb,qpd%nq_irr)) -! lo_allocate(dumdosbuf(opts%nf,dr%nb,qpd%nq_irr)) -! dumdos=0.0_flyt -! dumdosbuf=0.0_flyt -! do q1=1,lsmpi%nq -! lqp=lsmpi%ind(q1) -! ! get the actual self-energy -! call se%generate(qpd%ip(lqp),drd%iq(lqp),uc,fc,fct,fcf,qp,dr,loto,opts) -! ! and the intensity -! do mode=1,drd%nb -! call getintensity(se%faxis,se%im_3ph(:,mode)+se%im_iso(:,mode),& -! se%re_3ph(:,mode)+se%re_4ph(:,mode),se%p%omega(mode),se%faxis,& -! se%intensity(:,mode)) -! f0=lo_trapezoid_integration(se%faxis,se%intensity(:,mode)) -! ! if it's tiny, add a really narry gaussian instead. -! if ( f0 .lt. lo_tol ) then -! if ( drd%iq(q1)%omega(mode) .gt. drd%omega_min*0.5_flyt ) then -! do i=1,se%nf -! se%intensity(i,mode)=lo_gauss(se%faxis(i),drd%iq(lqp)%omega(mode),abs(se%faxis(3)-se%faxis(1))) -! enddo -! endif -! endif -! ! store the intensities -! dumdosbuf(:,mode,lqp)=dumdosbuf(:,mode,lqp)+se%intensity(:,mode) -! enddo -! ! -! if ( mw%talk ) call lo_progressbar(' ... calculating phonon dos',q1,lsmpi%nq,mpi_wtime()-t0) -! ! -! enddo -! -! ! Sum it up -! call mpi_allreduce(dumdosbuf,dumdos,qpd%nq_irr*opts%nf*dr%nb,MPI_DOUBLE_PRECISION,MPI_SUM,mw%comm,mw%error) -! -! ! Build the phonon dos structure -! lo_allocate(pd%omega(opts%nf)) -! lo_allocate(pd%pdos_site(opts%nf,uc%na)) -! lo_allocate(pd%pdos_mode(opts%nf,dr%nb)) -! lo_allocate(pd%dos(opts%nf)) -! pd%na=uc%na -! pd%nb=dr%nb -! pd%ndos=opts%nf -! pd%enhet=opts%enhet -! pd%omega=se%intensityaxis -! pd%pdos_site=0.0_flyt -! pd%pdos_mode=0.0_flyt -! pd%dos=0.0_flyt -! pd%dosprojection=.true. -! pd%dossmear=drd%default_smearing() -! pd%dosmax=maxval(pd%omega) -! -! t0=mpi_wtime() -! ! Add it up, with a little smearing -! lo_allocate(dum_site(pd%ndos,pd%na)) -! lo_allocate(dum_mode(pd%ndos,pd%nb)) -! lo_allocate(dum(pd%ndos)) -! dum_site=0.0_flyt -! dum_mode=0.0_flyt -! if ( mw%talk ) call lo_progressbar_init() -! do q1=1,lsmpi%nq -! lqp=lsmpi%ind(q1) -! weight=qpd%ip(lqp)%weight -! ! -! do mode=1,drd%nb -! ! skip acoustic at gamma -! if ( drd%iq(q1)%omega(mode) .lt. drd%omega_min*0.5_flyt ) cycle -! ! ok, smear a little -! sigma=qpd%smearingparameter(drd%iq(lqp)%vel(:,mode),pd%dossmear,opts%sigma) -! call lo_put_function_on_new_axis(se%faxis,dumdos(:,mode,lqp),pd%omega,dum,sigma) -! ! make sure it's normalized after convolution -! dum=dum/lo_trapezoid_integration(pd%omega,dum) -! dum=dum*weight -! ! add it to the mode-projected -! dum_mode(:,mode)=dum_mode(:,mode)+dum -! ! get the site-projection thing -! do i=1,uc%na -! cv0=drd%iq(lqp)%egv((i-1)*3+1:i*3,mode) -! f0=abs(dot_product(cv0,conjg(cv0))) -! dum_site(:,i)=dum_site(:,i)+f0*dum -! enddo -! enddo -! ! -! if ( mw%talk ) call lo_progressbar(' ... integrating phonon dos',q1,lsmpi%nq,mpi_wtime()-t0) -! ! -! enddo -! -! ! Add things together -! call mpi_allreduce(dum_site,pd%pdos_site,opts%nf*uc%na,MPI_DOUBLE_PRECISION,MPI_SUM,mw%comm,mw%error) -! call mpi_allreduce(dum_mode,pd%pdos_mode,opts%nf*dr%nb,MPI_DOUBLE_PRECISION,MPI_SUM,mw%comm,mw%error) -! -! if ( mw%r .eq. 0 ) then -! ! Start normalizing, first the whole thing -! do mode=1,drd%nb -! pd%dos=pd%dos+pd%pdos_mode(:,mode) -! f0=lo_trapezoid_integration(pd%omega,pd%pdos_mode(:,mode)) -! pd%pdos_mode=pd%pdos_mode/f0 -! enddo -! ! remove stupid stuff -! f1=pd%dos(1) -! do i=1,pd%ndos -! f0=(pd%ndos-i)*1.0_flyt/( (pd%ndos-1)*1.0_flyt ) -! f0=f0**2 -! pd%dos(i)=pd%dos(i)-f0*f1 -! if ( pd%dos(i) .lt. 0.0_flyt ) pd%dos(i)=0.0_flyt -! enddo -! pd%dos(1)=0.0_flyt -! ! -! f0=lo_trapezoid_integration(pd%omega,pd%dos) -! pd%dos=pd%dos*dr%nb/f0 -! ! and the site-projected -! do i=1,uc%na -! f0=lo_trapezoid_integration(pd%omega,pd%pdos_site(:,i)) -! pd%pdos_site(:,i)=pd%pdos_site(:,i)/f0 -! enddo -! ! make sure the pojected adds up to the total -! do i=1,pd%ndos -! if ( pd%dos(i) .gt. lo_tol/lo_twopi/1E12_flyt ) then -! f0=sum(pd%pdos_mode(i,:)) -! pd%pdos_mode(i,:)=pd%pdos_mode(i,:)*pd%dos(i)/f0 -! f0=sum(pd%pdos_site(i,:)) -! pd%pdos_site(i,:)=pd%pdos_site(i,:)*pd%dos(i)/f0 -! endif -! enddo -! ! Write it to file -! call pd%write_to_file(uc,opts%enhet,pdfplot=.false.,modeproj=.false.,& -! filename='outfile.phonon_dos_lineshape') -! ! -! endif -! -!end subroutine - diff --git a/src/anharmonic_free_energy/epot.f90 b/src/anharmonic_free_energy/epot.f90 index 7de7706a..c154fb87 100644 --- a/src/anharmonic_free_energy/epot.f90 +++ b/src/anharmonic_free_energy/epot.f90 @@ -162,11 +162,6 @@ subroutine setup_potential_energy_differences(pot, uc, ss, fc2, fc3, fc4, mw, ve t0 = timer t1 = timer - if (verbosity .gt. 0) then - write (*, *) '' - write (*, *) 'PREPARING POTENTIAL ENERGY DIFFERENCES' - end if - call fc2%remap(uc, ss, pot%fc2) if (verbosity .gt. 0) then t1 = walltime() @@ -243,6 +238,8 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, mw) ediff = 0.0_r8 sdiff = 0.0_r8 + if (mw%talk) write(*, *) '... computing energy differences' + ! Let's compute energies and stress differences do i=1, sim%nt if (mod(i, mw%n) .ne. mw%r) cycle @@ -258,7 +255,10 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, mw) sdiff(i, :, :, 1) = sim%stat%stress(:, :, i) sdiff(i, :, :, 2) = sim%stat%stress(:, :, i) - s3 end do + call mw%allreduce('sum', ediff) + call mw%allreduce('sum', sdiff) + if (mw%talk) write(*, *) '... computing free energy correction' allocate(buf(3, nblocks)) allocate(buf_stress(3, 3, nblocks)) @@ -274,7 +274,7 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, mw) ! First, let's compute properties for each blocks do j=1, nblocks istart = blocksize*j - iend = min(blocksize*j + 1, sim%nt) + iend = min(blocksize*(j+1), sim%nt) f0 = lo_mean(ediff(istart:iend, i)) buf(1, j) = lo_mean(ediff(istart:iend, i)) @@ -289,26 +289,27 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, mw) end do ! First order cumulant cumulant(1, i) = lo_mean(buf(1, :)) - cumulant_var(1, i) = lo_mean((buf(1, :) - cumulant(1, i))**2) + cumulant_var(1, i) = sqrt(lo_mean((buf(1, :) - cumulant(1, i))**2)) ! Second order cumulant cumulant(2, i) = lo_mean(buf(2, :)) - cumulant_var(2, i) = lo_mean((buf(2, :) - cumulant(2, i))**2) + cumulant_var(2, i) = sqrt(lo_mean((buf(2, :) - cumulant(2, i))**2)) ! Third order cumulant cumulant(3, i) = lo_mean(buf(3, :)) - cumulant_var(3, i) = lo_mean((buf(3, :) - cumulant(3, i))**2) + cumulant_var(3, i) = sqrt(lo_mean((buf(3, :) - cumulant(3, i))**2)) ! Same for the stress if (i .lt. 3) then do a=1, 3 do b=1, 3 stress_pot(a, b, i) = lo_mean(buf_stress(a, b, :)) - stress_potvar(a, b, i) = lo_mean((buf_stress(a, b, :) - stress_pot(a, b, i))**2) + stress_potvar(a, b, i) = sqrt(lo_mean((buf_stress(a, b, :) - stress_pot(a, b, i))**2)) end do end do end if end do ! We add the prefactor for the cumulants cumulant = cumulant/real(ss%na, r8) + cumulant_var = cumulant_var/real(ss%na, r8) cumulant(2, :) = 0.5_r8 * cumulant(2, :) * inverse_kbt cumulant_var(2, :) = 0.5_r8 * cumulant_var(2, :) * inverse_kbt cumulant_var(3, :) = cumulant_var(3, :) * inverse_kbt**2 / 6.0_r8 @@ -329,7 +330,7 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, mw) thermo%stress_pot(:, :) = stress_pot(:, :, 1) thermo%stress_potvar(:, :) = stress_potvar(:, :, 1) thermo%stress_diff(:, :) = stress_pot(:, :, 2) - thermo%stress_potvar(:, :) = stress_potvar(:, :, 2) + thermo%stress_diffvar(:, :) = stress_potvar(:, :, 2) end subroutine end module diff --git a/src/anharmonic_free_energy/main.f90 b/src/anharmonic_free_energy/main.f90 index f839ac2e..4da09f6f 100644 --- a/src/anharmonic_free_energy/main.f90 +++ b/src/anharmonic_free_energy/main.f90 @@ -58,7 +58,7 @@ program anharmonic_free_energy write(*, *) 'Recap of the parameters governing the calculation' write(*, *) '' write (*, '(1X,A40,F20.12)') 'Temperature ', opts%temperature - write (*, '(1X,A40,L3)') 'Classical limit ', opts%quantum + write (*, '(1X,A40,L3)') 'Quantum limit ', opts%quantum write (*, '(1X,A40,I4,I4,I4)') 'Q-point grid Harmonic ', opts%qgrid write (*, '(1X,A40,I4,I4,I4)') 'Third order q-point grid ', opts%qg3ph write (*, '(1X,A40,I4,I4,I4)') 'Fourth order q-point grid ', opts%qg4ph @@ -162,35 +162,32 @@ program anharmonic_free_energy end block latdyn calcepot: block + !> The simulation type(lo_mdsim) :: sim + !> The potentiel energy helper type(lo_energy_differences) :: pot + !> The supercell type(lo_crystalstructure) :: ss - real(r8), dimension(:, :, :, :), allocatable :: sdiff - real(r8), dimension(:, :, :), allocatable :: buf_stress - real(r8), dimension(:, :), allocatable :: buf - real(r8), dimension(:, :), allocatable :: ediff - real(r8), dimension(3, 3) :: s3, sk2, sk3, sk4, skp - - real(r8) :: e2, e3, e4, ep, inverse_kbt, f0 - integer :: i, j, a, b, blocksize - real(r8) :: stol - if (mw%talk) write(*, *) '' if (lo_does_file_exist('infile.sim.hdf5') .or. lo_does_file_exist('infile.meta')) then havesim = .true. if (mw%talk) write(*, *) 'Computing energy differences' + if (mw%talk) write(*, *) '... reading simulation files' + ! Read the supercell call ss%readfromfile('infile.ssposcar') call ss%classify('supercell', uc) + ! Setup the ifc with the potential + if (mw%talk) write(*, *) '... preparing potential energy differences' call pot%setup(uc, ss, fc, fct, fcf, mw, opts%verbosity+1) ! We fetch the simulation data if (lo_does_file_exist('infile.sim.hdf5')) then - call sim%read_from_hdf5('infile.sim.hdf5', verbosity=opts%verbosity + 2, stride=-1) + call sim%read_from_hdf5('infile.sim.hdf5', verbosity=-1, stride=-1) else - call sim%read_from_file(verbosity=opts%verbosity + 2, stride=1, magnetic=.false., dielectric=.false., nrand=-1, mw=mw) + call sim%read_from_file(verbosity=-1, stride=1, magnetic=.false., dielectric=.false., nrand=-1, mw=mw) end if if (abs(opts%temperature - sim%temperature_thermostat) .gt. lo_tol .and. mw%talk) then @@ -202,25 +199,9 @@ program anharmonic_free_energy write(*, *) end if - if (thermo%temperature .gt. 1E-5_r8) then - inverse_kbt = 1.0_r8/lo_kb_Hartree/thermo%temperature - else - inverse_kbt = 0.0_r8 - end if - - if (mw%talk) write(*, *) '... computing energy differences' call pot%compute_realspace_thermo(ss, sim, thermo, opts%nblocks, mw) - stol = sum(abs(thermo%stress_pot)) * 1e-6_r8 - call lo_symmetrize_stress(thermo%stress_pot, uc) - thermo%stress_pot = lo_chop(thermo%stress_pot, stol) - call lo_symmetrize_stress(thermo%stress_potvar, uc) - thermo%stress_potvar = lo_chop(thermo%stress_potvar, stol) - call lo_symmetrize_stress(thermo%stress_diff, uc) - thermo%stress_diff = lo_chop(thermo%stress_diff, stol) - call lo_symmetrize_stress(thermo%stress_diffvar, uc) - thermo%stress_diffvar = lo_chop(thermo%stress_diffvar, stol) - + call tmr%tock('simulation') else havesim = .false. if (mw%talk) then @@ -296,8 +277,135 @@ program anharmonic_free_energy end block latdyn4ph summary: block + !> Properties at the harmonic level + real(r8) :: fharm, uharm, sharm, charm + !> Properties with first order cumulant, 2nd order IFC + real(r8) :: f2_1, vf2_1, u2_1, vu2_1, s2_1, vs2_1, c2_1, vc2_1 + !> Properties with second order cumulant, 2nd order IFC + real(r8) :: f2_2, vf2_2, u2_2, vu2_2, s2_2, vs2_2, c2_2, vc2_2 + !> Properties with first order cumulant, 3rd order IFC + real(r8) :: f3_1, vf3_1, u3_1, vu3_1, s3_1, vs3_1, c3_1, vc3_1 + !> The prefactor, depending if we have stochastic samples or not + real(r8) :: pref real(r8) :: f0, f1, f2 - character(len=1000) :: opf1, opf2 + real(r8), dimension(3, 3) :: sigma + character(len=1000) :: opfc, opff, opfs + !> A tolerance to clean-up stress results + real(r8) :: stol + integer :: i + + if (opts%stochastic) then + pref = -1.0_r8 + else + pref = 1.0_r8 + end if + + ! Clean and symmetrize every stress tensor + stol = sum(abs(thermo%stress_pot)) * 1e-6_r8 + call lo_symmetrize_stress(thermo%stress_pot, uc) + thermo%stress_pot = lo_chop(thermo%stress_pot, stol) + call lo_symmetrize_stress(thermo%stress_potvar, uc) + thermo%stress_potvar = lo_chop(thermo%stress_potvar, stol) + call lo_symmetrize_stress(thermo%stress_diff, uc) + thermo%stress_diff = lo_chop(thermo%stress_diff, stol) + call lo_symmetrize_stress(thermo%stress_diffvar, uc) + thermo%stress_diffvar = lo_chop(thermo%stress_diffvar, stol) + + fharm = thermo%f0 * lo_Hartree_to_eV + uharm = thermo%u0 * lo_Hartree_to_eV + sharm = thermo%s0 / lo_kB_Hartree + charm = thermo%cv0 / lo_kB_Hartree + + f2_1 = thermo%clt_ifc2_1(1) * lo_Hartree_to_eV + u2_1 = thermo%clt_ifc2_1(1) * lo_Hartree_to_eV + s2_1 = 0.0_r8 + c2_1 = 0.0_r8 + vf2_1 = pref * thermo%clt_ifc2_1(2) * lo_Hartree_to_eV + vu2_1 = pref * thermo%clt_ifc2_1(2) * lo_Hartree_to_eV + vs2_1 = 0.0_r8 + vc2_1 = 0.0_r8 + + f2_2 = thermo%clt_ifc2_2(1) * lo_Hartree_to_eV + u2_2 = thermo%clt_ifc2_2(1) * lo_Hartree_to_eV + s2_2 = 0.0_r8 + c2_2 = 0.0_r8 + vf2_2 = pref * thermo%clt_ifc2_2(2) * lo_Hartree_to_eV + vu2_2 = pref * thermo%clt_ifc2_2(2) * lo_Hartree_to_eV + vs2_2 = 0.0_r8 + vc2_2 = 0.0_r8 + + f3_1 = thermo%clt_ifc3_1(1) * lo_Hartree_to_eV + u3_1 = thermo%clt_ifc3_1(1) * lo_Hartree_to_eV + s3_1 = 0.0_r8 + c3_1 = 0.0_r8 + vf3_1 = pref * thermo%clt_ifc3_1(2) * lo_Hartree_to_eV + vu3_1 = pref * thermo%clt_ifc3_1(2) * lo_Hartree_to_eV + vs3_1 = 0.0_r8 + vc3_1 = 0.0_r8 + + if (mw%talk) then + opfc = '(4(1X,A24))' + opff = '(4(1X,F24.12))' + opfs = '(3(1X,F24.12))' + write(*, *) '' + write(*, *) 'SUMMARY OF RESULTS' + write(*, *) '' + write(*, *) 'Effective harmonic contribution' + write(*, opfc) 'Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' + write(*, opff) fharm, uharm, sharm, charm + + write(*, *) '' + write(*, *) 'With first order cumulant correction, 2nd order IFC' + write(*, opfc) 'Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' + write(*, opff) fharm + f2_1, uharm+u2_1, sharm+s2_1, charm+c2_1 + write(*, opff) vf2_1, vu2_1, vs2_1, vc2_1 + + write(*, *) '' + write(*, *) 'With second order cumulant correction, 2nd order IFC' + write(*, opfc) 'Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' + write(*, opff) fharm+f2_1+f2_2, uharm+u2_1+u2_2, sharm+s2_1+s2_2, charm+c2_1+c2_2 + write(*, opff) vf2_1+vf2_2, vu2_1+vu2_2, vs2_1+vs2_2, vc2_1+vc2_2 + + if (opts%thirdorder) then + write(*, *) '' + write(*, *) 'With first order cumulant correction, 2nd+3rd order IFC' + write(*, opfc) 'Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' + write(*, opff) fharm + f3_1, uharm+u3_1, sharm+s3_1, charm+c3_1 + write(*, opff) vf3_1, vu3_1, vs3_1, vc3_1 + end if + + + write(*, *) '' + sigma = (thermo%stress_pot + thermo%stress_kin) * lo_pressure_HartreeBohr_to_GPa + write(*, *) 'Stress tensor [GPa]' + do i=1, 3 + write(*, opfs) sigma(i, :) + end do + sigma = (thermo%stress_potvar) * lo_pressure_HartreeBohr_to_GPa + write(*, *) 'Uuncertainty [GPa]' + do i=1, 3 + write(*, opfs) sigma(i, :) + end do + write(*, *) '' + sigma = (thermo%stress_diff + thermo%stress_3ph + thermo%stress_kin) * lo_pressure_HartreeBohr_to_GPa + write(*, *) 'Stress tensor with third order correction [GPa]' + do i=1, 3 + write(*, opfs) sigma(i, :) + end do + sigma = (thermo%stress_diffvar) * lo_pressure_HartreeBohr_to_GPa + write(*, *) 'Uncertainty [GPa]' + do i=1, 3 + write(*, opfs) sigma(i, :) + end do + write(*, *) '' + sigma = thermo%alpha * 1e6_r8 + write(*, *) 'Anisotropic thermal expansion from third-order [1e-6/K]' + do i=1, 3 + write(*, opfs) sigma(i, :) + end do + write(*, *) 'Volumic thermal expansion [1e-6/K]' + write(*, '(1X,F24.12)') sigma(1, 1) + sigma(2, 2) + sigma(3, 3) + end if call tmr%stop() if (mw%talk) write(*, *) '' From 2b17875f0e7b923d62740231bd216e43c77f2cf8 Mon Sep 17 00:00:00 2001 From: =?UTF-8?q?Alo=C3=AFs=20Castellano?= Date: Sun, 16 Feb 2025 16:32:18 +0100 Subject: [PATCH 04/28] Actually computing correction to the heat capacity with first order cumulants --- src/anharmonic_free_energy/epot.f90 | 18 +++++- .../lo_thermodynamic_helpers.f90 | 2 + src/anharmonic_free_energy/main.f90 | 55 +++++++++++-------- 3 files changed, 49 insertions(+), 26 deletions(-) diff --git a/src/anharmonic_free_energy/epot.f90 b/src/anharmonic_free_energy/epot.f90 index c154fb87..894f7257 100644 --- a/src/anharmonic_free_energy/epot.f90 +++ b/src/anharmonic_free_energy/epot.f90 @@ -216,15 +216,16 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, mw) !> MPI type(lo_mpi_helper), intent(inout) :: mw - real(r8), dimension(3, 5) :: cumulant, cumulant_var + real(r8), dimension(3, 5) :: cumulant, cumulant_var, cumcv, cumcv_var real(r8), dimension(3, 3, 5) :: stress_pot, stress_potvar real(r8), dimension(:, :, :, :), allocatable :: sdiff real(r8), dimension(:, :, :), allocatable :: buf_stress real(r8), dimension(:, :), allocatable :: buf + real(r8), dimension(:, :), allocatable :: bufcv real(r8), dimension(:, :), allocatable :: ediff real(r8), dimension(3, 3) :: s3, sk2, sk3, sk4, skp - real(r8) :: e2, e3, e4, ep, inverse_kbt, f0 + real(r8) :: e2, e3, e4, ep, inverse_kbt, f0, f1 integer :: i, j, a, b, blocksize, istart, iend if (thermo%temperature .gt. 1E-5_r8) then @@ -260,6 +261,7 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, mw) if (mw%talk) write(*, *) '... computing free energy correction' allocate(buf(3, nblocks)) + allocate(bufcv(3, nblocks)) allocate(buf_stress(3, 3, nblocks)) cumulant = 0.0_r8 @@ -281,6 +283,9 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, mw) buf(2, j) = lo_mean((ediff(istart:iend, i) - f0)**2) buf(3, j) = lo_mean((ediff(istart:iend, i) - f0)**3) + f1 = lo_mean(ediff(istart:iend, 1)) + bufcv(1, j) = lo_mean(ediff(istart:iend, i)*ediff(istart:iend, i)) - f0*lo_mean(ediff(istart:iend,i)) + do a=1, 3 do b=1, 3 buf_stress(a, b, j) = lo_mean(sdiff(istart:iend, a, b, i)) @@ -297,6 +302,10 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, mw) cumulant(3, i) = lo_mean(buf(3, :)) cumulant_var(3, i) = sqrt(lo_mean((buf(3, :) - cumulant(3, i))**2)) + ! Correction for the heat capacity + cumcv(1, i) = lo_mean(bufcv(1, :)) + cumcv_var(1, i) = sqrt(lo_mean((bufcv(1, :) - cumcv(1, i))**2)) + ! Same for the stress if (i .lt. 3) then do a=1, 3 @@ -313,6 +322,8 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, mw) cumulant(2, :) = 0.5_r8 * cumulant(2, :) * inverse_kbt cumulant_var(2, :) = 0.5_r8 * cumulant_var(2, :) * inverse_kbt cumulant_var(3, :) = cumulant_var(3, :) * inverse_kbt**2 / 6.0_r8 + cumcv = cumcv*inverse_kbt/thermo%temperature/real(ss%na, r8) + cumcv_var = cumcv_var*inverse_kbt/thermo%temperature/real(ss%na, r8) ! And we can store everything thermo%clt_ifc2_1(1) = cumulant(1, 3) thermo%clt_ifc2_1(2) = cumulant_var(1, 3) @@ -326,6 +337,9 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, mw) thermo%clt_ifc4_1(2) = cumulant_var(1, 5) thermo%clt_ifc4_2(1) = cumulant(2, 5) thermo%clt_ifc4_2(2) = cumulant_var(2, 5) + ! And the cv + thermo%cv_ifc2_1(1) = cumcv(1, 3) + thermo%cv_ifc2_1(2) = cumcv_var(1, 3) ! Stress included thermo%stress_pot(:, :) = stress_pot(:, :, 1) thermo%stress_potvar(:, :) = stress_potvar(:, :, 1) diff --git a/src/anharmonic_free_energy/lo_thermodynamic_helpers.f90 b/src/anharmonic_free_energy/lo_thermodynamic_helpers.f90 index f19249b3..967d9826 100644 --- a/src/anharmonic_free_energy/lo_thermodynamic_helpers.f90 +++ b/src/anharmonic_free_energy/lo_thermodynamic_helpers.f90 @@ -30,6 +30,8 @@ module lo_thermodynamic_helpers real(r8), dimension(2) :: clt_ifc2_1, clt_ifc2_2 real(r8), dimension(2) :: clt_ifc3_1, clt_ifc3_2 real(r8), dimension(2) :: clt_ifc4_1, clt_ifc4_2 + !> Also for the heat capacity + real(r8), dimension(2) :: cv_ifc2_1 !> The pressure real(r8) :: p=-lo_huge !> The stress tensor diff --git a/src/anharmonic_free_energy/main.f90 b/src/anharmonic_free_energy/main.f90 index 4da09f6f..0f185b90 100644 --- a/src/anharmonic_free_energy/main.f90 +++ b/src/anharmonic_free_energy/main.f90 @@ -59,6 +59,7 @@ program anharmonic_free_energy write(*, *) '' write (*, '(1X,A40,F20.12)') 'Temperature ', opts%temperature write (*, '(1X,A40,L3)') 'Quantum limit ', opts%quantum + write (*, '(1X,A40,L3)') 'Stochastic sampling ', opts%stochastic write (*, '(1X,A40,I4,I4,I4)') 'Q-point grid Harmonic ', opts%qgrid write (*, '(1X,A40,I4,I4,I4)') 'Third order q-point grid ', opts%qg3ph write (*, '(1X,A40,I4,I4,I4)') 'Fourth order q-point grid ', opts%qg4ph @@ -319,11 +320,11 @@ program anharmonic_free_energy f2_1 = thermo%clt_ifc2_1(1) * lo_Hartree_to_eV u2_1 = thermo%clt_ifc2_1(1) * lo_Hartree_to_eV s2_1 = 0.0_r8 - c2_1 = 0.0_r8 + c2_1 = pref * thermo%cv_ifc2_1(1) / lo_kB_Hartree vf2_1 = pref * thermo%clt_ifc2_1(2) * lo_Hartree_to_eV vu2_1 = pref * thermo%clt_ifc2_1(2) * lo_Hartree_to_eV vs2_1 = 0.0_r8 - vc2_1 = 0.0_r8 + vc2_1 = pref * thermo%cv_ifc2_1(2) / lo_kb_Hartree f2_2 = thermo%clt_ifc2_2(1) * lo_Hartree_to_eV u2_2 = thermo%clt_ifc2_2(1) * lo_Hartree_to_eV @@ -350,18 +351,22 @@ program anharmonic_free_energy write(*, *) '' write(*, *) 'SUMMARY OF RESULTS' write(*, *) '' - write(*, *) 'Effective harmonic contribution' + write(*, *) 'Effective harmonic contribution: F = F_harm' write(*, opfc) 'Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' write(*, opff) fharm, uharm, sharm, charm write(*, *) '' - write(*, *) 'With first order cumulant correction, 2nd order IFC' + write(*, *) 'Gibbs-Bogoliubov approximation: F = F_harm + ' write(*, opfc) 'Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' write(*, opff) fharm + f2_1, uharm+u2_1, sharm+s2_1, charm+c2_1 write(*, opff) vf2_1, vu2_1, vs2_1, vc2_1 write(*, *) '' - write(*, *) 'With second order cumulant correction, 2nd order IFC' + if (opts%stochastic) then + write(*, *) 'With second order cumulant correction: F = F_harm + - <(V-V_harm)^2> / 2kBT' + else + write(*, *) 'With second order cumulant correction: F = F_harm + + <(V-V_harm)^2> / 2kBT' + end if write(*, opfc) 'Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' write(*, opff) fharm+f2_1+f2_2, uharm+u2_1+u2_2, sharm+s2_1+s2_2, charm+c2_1+c2_2 write(*, opff) vf2_1+vf2_2, vu2_1+vu2_2, vs2_1+vs2_2, vc2_1+vc2_2 @@ -386,25 +391,27 @@ program anharmonic_free_energy do i=1, 3 write(*, opfs) sigma(i, :) end do - write(*, *) '' - sigma = (thermo%stress_diff + thermo%stress_3ph + thermo%stress_kin) * lo_pressure_HartreeBohr_to_GPa - write(*, *) 'Stress tensor with third order correction [GPa]' - do i=1, 3 - write(*, opfs) sigma(i, :) - end do - sigma = (thermo%stress_diffvar) * lo_pressure_HartreeBohr_to_GPa - write(*, *) 'Uncertainty [GPa]' - do i=1, 3 - write(*, opfs) sigma(i, :) - end do - write(*, *) '' - sigma = thermo%alpha * 1e6_r8 - write(*, *) 'Anisotropic thermal expansion from third-order [1e-6/K]' - do i=1, 3 - write(*, opfs) sigma(i, :) - end do - write(*, *) 'Volumic thermal expansion [1e-6/K]' - write(*, '(1X,F24.12)') sigma(1, 1) + sigma(2, 2) + sigma(3, 3) + if (opts%thirdorder) then + write(*, *) '' + sigma = (thermo%stress_diff + thermo%stress_3ph + thermo%stress_kin) * lo_pressure_HartreeBohr_to_GPa + write(*, *) 'Stress tensor with third order correction [GPa]' + do i=1, 3 + write(*, opfs) sigma(i, :) + end do + sigma = (thermo%stress_diffvar) * lo_pressure_HartreeBohr_to_GPa + write(*, *) 'Uncertainty [GPa]' + do i=1, 3 + write(*, opfs) sigma(i, :) + end do + write(*, *) '' + sigma = thermo%alpha * 1e6_r8 + write(*, *) 'Anisotropic thermal expansion from third-order [1e-6/K]' + do i=1, 3 + write(*, opfs) sigma(i, :) + end do + write(*, *) 'Volumic thermal expansion [1e-6/K]' + write(*, '(1X,F24.12)') sigma(1, 1) + sigma(2, 2) + sigma(3, 3) + end if end if call tmr%stop() From c3e0ecb8b2d2b50b48a23b83ccd7a12bfb779bfa Mon Sep 17 00:00:00 2001 From: =?UTF-8?q?Alo=C3=AFs=20Castellano?= Date: Mon, 17 Feb 2025 14:53:30 +0100 Subject: [PATCH 05/28] Faster elastic properties with third order, correcting some typos and more readable code --- src/anharmonic_free_energy/epot.f90 | 1 + src/anharmonic_free_energy/fourthorder.f90 | 128 ++++++++++++------ src/anharmonic_free_energy/main.f90 | 10 +- src/anharmonic_free_energy/thirdorder.f90 | 146 ++++++++++++++------- 4 files changed, 188 insertions(+), 97 deletions(-) diff --git a/src/anharmonic_free_energy/epot.f90 b/src/anharmonic_free_energy/epot.f90 index 894f7257..f3481605 100644 --- a/src/anharmonic_free_energy/epot.f90 +++ b/src/anharmonic_free_energy/epot.f90 @@ -324,6 +324,7 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, mw) cumulant_var(3, :) = cumulant_var(3, :) * inverse_kbt**2 / 6.0_r8 cumcv = cumcv*inverse_kbt/thermo%temperature/real(ss%na, r8) cumcv_var = cumcv_var*inverse_kbt/thermo%temperature/real(ss%na, r8) + ! And we can store everything thermo%clt_ifc2_1(1) = cumulant(1, 3) thermo%clt_ifc2_1(2) = cumulant_var(1, 3) diff --git a/src/anharmonic_free_energy/fourthorder.f90 b/src/anharmonic_free_energy/fourthorder.f90 index 7fa710a1..00b246f1 100644 --- a/src/anharmonic_free_energy/fourthorder.f90 +++ b/src/anharmonic_free_energy/fourthorder.f90 @@ -94,25 +94,33 @@ subroutine free_energy_fourthorder(uc, fcf, qp, dr, temperature, df4, s4, cv4, q psisq = real(dot_product(evp3, ptf), r8) if (quantum) then + ! Phonon occupation n1 = lo_planck(temperature, om1) n2 = lo_planck(temperature, om2) + ! First derivative with respect to temperature dn1 = lo_planck_deriv(temperature, om1) dn2 = lo_planck_deriv(temperature, om2) + ! Second derivative with respect to temperature ddn1 = lo_planck_secondderiv(temperature, om1) ddn2 = lo_planck_secondderiv(temperature, om2) + ! The free energy f0 = (2.0_r8 * n1 + 1.0_r8) * (2.0_r8 * n2 + 1.0_r8) * psisq * prefactor / 32.0_r8 - + ! The entropy df0 = 2.0_r8 * dn1 * (2.0_r8 * n2 + 1.0_r8) + (2.0_r8 * n1 + 1.0_r8) * 2.0_r8 * dn2 df0 = df0 * psisq * prefactor / 32.0_r8 - - f1 = 2.0_r8 * ddn1 * (2.0_r8 * n2 + 1.0_r8) + 2.0_r8 * ddn2 * (2.0_r8 * n1 + 1.0_r8) + & + ddf0 = 2.0_r8 * ddn1 * (2.0_r8 * n2 + 1.0_r8) + 2.0_r8 * ddn2 * (2.0_r8 * n1 + 1.0_r8) + & 8.0_r8 * dn1 * dn2 ddf0 = ddf0 * temperature * psisq * prefactor / 32.0_r8 else + ! Much simpler in the classical case + ! Free energy f0 = (lo_kb_Hartree*temperature)**2 / (om1*om2) / 8.0_r8 + ! Entropy df0 = lo_kb_Hartree**2 * temperature / (om1*om2) / 4.0_r8 + ! Heat capacity ddf0 = lo_kb_Hartree**2 * temperature / (om1*om2) / 4.0_r8 end if + ! And we accumulate df4 = df4 + f0 * psisq * prefactor s4 = s4 - df0 * psisq * prefactor cv4 = cv4 - df0 * psisq * prefactor @@ -127,10 +135,12 @@ subroutine free_energy_fourthorder(uc, fcf, qp, dr, temperature, df4, s4, cv4, q if (mw%talk) then call lo_progressbar(' ... fourth order', qp%n_irr_point, qp%n_irr_point, walltime() - t0) end if + ! Reduce on all ranks call mw%allreduce('sum', df4) call mw%allreduce('sum', s4) call mw%allreduce('sum', cv4) + ! And deallocate call mem%deallocate(ptf, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) call mem%deallocate(evp1, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) call mem%deallocate(evp2, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) @@ -161,14 +171,20 @@ subroutine free_energy_fourthorder_secondorder(uc, fcf, qp, dr, temperature, fe4 !> memory tracker type(lo_mem_helper), intent(inout) :: mem + !> For the smearing parameters + real(r8), dimension(:, :), allocatable :: sigsq !> Frequency scaled eigenvectors complex(r8), dimension(:), allocatable :: egv1, egv2, egv3, egv4 !> Helper for Fourier transform of psi3 complex(r8), dimension(:), allocatable :: ptf, evp1, evp2, evp3 + !> Phonon occupations + real(r8), dimension(4) :: n, dn, ddn !> Frequencies, bose-einstein occupation and scattering strength and some other buffer - real(r8) :: sigma, om1, om2, om3, om4, n1, n2, n3, n4, psisq, f0, f1, f2, f3, t0, prefactor + real(r8) :: sigma, om1, om2, om3, om4, psisq, f0, f1, f2, f3, t0, prefactor !> - real(r8) :: s1, s2, s3, mult, dn1, dn2, ddn1, ddn2, df0, ddf0, np1, np2, np3, np4, sig, sig1, sig2, sig3, sig4 + real(r8) :: s1, s2, s3, mult, df0, ddf0, sig, sig1, sig2, sig3, sig4 + !> The phonon occupation plus 1 + real(r8) :: np1, np2, np3, np4 !> The multiplicities real(r8) :: m0, m1, m2, m3 !> The complex threephonon matrix element @@ -187,13 +203,10 @@ subroutine free_energy_fourthorder_secondorder(uc, fcf, qp, dr, temperature, fe4 call mem%allocate(egv2, dr%n_mode, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) call mem%allocate(egv3, dr%n_mode, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) call mem%allocate(egv4, dr%n_mode, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%allocate(sigsq, [qp%n_irr_point, dr%n_mode], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) t0 = walltime() - fe4 = 0.0_r8 - s4 = 0.0_r8 - cv4 = 0.0_r8 - select type (qp) class is (lo_fft_mesh) dims = qp%griddensity @@ -201,6 +214,22 @@ subroutine free_energy_fourthorder_secondorder(uc, fcf, qp, dr, temperature, fe4 call lo_stop_gracefully(['This routine only works with FFT meshes'], lo_exitcode_param, __FILE__, __LINE__) end select + fe4 = 0.0_r8 + s4 = 0.0_r8 + cv4 = 0.0_r8 + + ! First we compute the broadening parameter for each modes + sigsq = 0.0_r8 + do q1=1, qp%n_irr_point + do b1=1, dr%n_mode + sigsq(q1, b1) = qp%smearingparameter(dr%iq(q1)%vel(:, b1), dr%default_smearing(b1), 1.0_r8)**2 + end do + end do + + n = 0.0_r8 + dn = 0.0_r8 + ddn = 0.0_r8 + do q1=1, qp%n_irr_point do q2=1, qp%n_full_point do q3=1, qp%n_full_point @@ -211,6 +240,7 @@ subroutine free_energy_fourthorder_secondorder(uc, fcf, qp, dr, temperature, fe4 if (q3 .lt. q2) cycle if (q4 .lt. q3) cycle + ! Prefactors to account for equivalent points if (q2 .eq. q3 .and. q3 .eq. q4) then m0 = 1.0_r8 m1 = 1.0_r8 @@ -235,72 +265,84 @@ subroutine free_energy_fourthorder_secondorder(uc, fcf, qp, dr, temperature, fe4 call pretransform_phi4(fcf, qp%ap(q2)%r, qp%ap(q3)%r, qp%ap(q4)%r, ptf) do b1=1, dr%n_mode + ! Get first phonon om1 = dr%iq(q1)%omega(b1) if (om1 .lt. lo_freqtol) cycle + n(1) = lo_planck(temperature, om1) + dn(1) = lo_planck_deriv(temperature, om1) + ddn(1) = lo_planck_secondderiv(temperature, om1) egv1 = dr%iq(q1)%egv(:, b1)/sqrt(om1) do b2=1, dr%n_mode + ! Get second phonon om2 = dr%aq(q2)%omega(b2) if (om2 .lt. lo_freqtol) cycle - + n(2) = lo_planck(temperature, om2) + dn(2) = lo_planck_deriv(temperature, om2) + ddn(2) = lo_planck_secondderiv(temperature, om2) egv2 = dr%aq(q2)%egv(:, b2)/sqrt(om2) + + ! Multiply first and second phonon evp1 = 0.0_r8 call zgeru(dr%n_mode, dr%n_mode, (1.0_r8, 0.0_r8), egv2, 1, egv1, 1, evp1, dr%n_mode) do b3=1, dr%n_mode + ! Get third phonon om3 = dr%aq(q3)%omega(b3) if (om3 .lt. lo_freqtol) cycle - + n(3) = lo_planck(temperature, om3) + dn(3) = lo_planck_deriv(temperature, om3) + ddn(3) = lo_planck_secondderiv(temperature, om3) egv3 = dr%aq(q3)%egv(:, b3)/sqrt(om3) + + ! Project on third phonon evp2 = 0.0_r8 call zgeru(dr%n_mode, dr%n_mode**2, (1.0_r8, 0.0_r8), egv3, 1, evp1, 1, evp2, dr%n_mode) do b4=1, dr%n_mode + ! Get fourth phonon om4 = dr%aq(q4)%omega(b4) if (om4 .lt. lo_freqtol) cycle - + n(4) = lo_planck(temperature, om4) + dn(4) = lo_planck_deriv(temperature, om4) + ddn(4) = lo_planck_secondderiv(temperature, om4) egv4 = dr%aq(q4)%egv(:, b4)/sqrt(om4) + + ! Project on fourth phonon evp3 = 0.0_r8 call zgeru(dr%n_mode, dr%n_mode**3, (1.0_r8, 0.0_r8), egv4, 1, evp2, 1, evp3, dr%n_mode) evp3 = conjg(evp3) + + ! Compute the scattering matrix element c0 = dot_product(evp3, ptf) psisq = abs(c0*conjg(c0))*prefactor - if (om4 .lt. lo_freqtol) cycle - if (quantum) then - n1 = lo_planck(temperature, om1) - n2 = lo_planck(temperature, om2) - n3 = lo_planck(temperature, om3) - n4 = lo_planck(temperature, om4) - np1 = n1 + 1.0_r8 - np2 = n2 + 1.0_r8 - np3 = n3 + 1.0_r8 - np4 = n4 + 1.0_r8 - - f1 = np1*np2*np3*np4 - n1*n2*n3*n4 / (om1+om2+om3+om4) - if (abs(-om1+om2+om3+om4) .lt. lo_freqtol) then - sig1 = dr%default_smearing(b1) - sig2 = dr%default_smearing(b2) - sig3 = dr%default_smearing(b3) - sig = sqrt(sig1**2 + sig2**2 + sig3**2 + sig4**2) - f2 = 4.0_r8*(n1*np2*np3*np4 - np1*n2*n3*n4) * real(1.0/(-om1+om2+om3+om4 + lo_imag*sig)) - else - f2 = 4.0_r8*(n1*np2*np3*np4 - np1*n2*n3*n4) / (-om1+om2+om3+om4) - end if - if (abs(om1+om2-om3-om4) .lt. lo_freqtol) then - sig1 = dr%default_smearing(b1) - sig2 = dr%default_smearing(b2) - sig3 = dr%default_smearing(b3) - sig = sqrt(sig1**2 + sig2**2 + sig3**2 + sig4**2) - f3 = 3.0_r8*(n1*n2*(n3+n4+1.0_r8) - n3*n4*(n1+n2+1.0_r8))*real(1.0/(om1+om2-om3-om4 + lo_imag*sig)) - else - f3 = 3.0_r8*(n1*n2*(n3+n4+1.0_r8) - n3*n4*(n1+n2+1.0_r8)) / (om1+om2-om3-om4) - end if + ! Phonon occupation + np1 = n(1) + 1.0_r8 + np2 = n(2) + 1.0_r8 + np3 = n(3) + 1.0_r8 + np4 = n(4) + 1.0_r8 + + ! We get the broadening parameter + sig1 = sigsq(q1, b1) + sig2 = sigsq(qp%ap(q2)%irreducible_index, b2) + sig3 = sigsq(qp%ap(q3)%irreducible_index, b3) + sig4 = sigsq(qp%ap(q4)%irreducible_index, b3) + sig = sqrt(sig1 + sig2 + sig3 + sig4) + + f1 = (np1*np2*np3*np4 - n(1)*n(2)*n(3)*n(4)) / real(1.0_r8/(om1+om2+om3+om4+lo_imag*sig), r8) + f2 = 4.0_r8*(n(1)*np2*np3*np4 - np1*n(2)*n(3)*n(4)) * real(1.0/(-om1+om2+om3+om4 + lo_imag*sig)) + f3 = 3.0_r8*(n(1)*n(2)*(n(3)+n(4)+1.0_r8) - n(3)*n(4)*(n(1)+n(2)+1.0_r8))*real(1.0/(om1+om2-om3-om4 + lo_imag*sig)) f0 = (f1 + f2 + f3) / 768.0_r8 else + ! Much simpler in the classical case + ! Free energy f0 = (lo_kb_Hartree*temperature)**3 / (om1*om2*om3*om4) / 48.0_r8 + ! Entropy df0 = lo_kb_Hartree**3*temperature**2 / (om1*om2*om3*om4) / 16.0_r8 + ! Heat capacity ddf0 = lo_kb_Hartree**3*temperature**2 / (om1*om2*om3*om4) / 8.0_r8 end if + ! And we accumulate fe4 = fe4 - f0 * psisq s4 = s4 + df0 * psisq cv4 = cv4 + ddf0 * psisq @@ -318,10 +360,12 @@ subroutine free_energy_fourthorder_secondorder(uc, fcf, qp, dr, temperature, fe4 if (mw%talk) then call lo_progressbar(' ... fourth order', qp%n_irr_point, qp%n_irr_point, walltime() - t0) end if + ! Reduce on all ranks call mw%allreduce('sum', fe4) call mw%allreduce('sum', s4) call mw%allreduce('sum', cv4) + ! And deallocate memory call mem%deallocate(ptf, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) call mem%deallocate(evp1, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) call mem%deallocate(evp2, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) diff --git a/src/anharmonic_free_energy/main.f90 b/src/anharmonic_free_energy/main.f90 index 0f185b90..47c90eee 100644 --- a/src/anharmonic_free_energy/main.f90 +++ b/src/anharmonic_free_energy/main.f90 @@ -372,11 +372,11 @@ program anharmonic_free_energy write(*, opff) vf2_1+vf2_2, vu2_1+vu2_2, vs2_1+vs2_2, vc2_1+vc2_2 if (opts%thirdorder) then - write(*, *) '' - write(*, *) 'With first order cumulant correction, 2nd+3rd order IFC' - write(*, opfc) 'Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' - write(*, opff) fharm + f3_1, uharm+u3_1, sharm+s3_1, charm+c3_1 - write(*, opff) vf3_1, vu3_1, vs3_1, vc3_1 + write(*, *) '' + write(*, *) 'With first order cumulant correction, 2nd+3rd order IFC' + write(*, opfc) 'Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' + write(*, opff) fharm + f3_1, uharm+u3_1, sharm+s3_1, charm+c3_1 + write(*, opff) vf3_1, vu3_1, vs3_1, vc3_1 end if diff --git a/src/anharmonic_free_energy/thirdorder.f90 b/src/anharmonic_free_energy/thirdorder.f90 index e7fc65c5..deadab83 100644 --- a/src/anharmonic_free_energy/thirdorder.f90 +++ b/src/anharmonic_free_energy/thirdorder.f90 @@ -11,6 +11,7 @@ module thirdorder use type_forceconstant_secondorder, only: lo_forceconstant_secondorder use type_forceconstant_thirdorder, only: lo_forceconstant_thirdorder use type_phonon_dispersions, only: lo_phonon_dispersions +use type_symmetryoperation, only: lo_operate_on_secondorder_tensor use lo_timetracker, only: lo_timer use lo_thermodynamic_helpers, only: lo_full_to_voigt @@ -44,31 +45,42 @@ subroutine elastic_thirdorder(uc, fc, fct, qp, dr, temperature, p3ph, alpha, qua !> memory tracker type(lo_mem_helper), intent(inout) :: mem + !> The eigenvector for the current mode complex(r8), dimension(:), allocatable :: egv + !> Complex coefficients for gruneisen complex(r8), dimension(3, 3) :: c0 + !> stiffness and compliance tensors, in voigt notation real(r8), dimension(6, 6) :: cij, sij - real(r8), dimension(3, 3) :: grun, buf + !> Buffers for Gruneisen and thermal expansion, with full anisotropy + real(r8), dimension(3, 3) :: grun, bufalpha, grunbuf + !> q-points and lattice distances real(r8), dimension(3) :: qv, rv2, rv3 - real(r8), dimension(2) :: d + !> Phase factor for Fourier transform and product of eigenvectors complex(r8) :: expiqr, evprod + !> Harmonic stuffs real(r8) :: om, iqr, invsqrtmass, u0, cv0 - integer :: q1, b1, a1, t, a2, a3, i, j, k, l, ivoigt, jvoigt, ctr + !> Integers for do loops + integer :: q1, b1, a1, t, a2, a3, i, j, k, l, ivoigt, jvoigt, ctr, ifull - allocate(egv(dr%n_mode)) + ! We start by allocating space for the eigenvector + call mem%allocate(egv, dr%n_mode, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + ! Set everything to zero p3ph = 0.0_r8 - buf = 0.0_r8 + bufalpha = 0.0_r8 + ! And here we go ctr = 0 - do q1=1, qp%n_full_point - qv = qp%ap(q1)%r * lo_twopi + do q1=1, qp%n_irr_point + qv = qp%ip(q1)%r * lo_twopi do b1=1, dr%n_mode ctr = ctr + 1 if (mod(ctr, mw%n) .ne. mw%r) cycle - om = dr%aq(q1)%omega(b1) + ! We start by computing the mode Gruneisen parameter, with full anisotropy + om = dr%iq(q1)%omega(b1) if (om .lt. lo_freqtol) cycle c0 = 0.0_r8 - egv = dr%aq(q1)%egv(:, b1) + egv = dr%iq(q1)%egv(:, b1) do a1=1, fct%na do t=1, fct%atom(a1)%n a2 = fct%atom(a1)%triplet(t)%i2 @@ -92,6 +104,13 @@ subroutine elastic_thirdorder(uc, fc, fct, qp, dr, temperature, p3ph, alpha, qua end do grun = -real(c0, r8) / (6.0_r8 * om**2) + ! Here we sum over all symmetry equivalent q-point, taking into account the symop + grunbuf = 0.0_r8 + do ifull=1, qp%ip(q1)%n_full_point + grunbuf = grunbuf + lo_operate_on_secondorder_tensor(uc%sym%op(ifull), grun) + end do + grun = grunbuf + ! Now we can accumulate things using the Gruneisen parameter if (quantum) then u0 = lo_harmonic_oscillator_internal_energy(temperature, om) @@ -101,22 +120,21 @@ subroutine elastic_thirdorder(uc, fc, fct, qp, dr, temperature, p3ph, alpha, qua cv0 = lo_kb_Hartree end if - p3ph(:, :) = p3ph(:, :) - grun(:, :) * u0 * qp%ap(q1)%integration_weight / uc%volume - do i=1, 3 - do j=1, 3 - buf(i, j) = buf(i, j) + cv0 * grun(i, j) * qp%ap(q1)%integration_weight - end do - end do - + ! And we accumulate + p3ph(:, :) = p3ph(:, :) - grun(:, :) * u0 / uc%volume / qp%n_full_point + bufalpha(:, :) = bufalpha(:, :) + cv0 * grun(:, :) / qp%n_full_point end do end do + ! Reduce the calculation call mw%allreduce('sum', p3ph) - call mw%allreduce('sum', buf) + call mw%allreduce('sum', bufalpha) + ! We need the compliance tensor to get the thermal expansion call fc%get_elastic_constants(uc, mw, -1) cij = fc%elastic_constants_voigt + fc%elastic_constants_voigt_longrange call lo_invert_real_matrix(cij, sij) + ! And we just have to add the compliance tensor part to get the thermal expansion alpha = 0.0_r8 do i=1, 3 do j=1, 3 @@ -125,11 +143,13 @@ subroutine elastic_thirdorder(uc, fc, fct, qp, dr, temperature, p3ph, alpha, qua ivoigt = lo_full_to_voigt(i, j) jvoigt = lo_full_to_voigt(k, l) - alpha(i, j) = alpha(i, j) + sij(ivoigt, jvoigt) * buf(k, l) / uc%volume + ! That's simply the formula + alpha(i, j) = alpha(i, j) + sij(ivoigt, jvoigt) * bufalpha(k, l) / uc%volume end do end do end do end do + call mem%deallocate(egv, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) end subroutine @@ -154,6 +174,8 @@ subroutine free_energy_thirdorder(uc, fct, qp, dr, temperature, fe3, s3, cv3, qu !> memory tracker type(lo_mem_helper), intent(inout) :: mem + !> For the smearing parameters + real(r8), dimension(:, :), allocatable :: sigsq !> Frequency scaled eigenvectors complex(r8), dimension(:), allocatable :: egv1, egv2, egv3 !> Helper for Fourier transform of psi3 @@ -176,6 +198,7 @@ subroutine free_energy_thirdorder(uc, fct, qp, dr, temperature, fe3, s3, cv3, qu call mem%allocate(egv1, dr%n_mode, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) call mem%allocate(egv2, dr%n_mode, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) call mem%allocate(egv3, dr%n_mode, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%allocate(sigsq, [qp%n_irr_point, dr%n_mode], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) t0 = walltime() @@ -189,6 +212,14 @@ subroutine free_energy_thirdorder(uc, fct, qp, dr, temperature, fe3, s3, cv3, qu fe3 = 0.0_r8 cv3 = 0.0_r8 + ! First we compute the broadening parameter for each modes + sigsq = 0.0_r8 + do q1=1, qp%n_irr_point + do b1=1, dr%n_mode + sigsq(q1, b1) = qp%smearingparameter(dr%iq(q1)%vel(:, b1), dr%default_smearing(b1), 1.0_r8)**2 + end do + end do + do q1=1, qp%n_irr_point do q2=1, qp%n_full_point ctr = ctr + 1 @@ -208,79 +239,84 @@ subroutine free_energy_thirdorder(uc, fct, qp, dr, temperature, fe3, s3, cv3, qu call pretransform_phi3(fct, qp%ap(q2)%r, qp%ap(q3)%r, ptf) do b1=1, dr%n_mode + ! Get first phonon om1 = dr%iq(q1)%omega(b1) if (om1 .lt. lo_freqtol) cycle + n1 = lo_planck(temperature, om1) + dn1 = lo_planck_deriv(temperature, om1) + ddn1 = lo_planck_secondderiv(temperature, om1) egv1 = dr%iq(q1)%egv(:, b1)/sqrt(om1) do b2=1, dr%n_mode + ! Get second phonon om2 = dr%aq(q2)%omega(b2) if (om2 .lt. lo_freqtol) cycle - + n2 = lo_planck(temperature, om2) + dn2 = lo_planck_deriv(temperature, om2) + ddn2 = lo_planck_secondderiv(temperature, om2) egv2 = dr%aq(q2)%egv(:, b2)/sqrt(om2) + + ! Multiply first and second phonon evp1 = 0.0_r8 call zgeru(dr%n_mode, dr%n_mode, (1.0_r8, 0.0_r8), egv2, 1, egv1, 1, evp1, dr%n_mode) do b3=1, dr%n_mode + ! Get third phonon om3 = dr%aq(q3)%omega(b3) if (om3 .lt. lo_freqtol) cycle + n3 = lo_planck(temperature, om3) + dn3 = lo_planck_deriv(temperature, om3) + ddn3 = lo_planck_secondderiv(temperature, om3) egv3 = dr%aq(q3)%egv(:, b3)/sqrt(om3) + ! Project on third phonon evp2 = 0.0_r8 call zgeru(dr%n_mode, dr%n_mode**2, (1.0_r8, 0.0_r8), egv3, 1, evp1, 1, evp2, dr%n_mode) evp2 = conjg(evp2) + + ! Compute the scattering matrix element c0 = dot_product(evp2, ptf) psisq = real(conjg(c0)*c0, r8) * prefactor if (quantum) then - n1 = lo_planck(temperature, om1) - n2 = lo_planck(temperature, om2) - n3 = lo_planck(temperature, om3) - - dn1 = lo_planck_deriv(temperature, om1) - dn2 = lo_planck_deriv(temperature, om1) - dn3 = lo_planck_deriv(temperature, om1) - - ddn1 = lo_planck_secondderiv(temperature, om1) - ddn2 = lo_planck_secondderiv(temperature, om1) - ddn3 = lo_planck_secondderiv(temperature, om1) + ! Get a smearing parameter + sig1 = sigsq(q1, b1) + sig2 = sigsq(qp%ap(q2)%irreducible_index, b2) + sig3 = sigsq(qp%ap(q3)%irreducible_index, b3) + sigma = sqrt(sig1 + sig2 + sig3) ! This are the formula to get the free energy f1 = (n1 + 1.0_r8)*(n2 + n3 + 1.0_r8) + n2*n3 f2 = n1*n2 + n1*n3 - n2*n3 + 1.0_r8 - ! Here is for the entropy df1 = dn1 * (n2 + n3 + 1.0_r8) + (n1 + 1.0_r8) * (dn2 + dn3) + dn2 * n3 + n2 * dn3 df2 = dn1 * n2 + n1 * dn2 + dn1 * n3 + n1 * dn3 - dn2 * n3 - n2 * dn3 - ! And the heat capacity ddf1 = ddn1 * (n2 + n3 + 1.0_r8) + 2.0_r8 * dn1 * (dn2 + dn3) + (n1 + 1.0_r8) * (ddn2 + ddn3) + & ddn2 * n3 + n2 * ddn3 + 2.0_r8 * dn2 * dn3 ddf2 = ddn1 * n2 + n1 * ddn2 + 2.0_r8 * dn1 * dn2 + ddn1 * n3 + n1 * ddn3 + 2.0_r8 * dn1 * dn3 - & ddn2 * n3 - n2 * ddn3 - 2.0_r8 * dn2 * dn3 - f1 = f1/(om1 + om2 + om3) - df1 = df1/(om1 + om2 + om3) - ddf1 = ddf1/(om1 + om2 + om3) - if (abs(om1 + om2 - om3) .lt. lo_freqtol) then - ! Get a smearing parameter - sig1 = dr%default_smearing(b1) - sig2 = dr%default_smearing(b2) - sig3 = dr%default_smearing(b3) - sigma = sqrt(sig1**2 + sig2**2 + sig3**2) - f2 = 3*f2*real(1.0/(om1 + om2 - om3 + lo_imag*sigma), r8) - df2 = 3.0_r8 * df2 * real(1.0/(om1 + om2 - om3 + lo_imag*sigma), r8) - ddf2 = 3.0_r8 * ddf2 * real(1.0/(om1 + om2 - om3 + lo_imag*sigma), r8) - else - f2 = 3.0_r8 * f2 / (om1 + om2 - om3) - df2 = 3.0_r8 * df2 / (om1 + om2 - om3) - ddf2 = 3.0_r8 * ddf2 / (om1 + om2 - om3) - end if + ! Compute the principal values + f1 = f1*real(1.0_r8/(om1 + om2 + om3 + lo_imag*sigma), r8) + df1 = df1*real(1.0_r8/(om1 + om2 + om3 + lo_imag*sigma), r8) + ddf1 = ddf1*real(1.0_r8/(om1 + om2 + om3 + lo_imag*sigma), r8) + f2 = 3*f2*real(1.0/(om1 + om2 - om3 + lo_imag*sigma), r8) + df2 = 3.0_r8 * df2 * real(1.0/(om1 + om2 - om3 + lo_imag*sigma), r8) + ddf2 = 3.0_r8 * ddf2 * real(1.0/(om1 + om2 - om3 + lo_imag*sigma), r8) + + ! Get everything together f0 = (f1 + f2) / 48.0_r8 df0 = (df1 + df2) / 48.0_r8 ddf0 = (ddf1 + ddf2) * temperature / 48.0_r8 else + ! It's much simpler in the classical case + ! Free energy f0 = (lo_kb_Hartree*temperature)**2 / (om1*om2*om3) / 12.0_r8 + ! Entropy df0 = lo_kb_Hartree**2 * temperature / (om1*om2*om3) / 6.0_r8 + ! Heat capacity ddf0 = lo_kb_Hartree**2 * temperature / (om1*om2*om3) / 6.0_r8 end if + ! And accumulate fe3 = fe3 - f0 * psisq s3 = s3 + df0 * psisq cv3 = cv3 + ddf0 * psisq @@ -295,9 +331,19 @@ subroutine free_energy_thirdorder(uc, fct, qp, dr, temperature, fe3, s3, cv3, qu if (mw%talk) then call lo_progressbar(' ... third order', qp%n_irr_point, qp%n_irr_point, walltime() - t0) end if - + ! Reduce on all ranks call mw%allreduce('sum', fe3) + call mw%allreduce('sum', s3) call mw%allreduce('sum', cv3) + + ! And we can deallocate everything + call mem%deallocate(ptf, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%deallocate(evp1, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%deallocate(evp2, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%deallocate(egv1, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%deallocate(egv2, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%deallocate(egv3, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%deallocate(sigsq, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) end subroutine !> Get the Fourier transform of the third order matrix element From 396ed744f7874fb85ed551710784699f5471fca8 Mon Sep 17 00:00:00 2001 From: =?UTF-8?q?Alo=C3=AFs=20Castellano?= Date: Tue, 18 Feb 2025 09:17:57 +0100 Subject: [PATCH 06/28] Getting closer to a clean anharmonic_free_energy --- src/anharmonic_free_energy/epot.f90 | 98 +++++++++++-------- .../lo_thermodynamic_helpers.f90 | 12 +-- src/anharmonic_free_energy/main.f90 | 97 +++++++++++------- 3 files changed, 120 insertions(+), 87 deletions(-) diff --git a/src/anharmonic_free_energy/epot.f90 b/src/anharmonic_free_energy/epot.f90 index f3481605..c304322b 100644 --- a/src/anharmonic_free_energy/epot.f90 +++ b/src/anharmonic_free_energy/epot.f90 @@ -3,7 +3,7 @@ module epot use konstanter, only: r8, lo_pi, lo_twopi, lo_tol, lo_sqtol, lo_status, lo_Hartree_to_eV, lo_kb_hartree use gottochblandat, only: tochar, walltime, lo_chop, lo_trueNtimes, lo_progressbar_init, & lo_progressbar, lo_frobnorm, open_file, lo_flattentensor, lo_sqnorm, lo_outerproduct, lo_mean, & - lo_points_on_sphere, lo_mean, lo_stddev + lo_points_on_sphere, lo_mean, lo_stddev, lo_outerproduct use mpi_wrappers, only: lo_mpi_helper, lo_stop_gracefully use lo_memtracker, only: lo_mem_helper !use geometryfunctions, only: lo_inscribed_sphere_in_box @@ -202,7 +202,7 @@ subroutine setup_potential_energy_differences(pot, uc, ss, fc2, fc3, fc4, mw, ve end if end subroutine -subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, mw) +subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, mw, mem) !> container for potential energy differences class(lo_energy_differences), intent(in) :: pot !> The supercell @@ -215,29 +215,45 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, mw) integer, intent(in) :: nblocks !> MPI type(lo_mpi_helper), intent(inout) :: mw + !> memory tracker + type(lo_mem_helper), intent(inout) :: mem - real(r8), dimension(3, 5) :: cumulant, cumulant_var, cumcv, cumcv_var - real(r8), dimension(3, 3, 5) :: stress_pot, stress_potvar + real(r8), dimension(3, 4) :: cumulant, cumulant_var, cumcv, cumcv_var + real(r8), dimension(3, 3, 4) :: stress_pot, stress_potvar + !> The stress difference between true and ifcs real(r8), dimension(:, :, :, :), allocatable :: sdiff + !> A little buffer for the stress real(r8), dimension(:, :, :), allocatable :: buf_stress - real(r8), dimension(:, :), allocatable :: buf - real(r8), dimension(:, :), allocatable :: bufcv + !> The energy difference between true and ifcs real(r8), dimension(:, :), allocatable :: ediff - real(r8), dimension(3, 3) :: s3, sk2, sk3, sk4, skp + !> Little buffers for the blocks + real(r8), dimension(:, :), allocatable :: buf, bufcv + !> The third order contribution to the stress + real(r8), dimension(3, 3) :: s3 + !> Some buffers: energy, inverse kbt blabla real(r8) :: e2, e3, e4, ep, inverse_kbt, f0, f1 + !> Some integers for do loops integer :: i, j, a, b, blocksize, istart, iend + !> Let's get the inverse temperature if (thermo%temperature .gt. 1E-5_r8) then inverse_kbt = 1.0_r8/lo_kb_Hartree/thermo%temperature else inverse_kbt = 0.0_r8 end if - allocate(ediff(sim%nt, 5)) - allocate(sdiff(sim%nt, 3, 3, 2)) + ! Allocate stuffs + call mem%allocate(ediff, [sim%nt, 4], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%allocate(sdiff, [sim%nt, 3, 3, 2], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%allocate(buf, [3, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%allocate(bufcv, [3, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%allocate(buf_stress, [3, 3, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) ediff = 0.0_r8 sdiff = 0.0_r8 + buf = 0.0_r8 + bufcv = 0.0_r8 + buf_stress = 0.0_r8 if (mw%talk) write(*, *) '... computing energy differences' @@ -247,45 +263,44 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, mw) call pot%energies_and_forces(ss, sim%u(:, :, i), e2, e3, e4, ep, s3) ! We store the energy differences ediff(i, 1) = sim%stat%potential_energy(i) - ediff(i, 2) = sim%stat%potential_energy(i) - e2 - ediff(i, 3) = sim%stat%potential_energy(i) - e2 - ep - ediff(i, 4) = sim%stat%potential_energy(i) - e2 - ep - e3 - ediff(i, 5) = sim%stat%potential_energy(i) - e2 - ep - e3 - e4 + ediff(i, 2) = sim%stat%potential_energy(i) - e2 - ep + ediff(i, 3) = sim%stat%potential_energy(i) - e2 - ep - e3 + ediff(i, 4) = sim%stat%potential_energy(i) - e2 - ep - e3 - e4 - ! But also the stress + ! But also the stress differences sdiff(i, :, :, 1) = sim%stat%stress(:, :, i) sdiff(i, :, :, 2) = sim%stat%stress(:, :, i) - s3 end do + ! And reduce everything call mw%allreduce('sum', ediff) call mw%allreduce('sum', sdiff) if (mw%talk) write(*, *) '... computing free energy correction' - allocate(buf(3, nblocks)) - allocate(bufcv(3, nblocks)) - allocate(buf_stress(3, 3, nblocks)) + ! Ok now the messy part, here we compute the various correction + ! We also estimate the uncertainty through block averaging + ! TODO: is there a way to automatize the optimal number of blocks ? + ! Need to look what math people think of this cumulant = 0.0_r8 cumulant_var = 0.0_r8 stress_pot = 0.0_r8 stress_potvar = 0.0_r8 blocksize = floor((real(sim%nt, r8)) / real(nblocks)) - buf = 0.0_r8 - buf_stress = 0.0_r8 - - do i=1, 5 + do i=1, 4 ! First, let's compute properties for each blocks do j=1, nblocks + ! Index for the blocks istart = blocksize*j iend = min(blocksize*(j+1), sim%nt) - + ! We compute the averages for each block f0 = lo_mean(ediff(istart:iend, i)) + f1 = lo_mean(ediff(istart:iend, 1)) buf(1, j) = lo_mean(ediff(istart:iend, i)) buf(2, j) = lo_mean((ediff(istart:iend, i) - f0)**2) buf(3, j) = lo_mean((ediff(istart:iend, i) - f0)**3) - - f1 = lo_mean(ediff(istart:iend, 1)) - bufcv(1, j) = lo_mean(ediff(istart:iend, i)*ediff(istart:iend, i)) - f0*lo_mean(ediff(istart:iend,i)) - + bufcv(1, j) = lo_mean(ediff(istart:iend, 1)*ediff(istart:iend, i)) - f1*lo_mean(ediff(istart:iend,i)) + bufcv(2, j) = lo_mean(ediff(istart:iend, 1)*ediff(istart:iend, i)**2) - f1*lo_mean(ediff(istart:iend,i)**2) + ! Including the stress do a=1, 3 do b=1, 3 buf_stress(a, b, j) = lo_mean(sdiff(istart:iend, a, b, i)) @@ -301,11 +316,9 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, mw) ! Third order cumulant cumulant(3, i) = lo_mean(buf(3, :)) cumulant_var(3, i) = sqrt(lo_mean((buf(3, :) - cumulant(3, i))**2)) - ! Correction for the heat capacity cumcv(1, i) = lo_mean(bufcv(1, :)) cumcv_var(1, i) = sqrt(lo_mean((bufcv(1, :) - cumcv(1, i))**2)) - ! Same for the stress if (i .lt. 3) then do a=1, 3 @@ -321,31 +334,30 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, mw) cumulant_var = cumulant_var/real(ss%na, r8) cumulant(2, :) = 0.5_r8 * cumulant(2, :) * inverse_kbt cumulant_var(2, :) = 0.5_r8 * cumulant_var(2, :) * inverse_kbt + cumulant(3, :) = cumulant(3, :) * inverse_kbt**2 / 6.0_r8 cumulant_var(3, :) = cumulant_var(3, :) * inverse_kbt**2 / 6.0_r8 cumcv = cumcv*inverse_kbt/thermo%temperature/real(ss%na, r8) cumcv_var = cumcv_var*inverse_kbt/thermo%temperature/real(ss%na, r8) ! And we can store everything - thermo%clt_ifc2_1(1) = cumulant(1, 3) - thermo%clt_ifc2_1(2) = cumulant_var(1, 3) - thermo%clt_ifc2_2(1) = cumulant(2, 3) - thermo%clt_ifc2_2(2) = cumulant_var(2, 3) - thermo%clt_ifc3_1(1) = cumulant(1, 4) - thermo%clt_ifc3_1(2) = cumulant_var(1, 4) - thermo%clt_ifc3_2(1) = cumulant(2, 4) - thermo%clt_ifc3_2(2) = cumulant_var(2, 4) - thermo%clt_ifc4_1(1) = cumulant(1, 5) - thermo%clt_ifc4_1(2) = cumulant_var(1, 5) - thermo%clt_ifc4_2(1) = cumulant(2, 5) - thermo%clt_ifc4_2(2) = cumulant_var(2, 5) - ! And the cv - thermo%cv_ifc2_1(1) = cumcv(1, 3) - thermo%cv_ifc2_1(2) = cumcv_var(1, 3) + thermo%corr_fe = cumulant + thermo%corr_fe_var = cumulant_var +! thermo%corr_s = s +! thermo%corr_s_var = s_var + thermo%corr_cv = cumcv + thermo%corr_cv_var = cumcv_var ! Stress included thermo%stress_pot(:, :) = stress_pot(:, :, 1) thermo%stress_potvar(:, :) = stress_potvar(:, :, 1) thermo%stress_diff(:, :) = stress_pot(:, :, 2) thermo%stress_diffvar(:, :) = stress_potvar(:, :, 2) + + ! And we can deallocate + call mem%deallocate(ediff, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%deallocate(sdiff, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%deallocate(buf, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%deallocate(bufcv, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%deallocate(buf_stress, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) end subroutine end module diff --git a/src/anharmonic_free_energy/lo_thermodynamic_helpers.f90 b/src/anharmonic_free_energy/lo_thermodynamic_helpers.f90 index 967d9826..2f45cad8 100644 --- a/src/anharmonic_free_energy/lo_thermodynamic_helpers.f90 +++ b/src/anharmonic_free_energy/lo_thermodynamic_helpers.f90 @@ -26,12 +26,10 @@ module lo_thermodynamic_helpers real(r8) :: cv0, cv3, cv4 !> The heat capacity at constant pressure real(r8) :: cp0, cp3, cp4 - !> The cumulant contributions - real(r8), dimension(2) :: clt_ifc2_1, clt_ifc2_2 - real(r8), dimension(2) :: clt_ifc3_1, clt_ifc3_2 - real(r8), dimension(2) :: clt_ifc4_1, clt_ifc4_2 - !> Also for the heat capacity - real(r8), dimension(2) :: cv_ifc2_1 + !> The cumulant corrections, first dimension is IFC, second is cumulant order + real(r8), dimension(3, 4) :: corr_fe=0.0_r8, corr_s=0.0_r8, corr_u=0.0_r8, corr_cv=0.0_r8 + !> The uncertainty for the cumulant corrections + real(r8), dimension(3, 4) :: corr_fe_var=0.0_r8, corr_s_var=0.0_r8, corr_u_var=0.0_r8, corr_cv_var=0.0_r8 !> The pressure real(r8) :: p=-lo_huge !> The stress tensor @@ -42,6 +40,7 @@ module lo_thermodynamic_helpers end type contains +! Symmetrize 3x3 tensors subroutine lo_symmetrize_stress(m, uc) !> The input matrix real(r8), dimension(3, 3), intent(inout) :: m @@ -58,6 +57,7 @@ subroutine lo_symmetrize_stress(m, uc) m = tmp / real(uc%sym%n, r8) end subroutine +! Go from full 3x3 real space to 6 voigt notation function lo_full_to_voigt(i, j) result(k) !> Inputs integer, intent(in) :: i diff --git a/src/anharmonic_free_energy/main.f90 b/src/anharmonic_free_energy/main.f90 index 47c90eee..2e5f3e10 100644 --- a/src/anharmonic_free_energy/main.f90 +++ b/src/anharmonic_free_energy/main.f90 @@ -1,9 +1,10 @@ program anharmonic_free_energy !!{!src/anharmonic_free_energy/manual.md!} -use konstanter, only: r8, lo_Hartree_to_eV, lo_kb_Hartree, lo_pressure_HartreeBohr_to_GPa, lo_tol, lo_status, lo_freqtol, lo_twopi +use konstanter, only: r8, lo_Hartree_to_eV, lo_kb_Hartree, lo_pressure_HartreeBohr_to_GPa, lo_tol, lo_status, lo_freqtol, & +lo_twopi, lo_time_au_to_fs use gottochblandat, only: open_file, walltime, lo_linspace, lo_progressbar_init, lo_progressbar, tochar, & lo_does_file_exist, lo_mean, lo_stddev, lo_harmonic_oscillator_internal_energy, lo_chop, & - lo_invert_real_matrix, lo_harmonic_oscillator_cv + lo_invert_real_matrix, lo_harmonic_oscillator_cv, tochar use mpi_wrappers, only: lo_mpi_helper use lo_memtracker, only: lo_mem_helper use lo_timetracker, only: lo_timer @@ -191,6 +192,14 @@ program anharmonic_free_energy call sim%read_from_file(verbosity=-1, stride=1, magnetic=.false., dielectric=.false., nrand=-1, mw=mw) end if + ! Let's recap info on the simulation + if (mw%talk) then + write (*, *) '... short summary of simulation:' + write (*, *) ' number of atoms: ', tochar(sim%na) + write (*, *) ' number of configurations: ', tochar(sim%nt) + write (*, *) ' thermostat set to (K): ', tochar(sim%temperature_thermostat) + end if + if (abs(opts%temperature - sim%temperature_thermostat) .gt. lo_tol .and. mw%talk) then write(*, *) write(*, *) 'WARNING: input and simulation temperatures do not match' @@ -200,7 +209,7 @@ program anharmonic_free_energy write(*, *) end if - call pot%compute_realspace_thermo(ss, sim, thermo, opts%nblocks, mw) + call pot%compute_realspace_thermo(ss, sim, thermo, opts%nblocks, mw, mem) call tmr%tock('simulation') else @@ -278,6 +287,14 @@ program anharmonic_free_energy end block latdyn4ph summary: block + !> The thermodynamic properties + real(r8), dimension(3, 4) :: fe, s, u, cv + !> The second order cumulants + real(r8), dimension(3, 4) :: fe2, s2, u2, cv2 + !> And their uncertainty + real(r8), dimension(3, 4) :: fe_unc, s_unc, u_unc, cv_unc + !> The thermodynamic properties + real(r8), dimension(3, 4) :: corr, corr_s, corr_cv !> Properties at the harmonic level real(r8) :: fharm, uharm, sharm, charm !> Properties with first order cumulant, 2nd order IFC @@ -312,37 +329,37 @@ program anharmonic_free_energy call lo_symmetrize_stress(thermo%stress_diffvar, uc) thermo%stress_diffvar = lo_chop(thermo%stress_diffvar, stol) - fharm = thermo%f0 * lo_Hartree_to_eV - uharm = thermo%u0 * lo_Hartree_to_eV - sharm = thermo%s0 / lo_kB_Hartree - charm = thermo%cv0 / lo_kB_Hartree - - f2_1 = thermo%clt_ifc2_1(1) * lo_Hartree_to_eV - u2_1 = thermo%clt_ifc2_1(1) * lo_Hartree_to_eV - s2_1 = 0.0_r8 - c2_1 = pref * thermo%cv_ifc2_1(1) / lo_kB_Hartree - vf2_1 = pref * thermo%clt_ifc2_1(2) * lo_Hartree_to_eV - vu2_1 = pref * thermo%clt_ifc2_1(2) * lo_Hartree_to_eV - vs2_1 = 0.0_r8 - vc2_1 = pref * thermo%cv_ifc2_1(2) / lo_kb_Hartree - - f2_2 = thermo%clt_ifc2_2(1) * lo_Hartree_to_eV - u2_2 = thermo%clt_ifc2_2(1) * lo_Hartree_to_eV - s2_2 = 0.0_r8 - c2_2 = 0.0_r8 - vf2_2 = pref * thermo%clt_ifc2_2(2) * lo_Hartree_to_eV - vu2_2 = pref * thermo%clt_ifc2_2(2) * lo_Hartree_to_eV - vs2_2 = 0.0_r8 - vc2_2 = 0.0_r8 - - f3_1 = thermo%clt_ifc3_1(1) * lo_Hartree_to_eV - u3_1 = thermo%clt_ifc3_1(1) * lo_Hartree_to_eV - s3_1 = 0.0_r8 - c3_1 = 0.0_r8 - vf3_1 = pref * thermo%clt_ifc3_1(2) * lo_Hartree_to_eV - vu3_1 = pref * thermo%clt_ifc3_1(2) * lo_Hartree_to_eV - vs3_1 = 0.0_r8 - vc3_1 = 0.0_r8 + ! The harmonic values + fharm = thermo%f0 + uharm = thermo%u0 + sharm = thermo%s0 + charm = thermo%cv0 + ! This are all the values with the corrections + fe(1, :) = fharm + thermo%corr_fe(1, :) + s(1, :) = sharm + thermo%corr_s(1, :) + u(1, :) = uharm + thermo%corr_u(1, :) + cv(1, :) = charm + thermo%corr_cv(1, :) + ! And the second order cumulants + fe(2, :) = fharm + thermo%corr_fe(1, :) + pref * thermo%corr_fe(2, :) + s(2, :) = sharm + thermo%corr_s(1, :) + pref * thermo%corr_s(2, :) + u(2, :) = uharm + thermo%corr_u(1, :) + pref * thermo%corr_u(2, :) + cv(2, :) = charm + thermo%corr_cv(1, :) + pref * thermo%corr_cv(2, :) + + ! And now we add the other little corrections + fe(2, 3) = fe(2, 3) + thermo%f3 + s(2, 3) = s(2, 3) + thermo%s3 + u(2, 3) = u(2, 3) + thermo%u3 + cv(2, 3) = cv(2, 3) + thermo%s3 + + ! And nice units for display + fharm = fharm * lo_Hartree_to_eV + uharm = uharm * lo_Hartree_to_eV + sharm = sharm / lo_kb_Hartree + charm = charm / lo_kb_Hartree + fe = fe * lo_Hartree_to_eV + u = u * lo_Hartree_to_eV + s = s / lo_kb_Hartree + cv = cv / lo_kb_Hartree if (mw%talk) then opfc = '(4(1X,A24))' @@ -358,7 +375,7 @@ program anharmonic_free_energy write(*, *) '' write(*, *) 'Gibbs-Bogoliubov approximation: F = F_harm + ' write(*, opfc) 'Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' - write(*, opff) fharm + f2_1, uharm+u2_1, sharm+s2_1, charm+c2_1 + write(*, opff) fe(1, 2), u(1, 2), s(1, 2), cv(1, 2) write(*, opff) vf2_1, vu2_1, vs2_1, vc2_1 write(*, *) '' @@ -368,14 +385,19 @@ program anharmonic_free_energy write(*, *) 'With second order cumulant correction: F = F_harm + + <(V-V_harm)^2> / 2kBT' end if write(*, opfc) 'Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' - write(*, opff) fharm+f2_1+f2_2, uharm+u2_1+u2_2, sharm+s2_1+s2_2, charm+c2_1+c2_2 + write(*, opff) fe(2, 2), u(2, 2), s(2, 2), cv(2, 2) write(*, opff) vf2_1+vf2_2, vu2_1+vu2_2, vs2_1+vs2_2, vc2_1+vc2_2 if (opts%thirdorder) then write(*, *) '' write(*, *) 'With first order cumulant correction, 2nd+3rd order IFC' write(*, opfc) 'Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' - write(*, opff) fharm + f3_1, uharm+u3_1, sharm+s3_1, charm+c3_1 + write(*, opff) fe(1, 3), u(1, 3), s(1, 3), cv(1, 3) + write(*, opff) vf3_1, vu3_1, vs3_1, vc3_1 + write(*, *) '' + write(*, *) 'With Second order cumulant correction, 2nd+3rd order IFC' + write(*, opfc) 'Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' + write(*, opff) fe(2, 3), u(2, 3), s(2, 3), cv(2, 3) write(*, opff) vf3_1, vu3_1, vs3_1, vc3_1 end if @@ -417,7 +439,6 @@ program anharmonic_free_energy call tmr%stop() if (mw%talk) write(*, *) '' call tmr%dump(mw, 'Timings:') - end block summary ! And we are done! From 34976828a737b1af3ec9d29387032651af6e9da2 Mon Sep 17 00:00:00 2001 From: =?UTF-8?q?Alo=C3=AFs=20Castellano?= Date: Wed, 2 Apr 2025 00:07:13 +0200 Subject: [PATCH 07/28] Correcting a qpoint fetch on the full grid instead of the irreducible one --- src/anharmonic_free_energy/fourthorder.f90 | 2 +- src/anharmonic_free_energy/main.f90 | 11 ++++++----- 2 files changed, 7 insertions(+), 6 deletions(-) diff --git a/src/anharmonic_free_energy/fourthorder.f90 b/src/anharmonic_free_energy/fourthorder.f90 index 00b246f1..5cea071e 100644 --- a/src/anharmonic_free_energy/fourthorder.f90 +++ b/src/anharmonic_free_energy/fourthorder.f90 @@ -73,7 +73,7 @@ subroutine free_energy_fourthorder(uc, fcf, qp, dr, temperature, df4, s4, cv4, q prefactor = qp%ip(q1)%integration_weight*qp%ap(q2)%integration_weight/uc%na ! pre-transform the matrix element - call pretransform_phi4_first(fcf, qp%ap(q1)%r, qp%ap(q2)%r, ptf) + call pretransform_phi4_first(fcf, qp%ip(q1)%r, qp%ap(q2)%r, ptf) do b1=1, dr%n_mode om1 = dr%iq(q1)%omega(b1) diff --git a/src/anharmonic_free_energy/main.f90 b/src/anharmonic_free_energy/main.f90 index 2e5f3e10..515cb310 100644 --- a/src/anharmonic_free_energy/main.f90 +++ b/src/anharmonic_free_energy/main.f90 @@ -276,11 +276,12 @@ program anharmonic_free_energy thermo%u4 = (fe4 + opts%temperature * s4) thermo%cv4 = cv4 - call free_energy_fourthorder_secondorder(uc, fcf, qp, dr, opts%temperature, fe4, s4, cv4, opts%quantum, mw, mem) - thermo%f4 = thermo%f4 + fe4 - thermo%s4 = thermo%s4 + s4 - thermo%u4 = thermo%u4 + (fe4 + opts%temperature * s4) - thermo%cv4 = thermo%cv4 + cv4 + ! TODO set fourthorder, second order cumulant its own qpoint grid density +! call free_energy_fourthorder_secondorder(uc, fcf, qp, dr, opts%temperature, fe4, s4, cv4, opts%quantum, mw, mem) +! thermo%f4 = thermo%f4 + fe4 +! thermo%s4 = thermo%s4 + s4 +! thermo%u4 = thermo%u4 + (fe4 + opts%temperature * s4) +! thermo%cv4 = thermo%cv4 + cv4 end if call tmr%tock('four-phonon') From d84de6ab9163ebf4ef2907c14ddc8e48533d7d84 Mon Sep 17 00:00:00 2001 From: =?UTF-8?q?Alo=C3=AFs=20Castellano?= Date: Fri, 4 Apr 2025 10:14:45 +0200 Subject: [PATCH 08/28] Setting real to right precision --- src/anharmonic_free_energy/epot.f90 | 2 +- src/anharmonic_free_energy/fourthorder.f90 | 4 ++-- 2 files changed, 3 insertions(+), 3 deletions(-) diff --git a/src/anharmonic_free_energy/epot.f90 b/src/anharmonic_free_energy/epot.f90 index c304322b..03f29dca 100644 --- a/src/anharmonic_free_energy/epot.f90 +++ b/src/anharmonic_free_energy/epot.f90 @@ -285,7 +285,7 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, mw, mem) cumulant_var = 0.0_r8 stress_pot = 0.0_r8 stress_potvar = 0.0_r8 - blocksize = floor((real(sim%nt, r8)) / real(nblocks)) + blocksize = floor((real(sim%nt, r8)) / real(nblocks, r8)) do i=1, 4 ! First, let's compute properties for each blocks do j=1, nblocks diff --git a/src/anharmonic_free_energy/fourthorder.f90 b/src/anharmonic_free_energy/fourthorder.f90 index 5cea071e..73935fbc 100644 --- a/src/anharmonic_free_energy/fourthorder.f90 +++ b/src/anharmonic_free_energy/fourthorder.f90 @@ -329,8 +329,8 @@ subroutine free_energy_fourthorder_secondorder(uc, fcf, qp, dr, temperature, fe4 sig = sqrt(sig1 + sig2 + sig3 + sig4) f1 = (np1*np2*np3*np4 - n(1)*n(2)*n(3)*n(4)) / real(1.0_r8/(om1+om2+om3+om4+lo_imag*sig), r8) - f2 = 4.0_r8*(n(1)*np2*np3*np4 - np1*n(2)*n(3)*n(4)) * real(1.0/(-om1+om2+om3+om4 + lo_imag*sig)) - f3 = 3.0_r8*(n(1)*n(2)*(n(3)+n(4)+1.0_r8) - n(3)*n(4)*(n(1)+n(2)+1.0_r8))*real(1.0/(om1+om2-om3-om4 + lo_imag*sig)) + f2 = 4.0_r8*(n(1)*np2*np3*np4 - np1*n(2)*n(3)*n(4)) * real(1.0/(-om1+om2+om3+om4 + lo_imag*sig), r8) + f3 = 3.0_r8*(n(1)*n(2)*(n(3)+n(4)+1.0_r8) - n(3)*n(4)*(n(1)+n(2)+1.0_r8))*real(1.0/(om1+om2-om3-om4 + lo_imag*sig), r8) f0 = (f1 + f2 + f3) / 768.0_r8 else From e32d7b31ef812bc7e6dfe51ba686aca72f0bef5e Mon Sep 17 00:00:00 2001 From: =?UTF-8?q?Alo=C3=AFs=20Castellano?= Date: Fri, 4 Apr 2025 17:21:57 +0200 Subject: [PATCH 09/28] Fix some prefactor for quantum fourthorder --- src/anharmonic_free_energy/fourthorder.f90 | 6 +++--- 1 file changed, 3 insertions(+), 3 deletions(-) diff --git a/src/anharmonic_free_energy/fourthorder.f90 b/src/anharmonic_free_energy/fourthorder.f90 index 73935fbc..00884ecc 100644 --- a/src/anharmonic_free_energy/fourthorder.f90 +++ b/src/anharmonic_free_energy/fourthorder.f90 @@ -107,10 +107,10 @@ subroutine free_energy_fourthorder(uc, fcf, qp, dr, temperature, df4, s4, cv4, q f0 = (2.0_r8 * n1 + 1.0_r8) * (2.0_r8 * n2 + 1.0_r8) * psisq * prefactor / 32.0_r8 ! The entropy df0 = 2.0_r8 * dn1 * (2.0_r8 * n2 + 1.0_r8) + (2.0_r8 * n1 + 1.0_r8) * 2.0_r8 * dn2 - df0 = df0 * psisq * prefactor / 32.0_r8 + df0 = df0 / 32.0_r8 ddf0 = 2.0_r8 * ddn1 * (2.0_r8 * n2 + 1.0_r8) + 2.0_r8 * ddn2 * (2.0_r8 * n1 + 1.0_r8) + & 8.0_r8 * dn1 * dn2 - ddf0 = ddf0 * temperature * psisq * prefactor / 32.0_r8 + ddf0 = ddf0 * temperature / 32.0_r8 else ! Much simpler in the classical case ! Free energy @@ -123,7 +123,7 @@ subroutine free_energy_fourthorder(uc, fcf, qp, dr, temperature, df4, s4, cv4, q ! And we accumulate df4 = df4 + f0 * psisq * prefactor s4 = s4 - df0 * psisq * prefactor - cv4 = cv4 - df0 * psisq * prefactor + cv4 = cv4 - ddf0 * psisq * prefactor end do end do end do From c16073dd77ab903a5c6fdf6f93a05887d22b1175 Mon Sep 17 00:00:00 2001 From: =?UTF-8?q?Alo=C3=AFs=20Castellano?= Date: Tue, 8 Apr 2025 09:05:30 +0200 Subject: [PATCH 10/28] Fixing Fourier transform fourthorder --- src/anharmonic_free_energy/fourthorder.f90 | 5 +++-- 1 file changed, 3 insertions(+), 2 deletions(-) diff --git a/src/anharmonic_free_energy/fourthorder.f90 b/src/anharmonic_free_energy/fourthorder.f90 index 00884ecc..88cfd337 100644 --- a/src/anharmonic_free_energy/fourthorder.f90 +++ b/src/anharmonic_free_energy/fourthorder.f90 @@ -64,8 +64,10 @@ subroutine free_energy_fourthorder(uc, fcf, qp, dr, temperature, df4, s4, cv4, q t0 = walltime() df4 = 0.0_r8 + s4 = 0.0_r8 cv4 = 0.0_r8 + ctr = 0 do q1=1, qp%n_irr_point do q2=1, qp%n_full_point ctr = ctr + 1 @@ -147,7 +149,6 @@ subroutine free_energy_fourthorder(uc, fcf, qp, dr, temperature, df4, s4, cv4, q call mem%deallocate(evp3, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) call mem%deallocate(egv1, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) call mem%deallocate(egv2, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - end subroutine !> Calculate the fourth order free energy @@ -405,7 +406,7 @@ subroutine pretransform_phi4_first(fcf, q1, q2, ptf) rv4 = fcf%atom(a1)%quartet(q)%lv4 iqr = -dot_product(q1, rv2) + dot_product(q2, rv3) - dot_product(q2, rv4) - iqr = -iqr*lo_twopi + iqr = iqr*lo_twopi expiqr = cmplx(cos(iqr), sin(iqr), r8) do l = 1, 3 do k = 1, 3 From 315ebb5085238ed23579d0ed1ebbd6cbce356b98 Mon Sep 17 00:00:00 2001 From: =?UTF-8?q?Alo=C3=AFs=20Castellano?= Date: Tue, 20 May 2025 16:17:04 +0200 Subject: [PATCH 11/28] First part of big cleanup: MD-TDEP --- src/anharmonic_free_energy/epot.f90 | 393 ++++++++++++------ .../lo_thermodynamic_helpers.f90 | 36 +- src/anharmonic_free_energy/main.f90 | 234 ++++------- src/anharmonic_free_energy/options.f90 | 12 +- 4 files changed, 380 insertions(+), 295 deletions(-) diff --git a/src/anharmonic_free_energy/epot.f90 b/src/anharmonic_free_energy/epot.f90 index 03f29dca..a3c527af 100644 --- a/src/anharmonic_free_energy/epot.f90 +++ b/src/anharmonic_free_energy/epot.f90 @@ -202,7 +202,166 @@ subroutine setup_potential_energy_differences(pot, uc, ss, fc2, fc3, fc4, mw, ve end if end subroutine -subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, mw, mem) +! subroutine old_compute_realspace_thermo(pot, ss, sim, thermo, nblocks, mw, mem) +! !> container for potential energy differences +! class(lo_energy_differences), intent(in) :: pot +! !> The supercell +! type(lo_crystalstructure), intent(in) :: ss +! !> The simulation +! type(lo_mdsim), intent(in) :: sim +! !> The thermodynamic helper +! type(lo_thermodynamics), intent(inout) :: thermo +! !> Number of blocks +! integer, intent(in) :: nblocks +! !> MPI +! type(lo_mpi_helper), intent(inout) :: mw +! !> memory tracker +! type(lo_mem_helper), intent(inout) :: mem + +! real(r8), dimension(3, 4) :: cumulant, cumulant_var, cumcv, cumcv_var +! real(r8), dimension(3, 3, 4) :: stress_pot, stress_potvar +! !> The stress difference between true and ifcs +! real(r8), dimension(:, :, :, :), allocatable :: sdiff +! !> A little buffer for the stress +! real(r8), dimension(:, :, :), allocatable :: buf_stress +! !> The energy difference between true and ifcs +! real(r8), dimension(:, :), allocatable :: ediff +! !> Little buffers for the blocks +! real(r8), dimension(:, :), allocatable :: buf, bufcv +! !> The third order contribution to the stress +! real(r8), dimension(3, 3) :: s3 + +! !> Some buffers: energy, inverse kbt blabla +! real(r8) :: e2, e3, e4, ep, inverse_kbt, f0, f1 +! !> Some integers for do loops +! integer :: i, j, a, b, blocksize, istart, iend + +! !> Let's get the inverse temperature +! if (thermo%temperature .gt. 1E-5_r8) then +! inverse_kbt = 1.0_r8/lo_kb_Hartree/thermo%temperature +! else +! inverse_kbt = 0.0_r8 +! end if + +! ! Allocate stuffs +! call mem%allocate(ediff, [sim%nt, 4], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) +! call mem%allocate(sdiff, [sim%nt, 3, 3, 2], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) +! call mem%allocate(buf, [3, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) +! call mem%allocate(bufcv, [3, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) +! call mem%allocate(buf_stress, [3, 3, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) +! ediff = 0.0_r8 +! sdiff = 0.0_r8 +! buf = 0.0_r8 +! bufcv = 0.0_r8 +! buf_stress = 0.0_r8 + +! if (mw%talk) write(*, *) '... computing energy differences' + +! ! Let's compute energies and stress differences +! do i=1, sim%nt +! if (mod(i, mw%n) .ne. mw%r) cycle +! call pot%energies_and_forces(ss, sim%u(:, :, i), e2, e3, e4, ep, s3) +! ! We store the energy differences +! ediff(i, 1) = sim%stat%potential_energy(i) +! ediff(i, 2) = sim%stat%potential_energy(i) - e2 - ep +! ediff(i, 3) = sim%stat%potential_energy(i) - e2 - ep - e3 +! ediff(i, 4) = sim%stat%potential_energy(i) - e2 - ep - e3 - e4 + +! ! But also the stress differences +! sdiff(i, :, :, 1) = sim%stat%stress(:, :, i) +! sdiff(i, :, :, 2) = sim%stat%stress(:, :, i) - s3 +! end do +! ! And reduce everything +! call mw%allreduce('sum', ediff) +! call mw%allreduce('sum', sdiff) + +! if (mw%talk) write(*, *) '... computing free energy correction' + +! ! Ok now the messy part, here we compute the various correction +! ! We also estimate the uncertainty through block averaging +! ! TODO: is there a way to automatize the optimal number of blocks ? +! ! Need to look what math people think of this +! cumulant = 0.0_r8 +! cumulant_var = 0.0_r8 +! stress_pot = 0.0_r8 +! stress_potvar = 0.0_r8 +! blocksize = floor((real(sim%nt, r8)) / real(nblocks, r8)) +! do i=1, 4 +! ! First, let's compute properties for each blocks +! do j=1, nblocks +! ! Index for the blocks +! istart = blocksize*j +! iend = min(blocksize*(j+1), sim%nt) +! ! We compute the averages for each block +! f0 = lo_mean(ediff(istart:iend, i)) +! f1 = lo_mean(ediff(istart:iend, 1)) +! buf(1, j) = lo_mean(ediff(istart:iend, i)) +! buf(2, j) = lo_mean((ediff(istart:iend, i) - f0)**2) +! buf(3, j) = lo_mean((ediff(istart:iend, i) - f0)**3) +! bufcv(1, j) = lo_mean(ediff(istart:iend, 1)*ediff(istart:iend, i)) - f1*lo_mean(ediff(istart:iend,i)) +! bufcv(2, j) = lo_mean(ediff(istart:iend, 1)*ediff(istart:iend, i)**2) - f1*lo_mean(ediff(istart:iend,i)**2) +! ! Including the stress +! do a=1, 3 +! do b=1, 3 +! buf_stress(a, b, j) = lo_mean(sdiff(istart:iend, a, b, i)) +! end do +! end do +! end do +! ! First order cumulant +! cumulant(1, i) = lo_mean(buf(1, :)) +! cumulant_var(1, i) = sqrt(lo_mean((buf(1, :) - cumulant(1, i))**2)) +! ! Second order cumulant +! cumulant(2, i) = lo_mean(buf(2, :)) +! cumulant_var(2, i) = sqrt(lo_mean((buf(2, :) - cumulant(2, i))**2)) +! ! Third order cumulant +! cumulant(3, i) = lo_mean(buf(3, :)) +! cumulant_var(3, i) = sqrt(lo_mean((buf(3, :) - cumulant(3, i))**2)) +! ! Correction for the heat capacity +! cumcv(1, i) = lo_mean(bufcv(1, :)) +! cumcv_var(1, i) = sqrt(lo_mean((bufcv(1, :) - cumcv(1, i))**2)) +! ! Same for the stress +! if (i .lt. 3) then +! do a=1, 3 +! do b=1, 3 +! stress_pot(a, b, i) = lo_mean(buf_stress(a, b, :)) +! stress_potvar(a, b, i) = sqrt(lo_mean((buf_stress(a, b, :) - stress_pot(a, b, i))**2)) +! end do +! end do +! end if +! end do +! ! We add the prefactor for the cumulants +! cumulant = cumulant/real(ss%na, r8) +! cumulant_var = cumulant_var/real(ss%na, r8) +! cumulant(2, :) = 0.5_r8 * cumulant(2, :) * inverse_kbt +! cumulant_var(2, :) = 0.5_r8 * cumulant_var(2, :) * inverse_kbt +! cumulant(3, :) = cumulant(3, :) * inverse_kbt**2 / 6.0_r8 +! cumulant_var(3, :) = cumulant_var(3, :) * inverse_kbt**2 / 6.0_r8 +! cumcv = cumcv*inverse_kbt/thermo%temperature/real(ss%na, r8) +! cumcv_var = cumcv_var*inverse_kbt/thermo%temperature/real(ss%na, r8) + +! ! And we can store everything +! thermo%corr_fe = cumulant +! thermo%corr_fe_var = cumulant_var +! ! thermo%corr_s = s +! ! thermo%corr_s_var = s_var +! thermo%corr_cv = cumcv +! thermo%corr_cv_var = cumcv_var +! ! Stress included +! thermo%stress_pot(:, :) = stress_pot(:, :, 1) +! thermo%stress_potvar(:, :) = stress_potvar(:, :, 1) +! thermo%stress_diff(:, :) = stress_pot(:, :, 2) +! thermo%stress_diffvar(:, :) = stress_potvar(:, :, 2) + +! ! And we can deallocate +! call mem%deallocate(ediff, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) +! call mem%deallocate(sdiff, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) +! call mem%deallocate(buf, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) +! call mem%deallocate(bufcv, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) +! call mem%deallocate(buf_stress, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) +! end subroutine + + +subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, stochastic, mw, mem) !> container for potential energy differences class(lo_energy_differences), intent(in) :: pot !> The supercell @@ -213,151 +372,137 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, mw, mem) type(lo_thermodynamics), intent(inout) :: thermo !> Number of blocks integer, intent(in) :: nblocks + !> Are we within a stochastic sampling approach ? + logical, intent(in) :: stochastic !> MPI type(lo_mpi_helper), intent(inout) :: mw !> memory tracker type(lo_mem_helper), intent(inout) :: mem - real(r8), dimension(3, 4) :: cumulant, cumulant_var, cumcv, cumcv_var - real(r8), dimension(3, 3, 4) :: stress_pot, stress_potvar !> The stress difference between true and ifcs real(r8), dimension(:, :, :, :), allocatable :: sdiff - !> A little buffer for the stress - real(r8), dimension(:, :, :), allocatable :: buf_stress !> The energy difference between true and ifcs real(r8), dimension(:, :), allocatable :: ediff - !> Little buffers for the blocks - real(r8), dimension(:, :), allocatable :: buf, bufcv - !> The third order contribution to the stress - real(r8), dimension(3, 3) :: s3 - - !> Some buffers: energy, inverse kbt blabla - real(r8) :: e2, e3, e4, ep, inverse_kbt, f0, f1 - !> Some integers for do loops - integer :: i, j, a, b, blocksize, istart, iend - - !> Let's get the inverse temperature - if (thermo%temperature .gt. 1E-5_r8) then - inverse_kbt = 1.0_r8/lo_kb_Hartree/thermo%temperature - else - inverse_kbt = 0.0_r8 - end if ! Allocate stuffs call mem%allocate(ediff, [sim%nt, 4], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) call mem%allocate(sdiff, [sim%nt, 3, 3, 2], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%allocate(buf, [3, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%allocate(bufcv, [3, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%allocate(buf_stress, [3, 3, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) ediff = 0.0_r8 sdiff = 0.0_r8 - buf = 0.0_r8 - bufcv = 0.0_r8 - buf_stress = 0.0_r8 - - if (mw%talk) write(*, *) '... computing energy differences' ! Let's compute energies and stress differences - do i=1, sim%nt - if (mod(i, mw%n) .ne. mw%r) cycle - call pot%energies_and_forces(ss, sim%u(:, :, i), e2, e3, e4, ep, s3) - ! We store the energy differences - ediff(i, 1) = sim%stat%potential_energy(i) - ediff(i, 2) = sim%stat%potential_energy(i) - e2 - ep - ediff(i, 3) = sim%stat%potential_energy(i) - e2 - ep - e3 - ediff(i, 4) = sim%stat%potential_energy(i) - e2 - ep - e3 - e4 - - ! But also the stress differences - sdiff(i, :, :, 1) = sim%stat%stress(:, :, i) - sdiff(i, :, :, 2) = sim%stat%stress(:, :, i) - s3 - end do - ! And reduce everything - call mw%allreduce('sum', ediff) - call mw%allreduce('sum', sdiff) - - if (mw%talk) write(*, *) '... computing free energy correction' - - ! Ok now the messy part, here we compute the various correction - ! We also estimate the uncertainty through block averaging - ! TODO: is there a way to automatize the optimal number of blocks ? - ! Need to look what math people think of this - cumulant = 0.0_r8 - cumulant_var = 0.0_r8 - stress_pot = 0.0_r8 - stress_potvar = 0.0_r8 - blocksize = floor((real(sim%nt, r8)) / real(nblocks, r8)) - do i=1, 4 - ! First, let's compute properties for each blocks - do j=1, nblocks - ! Index for the blocks - istart = blocksize*j - iend = min(blocksize*(j+1), sim%nt) - ! We compute the averages for each block - f0 = lo_mean(ediff(istart:iend, i)) - f1 = lo_mean(ediff(istart:iend, 1)) - buf(1, j) = lo_mean(ediff(istart:iend, i)) - buf(2, j) = lo_mean((ediff(istart:iend, i) - f0)**2) - buf(3, j) = lo_mean((ediff(istart:iend, i) - f0)**3) - bufcv(1, j) = lo_mean(ediff(istart:iend, 1)*ediff(istart:iend, i)) - f1*lo_mean(ediff(istart:iend,i)) - bufcv(2, j) = lo_mean(ediff(istart:iend, 1)*ediff(istart:iend, i)**2) - f1*lo_mean(ediff(istart:iend,i)**2) - ! Including the stress + energy_computation: block + !> The stress contributions + real(r8), dimension(3, 3) :: s3 + !> The individual energy contributions + real(r8) :: e2, e3, e4, ep + !> Some integers + integer :: i + + do i=1, sim%nt + if (mod(i, mw%n) .ne. mw%r) cycle + call pot%energies_and_forces(ss, sim%u(:, :, i), e2, e3, e4, ep, s3) + ! We store the energy differences + ediff(i, 1) = sim%stat%potential_energy(i) + ediff(i, 2) = sim%stat%potential_energy(i) - e2 - ep + ediff(i, 3) = sim%stat%potential_energy(i) - e2 - ep - e3 + ediff(i, 4) = sim%stat%potential_energy(i) - e2 - ep - e3 - e4 + + ! But also the stress differences + sdiff(i, :, :, 1) = sim%stat%stress(:, :, i) + sdiff(i, :, :, 2) = sim%stat%stress(:, :, i) - s3 + end do + ! And reduce everything + call mw%allreduce('sum', ediff) + call mw%allreduce('sum', sdiff) + + if (mw%talk) write(*, *) '... computing energy differences' + end block energy_computation + + + averaging: block + !> Little buffers for the blocks + real(r8), dimension(:, :), allocatable :: buf, bufcv + !> A little buffer for the stress + real(r8), dimension(:, :, :), allocatable :: buf_stress + !> Some buffers: energy, inverse kbt blabla + real(r8) :: inverse_kbt, f0, f1, f2 + !> Some integers + integer :: i, j, a, b, blocksize, istart, iend + + real(r8), dimension(3, 3, 2) :: stress + real(r8), dimension(2) :: F, S, Cv, U0 + + !> Let's get the inverse temperature + if (thermo%temperature .gt. 1E-5_r8) then + inverse_kbt = 1.0_r8/lo_kb_Hartree/thermo%temperature + else + inverse_kbt = 0.0_r8 + end if + + call mem%allocate(buf, [3, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%allocate(bufcv, [3, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%allocate(buf_stress, [3, 3, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + buf = 0.0_r8 + bufcv = 0.0_r8 + buf_stress = 0.0_r8 + + ! We need the length of each block for the block averaging + blocksize = floor((real(sim%nt, r8)) / real(nblocks, r8)) + if (stochastic) then + else + do j=1, nblocks + ! Index for the block + istart = blocksize*j + iend = min(blocksize*(j+1), sim%nt) + ! Now we compute the average for each block + ! This is to get the U0 + f0 = lo_mean(ediff(istart:iend, 2)) + f1 = lo_mean(ediff(istart:iend, 1)) + buf(1, j) = f0 + ! This is to get the correction to the entropy + buf(2, j) = lo_mean((ediff(istart:iend, 2) - f0)**2) + ! This is to get the correction to the heat capacity + bufcv(1, j) = lo_mean((ediff(istart:iend, 1) - f1) * (ediff(istart:iend, 2) - f0)) + ! And the stress + do a=1, 3 + do b=1, 3 + buf_stress(a, b, j) = lo_mean(sdiff(istart:iend, a, b, 1)) + end do + end do + end do + ! First we get the U0 term + U0(1) = lo_mean(buf(1, :)) + U0(2) = sqrt(lo_mean((buf(1, :) - U0(1))**2)) + U0 = U0 / sim%na + + ! Now we need the entropy correction + S(1) = lo_mean(buf(2, :)) + S(2) = sqrt(lo_mean((buf(2, :) - S(1))**2)) + S = 0.5_r8 * lo_kb_Hartree * S * inverse_kbt**2 / sim%na + + ! And the heat capacity correction + Cv(1) = lo_mean(bufcv(1, :)) + Cv(2) = sqrt(lo_mean((bufcv(1, :) - Cv(1))**2)) + Cv = Cv * inverse_kbt / thermo%temperature / sim%na + + ! And the stress do a=1, 3 do b=1, 3 - buf_stress(a, b, j) = lo_mean(sdiff(istart:iend, a, b, i)) + stress(a, b, 1) = lo_mean(buf_stress(a, b, :)) + stress(a, b, 2) = sqrt(lo_mean((buf_stress(a, b, :) - stress(a, b, 1))**2)) end do end do - end do - ! First order cumulant - cumulant(1, i) = lo_mean(buf(1, :)) - cumulant_var(1, i) = sqrt(lo_mean((buf(1, :) - cumulant(1, i))**2)) - ! Second order cumulant - cumulant(2, i) = lo_mean(buf(2, :)) - cumulant_var(2, i) = sqrt(lo_mean((buf(2, :) - cumulant(2, i))**2)) - ! Third order cumulant - cumulant(3, i) = lo_mean(buf(3, :)) - cumulant_var(3, i) = sqrt(lo_mean((buf(3, :) - cumulant(3, i))**2)) - ! Correction for the heat capacity - cumcv(1, i) = lo_mean(bufcv(1, :)) - cumcv_var(1, i) = sqrt(lo_mean((bufcv(1, :) - cumcv(1, i))**2)) - ! Same for the stress - if (i .lt. 3) then - do a=1, 3 - do b=1, 3 - stress_pot(a, b, i) = lo_mean(buf_stress(a, b, :)) - stress_potvar(a, b, i) = sqrt(lo_mean((buf_stress(a, b, :) - stress_pot(a, b, i))**2)) - end do - end do + + ! And we store the results + thermo%first_order%F = U0 + thermo%second_order%F = -thermo%temperature * S + thermo%first_order%U = U0 + thermo%second_order%S = S + thermo%second_order%Cv = Cv + thermo%first_order%stress = stress end if - end do - ! We add the prefactor for the cumulants - cumulant = cumulant/real(ss%na, r8) - cumulant_var = cumulant_var/real(ss%na, r8) - cumulant(2, :) = 0.5_r8 * cumulant(2, :) * inverse_kbt - cumulant_var(2, :) = 0.5_r8 * cumulant_var(2, :) * inverse_kbt - cumulant(3, :) = cumulant(3, :) * inverse_kbt**2 / 6.0_r8 - cumulant_var(3, :) = cumulant_var(3, :) * inverse_kbt**2 / 6.0_r8 - cumcv = cumcv*inverse_kbt/thermo%temperature/real(ss%na, r8) - cumcv_var = cumcv_var*inverse_kbt/thermo%temperature/real(ss%na, r8) - - ! And we can store everything - thermo%corr_fe = cumulant - thermo%corr_fe_var = cumulant_var -! thermo%corr_s = s -! thermo%corr_s_var = s_var - thermo%corr_cv = cumcv - thermo%corr_cv_var = cumcv_var - ! Stress included - thermo%stress_pot(:, :) = stress_pot(:, :, 1) - thermo%stress_potvar(:, :) = stress_potvar(:, :, 1) - thermo%stress_diff(:, :) = stress_pot(:, :, 2) - thermo%stress_diffvar(:, :) = stress_potvar(:, :, 2) - - ! And we can deallocate - call mem%deallocate(ediff, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%deallocate(sdiff, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%deallocate(buf, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%deallocate(bufcv, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%deallocate(buf_stress, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + end block averaging end subroutine end module diff --git a/src/anharmonic_free_energy/lo_thermodynamic_helpers.f90 b/src/anharmonic_free_energy/lo_thermodynamic_helpers.f90 index 2f45cad8..51f0a7fc 100644 --- a/src/anharmonic_free_energy/lo_thermodynamic_helpers.f90 +++ b/src/anharmonic_free_energy/lo_thermodynamic_helpers.f90 @@ -1,6 +1,7 @@ #include "precompilerdefinitions" module lo_thermodynamic_helpers use konstanter, only: r8, lo_huge +use gottochblandat, only: lo_chop use type_crystalstructure, only: lo_crystalstructure use type_symmetryoperation, only: lo_operate_on_secondorder_tensor @@ -10,31 +11,27 @@ module lo_thermodynamic_helpers public :: lo_symmetrize_stress public :: lo_full_to_voigt +type lo_thermodynamic_contribution + ! The different contributions. First dimension is the result, second one the uncertainty + real(r8), dimension(2) :: F=0.0_r8 + real(r8), dimension(2) :: U=0.0_r8 + real(r8), dimension(2) :: S=0.0_r8 + real(r8), dimension(2) :: Cv=0.0_r8 + real(r8), dimension(3, 3, 2) :: stress=0.0_r8 +end type + !> A container for all thermodynamic results type lo_thermodynamics !> The temperature at which everything is evaluated real(r8) :: temperature=-lo_huge !> The volume real(r8) :: volume=-lo_huge - !> The free energies - real(r8) :: f0, f3, f4 - !> The internal energy - real(r8) :: u0, u3, u4 - !> The entropy - real(r8) :: s0, s3, s4 - !> The heat capacity at constant volume - real(r8) :: cv0, cv3, cv4 - !> The heat capacity at constant pressure - real(r8) :: cp0, cp3, cp4 - !> The cumulant corrections, first dimension is IFC, second is cumulant order - real(r8), dimension(3, 4) :: corr_fe=0.0_r8, corr_s=0.0_r8, corr_u=0.0_r8, corr_cv=0.0_r8 - !> The uncertainty for the cumulant corrections - real(r8), dimension(3, 4) :: corr_fe_var=0.0_r8, corr_s_var=0.0_r8, corr_u_var=0.0_r8, corr_cv_var=0.0_r8 - !> The pressure - real(r8) :: p=-lo_huge - !> The stress tensor - real(r8), dimension(3, 3) :: stress_pot, stress_kin, stress_potvar - real(r8), dimension(3, 3) :: stress_3ph, stress_diff, stress_diffvar + ! The things to hold results + type(lo_thermodynamic_contribution) :: harmonic + type(lo_thermodynamic_contribution) :: first_order + type(lo_thermodynamic_contribution) :: second_order + type(lo_thermodynamic_contribution) :: threephonon + type(lo_thermodynamic_contribution) :: fourphonon !> The thermal expansion real(r8), dimension(3, 3) :: alpha end type @@ -55,6 +52,7 @@ subroutine lo_symmetrize_stress(m, uc) tmp = tmp + lo_operate_on_secondorder_tensor(uc%sym%op(iop), m) end do m = tmp / real(uc%sym%n, r8) + m = lo_chop(m, sum(abs(m))*1e-6_r8) end subroutine ! Go from full 3x3 real space to 6 voigt notation diff --git a/src/anharmonic_free_energy/main.f90 b/src/anharmonic_free_energy/main.f90 index 515cb310..024919a1 100644 --- a/src/anharmonic_free_energy/main.f90 +++ b/src/anharmonic_free_energy/main.f90 @@ -130,35 +130,32 @@ program anharmonic_free_energy if (mw%talk) write(*, *) '... computing thermodynamic properties with harmonic dispersion' ! We start by computing everything we can from the harmonic phonons if (opts%quantum) then - thermo%f0 = dr%phonon_free_energy(temperature) - thermo%s0 = dr%phonon_entropy(temperature) - thermo%u0 = thermo%f0 + temperature * thermo%s0 - thermo%cv0 = dr%phonon_cv(temperature) - call dr%phonon_kinetic_stress(qp, uc, temperature, thermo%stress_kin) + thermo%harmonic%F(1) = dr%phonon_free_energy(temperature) + thermo%harmonic%S(1) = dr%phonon_entropy(temperature) + thermo%harmonic%U(1) = thermo%harmonic%F(1) + temperature * thermo%harmonic%S(1) + thermo%harmonic%Cv(1) = dr%phonon_cv(temperature) + call dr%phonon_kinetic_stress(qp, uc, temperature, thermo%harmonic%stress(:, :, 1)) else - thermo%f0 = dr%phonon_free_energy_classical(temperature) - thermo%u0 = 3.0_r8 * lo_kb_Hartree * temperature - thermo%s0 = (thermo%u0 - thermo%f0) / temperature - thermo%cv0 = 3.0_r8 * lo_kb_Hartree - thermo%stress_kin = 0.0_r8 + thermo%harmonic%F(1) = dr%phonon_free_energy_classical(temperature) + thermo%harmonic%U(1) = 3.0_r8 * lo_kb_Hartree * temperature + thermo%harmonic%S(1) = (thermo%harmonic%U(1) - thermo%harmonic%F(1)) / temperature + thermo%harmonic%Cv(1) = 3.0_r8 * lo_kb_Hartree + thermo%harmonic%stress = 0.0_r8 do i=1, 3 - thermo%stress_kin(i, i) = lo_kb_Hartree * temperature * uc%na / uc%volume + thermo%harmonic%stress(i, i, 1) = lo_kb_Hartree * temperature * uc%na / uc%volume end do end if ! Usually not needed here, but always a good idea to clean - call lo_symmetrize_stress(thermo%stress_kin, uc) - thermo%stress_kin = lo_chop(thermo%stress_kin, sum(abs(thermo%stress_kin))*1e-6_r8) + call lo_symmetrize_stress(thermo%harmonic%stress(:, :, 1), uc) ! If we have third order IFC, might as well compute elastic things if (opts%thirdorder) then if (mw%talk) write(*, *) '... computing third order contribution to elastic properties' - call elastic_thirdorder(uc, fc, fct, qp, dr, opts%temperature, thermo%stress_3ph, thermo%alpha, opts%quantum, mw, mem) - ! Now we symmetrize and store everything - call lo_symmetrize_stress(thermo%stress_3ph, uc) - thermo%stress_3ph = lo_chop(thermo%stress_3ph, sum(abs(thermo%stress_3ph))*1e-6_r8) + call elastic_thirdorder(uc, fc, fct, qp, dr, opts%temperature, thermo%threephonon%stress(:, :, 1), thermo%alpha, opts%quantum, mw, mem) + ! Now we symmetrize + call lo_symmetrize_stress(thermo%threephonon%stress(:, :, 1), uc) call lo_symmetrize_stress(thermo%alpha, uc) - thermo%alpha = lo_chop(thermo%alpha, sum(abs(thermo%alpha))*1e-6_r8) end if call tmr%tock('harmonic properties') end block latdyn @@ -209,7 +206,12 @@ program anharmonic_free_energy write(*, *) end if - call pot%compute_realspace_thermo(ss, sim, thermo, opts%nblocks, mw, mem) + call pot%compute_realspace_thermo(ss, sim, thermo, opts%nblocks, opts%stochastic, mw, mem) + ! We also need to symmetrize the stress tensor + call lo_symmetrize_stress(thermo%first_order%stress(:, :, 1), uc) + call lo_symmetrize_stress(thermo%first_order%stress(:, :, 2), uc) + call lo_symmetrize_stress(thermo%second_order%stress(:, :, 1), uc) + call lo_symmetrize_stress(thermo%second_order%stress(:, :, 2), uc) call tmr%tock('simulation') else @@ -242,10 +244,10 @@ program anharmonic_free_energy call dr%generate(qp, fc, uc, mw=mw, mem=mem, verbosity=opts%verbosity) call free_energy_thirdorder(uc, fct, qp, dr, opts%temperature, fe3, s3, cv3, opts%quantum, mw, mem) - thermo%f3 = fe3 - thermo%s3 = s3 - thermo%u3 = (fe3 + opts%temperature * s3) - thermo%cv3 = cv3 + thermo%threephonon%F = fe3 + thermo%threephonon%S = s3 + thermo%threephonon%U = (fe3 + opts%temperature * s3) + thermo%threephonon%Cv = cv3 end if call tmr%tock('three-phonon') @@ -271,10 +273,10 @@ program anharmonic_free_energy call dr%generate(qp, fc, uc, mw=mw, mem=mem, verbosity=opts%verbosity) call free_energy_fourthorder(uc, fcf, qp, dr, opts%temperature, fe4, s4, cv4, opts%quantum, mw, mem) - thermo%f4 = fe4 - thermo%s4 = s4 - thermo%u4 = (fe4 + opts%temperature * s4) - thermo%cv4 = cv4 + thermo%fourphonon%F = fe4 + thermo%fourphonon%S = s4 + thermo%fourphonon%U = (fe4 + opts%temperature * s4) + thermo%fourphonon%Cv = cv4 ! TODO set fourthorder, second order cumulant its own qpoint grid density ! call free_energy_fourthorder_secondorder(uc, fcf, qp, dr, opts%temperature, fe4, s4, cv4, opts%quantum, mw, mem) @@ -288,153 +290,89 @@ program anharmonic_free_energy end block latdyn4ph summary: block - !> The thermodynamic properties - real(r8), dimension(3, 4) :: fe, s, u, cv - !> The second order cumulants - real(r8), dimension(3, 4) :: fe2, s2, u2, cv2 - !> And their uncertainty - real(r8), dimension(3, 4) :: fe_unc, s_unc, u_unc, cv_unc - !> The thermodynamic properties - real(r8), dimension(3, 4) :: corr, corr_s, corr_cv - !> Properties at the harmonic level - real(r8) :: fharm, uharm, sharm, charm - !> Properties with first order cumulant, 2nd order IFC - real(r8) :: f2_1, vf2_1, u2_1, vu2_1, s2_1, vs2_1, c2_1, vc2_1 - !> Properties with second order cumulant, 2nd order IFC - real(r8) :: f2_2, vf2_2, u2_2, vu2_2, s2_2, vs2_2, c2_2, vc2_2 - !> Properties with first order cumulant, 3rd order IFC - real(r8) :: f3_1, vf3_1, u3_1, vu3_1, s3_1, vs3_1, c3_1, vc3_1 - !> The prefactor, depending if we have stochastic samples or not - real(r8) :: pref - real(r8) :: f0, f1, f2 - real(r8), dimension(3, 3) :: sigma + !> Unit conversion factor + real(r8) :: f_unit, e_unit, s_unit, c_unit, p_unit + !> Buffer for the stress tensor + real(r8), dimension(3, 3, 2) :: sigma + !> The pressure + real(r8), dimension(2) :: pressure character(len=1000) :: opfc, opff, opfs !> A tolerance to clean-up stress results real(r8) :: stol integer :: i - - if (opts%stochastic) then - pref = -1.0_r8 - else - pref = 1.0_r8 - end if - - ! Clean and symmetrize every stress tensor - stol = sum(abs(thermo%stress_pot)) * 1e-6_r8 - call lo_symmetrize_stress(thermo%stress_pot, uc) - thermo%stress_pot = lo_chop(thermo%stress_pot, stol) - call lo_symmetrize_stress(thermo%stress_potvar, uc) - thermo%stress_potvar = lo_chop(thermo%stress_potvar, stol) - call lo_symmetrize_stress(thermo%stress_diff, uc) - thermo%stress_diff = lo_chop(thermo%stress_diff, stol) - call lo_symmetrize_stress(thermo%stress_diffvar, uc) - thermo%stress_diffvar = lo_chop(thermo%stress_diffvar, stol) - - ! The harmonic values - fharm = thermo%f0 - uharm = thermo%u0 - sharm = thermo%s0 - charm = thermo%cv0 - ! This are all the values with the corrections - fe(1, :) = fharm + thermo%corr_fe(1, :) - s(1, :) = sharm + thermo%corr_s(1, :) - u(1, :) = uharm + thermo%corr_u(1, :) - cv(1, :) = charm + thermo%corr_cv(1, :) - ! And the second order cumulants - fe(2, :) = fharm + thermo%corr_fe(1, :) + pref * thermo%corr_fe(2, :) - s(2, :) = sharm + thermo%corr_s(1, :) + pref * thermo%corr_s(2, :) - u(2, :) = uharm + thermo%corr_u(1, :) + pref * thermo%corr_u(2, :) - cv(2, :) = charm + thermo%corr_cv(1, :) + pref * thermo%corr_cv(2, :) - - ! And now we add the other little corrections - fe(2, 3) = fe(2, 3) + thermo%f3 - s(2, 3) = s(2, 3) + thermo%s3 - u(2, 3) = u(2, 3) + thermo%u3 - cv(2, 3) = cv(2, 3) + thermo%s3 - - ! And nice units for display - fharm = fharm * lo_Hartree_to_eV - uharm = uharm * lo_Hartree_to_eV - sharm = sharm / lo_kb_Hartree - charm = charm / lo_kb_Hartree - fe = fe * lo_Hartree_to_eV - u = u * lo_Hartree_to_eV - s = s / lo_kb_Hartree - cv = cv / lo_kb_Hartree + real(r8), dimension(4) :: buf, var + + f_unit = lo_Hartree_to_eV + e_unit = lo_Hartree_to_eV + s_unit = 1.0 / lo_kb_Hartree + c_unit = 1.0 / lo_kb_Hartree + p_unit = lo_pressure_HartreeBohr_to_GPa + + ! Get the stress tensor + sigma = (thermo%harmonic%stress + thermo%first_order%stress + thermo%second_order%stress) * p_unit + ! And the pressure + pressure = 0.0_r8 + do i=1, 3 + pressure = pressure + sigma(i, i, :) / 3.0_r8 + end do if (mw%talk) then opfc = '(4(1X,A24))' opff = '(4(1X,F24.12))' opfs = '(3(1X,F24.12))' + buf(1) = thermo%harmonic%F(1) * f_unit + buf(2) = thermo%harmonic%U(1) * e_unit + buf(3) = thermo%harmonic%S(1) * s_unit + buf(4) = thermo%harmonic%Cv(1) * c_unit + var = 0.0_r8 write(*, *) '' write(*, *) 'SUMMARY OF RESULTS' write(*, *) '' write(*, *) 'Effective harmonic contribution: F = F_harm' write(*, opfc) 'Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' - write(*, opff) fharm, uharm, sharm, charm - + write(*, opff) buf + write(*, opff) var + + buf(1) = buf(1) + thermo%first_order%F(1) * f_unit + buf(2) = buf(2) + thermo%first_order%U(1) * e_unit + buf(3) = buf(3) + thermo%first_order%S(1) * s_unit + buf(4) = buf(4) + thermo%first_order%Cv(1) * c_unit + var(1) = var(1) + thermo%first_order%F(2) * f_unit + var(2) = var(2) + thermo%first_order%U(2) * e_unit + var(3) = var(3) + thermo%first_order%S(2) * s_unit + var(4) = var(4) + thermo%first_order%Cv(2) * c_unit write(*, *) '' write(*, *) 'Gibbs-Bogoliubov approximation: F = F_harm + ' write(*, opfc) 'Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' - write(*, opff) fe(1, 2), u(1, 2), s(1, 2), cv(1, 2) - write(*, opff) vf2_1, vu2_1, vs2_1, vc2_1 - + write(*, opff) buf + write(*, opff) var + + buf(1) = buf(1) + thermo%second_order%F(1) * f_unit + buf(2) = buf(2) + thermo%second_order%U(1) * e_unit + buf(3) = buf(3) + thermo%second_order%S(1) * s_unit + buf(4) = buf(4) + thermo%second_order%Cv(1) * c_unit + var(1) = var(1) + thermo%second_order%F(2) * f_unit + var(2) = var(2) + thermo%second_order%U(2) * e_unit + var(3) = var(3) + thermo%second_order%S(2) * s_unit + var(4) = var(4) + thermo%second_order%Cv(2) * c_unit write(*, *) '' - if (opts%stochastic) then - write(*, *) 'With second order cumulant correction: F = F_harm + - <(V-V_harm)^2> / 2kBT' - else - write(*, *) 'With second order cumulant correction: F = F_harm + + <(V-V_harm)^2> / 2kBT' - end if + write(*, *) 'Second order cumulant approximation to the free energy' write(*, opfc) 'Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' - write(*, opff) fe(2, 2), u(2, 2), s(2, 2), cv(2, 2) - write(*, opff) vf2_1+vf2_2, vu2_1+vu2_2, vs2_1+vs2_2, vc2_1+vc2_2 - - if (opts%thirdorder) then - write(*, *) '' - write(*, *) 'With first order cumulant correction, 2nd+3rd order IFC' - write(*, opfc) 'Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' - write(*, opff) fe(1, 3), u(1, 3), s(1, 3), cv(1, 3) - write(*, opff) vf3_1, vu3_1, vs3_1, vc3_1 - write(*, *) '' - write(*, *) 'With Second order cumulant correction, 2nd+3rd order IFC' - write(*, opfc) 'Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' - write(*, opff) fe(2, 3), u(2, 3), s(2, 3), cv(2, 3) - write(*, opff) vf3_1, vu3_1, vs3_1, vc3_1 - end if - + write(*, opff) buf + write(*, opff) var write(*, *) '' - sigma = (thermo%stress_pot + thermo%stress_kin) * lo_pressure_HartreeBohr_to_GPa + write(*, *) 'Elastic properties' + write(*, '(2(1X,A24))') 'Pressure [GPa]', 'Uncertainty [GPa]' + write(*, '(2(1X,F24.12))') -pressure(1), pressure(2) write(*, *) 'Stress tensor [GPa]' do i=1, 3 - write(*, opfs) sigma(i, :) + write(*, opfs) sigma(i, :, 1) end do - sigma = (thermo%stress_potvar) * lo_pressure_HartreeBohr_to_GPa - write(*, *) 'Uuncertainty [GPa]' + write(*, *) 'Uncertainty [GPa]' do i=1, 3 - write(*, opfs) sigma(i, :) + write(*, opfs) sigma(i, :, 2) end do - if (opts%thirdorder) then - write(*, *) '' - sigma = (thermo%stress_diff + thermo%stress_3ph + thermo%stress_kin) * lo_pressure_HartreeBohr_to_GPa - write(*, *) 'Stress tensor with third order correction [GPa]' - do i=1, 3 - write(*, opfs) sigma(i, :) - end do - sigma = (thermo%stress_diffvar) * lo_pressure_HartreeBohr_to_GPa - write(*, *) 'Uncertainty [GPa]' - do i=1, 3 - write(*, opfs) sigma(i, :) - end do - write(*, *) '' - sigma = thermo%alpha * 1e6_r8 - write(*, *) 'Anisotropic thermal expansion from third-order [1e-6/K]' - do i=1, 3 - write(*, opfs) sigma(i, :) - end do - write(*, *) 'Volumic thermal expansion [1e-6/K]' - write(*, '(1X,F24.12)') sigma(1, 1) + sigma(2, 2) + sigma(3, 3) - end if end if call tmr%stop() diff --git a/src/anharmonic_free_energy/options.f90 b/src/anharmonic_free_energy/options.f90 index af8f1f8a..71ef2fa8 100644 --- a/src/anharmonic_free_energy/options.f90 +++ b/src/anharmonic_free_energy/options.f90 @@ -108,11 +108,15 @@ subroutine parse(opts) call cli%get(switch='--qpoint_grid4ph', val=opts%qg4ph, error=lo_status); errctr = errctr + lo_status call cli%get(switch='--nblocks', val=opts%nblocks, error=lo_status); errctr = errctr + lo_status - ! If we have fourthorder we should also have thirdorder -! if (opts%fourthorder) opts%thirdorder = .true. - if (errctr .ne. 0) call lo_stop_gracefully(['Failed parsing the command line options'], lo_exitcode_baddim) + ! If we have MD data, makes no sense to use the high order correction + if (.not. opts%stochastic .and. (opts%thirdorder .or. opts%fourthorder)) then + write(*, *) 'Makes no sense to use higher order IFC if the configurations are not from a stochastic sampling' + stop + end if + + ! We have to enable thirdorder to use the qg3ph flag if (maxval(opts%qg3ph) .gt. 0 .and. .not. opts%thirdorder) then write(*, *) 'You have to enable thirdorder to use a three-phonon q-grid, stopping calculation.' stop @@ -121,6 +125,7 @@ subroutine parse(opts) opts%qg3ph = opts%qgrid end if + ! We have to enable fourthorder to use the qg4ph flag if (maxval(opts%qg4ph) .gt. 0 .and. .not. opts%fourthorder) then write(*, *) 'You have to enable fourthorder to use a four-phonon q-grid, stopping calculation.' stop @@ -129,7 +134,6 @@ subroutine parse(opts) write(*, *) opts%qg4ph opts%qg4ph = opts%qgrid end if - end subroutine end module From 18aafb364f02c398c4850d7aa9138d081e50b09b Mon Sep 17 00:00:00 2001 From: =?UTF-8?q?Alo=C3=AFs=20Castellano?= Date: Tue, 20 May 2025 17:20:44 +0200 Subject: [PATCH 12/28] forgot to add the main.f90 --- src/anharmonic_free_energy/epot.f90 | 41 ++++++++++++++++++++++++++++- src/anharmonic_free_energy/main.f90 | 27 +++++++++++++++---- 2 files changed, 62 insertions(+), 6 deletions(-) diff --git a/src/anharmonic_free_energy/epot.f90 b/src/anharmonic_free_energy/epot.f90 index a3c527af..cb5407c4 100644 --- a/src/anharmonic_free_energy/epot.f90 +++ b/src/anharmonic_free_energy/epot.f90 @@ -361,7 +361,7 @@ subroutine setup_potential_energy_differences(pot, uc, ss, fc2, fc3, fc4, mw, ve ! end subroutine -subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, stochastic, mw, mem) +subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, stochastic, thirdorder, fourthorder, mw, mem) !> container for potential energy differences class(lo_energy_differences), intent(in) :: pot !> The supercell @@ -374,6 +374,10 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, stochastic, m integer, intent(in) :: nblocks !> Are we within a stochastic sampling approach ? logical, intent(in) :: stochastic + !> Are we using thirdorder ? + logical, intent(in) :: thirdorder + !> Are we using fourthorder ? + logical, intent(in) :: fourthorder !> MPI type(lo_mpi_helper), intent(inout) :: mw !> memory tracker @@ -450,6 +454,41 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, stochastic, m ! We need the length of each block for the block averaging blocksize = floor((real(sim%nt, r8)) / real(nblocks, r8)) if (stochastic) then + ! For the stochastic, what we compute depends on the order included + do j=1, nblocks + ! Index for the block + istart = blocksize*j + iend = min(blocksize*(j+1), sim%nt) + ! Now we compute the average for each block + if (fourthorder) then + f0 = lo_mean(ediff(istart:iend, 4)) + else if (thirdorder) then + f0 = lo_mean(ediff(istart:iend, 3)) + else + f0 = lo_mean(ediff(istart:iend, 2)) + end if + buf(1, j) = f0 + + ! And the stress + if (fourthorder .or. thirdorder) then + do a=1, 3 + do b=1, 3 + buf_stress(a, b, j) = lo_mean(sdiff(istart:iend, a, b, 2)) + end do + end do + else + do a=1, 3 + do b=1, 3 + buf_stress(a, b, j) = lo_mean(sdiff(istart:iend, a, b, 1)) + end do + end do + end if + end do + ! First we get the U0 term + U0(1) = lo_mean(buf(1, :)) + U0(2) = sqrt(lo_mean((buf(1, :) - U0(1))**2)) + U0 = U0 / sim%na + ! Then the else do j=1, nblocks ! Index for the block diff --git a/src/anharmonic_free_energy/main.f90 b/src/anharmonic_free_energy/main.f90 index 024919a1..e38aa498 100644 --- a/src/anharmonic_free_energy/main.f90 +++ b/src/anharmonic_free_energy/main.f90 @@ -206,7 +206,8 @@ program anharmonic_free_energy write(*, *) end if - call pot%compute_realspace_thermo(ss, sim, thermo, opts%nblocks, opts%stochastic, mw, mem) + call pot%compute_realspace_thermo(ss, sim, thermo, opts%nblocks, & + opts%thirdorder, opts%fourthorder, opts%thirdorder, mw, mem) ! We also need to symmetrize the stress tensor call lo_symmetrize_stress(thermo%first_order%stress(:, :, 1), uc) call lo_symmetrize_stress(thermo%first_order%stress(:, :, 2), uc) @@ -244,10 +245,18 @@ program anharmonic_free_energy call dr%generate(qp, fc, uc, mw=mw, mem=mem, verbosity=opts%verbosity) call free_energy_thirdorder(uc, fct, qp, dr, opts%temperature, fe3, s3, cv3, opts%quantum, mw, mem) - thermo%threephonon%F = fe3 - thermo%threephonon%S = s3 - thermo%threephonon%U = (fe3 + opts%temperature * s3) - thermo%threephonon%Cv = cv3 + thermo%threephonon%F(1) = fe3 + thermo%threephonon%S(1) = s3 + thermo%threephonon%U(1) = (fe3 + opts%temperature * s3) + thermo%threephonon%Cv(1) = cv3 + ! If we are in the stochastic mode, we have to add it to the result + ! It's a second order correction + if (opts%stochastic) then + thermo%second_order%F(1) = thermo%second_order%F(1) +thermo%threephonon%F(1) + thermo%second_order%S(1) = thermo%second_order%S(1) +thermo%threephonon%S(1) + thermo%second_order%U(1) = thermo%second_order%U(1) +thermo%threephonon%U(1) + thermo%second_order%Cv(1) = thermo%second_order%Cv(1) + thermo%threephonon%Cv(1) + end if end if call tmr%tock('three-phonon') @@ -277,6 +286,14 @@ program anharmonic_free_energy thermo%fourphonon%S = s4 thermo%fourphonon%U = (fe4 + opts%temperature * s4) thermo%fourphonon%Cv = cv4 + ! If we are in the stochastic mode, we have to add it to the result + ! It's a first order correction + if (opts%stochastic) then + thermo%first_order%F(1) = thermo%first_order%F(1) + thermo%fourphonon%F(1) + thermo%first_order%U(1) = thermo%first_order%U(1) + thermo%fourphonon%U(1) + thermo%first_order%S(1) = thermo%first_order%S(1) + thermo%fourphonon%S(1) + thermo%first_order%Cv(1) = thermo%first_order%Cv(1) + thermo%fourphonon%Cv(1) + end if ! TODO set fourthorder, second order cumulant its own qpoint grid density ! call free_energy_fourthorder_secondorder(uc, fcf, qp, dr, opts%temperature, fe4, s4, cv4, opts%quantum, mw, mem) From e95f9db50b4acdeb97614d99650f61c5d5fa3334 Mon Sep 17 00:00:00 2001 From: =?UTF-8?q?Alo=C3=AFs=20Castellano?= Date: Tue, 20 May 2025 18:09:33 +0200 Subject: [PATCH 13/28] Fix for the block averaging in anharmonic_free_energy --- src/anharmonic_free_energy/epot.f90 | 28 +++++++++++++++------------- 1 file changed, 15 insertions(+), 13 deletions(-) diff --git a/src/anharmonic_free_energy/epot.f90 b/src/anharmonic_free_energy/epot.f90 index cb5407c4..f184be6a 100644 --- a/src/anharmonic_free_energy/epot.f90 +++ b/src/anharmonic_free_energy/epot.f90 @@ -425,17 +425,18 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, stochastic, t averaging: block + !> Buffer for the stress tensor + real(r8), dimension(3, 3, 2) :: stress + !> Buffer for the thermodynamic quantities + real(r8), dimension(2) :: F, S, Cv, U0 !> Little buffers for the blocks real(r8), dimension(:, :), allocatable :: buf, bufcv !> A little buffer for the stress real(r8), dimension(:, :, :), allocatable :: buf_stress !> Some buffers: energy, inverse kbt blabla - real(r8) :: inverse_kbt, f0, f1, f2 + real(r8) :: inverse_kbt, f0, f1, f2, blocksize !> Some integers - integer :: i, j, a, b, blocksize, istart, iend - - real(r8), dimension(3, 3, 2) :: stress - real(r8), dimension(2) :: F, S, Cv, U0 + integer :: i, j, a, b, istart, iend !> Let's get the inverse temperature if (thermo%temperature .gt. 1E-5_r8) then @@ -444,21 +445,21 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, stochastic, t inverse_kbt = 0.0_r8 end if - call mem%allocate(buf, [3, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%allocate(bufcv, [3, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%allocate(buf, [2, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%allocate(bufcv, [2, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) call mem%allocate(buf_stress, [3, 3, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) buf = 0.0_r8 bufcv = 0.0_r8 buf_stress = 0.0_r8 ! We need the length of each block for the block averaging - blocksize = floor((real(sim%nt, r8)) / real(nblocks, r8)) + blocksize = real(sim%nt, r8) / real(nblocks, r8) if (stochastic) then ! For the stochastic, what we compute depends on the order included do j=1, nblocks ! Index for the block - istart = blocksize*j - iend = min(blocksize*(j+1), sim%nt) + istart = ceiling(blocksize*(j-1) + 1) + iend = min(ceiling(blocksize*j), sim%nt) ! Now we compute the average for each block if (fourthorder) then f0 = lo_mean(ediff(istart:iend, 4)) @@ -492,8 +493,8 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, stochastic, t else do j=1, nblocks ! Index for the block - istart = blocksize*j - iend = min(blocksize*(j+1), sim%nt) + istart = ceiling(blocksize*(j-1) + 1) + iend = min(ceiling(blocksize*j), sim%nt) ! Now we compute the average for each block ! This is to get the U0 f0 = lo_mean(ediff(istart:iend, 2)) @@ -535,7 +536,8 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, stochastic, t ! And we store the results thermo%first_order%F = U0 - thermo%second_order%F = -thermo%temperature * S + thermo%second_order%F(1) = -thermo%temperature * S(1) + thermo%second_order%F(2) = thermo%temperature * S(2) thermo%first_order%U = U0 thermo%second_order%S = S thermo%second_order%Cv = Cv From 3c58dcca950e5c8b589e0631448c8d184d4a0e30 Mon Sep 17 00:00:00 2001 From: =?UTF-8?q?Alo=C3=AFs=20Castellano?= Date: Tue, 20 May 2025 21:07:46 +0200 Subject: [PATCH 14/28] A little bit of cleaning --- src/anharmonic_free_energy/energy.f90 | 522 ------------------------ src/anharmonic_free_energy/epot.f90 | 168 +------- src/anharmonic_free_energy/main.f90 | 39 +- src/anharmonic_free_energy/old.main.f90 | 253 ------------ src/anharmonic_free_energy/options.f90 | 3 +- 5 files changed, 31 insertions(+), 954 deletions(-) delete mode 100644 src/anharmonic_free_energy/energy.f90 delete mode 100644 src/anharmonic_free_energy/old.main.f90 diff --git a/src/anharmonic_free_energy/energy.f90 b/src/anharmonic_free_energy/energy.f90 deleted file mode 100644 index eaa52a9c..00000000 --- a/src/anharmonic_free_energy/energy.f90 +++ /dev/null @@ -1,522 +0,0 @@ -module energy -!! get the anharmonic free energy -use konstanter, only: r8, i8, lo_twopi, lo_freqtol, lo_imag, lo_sqtol, lo_status, lo_kb_Hartree -use gottochblandat, only: lo_stop_gracefully, tochar, walltime, lo_chop, lo_trueNtimes, & - lo_progressbar_init, lo_progressbar, lo_planck, lo_trapezoid_integration, open_file, & - lo_flattentensor, lo_sqnorm, lo_linspace, lo_mean, lo_clean_fractional_coordinates -use mpi_wrappers, only: lo_mpi_helper, MPI_DOUBLE_PRECISION, MPI_SUM, MPI_DOUBLE_COMPLEX, MPI_IN_PLACE -use lo_memtracker, only: lo_mem_helper -use type_crystalstructure, only: lo_crystalstructure -use type_forceconstant_secondorder, only: lo_forceconstant_secondorder -use type_forceconstant_thirdorder, only: lo_forceconstant_thirdorder -use type_forceconstant_fourthorder, only: lo_forceconstant_fourthorder -use type_qpointmesh, only: lo_fft_mesh -use type_phonon_dispersions, only: lo_phonon_dispersions - -implicit none -private - -public :: perturbative_anharmonic_free_energy - -contains - -!> Calculates the anharmonic contributions to the free energy -subroutine perturbative_anharmonic_free_energy(p, fct, fcf, qp, dr, temperature, free_energy_thirdorder, free_energy_fourthorder, & - fourthorder, quantum, mw, mem, verbosity) - !> crystal structure - type(lo_crystalstructure), intent(in) :: p - !> third order force constant - type(lo_forceconstant_thirdorder), intent(in) :: fct - !> fourth order force constant - type(lo_forceconstant_fourthorder), intent(in) :: fcf - !> q-point mesh - type(lo_fft_mesh), intent(in) :: qp - !> dispersions - type(lo_phonon_dispersions), intent(in) :: dr - !> temperature - real(r8) :: temperature - !> free energies - real(r8), intent(out) :: free_energy_thirdorder, free_energy_fourthorder - !> what to compute - logical, intent(in) :: quantum, fourthorder - !> mpi helper - type(lo_mpi_helper), intent(inout) :: mw - !> memory tracker - type(lo_mem_helper), intent(inout) :: mem - !> talk a lot? - integer, intent(in) :: verbosity - - complex(r8), dimension(:, :, :), allocatable :: nuvec1, nuvec2 - real(r8), dimension(:, :), allocatable :: en3, en4 - real(r8) :: t0, t1, timer - - ! Start timers - timer = walltime() - t0 = timer - t1 = timer - - ! Set basic things - init: block - real(r8) :: f0, f1 - integer :: iq, imode, ctr, iatom, ix, ialpha - - if (verbosity .gt. 0) then - write (*, *) '' - write (*, *) 'CALCULATING ANHARMONIC FREE ENERGY' - end if - - ! Get the scaled eigenvectors - call mem%allocate(nuvec1, [dr%n_mode, dr%n_mode, qp%n_irr_point], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%allocate(nuvec2, [dr%n_mode, dr%n_mode, qp%n_full_point], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - nuvec1 = 0.0_r8 - nuvec2 = 0.0_r8 - - ctr = 0 - do iq = 1, qp%n_irr_point - do imode = 1, dr%n_mode - ctr = ctr + 1 - if (mod(ctr, mw%n) .ne. mw%r) cycle - if (dr%iq(iq)%omega(imode) .gt. lo_freqtol) then - f0 = 1.0_r8/sqrt(dr%iq(iq)%omega(imode)) - else - f0 = 0.0_r8 - end if - do iatom = 1, p%na - f1 = p%invsqrtmass(iatom) - do ix = 1, 3 - ialpha = (iatom - 1)*3 + ix - nuvec1(ialpha, imode, iq) = dr%iq(iq)%egv(ialpha, imode)*f0*f1 - end do - end do - end do - end do - do iq = 1, qp%n_full_point - do imode = 1, dr%n_mode - ctr = ctr + 1 - if (mod(ctr, mw%n) .ne. mw%r) cycle - if (dr%aq(iq)%omega(imode) .gt. lo_freqtol) then - f0 = 1.0_r8/sqrt(dr%aq(iq)%omega(imode)) - else - f0 = 0.0_r8 - end if - do iatom = 1, p%na - f1 = p%invsqrtmass(iatom) - do ix = 1, 3 - ialpha = (iatom - 1)*3 + ix - nuvec2(ialpha, imode, iq) = dr%aq(iq)%egv(ialpha, imode)*f0*f1 - end do - end do - end do - end do - call mw%allreduce('sum', nuvec1) - call mw%allreduce('sum', nuvec2) - - ! Space for free energies per mode - call mem%allocate(en3, [dr%n_mode, qp%n_irr_point], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%allocate(en4, [dr%n_mode, qp%n_irr_point], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - en3 = 0.0_r8 - en4 = 0.0_r8 - - if (verbosity .gt. 0) then - t1 = walltime() - write (*, *) '... scaled vectors and made space (', tochar(t1 - t0), 's)' - t0 = t1 - end if - end block init - - ! Integrate out the free energy - third: block - real(r8), external :: zdotu - real(r8), parameter :: threephonon_prefactor = -1.0_r8/48.0_r8 - real(r8), parameter :: fourphonon_prefactor = 1.0_r8/32.0_r8 - real(r8), parameter :: onethird = 1.0_r8/3.0_r8 - complex(r8), dimension(:, :), allocatable :: buf_ev1, buf_ev2, buf_ev3 - complex(r8), dimension(:), allocatable :: evp1, evp2, evp3, ptf - complex(r8) :: c0 - real(r8), dimension(3) :: qv1, qv2, qv3 - real(r8) :: psisq, sigma, om1, om2, om3, n1, n2, n3, f1, f2, prefactor, s1, s2, s3 - integer :: ctr, b1, b2, b3, q1, q2, q3 - - ! Space for intermediate products - call mem%allocate(evp1, dr%n_mode**2, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%allocate(evp2, dr%n_mode**3, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%allocate(ptf, dr%n_mode**3, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%allocate(buf_ev1, [dr%n_mode, dr%n_mode], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%allocate(buf_ev2, [dr%n_mode, dr%n_mode], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%allocate(buf_ev3, [dr%n_mode, dr%n_mode], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - !call mem%allocate(buf_ev4,[dr%n_mode,dr%n_mode],persistent=.false.,scalable=.false.,file=__FILE__,line=__LINE__) - evp1 = 0.0_r8 - evp2 = 0.0_r8 - ptf = 0.0_r8 - buf_ev1 = 0.0_r8 - buf_ev2 = 0.0_r8 - buf_ev3 = 0.0_r8 - !buf_ev4=0.0_r8 - - ! Optimizations: - ! 1) check the prefactors, can maybe do those before in a neater way - ! 2) only have to go over half the q-vectors I think. - if (verbosity .gt. 0) call lo_progressbar_init() - en3 = 0.0_r8 - ctr = 0 - do q1 = 1, qp%n_irr_point - do q2 = 1, qp%n_full_point - ! make it parallel - ctr = ctr + 1 - if (mod(ctr, mw%n) .ne. mw%r) cycle - ! locate third q-vector - q3 = fft_third_grid_index(qp%ip(q1)%full_index, q2, qp%griddensity) - - qv1 = qp%ip(q1)%r - qv2 = qp%ap(q2)%r - qv3 = qp%ap(q3)%r - - prefactor = threephonon_prefactor*qp%ap(q2)%integration_weight - - ! pre-transform the matrix element - call pretransform_phi3(fct, qv2, qv3, ptf) - ! pre-fetch eigenvectors. Maybe a speedup, dunno. - buf_ev1 = nuvec1(:, :, q1) - buf_ev2 = nuvec2(:, :, q2) - buf_ev3 = nuvec2(:, :, q3) - - do b1 = 1, dr%n_mode - do b2 = 1, dr%n_mode - evp1 = 0.0_r8 - call zgeru(dr%n_mode, dr%n_mode, (1.0_r8, 0.0_r8), buf_ev2(:, b2), 1, buf_ev1(:, b1), 1, evp1, dr%n_mode) - do b3 = 1, dr%n_mode - evp2 = 0.0_r8 - call zgeru(dr%n_mode, dr%n_mode*dr%n_mode, (1.0_r8, 0.0_r8), buf_ev3(:, b3), 1, evp1, 1, evp2, dr%n_mode) - evp2 = conjg(evp2) - c0 = dot_product(evp2, ptf) - !c0=zdotu(dr%n_mode**3,evp2,1,ptf,1) - ! And now we have the matrix element. - psisq = real(conjg(c0)*c0, r8) - ! Get a smearing parameter - s1 = dr%default_smearing(b1) - s2 = dr%default_smearing(b2) - s3 = dr%default_smearing(b3) - sigma = sqrt(s1**2 + s2**2 + s3**2) - ! Same sigma as the usual case for debugging. - !sigma=lo_mean(dr%default_smearing) - om1 = dr%iq(q1)%omega(b1) - om2 = dr%aq(q2)%omega(b2) - om3 = dr%aq(q3)%omega(b3) - if (om1 .lt. lo_freqtol) cycle - if (om2 .lt. lo_freqtol) cycle - if (om3 .lt. lo_freqtol) cycle - ! Decide if we take the classical limit for the occupations - if (quantum) then - n1 = lo_planck(temperature, om1) - n2 = lo_planck(temperature, om2) - n3 = lo_planck(temperature, om3) - - ! This is the Wallace expression - ! f1=n1*n2+n1+onethird - ! f1=3*f1*real(1.0_r8/( om1+om2+om3+lo_imag*sigma )) - ! f2=2*n1*n3-n1*n2+n3 - ! f2=3*f2*real(1.0_r8/( om1+om2-om3+lo_imag*sigma )) - ! en3(b1,q1)=en3(b1,q1)+( (f1+f2)*psisq )*prefactor - - ! Try the Cowley expression instead? - else - n1 = lo_kb_Hartree*temperature/om1 - n2 = lo_kb_Hartree*temperature/om2 - n3 = lo_kb_Hartree*temperature/om3 - end if - f1 = (n1 + 1)*(n2 + n3 + 1) + n2*n3 - f2 = n1*n2 + n1*n3 - n2*n3 + 1 - f2 = 3*f2*real(1.0_r8/(om1 + om2 - om3 + lo_imag*sigma)) - f1 = f1*real(1.0_r8/(om1 + om2 + om3 + lo_imag*sigma)) - en3(b1, q1) = en3(b1, q1) + ((f1 + f2)*psisq)*prefactor - end do - end do - end do - end do - if (verbosity .gt. 0 .and. q1 .lt. qp%n_irr_point) then - call lo_progressbar(' ... third order', q1, qp%n_irr_point, walltime() - t0) - end if - end do - - ! Some cleanup - call mem%deallocate(evp1, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%deallocate(evp2, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%deallocate(ptf, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - - if (verbosity .gt. 0) then - t1 = walltime() - call lo_progressbar(' ... third order', qp%n_irr_point, qp%n_irr_point, t1 - t0) - t0 = t1 - end if - call mw%allreduce('sum', en3) - - if (fourthorder) then - ! Do the fourth order? Might as well. - call mem%allocate(evp1, dr%n_mode**2, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%allocate(evp2, dr%n_mode**2, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%allocate(evp3, dr%n_mode**4, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%allocate(ptf, dr%n_mode**4, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - evp1 = 0.0_r8 - evp2 = 0.0_r8 - evp3 = 0.0_r8 - ptf = 0.0_r8 - - if (verbosity .gt. 0) call lo_progressbar_init() - en4 = 0.0_r8 - ctr = 0 - do q1 = 1, qp%n_irr_point - do q2 = 1, qp%n_full_point - ! make it parallel - ctr = ctr + 1 - if (mod(ctr, mw%n) .ne. mw%r) cycle - qv1 = qp%ip(q1)%r - qv2 = qp%ap(q2)%r - prefactor = fourphonon_prefactor*qp%ap(q2)%integration_weight - - ! pre-transform the matrix element - call pretransform_phi4(fcf, qv1, qv2, ptf) - ! pre-fetch eigenvectors. Maybe a speedup, dunno. - buf_ev1 = nuvec1(:, :, q1) - buf_ev2 = nuvec2(:, :, q2) - do b1 = 1, dr%n_mode - do b2 = 1, dr%n_mode - om1 = dr%iq(q1)%omega(b1) - om2 = dr%aq(q2)%omega(b2) - if (om1 .lt. lo_freqtol) cycle - if (om2 .lt. lo_freqtol) cycle - ! Decide if we take the classical limit for the occupations - if (quantum) then - n1 = lo_planck(temperature, om1) - n2 = lo_planck(temperature, om2) - else - n1 = lo_kb_Hartree*temperature/om1 - n2 = lo_kb_Hartree*temperature/om2 - end if - ! Now to get - evp1 = 0.0_r8 - evp2 = 0.0_r8 - evp3 = 0.0_r8 - call zgerc(dr%n_mode, dr%n_mode, (1.0_r8, 0.0_r8), buf_ev1(:, b1), 1, buf_ev1(:, b1), 1, evp1, dr%n_mode) - call zgerc(dr%n_mode, dr%n_mode, (1.0_r8, 0.0_r8), buf_ev2(:, b2), 1, buf_ev2(:, b2), 1, evp2, dr%n_mode) - call zgeru(dr%n_mode**2, dr%n_mode**2, (1.0_r8, 0.0_r8), evp2, 1, evp1, 1, evp3, dr%n_mode**2) - evp3 = conjg(evp3) - psisq = real(dot_product(evp3, ptf), r8) - f1 = (2*n1 + 1)*(2*n2 + 1)*psisq*prefactor - - en4(b1, q1) = en4(b1, q1) + f1 - end do - end do - end do - if (verbosity .gt. 0 .and. q1 .lt. qp%n_irr_point) then - call lo_progressbar(' ... fourth order', q1, qp%n_irr_point, walltime() - t0) - end if - end do - - call mem%deallocate(evp1, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%deallocate(evp2, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%deallocate(evp3, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%deallocate(ptf, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%deallocate(buf_ev1, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%deallocate(buf_ev2, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%deallocate(buf_ev3, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - - if (verbosity .gt. 0) then - t1 = walltime() - call lo_progressbar(' ... fourth order', qp%n_irr_point, qp%n_irr_point, t1 - t0) - t0 = t1 - end if - call mw%allreduce('sum', en4) - end if - end block third - - ! add things up - finalize: block - integer :: q1 - - ! Add it up - free_energy_thirdorder = 0.0_r8 - free_energy_fourthorder = 0.0_r8 - do q1 = 1, qp%n_irr_point - free_energy_thirdorder = free_energy_thirdorder + sum(en3(:, q1))*qp%ip(q1)%integration_weight - if (fourthorder) then - free_energy_fourthorder = free_energy_fourthorder + sum(en4(:, q1))*qp%ip(q1)%integration_weight - end if - end do - ! And normalize it to be per atom - free_energy_thirdorder = free_energy_thirdorder/p%na - free_energy_fourthorder = free_energy_fourthorder/p%na - - ! and cleanup - call mem%deallocate(nuvec1, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%deallocate(nuvec2, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%deallocate(en3, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%deallocate(en4, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - end block finalize - - if (verbosity .gt. 0) then - t1 = walltime() - write (*, *) '... got anharmonic free energy (', tochar(t1 - timer), 's)' - end if - -end subroutine - -!> pre-transform to get half of the third order matrix element -subroutine pretransform_phi3(fct, q2, q3, ptf) - !> third order forceconstant - type(lo_forceconstant_thirdorder), intent(in) :: fct - !> q-vectors - real(r8), dimension(3), intent(in) :: q2, q3 - !> flattened, pretransformed matrix element - complex(r8), dimension(:), intent(out) :: ptf - - integer :: i, j, k, l - - complex(r8) :: expiqr - real(r8), dimension(3) :: rv2, rv3 - real(r8) :: iqr - integer :: a1, a2, a3, ia, ib, ic, t, nb - - nb = fct%na*3 - ptf = 0.0_r8 - do a1 = 1, fct%na - do t = 1, fct%atom(a1)%n - a2 = fct%atom(a1)%triplet(t)%i2 - a3 = fct%atom(a1)%triplet(t)%i3 - - rv2 = fct%atom(a1)%triplet(t)%lv2 - rv3 = fct%atom(a1)%triplet(t)%lv3 - - iqr = dot_product(q2, rv2) + dot_product(q3, rv3) - iqr = -iqr*lo_twopi - expiqr = cmplx(cos(iqr), sin(iqr), r8) - do i = 1, 3 - do j = 1, 3 - do k = 1, 3 - ia = (a1 - 1)*3 + i - ib = (a2 - 1)*3 + j - ic = (a3 - 1)*3 + k - ! Now for the grand flattening scheme, consistent with the zgeru operations above. - l = (ia - 1)*nb*nb + (ib - 1)*nb + ic - ptf(l) = ptf(l) + fct%atom(a1)%triplet(t)%m(i, j, k)*expiqr - end do - end do - end do - end do - end do -end subroutine - -!> pre-transform to get half of the fourth order matrix element -subroutine pretransform_phi4(fcf, q1, q2, ptf) - !> third order forceconstant - type(lo_forceconstant_fourthorder), intent(in) :: fcf - !> q-vectors - real(r8), dimension(3), intent(in) :: q1, q2 - !> flattened, pretransformed matrix element - complex(r8), dimension(:), intent(out) :: ptf - - integer :: i, j, k, l, m - - complex(r8) :: expiqr - real(r8), dimension(3) :: rv2, rv3, rv4 - real(r8) :: iqr - integer :: a1, a2, a3, a4, ia, ib, ic, id, q, nb - - nb = fcf%na*3 - ptf = 0.0_r8 - do a1 = 1, fcf%na - do q = 1, fcf%atom(a1)%n - a2 = fcf%atom(a1)%quartet(q)%i2 - a3 = fcf%atom(a1)%quartet(q)%i3 - a4 = fcf%atom(a1)%quartet(q)%i4 - - rv2 = fcf%atom(a1)%quartet(q)%lv2 - rv3 = fcf%atom(a1)%quartet(q)%lv3 - rv4 = fcf%atom(a1)%quartet(q)%lv4 - - iqr = -dot_product(q1, rv2) + dot_product(q2, rv3) - dot_product(q2, rv4) - iqr = -iqr*lo_twopi - expiqr = cmplx(cos(iqr), sin(iqr), r8) - do l = 1, 3 - do k = 1, 3 - do j = 1, 3 - do i = 1, 3 - ia = (a1 - 1)*3 + i - ib = (a2 - 1)*3 + j - ic = (a3 - 1)*3 + k - id = (a4 - 1)*3 + l - ! Now for the grand flattening scheme, consistent with the zgeru operations above. - m = (ia - 1)*nb*nb*nb + (ib - 1)*nb*nb + (ic - 1)*nb + id - ptf(m) = ptf(m) + fcf%atom(a1)%quartet(q)%m(i, j, k, l)*expiqr - end do - end do - end do - end do - end do - end do -end subroutine - -!> returns the index on the grid that gives q3=-q1-q2 -pure function fft_third_grid_index(i1, i2, dims) result(i3) - !> index to q1 - integer, intent(in) :: i1 - !> index to q2 - integer, intent(in) :: i2 - !> dimensions of the grid - integer, dimension(3), intent(in) :: dims - !> index to q3 - integer :: i3 - - integer, dimension(3) :: gi1, gi2, gi3 - integer :: l, k - - ! Convert triplet to singlet - gi1 = singlet_to_triplet(i1, dims(2), dims(3)) - gi2 = singlet_to_triplet(i2, dims(2), dims(3)) - do l = 1, 3 - gi3(l) = 3 - gi1(l) - gi2(l) - end do - do k = 1, 3 - do l = 1, 3 - if (gi3(l) .lt. 1) gi3(l) = gi3(l) + dims(l) - if (gi3(l) .gt. dims(l)) gi3(l) = gi3(l) - dims(l) - end do - end do - ! convert it back to a singlet - i3 = triplet_to_singlet(gi3, dims(2), dims(3)) - -contains - !> convert a linear index to a triplet - pure function singlet_to_triplet(l, ny, nz) result(gi) - !> linear index - integer, intent(in) :: l - !> second dimension - integer, intent(in) :: ny - !> third dimension - integer, intent(in) :: nz - !> grid-index - integer, dimension(3) :: gi - - integer :: i, j, k - - k = mod(l, nz) - if (k .eq. 0) k = nz - j = mod((l - k)/nz, ny) + 1 - i = (l - k - (j - 1)*nz)/(nz*ny) + 1 - gi = [i, j, k] - end function - !> convert a triplet index to a singlet - pure function triplet_to_singlet(gi, ny, nz) result(l) - !> grid-index - integer, dimension(3), intent(in) :: gi - !> second dimension - integer, intent(in) :: ny - !> third dimension - integer, intent(in) :: nz - !> linear index - integer :: l - - l = (gi(1) - 1)*ny*nz + (gi(2) - 1)*nz + gi(3) - end function -end function - -end module diff --git a/src/anharmonic_free_energy/epot.f90 b/src/anharmonic_free_energy/epot.f90 index f184be6a..b0fb8bd3 100644 --- a/src/anharmonic_free_energy/epot.f90 +++ b/src/anharmonic_free_energy/epot.f90 @@ -1,17 +1,15 @@ module epot !! Deal with many kinds of potential energy differences -use konstanter, only: r8, lo_pi, lo_twopi, lo_tol, lo_sqtol, lo_status, lo_Hartree_to_eV, lo_kb_hartree -use gottochblandat, only: tochar, walltime, lo_chop, lo_trueNtimes, lo_progressbar_init, & - lo_progressbar, lo_frobnorm, open_file, lo_flattentensor, lo_sqnorm, lo_outerproduct, lo_mean, & - lo_points_on_sphere, lo_mean, lo_stddev, lo_outerproduct +use konstanter, only: r8, lo_kb_hartree +use gottochblandat, only: tochar, walltime, lo_mean, lo_stddev use mpi_wrappers, only: lo_mpi_helper, lo_stop_gracefully use lo_memtracker, only: lo_mem_helper -!use geometryfunctions, only: lo_inscribed_sphere_in_box use type_crystalstructure, only: lo_crystalstructure use type_forceconstant_secondorder, only: lo_forceconstant_secondorder use type_forceconstant_thirdorder, only: lo_forceconstant_thirdorder use type_forceconstant_fourthorder, only: lo_forceconstant_fourthorder use type_mdsim, only: lo_mdsim + use lo_thermodynamic_helpers, only: lo_thermodynamics, lo_symmetrize_stress implicit none @@ -202,164 +200,6 @@ subroutine setup_potential_energy_differences(pot, uc, ss, fc2, fc3, fc4, mw, ve end if end subroutine -! subroutine old_compute_realspace_thermo(pot, ss, sim, thermo, nblocks, mw, mem) -! !> container for potential energy differences -! class(lo_energy_differences), intent(in) :: pot -! !> The supercell -! type(lo_crystalstructure), intent(in) :: ss -! !> The simulation -! type(lo_mdsim), intent(in) :: sim -! !> The thermodynamic helper -! type(lo_thermodynamics), intent(inout) :: thermo -! !> Number of blocks -! integer, intent(in) :: nblocks -! !> MPI -! type(lo_mpi_helper), intent(inout) :: mw -! !> memory tracker -! type(lo_mem_helper), intent(inout) :: mem - -! real(r8), dimension(3, 4) :: cumulant, cumulant_var, cumcv, cumcv_var -! real(r8), dimension(3, 3, 4) :: stress_pot, stress_potvar -! !> The stress difference between true and ifcs -! real(r8), dimension(:, :, :, :), allocatable :: sdiff -! !> A little buffer for the stress -! real(r8), dimension(:, :, :), allocatable :: buf_stress -! !> The energy difference between true and ifcs -! real(r8), dimension(:, :), allocatable :: ediff -! !> Little buffers for the blocks -! real(r8), dimension(:, :), allocatable :: buf, bufcv -! !> The third order contribution to the stress -! real(r8), dimension(3, 3) :: s3 - -! !> Some buffers: energy, inverse kbt blabla -! real(r8) :: e2, e3, e4, ep, inverse_kbt, f0, f1 -! !> Some integers for do loops -! integer :: i, j, a, b, blocksize, istart, iend - -! !> Let's get the inverse temperature -! if (thermo%temperature .gt. 1E-5_r8) then -! inverse_kbt = 1.0_r8/lo_kb_Hartree/thermo%temperature -! else -! inverse_kbt = 0.0_r8 -! end if - -! ! Allocate stuffs -! call mem%allocate(ediff, [sim%nt, 4], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) -! call mem%allocate(sdiff, [sim%nt, 3, 3, 2], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) -! call mem%allocate(buf, [3, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) -! call mem%allocate(bufcv, [3, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) -! call mem%allocate(buf_stress, [3, 3, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) -! ediff = 0.0_r8 -! sdiff = 0.0_r8 -! buf = 0.0_r8 -! bufcv = 0.0_r8 -! buf_stress = 0.0_r8 - -! if (mw%talk) write(*, *) '... computing energy differences' - -! ! Let's compute energies and stress differences -! do i=1, sim%nt -! if (mod(i, mw%n) .ne. mw%r) cycle -! call pot%energies_and_forces(ss, sim%u(:, :, i), e2, e3, e4, ep, s3) -! ! We store the energy differences -! ediff(i, 1) = sim%stat%potential_energy(i) -! ediff(i, 2) = sim%stat%potential_energy(i) - e2 - ep -! ediff(i, 3) = sim%stat%potential_energy(i) - e2 - ep - e3 -! ediff(i, 4) = sim%stat%potential_energy(i) - e2 - ep - e3 - e4 - -! ! But also the stress differences -! sdiff(i, :, :, 1) = sim%stat%stress(:, :, i) -! sdiff(i, :, :, 2) = sim%stat%stress(:, :, i) - s3 -! end do -! ! And reduce everything -! call mw%allreduce('sum', ediff) -! call mw%allreduce('sum', sdiff) - -! if (mw%talk) write(*, *) '... computing free energy correction' - -! ! Ok now the messy part, here we compute the various correction -! ! We also estimate the uncertainty through block averaging -! ! TODO: is there a way to automatize the optimal number of blocks ? -! ! Need to look what math people think of this -! cumulant = 0.0_r8 -! cumulant_var = 0.0_r8 -! stress_pot = 0.0_r8 -! stress_potvar = 0.0_r8 -! blocksize = floor((real(sim%nt, r8)) / real(nblocks, r8)) -! do i=1, 4 -! ! First, let's compute properties for each blocks -! do j=1, nblocks -! ! Index for the blocks -! istart = blocksize*j -! iend = min(blocksize*(j+1), sim%nt) -! ! We compute the averages for each block -! f0 = lo_mean(ediff(istart:iend, i)) -! f1 = lo_mean(ediff(istart:iend, 1)) -! buf(1, j) = lo_mean(ediff(istart:iend, i)) -! buf(2, j) = lo_mean((ediff(istart:iend, i) - f0)**2) -! buf(3, j) = lo_mean((ediff(istart:iend, i) - f0)**3) -! bufcv(1, j) = lo_mean(ediff(istart:iend, 1)*ediff(istart:iend, i)) - f1*lo_mean(ediff(istart:iend,i)) -! bufcv(2, j) = lo_mean(ediff(istart:iend, 1)*ediff(istart:iend, i)**2) - f1*lo_mean(ediff(istart:iend,i)**2) -! ! Including the stress -! do a=1, 3 -! do b=1, 3 -! buf_stress(a, b, j) = lo_mean(sdiff(istart:iend, a, b, i)) -! end do -! end do -! end do -! ! First order cumulant -! cumulant(1, i) = lo_mean(buf(1, :)) -! cumulant_var(1, i) = sqrt(lo_mean((buf(1, :) - cumulant(1, i))**2)) -! ! Second order cumulant -! cumulant(2, i) = lo_mean(buf(2, :)) -! cumulant_var(2, i) = sqrt(lo_mean((buf(2, :) - cumulant(2, i))**2)) -! ! Third order cumulant -! cumulant(3, i) = lo_mean(buf(3, :)) -! cumulant_var(3, i) = sqrt(lo_mean((buf(3, :) - cumulant(3, i))**2)) -! ! Correction for the heat capacity -! cumcv(1, i) = lo_mean(bufcv(1, :)) -! cumcv_var(1, i) = sqrt(lo_mean((bufcv(1, :) - cumcv(1, i))**2)) -! ! Same for the stress -! if (i .lt. 3) then -! do a=1, 3 -! do b=1, 3 -! stress_pot(a, b, i) = lo_mean(buf_stress(a, b, :)) -! stress_potvar(a, b, i) = sqrt(lo_mean((buf_stress(a, b, :) - stress_pot(a, b, i))**2)) -! end do -! end do -! end if -! end do -! ! We add the prefactor for the cumulants -! cumulant = cumulant/real(ss%na, r8) -! cumulant_var = cumulant_var/real(ss%na, r8) -! cumulant(2, :) = 0.5_r8 * cumulant(2, :) * inverse_kbt -! cumulant_var(2, :) = 0.5_r8 * cumulant_var(2, :) * inverse_kbt -! cumulant(3, :) = cumulant(3, :) * inverse_kbt**2 / 6.0_r8 -! cumulant_var(3, :) = cumulant_var(3, :) * inverse_kbt**2 / 6.0_r8 -! cumcv = cumcv*inverse_kbt/thermo%temperature/real(ss%na, r8) -! cumcv_var = cumcv_var*inverse_kbt/thermo%temperature/real(ss%na, r8) - -! ! And we can store everything -! thermo%corr_fe = cumulant -! thermo%corr_fe_var = cumulant_var -! ! thermo%corr_s = s -! ! thermo%corr_s_var = s_var -! thermo%corr_cv = cumcv -! thermo%corr_cv_var = cumcv_var -! ! Stress included -! thermo%stress_pot(:, :) = stress_pot(:, :, 1) -! thermo%stress_potvar(:, :) = stress_potvar(:, :, 1) -! thermo%stress_diff(:, :) = stress_pot(:, :, 2) -! thermo%stress_diffvar(:, :) = stress_potvar(:, :, 2) - -! ! And we can deallocate -! call mem%deallocate(ediff, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) -! call mem%deallocate(sdiff, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) -! call mem%deallocate(buf, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) -! call mem%deallocate(bufcv, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) -! call mem%deallocate(buf_stress, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) -! end subroutine - subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, stochastic, thirdorder, fourthorder, mw, mem) !> container for potential energy differences @@ -524,7 +364,7 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, stochastic, t ! And the heat capacity correction Cv(1) = lo_mean(bufcv(1, :)) Cv(2) = sqrt(lo_mean((bufcv(1, :) - Cv(1))**2)) - Cv = Cv * inverse_kbt / thermo%temperature / sim%na + Cv = Cv * inverse_kbt**2 * lo_kb_Hartree / sim%na ! And the stress do a=1, 3 diff --git a/src/anharmonic_free_energy/main.f90 b/src/anharmonic_free_energy/main.f90 index e38aa498..af78b723 100644 --- a/src/anharmonic_free_energy/main.f90 +++ b/src/anharmonic_free_energy/main.f90 @@ -1,10 +1,8 @@ program anharmonic_free_energy !!{!src/anharmonic_free_energy/manual.md!} -use konstanter, only: r8, lo_Hartree_to_eV, lo_kb_Hartree, lo_pressure_HartreeBohr_to_GPa, lo_tol, lo_status, lo_freqtol, & -lo_twopi, lo_time_au_to_fs -use gottochblandat, only: open_file, walltime, lo_linspace, lo_progressbar_init, lo_progressbar, tochar, & - lo_does_file_exist, lo_mean, lo_stddev, lo_harmonic_oscillator_internal_energy, lo_chop, & - lo_invert_real_matrix, lo_harmonic_oscillator_cv, tochar +use konstanter, only: r8, lo_Hartree_to_eV, lo_kb_Hartree, lo_pressure_HartreeBohr_to_GPa, & + lo_tol, lo_status +use gottochblandat, only: open_file, walltime, tochar, lo_does_file_exist, open_file use mpi_wrappers, only: lo_mpi_helper use lo_memtracker, only: lo_mem_helper use lo_timetracker, only: lo_timer @@ -13,10 +11,9 @@ program anharmonic_free_energy use type_forceconstant_thirdorder, only: lo_forceconstant_thirdorder use type_forceconstant_fourthorder, only: lo_forceconstant_fourthorder use type_mdsim, only: lo_mdsim -use type_qpointmesh, only: lo_qpoint_mesh, lo_generate_qmesh, lo_read_qmesh_from_file, lo_fft_mesh +use type_qpointmesh, only: lo_qpoint_mesh, lo_generate_qmesh use type_phonon_dispersions, only: lo_phonon_dispersions use lo_phonon_bandstructure_on_path, only: lo_phonon_bandstructure -use type_phonon_dos, only: lo_phonon_dos use options, only: lo_opts use thirdorder, only: free_energy_thirdorder, elastic_thirdorder @@ -295,12 +292,8 @@ program anharmonic_free_energy thermo%first_order%Cv(1) = thermo%first_order%Cv(1) + thermo%fourphonon%Cv(1) end if - ! TODO set fourthorder, second order cumulant its own qpoint grid density + ! TODO set fourthorder, second order cumulant its own qpoint grid density, too expensive otherwise ! call free_energy_fourthorder_secondorder(uc, fcf, qp, dr, opts%temperature, fe4, s4, cv4, opts%quantum, mw, mem) -! thermo%f4 = thermo%f4 + fe4 -! thermo%s4 = thermo%s4 + s4 -! thermo%u4 = thermo%u4 + (fe4 + opts%temperature * s4) -! thermo%cv4 = thermo%cv4 + cv4 end if call tmr%tock('four-phonon') @@ -316,7 +309,7 @@ program anharmonic_free_energy character(len=1000) :: opfc, opff, opfs !> A tolerance to clean-up stress results real(r8) :: stol - integer :: i + integer :: i, u real(r8), dimension(4) :: buf, var f_unit = lo_Hartree_to_eV @@ -334,6 +327,9 @@ program anharmonic_free_energy end do if (mw%talk) then + u = open_file('out', 'outfile.anharmonic_free_energy') + write(u, '(A2,A12,8X,E20.12)') '# ', 'Temperature:', opts%temperature + opfc = '(4(1X,A24))' opff = '(4(1X,F24.12))' opfs = '(3(1X,F24.12))' @@ -349,11 +345,17 @@ program anharmonic_free_energy write(*, opfc) 'Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' write(*, opff) buf write(*, opff) var + write(u, *) '# Effective harmonic contribution: F = F_harm' + write(u, opfc) '# Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' + write(u, opff) buf + write(u, opff) var + ! Update the values buf(1) = buf(1) + thermo%first_order%F(1) * f_unit buf(2) = buf(2) + thermo%first_order%U(1) * e_unit buf(3) = buf(3) + thermo%first_order%S(1) * s_unit buf(4) = buf(4) + thermo%first_order%Cv(1) * c_unit + ! And the uncertainty var(1) = var(1) + thermo%first_order%F(2) * f_unit var(2) = var(2) + thermo%first_order%U(2) * e_unit var(3) = var(3) + thermo%first_order%S(2) * s_unit @@ -363,11 +365,17 @@ program anharmonic_free_energy write(*, opfc) 'Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' write(*, opff) buf write(*, opff) var + write(u, *) '# Gibbs-Bogoliubov approximation: F = F_harm + ' + write(u, opfc) '# Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' + write(u, opff) buf + write(u, opff) var + ! Update the values buf(1) = buf(1) + thermo%second_order%F(1) * f_unit buf(2) = buf(2) + thermo%second_order%U(1) * e_unit buf(3) = buf(3) + thermo%second_order%S(1) * s_unit buf(4) = buf(4) + thermo%second_order%Cv(1) * c_unit + ! And the uncertainty var(1) = var(1) + thermo%second_order%F(2) * f_unit var(2) = var(2) + thermo%second_order%U(2) * e_unit var(3) = var(3) + thermo%second_order%S(2) * s_unit @@ -377,6 +385,10 @@ program anharmonic_free_energy write(*, opfc) 'Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' write(*, opff) buf write(*, opff) var + write(u, *) '# Second order cumulant approximation to the free energy' + write(u, opfc) '# Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' + write(u, opff) buf + write(u, opff) var write(*, *) '' write(*, *) 'Elastic properties' @@ -390,6 +402,7 @@ program anharmonic_free_energy do i=1, 3 write(*, opfs) sigma(i, :, 2) end do + close(u) end if call tmr%stop() diff --git a/src/anharmonic_free_energy/old.main.f90 b/src/anharmonic_free_energy/old.main.f90 deleted file mode 100644 index 29509e94..00000000 --- a/src/anharmonic_free_energy/old.main.f90 +++ /dev/null @@ -1,253 +0,0 @@ -program anharmonic_free_energy -!!{!src/anharmonic_free_energy/manual.md!} -use konstanter, only: r8, lo_Hartree_to_eV, lo_kb_Hartree, lo_pressure_HartreeBohr_to_GPa -use gottochblandat, only: open_file, walltime, lo_linspace, lo_progressbar_init, lo_progressbar, tochar, & - lo_does_file_exist, lo_mean, lo_stddev -use mpi_wrappers, only: lo_mpi_helper -use lo_memtracker, only: lo_mem_helper -use lo_timetracker, only: lo_timer -use type_crystalstructure, only: lo_crystalstructure -use type_forceconstant_secondorder, only: lo_forceconstant_secondorder -use type_forceconstant_thirdorder, only: lo_forceconstant_thirdorder -use type_forceconstant_fourthorder, only: lo_forceconstant_fourthorder -use type_mdsim, only: lo_mdsim -use type_qpointmesh, only: lo_qpoint_mesh, lo_generate_qmesh, lo_read_qmesh_from_file, lo_fft_mesh -use type_phonon_dispersions, only: lo_phonon_dispersions -use lo_phonon_bandstructure_on_path, only: lo_phonon_bandstructure -use type_phonon_dos, only: lo_phonon_dos - -use options, only: lo_opts -use energy, only: perturbative_anharmonic_free_energy -use epot, only: lo_energy_differences -use type_thermodynamics, only: lo_thermodynamics - -implicit none - -type(lo_opts) :: opts -type(lo_forceconstant_secondorder) :: fc -type(lo_forceconstant_thirdorder) :: fct -type(lo_forceconstant_fourthorder) :: fcf -type(lo_phonon_dispersions) :: dr -type(lo_crystalstructure) :: uc -class(lo_qpoint_mesh), allocatable :: qp -type(lo_mpi_helper) :: mw -type(lo_mem_helper) :: mem -type(lo_timer) :: tmr -type(lo_mdsim) :: sim - -type(lo_thermodynamics) :: thermo -real(r8), dimension(3, 5) :: cumulant -real(r8) :: timer_init, timer_total -real(r8) :: U0, U1, energy_unit_factor -logical :: havehighorder - -! Init MPI, timers and options -call mw%init() -timer_total = walltime() -timer_init = walltime() -call opts%parse() -call tmr%start() - -! set up all possible meshes and get all dispersions -init: block - integer :: t, u - - ! only be verbose on the first rank - if (.not. mw%talk) opts%verbosity = -10 - - ! Read structure - call uc%readfromfile('infile.ucposcar', verbosity=opts%verbosity) - call uc%classify('wedge', timereversal=.true.) - if (mw%talk) write (*, *) '... read unitcell' - - ! Read forceconstants - call fc%readfromfile(uc, 'infile.forceconstant', mem, verbosity=-1) - if (mw%talk) write (*, *) '... read second order forceconstant' - - if (opts%thirdorder) call fct%readfromfile(uc, 'infile.forceconstant_thirdorder') - if (opts%fourthorder) call fcf%readfromfile(uc, 'infile.forceconstant_fourthorder') - havehighorder = .false. - if (opts%thirdorder .or. opts%fourthorder) havehighorder = .true. - - call tmr%tock('reading input') - - ! Get a q-mesh for the integrations. Always an FFT mesh. - if (mw%talk) write (*, *) '... generating q-mesh' - call lo_generate_qmesh(qp, uc, opts%qgrid, 'fft', timereversal=.true., headrankonly=.false., mw=mw, mem=mem, verbosity=opts%verbosity) - - ! Dispersions for everyone! - call dr%generate(qp, fc, uc, mw=mw, mem=mem, verbosity=opts%verbosity) - if (mw%talk) write (*, *) '... got the full dispersion relations' - call tmr%tock('harmonic properties') - - ! Check for imaginary modes right away - if (dr%omega_min .lt. 0.0_r8) then - ! Dump the free energies - if (mw%talk) then - write (*, *) 'Found negative eigenvalues. Stopping prematurely since no free energy can be defined.' - end if - call mw%destroy() - stop - end if - timer_init = walltime() - timer_init - -end block init - -! We start with the potential energy terms since those are much faster -epotthings: block - type(lo_energy_differences) :: pot - type(lo_crystalstructure) :: ss - - real(r8), dimension(:, :), allocatable :: f2, f3, f4, fp - real(r8), dimension(:, :), allocatable :: ediff - - real(r8) :: e2, e3, e4, ep, inverse_kbt - integer :: i - - call ss%readfromfile('infile.ssposcar') - call ss%classify('supercell', uc) - call pot%setup(uc, ss, fc, fct, fcf, mw, opts%verbosity + 1) - - thermo%volume = uc%volume - - ! Fetch simulation data from file - if (lo_does_file_exist('infile.sim.hdf5')) then - call sim%read_from_hdf5('infile.sim.hdf5', verbosity=opts%verbosity + 2, stride=-1) - else - call sim%read_from_file(verbosity=opts%verbosity + 2, stride=1, magnetic=.false., dielectric=.false., nrand=-1, mw=mw) - end if - - allocate (f2(3, ss%na)) - allocate (f3(3, ss%na)) - allocate (f4(3, ss%na)) - allocate (fp(3, ss%na)) - - ! Calculate the baseline energy - allocate (ediff(sim%nt, 5)) - ediff = 0.0_r8 - - do i = 1, sim%nt - if (mod(i, mw%n) .ne. mw%r) cycle - call pot%energies_and_forces(sim%u(:, :, i), e2, e3, e4, ep, f2, f3, f4, fp) - ediff(i, 1) = sim%stat%potential_energy(i) - ediff(i, 2) = sim%stat%potential_energy(i) - e2 - ediff(i, 3) = sim%stat%potential_energy(i) - e2 - ep - ediff(i, 4) = sim%stat%potential_energy(i) - e2 - ep - e3 - ediff(i, 5) = sim%stat%potential_energy(i) - e2 - ep - e3 - e4 - end do - call mw%allreduce('sum', ediff) - - if (sim%temperature_thermostat .gt. 1E-5_r8) then - inverse_kbt = 1.0_r8/lo_kb_Hartree/sim%temperature_thermostat - else - inverse_kbt = 0.0_r8 - end if - - ! Compute the first and second order cumulants - do i = 1, 5 - cumulant(1, i) = lo_mean(ediff(:, i)) - cumulant(2, i) = lo_mean((ediff(:, i) - cumulant(1, i))**2) - cumulant(2, i) = cumulant(2, i)*inverse_kbt*0.5_r8 - cumulant(3, i) = lo_mean((ediff(:, i) - cumulant(1, i))**3) - cumulant(3, i) = cumulant(3, i)*inverse_kbt**2/6.0_r8 - end do - - ! And normalize it to be per atom - cumulant = cumulant/real(ss%na, r8) - - if (mw%talk) then - write (*, *) 'Temperature (K) (from infile.meta): ', sim%temperature_thermostat - write (*, *) 'Potential energy:' - write (*, "(1X,A,E21.14,1X,A,F21.14)") ' input: ', cumulant(1, 1)*lo_Hartree_to_eV, ' upper bound:', cumulant(2, 1)*lo_Hartree_to_eV - write (*, "(1X,A,E21.14,1X,A,F21.14)") ' E-fc2: ', cumulant(1, 2)*lo_Hartree_to_eV, ' upper bound:', cumulant(2, 2)*lo_Hartree_to_eV - write (*, "(1X,A,E21.14,1X,A,F21.14)") ' E-fc2-polar: ', cumulant(1, 3)*lo_Hartree_to_eV, ' upper bound:', cumulant(2, 3)*lo_Hartree_to_eV - if (opts%thirdorder) then - write (*, "(1X,A,E21.14,1X,A,F21.14)") ' E-fc2-polar-fc3: ', cumulant(1, 4)*lo_Hartree_to_eV, ' upper bound:', cumulant(2, 4)*lo_Hartree_to_eV - end if - if (opts%fourthorder) then - write (*, "(1X,A,E21.14,1X,A,F21.14)") ' E-fc2-polar-fc3-fc4: ', cumulant(1, 5)*lo_Hartree_to_eV, ' upper bound:', cumulant(2, 5)*lo_Hartree_to_eV - end if - end if -end block epotthings - -! Calculate the actual free energy -getenergy: block - real(r8) :: f_ph, ah3, ah4, fe2_1, fe2_2, fe3_1, fe3_2, fe4_1, fe4_2, pref - integer :: u - character(len=1000) :: opf - - ! Some heuristics to figure out what the temperature is. - if (opts%quantum) then - f_ph = dr%phonon_free_energy(sim%temperature_thermostat) - else - f_ph = dr%phonon_free_energy_classical(sim%temperature_thermostat) - end if - - if (havehighorder) then - select type (qp); type is (lo_fft_mesh) - call perturbative_anharmonic_free_energy(uc, fct, fcf, qp, dr, sim%temperature_thermostat, ah3, ah4, & - opts%fourthorder, opts%quantum, mw, mem, opts%verbosity + 1) - end select - else - ah3 = 0.0_r8 - ah4 = 0.0_r8 - end if - - if (opts%stochastic) then - pref = -1.0_r8 - else - pref = 1.0_r8 - end if - if (mw%talk) then - opf = '(1X,A23,1X,F20.7)' - ! Write on a file - u = open_file('out', 'outfile.anharmonic_free_energy') - fe2_1 = (cumulant(1, 3) + f_ph)*lo_Hartree_to_eV - fe2_2 = (cumulant(1, 3) + f_ph + pref*cumulant(2, 3))*lo_Hartree_to_eV - write (u, "(1X, A17, F8.2, 1X, A17)") '# Free energy at ', sim%temperature_thermostat, 'K, unit : eV/atom' - write (u, *) '# Lowest order (1st order cumulant, 2nd order cumulant)' - write (u, "(1X, 2(F25.10,' '))") fe2_1, fe2_2 - write (*, *) '' - write (*, *) 'Lowest order approximation to the free energy (eV/atom):' - write (*, *) 'Calculated as + F_phonon' - write (*, opf) 'F =', fe2_1 - write (*, opf) 'F_phonon =', f_ph*lo_Hartree_to_eV - write (*, opf) 'Second order cumulant =', cumulant(2, 3)*lo_Hartree_to_eV - write (*, opf) 'Third order cumulant =', cumulant(3, 3)*lo_Hartree_to_eV - if (opts%thirdorder .or. opts%fourthorder) then - fe3_1 = (cumulant(1, 4) + f_ph + ah3)*lo_Hartree_to_eV - fe3_2 = (cumulant(1, 4) + f_ph + ah3 + pref*cumulant(2, 4))*lo_Hartree_to_eV - write (u, *) '# Third order anharmonic corrections (1st order cumulant, 2nd order cumulant)' - write (u, "(1X, 2(F25.10,' '))") fe3_1, fe3_2 - write (*, *) '' - write (*, *) 'Free energy with third order anharmonic corrections (eV/atom):' - write (*, *) 'Calculated as + F_phonon + F_3' - write (*, opf) 'F =', fe3_1 - write (*, opf) 'F_phonon =', f_ph*lo_Hartree_to_eV - write (*, opf) 'F_3 =', ah3*lo_Hartree_to_eV - write (*, opf) 'Second order cumulant =', cumulant(2, 4)*lo_Hartree_to_eV - write (*, opf) 'Third order cumulant =', cumulant(3, 4)*lo_Hartree_to_eV - end if - if (opts%fourthorder) then - fe4_1 = (cumulant(1, 5) + f_ph + ah3 + ah4)*lo_Hartree_to_eV - fe4_2 = (cumulant(1, 5) + f_ph + ah3 + ah4 + pref*cumulant(2, 5))*lo_Hartree_to_eV - write (u, *) '# Fourth order anharmonic corrections (1st order cumulant, 2nd order cumulant)' - write (u, "(1X, 2(F25.10,' '))") fe4_1, fe4_2 - write (*, *) '' - write (*, *) 'Free energy with fourth order anharmonic corrections (eV/atom):' - write (*, *) 'Calculated as + F_phonon + F_3 + F_4' - write (*, opf) 'F =', fe4_1 - write (*, opf) 'F_phonon =', f_ph*lo_Hartree_to_eV - write (*, opf) 'F_3 =', ah3*lo_Hartree_to_eV - write (*, opf) 'F_4 =', ah4*lo_Hartree_to_eV - write (*, opf) 'Second order cumulant =', cumulant(2, 5)*lo_Hartree_to_eV - write (*, opf) 'Third order cumulant =', cumulant(3, 5)*lo_Hartree_to_eV - end if - end if - -end block getenergy - -! Kill MPI -call mw%destroy() - -end program diff --git a/src/anharmonic_free_energy/options.f90 b/src/anharmonic_free_energy/options.f90 index 71ef2fa8..c2e6383a 100644 --- a/src/anharmonic_free_energy/options.f90 +++ b/src/anharmonic_free_energy/options.f90 @@ -1,7 +1,6 @@ #include "precompilerdefinitions" module options -use konstanter, only: r8, lo_author, lo_version, lo_licence, lo_tiny, lo_status, lo_exitcode_baddim, lo_exitcode_param, & - lo_frequency_Hartree_to_THz, lo_frequency_Hartree_to_icm, lo_frequency_Hartree_to_meV +use konstanter, only: r8, lo_author, lo_version, lo_licence, lo_status, lo_exitcode_baddim use gottochblandat, only: lo_stop_gracefully use flap, only: command_line_interface implicit none From 32f68254883234875c991a186f6566d175b2efb5 Mon Sep 17 00:00:00 2001 From: =?UTF-8?q?Alo=C3=AFs=20Castellano?= Date: Wed, 21 May 2025 01:48:49 +0200 Subject: [PATCH 15/28] A bit of cleaning and some fix --- src/anharmonic_free_energy/epot.f90 | 78 +++++++++++++++---- .../lo_thermodynamic_helpers.f90 | 2 - src/anharmonic_free_energy/main.f90 | 46 ++++++----- src/anharmonic_free_energy/thirdorder.f90 | 67 +--------------- 4 files changed, 92 insertions(+), 101 deletions(-) diff --git a/src/anharmonic_free_energy/epot.f90 b/src/anharmonic_free_energy/epot.f90 index b0fb8bd3..09693fd2 100644 --- a/src/anharmonic_free_energy/epot.f90 +++ b/src/anharmonic_free_energy/epot.f90 @@ -1,7 +1,8 @@ module epot !! Deal with many kinds of potential energy differences use konstanter, only: r8, lo_kb_hartree -use gottochblandat, only: tochar, walltime, lo_mean, lo_stddev +use gottochblandat, only: tochar, walltime, lo_mean, lo_stddev, & + lo_trueNtimes, lo_progressbar_init, lo_progressbar use mpi_wrappers, only: lo_mpi_helper, lo_stop_gracefully use lo_memtracker, only: lo_mem_helper use type_crystalstructure, only: lo_crystalstructure @@ -10,6 +11,8 @@ module epot use type_forceconstant_fourthorder, only: lo_forceconstant_fourthorder use type_mdsim, only: lo_mdsim +use konstanter, only: lo_Hartree_to_eV + use lo_thermodynamic_helpers, only: lo_thermodynamics, lo_symmetrize_stress implicit none @@ -17,11 +20,13 @@ module epot public :: lo_energy_differences type lo_energy_differences - ! forceconstants needed for evaluation + !> forceconstants needed for evaluation type(lo_forceconstant_secondorder) :: fc2 type(lo_forceconstant_thirdorder) :: fc3 type(lo_forceconstant_fourthorder) :: fc4 + !> Holder for long range part of the force constants real(r8), dimension(:, :, :, :), allocatable :: fcp + !> Is it a polar material ? logical :: polar = .false. contains @@ -45,10 +50,15 @@ subroutine energies_and_forces(pot, ss, u, e2, e3, e4, ep, s3) !> stress real(r8), dimension(3, 3), intent(out) :: s3 + !> Fourth order IFC real(r8), dimension(3, 3, 3, 3) :: m4 + !> Third order IFC real(r8), dimension(3, 3, 3) :: m3 + !> Second order IFC real(r8), dimension(3, 3) :: m2 + !> Forces and displacements real(r8), dimension(3) :: v0, u1, u2, u3, u4 + !> Some integers integer :: a1, a2, a3, a4, i1, i2, i3, i4, i5, i e2 = 0.0_r8 @@ -200,7 +210,7 @@ subroutine setup_potential_energy_differences(pot, uc, ss, fc2, fc3, fc4, mw, ve end if end subroutine - +!> Compute the thermodynamic corrections from the data subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, stochastic, thirdorder, fourthorder, mw, mem) !> container for potential energy differences class(lo_energy_differences), intent(in) :: pot @@ -240,11 +250,24 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, stochastic, t real(r8), dimension(3, 3) :: s3 !> The individual energy contributions real(r8) :: e2, e3, e4, ep + !> The time + real(r8) :: t0 !> Some integers - integer :: i + integer :: i, j, ntot + + ! For a nice progressbar, we count the steps + ntot = 0 + do i=1, sim%nt + if (mod(i, mw%n) .ne. mw%r) cycle + ntot = ntot + 1 + end do + t0 = walltime() + if (mw%talk) call lo_progressbar_init() + j = 0 do i=1, sim%nt if (mod(i, mw%n) .ne. mw%r) cycle + j = j + 1 call pot%energies_and_forces(ss, sim%u(:, :, i), e2, e3, e4, ep, s3) ! We store the energy differences ediff(i, 1) = sim%stat%potential_energy(i) @@ -255,15 +278,18 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, stochastic, t ! But also the stress differences sdiff(i, :, :, 1) = sim%stat%stress(:, :, i) sdiff(i, :, :, 2) = sim%stat%stress(:, :, i) - s3 + if (mw%talk .and. lo_trueNtimes(i, 127, ntot)) then + call lo_progressbar(' ... computing energy from IFC', j, ntot, walltime() - t0) + end if end do + if (mw%talk) then + call lo_progressbar(' ... computing energy from IFC', ntot, ntot, walltime() - t0) + end if ! And reduce everything call mw%allreduce('sum', ediff) call mw%allreduce('sum', sdiff) - - if (mw%talk) write(*, *) '... computing energy differences' end block energy_computation - averaging: block !> Buffer for the stress tensor real(r8), dimension(3, 3, 2) :: stress @@ -278,6 +304,7 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, stochastic, t !> Some integers integer :: i, j, a, b, istart, iend + if (mw%talk) write(*, *) '... computing cumulant corrections' !> Let's get the inverse temperature if (thermo%temperature .gt. 1E-5_r8) then inverse_kbt = 1.0_r8/lo_kb_Hartree/thermo%temperature @@ -285,16 +312,15 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, stochastic, t inverse_kbt = 0.0_r8 end if - call mem%allocate(buf, [2, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%allocate(bufcv, [2, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%allocate(buf_stress, [3, 3, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - buf = 0.0_r8 - bufcv = 0.0_r8 - buf_stress = 0.0_r8 - ! We need the length of each block for the block averaging blocksize = real(sim%nt, r8) / real(nblocks, r8) if (stochastic) then + call mem%allocate(buf, [2, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%allocate(bufcv, [2, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%allocate(buf_stress, [3, 3, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + buf = 0.0_r8 + bufcv = 0.0_r8 + buf_stress = 0.0_r8 ! For the stochastic, what we compute depends on the order included do j=1, nblocks ! Index for the block @@ -303,12 +329,17 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, stochastic, t ! Now we compute the average for each block if (fourthorder) then f0 = lo_mean(ediff(istart:iend, 4)) + buf(1, j) = f0 + buf(2, j) = lo_mean((ediff(istart:iend, 3) - f0)**2) else if (thirdorder) then f0 = lo_mean(ediff(istart:iend, 3)) + buf(1, j) = f0 + buf(2, j) = lo_mean((ediff(istart:iend, 3) - f0)**2) else f0 = lo_mean(ediff(istart:iend, 2)) + buf(1, j) = f0 + buf(2, j) = lo_mean((ediff(istart:iend, 2) - f0)**2) end if - buf(1, j) = f0 ! And the stress if (fourthorder .or. thirdorder) then @@ -330,7 +361,24 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, stochastic, t U0(2) = sqrt(lo_mean((buf(1, :) - U0(1))**2)) U0 = U0 / sim%na ! Then the + + ! And the stress + do a=1, 3 + do b=1, 3 + stress(a, b, 1) = lo_mean(buf_stress(a, b, :)) + stress(a, b, 2) = sqrt(lo_mean((buf_stress(a, b, :) - stress(a, b, 1))**2)) + end do + end do + + thermo%first_order%F = U0 + thermo%first_order%stress = thermo%first_order%stress + stress else + call mem%allocate(buf, [2, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%allocate(bufcv, [2, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%allocate(buf_stress, [3, 3, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + buf = 0.0_r8 + bufcv = 0.0_r8 + buf_stress = 0.0_r8 do j=1, nblocks ! Index for the block istart = ceiling(blocksize*(j-1) + 1) diff --git a/src/anharmonic_free_energy/lo_thermodynamic_helpers.f90 b/src/anharmonic_free_energy/lo_thermodynamic_helpers.f90 index 51f0a7fc..0d5df52e 100644 --- a/src/anharmonic_free_energy/lo_thermodynamic_helpers.f90 +++ b/src/anharmonic_free_energy/lo_thermodynamic_helpers.f90 @@ -24,8 +24,6 @@ module lo_thermodynamic_helpers type lo_thermodynamics !> The temperature at which everything is evaluated real(r8) :: temperature=-lo_huge - !> The volume - real(r8) :: volume=-lo_huge ! The things to hold results type(lo_thermodynamic_contribution) :: harmonic type(lo_thermodynamic_contribution) :: first_order diff --git a/src/anharmonic_free_energy/main.f90 b/src/anharmonic_free_energy/main.f90 index af78b723..2c590d06 100644 --- a/src/anharmonic_free_energy/main.f90 +++ b/src/anharmonic_free_energy/main.f90 @@ -2,7 +2,7 @@ program anharmonic_free_energy !!{!src/anharmonic_free_energy/manual.md!} use konstanter, only: r8, lo_Hartree_to_eV, lo_kb_Hartree, lo_pressure_HartreeBohr_to_GPa, & lo_tol, lo_status -use gottochblandat, only: open_file, walltime, tochar, lo_does_file_exist, open_file +use gottochblandat, only: open_file, walltime, tochar, lo_does_file_exist, open_file, lo_trace use mpi_wrappers, only: lo_mpi_helper use lo_memtracker, only: lo_mem_helper use lo_timetracker, only: lo_timer @@ -53,17 +53,20 @@ program anharmonic_free_energy call tmr%start() if (mw%talk) then + write(*, *) 'ANHARMONIC FREE ENERGY' write(*, *) 'Recap of the parameters governing the calculation' write(*, *) '' - write (*, '(1X,A40,F20.12)') 'Temperature ', opts%temperature - write (*, '(1X,A40,L3)') 'Quantum limit ', opts%quantum - write (*, '(1X,A40,L3)') 'Stochastic sampling ', opts%stochastic - write (*, '(1X,A40,I4,I4,I4)') 'Q-point grid Harmonic ', opts%qgrid - write (*, '(1X,A40,I4,I4,I4)') 'Third order q-point grid ', opts%qg3ph - write (*, '(1X,A40,I4,I4,I4)') 'Fourth order q-point grid ', opts%qg4ph + write(*, '(1X,A40,F20.12)') 'Temperature ', opts%temperature + write(*, '(1X,A40,I4)') 'Number of blocks ', opts%nblocks + write(*, '(1X,A40,L3)') 'Quantum limit ', opts%quantum + write(*, '(1X,A40,L3)') 'Stochastic sampling ', opts%stochastic + write(*, '(1X,A40,I4,I4,I4)') 'Q-point grid Harmonic ', opts%qgrid + write(*, '(1X,A40,I4,I4,I4)') 'Third order q-point grid ', opts%qg3ph + write(*, '(1X,A40,I4,I4,I4)') 'Fourth order q-point grid ', opts%qg4ph write(*, *) '' end if + if (mw%talk) write(*, *) 'INITIALIZATION' if (mw%talk) write(*, *) '... reading input files' ! Read structure call uc%readfromfile('infile.ucposcar', verbosity=opts%verbosity) @@ -108,7 +111,8 @@ program anharmonic_free_energy end if if (mw%talk) write(*, *) '... generating q-mesh' - call lo_generate_qmesh(qp, uc, opts%qgrid, 'fft', timereversal=.true., headrankonly=.false., mw=mw, mem=mem, verbosity=opts%verbosity) + call lo_generate_qmesh(qp, uc, opts%qgrid, 'fft', timereversal=.true., & + headrankonly=.false., mw=mw, mem=mem, verbosity=opts%verbosity) if (mw%talk) write(*, *) '... generating harmonic dispersion' call dr%generate(qp, fc, uc, mw=mw, mem=mem, verbosity=opts%verbosity) @@ -149,10 +153,12 @@ program anharmonic_free_energy if (opts%thirdorder) then if (mw%talk) write(*, *) '... computing third order contribution to elastic properties' - call elastic_thirdorder(uc, fc, fct, qp, dr, opts%temperature, thermo%threephonon%stress(:, :, 1), thermo%alpha, opts%quantum, mw, mem) + call elastic_thirdorder(uc, fc, fct, qp, dr, opts%temperature, thermo%threephonon%stress(:, :, 1), & + thermo%alpha, opts%quantum, mw, mem) ! Now we symmetrize call lo_symmetrize_stress(thermo%threephonon%stress(:, :, 1), uc) call lo_symmetrize_stress(thermo%alpha, uc) + if (opts%stochastic) thermo%first_order%stress = thermo%threephonon%stress end if call tmr%tock('harmonic properties') end block latdyn @@ -169,7 +175,7 @@ program anharmonic_free_energy if (lo_does_file_exist('infile.sim.hdf5') .or. lo_does_file_exist('infile.meta')) then havesim = .true. - if (mw%talk) write(*, *) 'Computing energy differences' + if (mw%talk) write(*, *) 'REAL-SPACE ENERGY CORRECTIONS' if (mw%talk) write(*, *) '... reading simulation files' ! Read the supercell @@ -204,7 +210,7 @@ program anharmonic_free_energy end if call pot%compute_realspace_thermo(ss, sim, thermo, opts%nblocks, & - opts%thirdorder, opts%fourthorder, opts%thirdorder, mw, mem) + opts%stochastic, opts%thirdorder, opts%fourthorder, mw, mem) ! We also need to symmetrize the stress tensor call lo_symmetrize_stress(thermo%first_order%stress(:, :, 1), uc) call lo_symmetrize_stress(thermo%first_order%stress(:, :, 2), uc) @@ -237,7 +243,8 @@ program anharmonic_free_energy end if if (mw%talk) write(*, *) '... generating q-mesh' - call lo_generate_qmesh(qp, uc, opts%qg3ph, 'fft', timereversal=.true., headrankonly=.false., mw=mw, mem=mem, verbosity=opts%verbosity) + call lo_generate_qmesh(qp, uc, opts%qg3ph, 'fft', timereversal=.true., & + headrankonly=.false., mw=mw, mem=mem, verbosity=opts%verbosity) if (mw%talk) write(*, *) '... generating harmonic dispersion' call dr%generate(qp, fc, uc, mw=mw, mem=mem, verbosity=opts%verbosity) @@ -274,7 +281,8 @@ program anharmonic_free_energy end if if (mw%talk) write(*, *) '... generating q-mesh' - call lo_generate_qmesh(qp, uc, opts%qg4ph, 'fft', timereversal=.true., headrankonly=.false., mw=mw, mem=mem, verbosity=opts%verbosity) + call lo_generate_qmesh(qp, uc, opts%qg4ph, 'fft', timereversal=.true., & + headrankonly=.false., mw=mw, mem=mem, verbosity=opts%verbosity) if (mw%talk) write(*, *) '... generating harmonic dispersion' call dr%generate(qp, fc, uc, mw=mw, mem=mem, verbosity=opts%verbosity) @@ -296,7 +304,6 @@ program anharmonic_free_energy ! call free_energy_fourthorder_secondorder(uc, fcf, qp, dr, opts%temperature, fe4, s4, cv4, opts%quantum, mw, mem) end if call tmr%tock('four-phonon') - end block latdyn4ph summary: block @@ -304,13 +311,16 @@ program anharmonic_free_energy real(r8) :: f_unit, e_unit, s_unit, c_unit, p_unit !> Buffer for the stress tensor real(r8), dimension(3, 3, 2) :: sigma + !> Some buffer to print the results + real(r8), dimension(4) :: buf, var !> The pressure real(r8), dimension(2) :: pressure + !> To have a pretty logfile character(len=1000) :: opfc, opff, opfs !> A tolerance to clean-up stress results real(r8) :: stol + !> Some integers integer :: i, u - real(r8), dimension(4) :: buf, var f_unit = lo_Hartree_to_eV e_unit = lo_Hartree_to_eV @@ -321,10 +331,8 @@ program anharmonic_free_energy ! Get the stress tensor sigma = (thermo%harmonic%stress + thermo%first_order%stress + thermo%second_order%stress) * p_unit ! And the pressure - pressure = 0.0_r8 - do i=1, 3 - pressure = pressure + sigma(i, i, :) / 3.0_r8 - end do + pressure(1) = lo_trace(sigma(:, :, 1)) / 3.0_r8 + pressure(2) = lo_trace(sigma(:, :, 2)) / 3.0_r8 if (mw%talk) then u = open_file('out', 'outfile.anharmonic_free_energy') diff --git a/src/anharmonic_free_energy/thirdorder.f90 b/src/anharmonic_free_energy/thirdorder.f90 index deadab83..bf9900bd 100644 --- a/src/anharmonic_free_energy/thirdorder.f90 +++ b/src/anharmonic_free_energy/thirdorder.f90 @@ -13,6 +13,7 @@ module thirdorder use type_phonon_dispersions, only: lo_phonon_dispersions use type_symmetryoperation, only: lo_operate_on_secondorder_tensor use lo_timetracker, only: lo_timer +use lo_fftgrid_helper, only: fft_third_grid_index use lo_thermodynamic_helpers, only: lo_full_to_voigt @@ -152,7 +153,6 @@ subroutine elastic_thirdorder(uc, fc, fct, qp, dr, temperature, p3ph, alpha, qua call mem%deallocate(egv, persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) end subroutine - !> Calculate the third order free energy subroutine free_energy_thirdorder(uc, fct, qp, dr, temperature, fe3, s3, cv3, quantum, mw, mem) !> crystal structure @@ -220,6 +220,7 @@ subroutine free_energy_thirdorder(uc, fct, qp, dr, temperature, fe3, s3, cv3, qu end do end do + if (mw%talk) call lo_progressbar_init() do q1=1, qp%n_irr_point do q2=1, qp%n_full_point ctr = ctr + 1 @@ -390,68 +391,4 @@ subroutine pretransform_phi3(fct, q2, q3, ptf) end do end do end subroutine - -!> returns the index on the grid that gives q3=-q1-q2 -pure function fft_third_grid_index(i1, i2, dims) result(i3) - !> index to q1 - integer, intent(in) :: i1 - !> index to q2 - integer, intent(in) :: i2 - !> dimensions of the grid - integer, dimension(3), intent(in) :: dims - !> index to q3 - integer :: i3 - - integer, dimension(3) :: gi1, gi2, gi3 - integer :: l, k - - ! Convert triplet to singlet - gi1 = singlet_to_triplet(i1, dims(2), dims(3)) - gi2 = singlet_to_triplet(i2, dims(2), dims(3)) - do l = 1, 3 - gi3(l) = 3 - gi1(l) - gi2(l) - end do - do k = 1, 3 - do l = 1, 3 - if (gi3(l) .lt. 1) gi3(l) = gi3(l) + dims(l) - if (gi3(l) .gt. dims(l)) gi3(l) = gi3(l) - dims(l) - end do - end do - ! convert it back to a singlet - i3 = triplet_to_singlet(gi3, dims(2), dims(3)) - -contains - !> convert a linear index to a triplet - pure function singlet_to_triplet(l, ny, nz) result(gi) - !> linear index - integer, intent(in) :: l - !> second dimension - integer, intent(in) :: ny - !> third dimension - integer, intent(in) :: nz - !> grid-index - integer, dimension(3) :: gi - - integer :: i, j, k - - k = mod(l, nz) - if (k .eq. 0) k = nz - j = mod((l - k)/nz, ny) + 1 - i = (l - k - (j - 1)*nz)/(nz*ny) + 1 - gi = [i, j, k] - end function - !> convert a triplet index to a singlet - pure function triplet_to_singlet(gi, ny, nz) result(l) - !> grid-index - integer, dimension(3), intent(in) :: gi - !> second dimension - integer, intent(in) :: ny - !> third dimension - integer, intent(in) :: nz - !> linear index - integer :: l - - l = (gi(1) - 1)*ny*nz + (gi(2) - 1)*nz + gi(3) - end function -end function end module From 3a8c5d7e0e203217b7e60c50dd39f870a72f4c79 Mon Sep 17 00:00:00 2001 From: =?UTF-8?q?Alo=C3=AFs=20Castellano?= Date: Wed, 21 May 2025 11:16:19 +0200 Subject: [PATCH 16/28] More cleaning, and work in Voigt notation for stress --- src/anharmonic_free_energy/epot.f90 | 103 ++++++++---------- .../lo_thermodynamic_helpers.f90 | 49 +++++++++ src/anharmonic_free_energy/main.f90 | 6 +- 3 files changed, 99 insertions(+), 59 deletions(-) diff --git a/src/anharmonic_free_energy/epot.f90 b/src/anharmonic_free_energy/epot.f90 index 09693fd2..6fe171c7 100644 --- a/src/anharmonic_free_energy/epot.f90 +++ b/src/anharmonic_free_energy/epot.f90 @@ -13,7 +13,7 @@ module epot use konstanter, only: lo_Hartree_to_eV -use lo_thermodynamic_helpers, only: lo_thermodynamics, lo_symmetrize_stress +use lo_thermodynamic_helpers, only: lo_thermodynamics, lo_full_to_voigt_33, lo_voigt_to_full_33 implicit none private @@ -211,7 +211,7 @@ subroutine setup_potential_energy_differences(pot, uc, ss, fc2, fc3, fc4, mw, ve end subroutine !> Compute the thermodynamic corrections from the data -subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, stochastic, thirdorder, fourthorder, mw, mem) +subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, mw, mem) !> container for potential energy differences class(lo_energy_differences), intent(in) :: pot !> The supercell @@ -222,25 +222,19 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, stochastic, t type(lo_thermodynamics), intent(inout) :: thermo !> Number of blocks integer, intent(in) :: nblocks - !> Are we within a stochastic sampling approach ? - logical, intent(in) :: stochastic - !> Are we using thirdorder ? - logical, intent(in) :: thirdorder - !> Are we using fourthorder ? - logical, intent(in) :: fourthorder !> MPI type(lo_mpi_helper), intent(inout) :: mw !> memory tracker type(lo_mem_helper), intent(inout) :: mem !> The stress difference between true and ifcs - real(r8), dimension(:, :, :, :), allocatable :: sdiff + real(r8), dimension(:, :, :), allocatable :: sdiff !> The energy difference between true and ifcs real(r8), dimension(:, :), allocatable :: ediff ! Allocate stuffs call mem%allocate(ediff, [sim%nt, 4], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%allocate(sdiff, [sim%nt, 3, 3, 2], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%allocate(sdiff, [sim%nt, 6, 2], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) ediff = 0.0_r8 sdiff = 0.0_r8 @@ -253,13 +247,12 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, stochastic, t !> The time real(r8) :: t0 !> Some integers - integer :: i, j, ntot + integer :: i, j, ntot, a, b - ! For a nice progressbar, we count the steps + ! For a nice progressbar, we count the number of configuration on the rank ntot = 0 do i=1, sim%nt - if (mod(i, mw%n) .ne. mw%r) cycle - ntot = ntot + 1 + if (mod(i, mw%n) .eq. mw%r) ntot = ntot + 1 end do t0 = walltime() @@ -275,9 +268,9 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, stochastic, t ediff(i, 3) = sim%stat%potential_energy(i) - e2 - ep - e3 ediff(i, 4) = sim%stat%potential_energy(i) - e2 - ep - e3 - e4 - ! But also the stress differences - sdiff(i, :, :, 1) = sim%stat%stress(:, :, i) - sdiff(i, :, :, 2) = sim%stat%stress(:, :, i) - s3 + ! But also the stress differences, in Voigt notation + sdiff(i, :, 1) = lo_full_to_voigt_33(sim%stat%stress(:, :, i)) + sdiff(i, :, 2) = lo_full_to_voigt_33(sim%stat%stress(:, :, i) - s3) if (mw%talk .and. lo_trueNtimes(i, 127, ntot)) then call lo_progressbar(' ... computing energy from IFC', j, ntot, walltime() - t0) end if @@ -292,15 +285,13 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, stochastic, t averaging: block !> Buffer for the stress tensor - real(r8), dimension(3, 3, 2) :: stress + real(r8), dimension(6, 2) :: stress_voigt !> Buffer for the thermodynamic quantities real(r8), dimension(2) :: F, S, Cv, U0 !> Little buffers for the blocks - real(r8), dimension(:, :), allocatable :: buf, bufcv - !> A little buffer for the stress - real(r8), dimension(:, :, :), allocatable :: buf_stress + real(r8), dimension(:, :), allocatable :: buf, bufcv, bufstress !> Some buffers: energy, inverse kbt blabla - real(r8) :: inverse_kbt, f0, f1, f2, blocksize + real(r8) :: inverse_kbt, f0, f1, f2, blocksize, sqnm1 !> Some integers integer :: i, j, a, b, istart, iend @@ -314,24 +305,24 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, stochastic, t ! We need the length of each block for the block averaging blocksize = real(sim%nt, r8) / real(nblocks, r8) - if (stochastic) then + if (thermo%stochastic) then call mem%allocate(buf, [2, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) call mem%allocate(bufcv, [2, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%allocate(buf_stress, [3, 3, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%allocate(bufstress, [6, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) buf = 0.0_r8 bufcv = 0.0_r8 - buf_stress = 0.0_r8 + bufstress = 0.0_r8 ! For the stochastic, what we compute depends on the order included do j=1, nblocks ! Index for the block istart = ceiling(blocksize*(j-1) + 1) iend = min(ceiling(blocksize*j), sim%nt) ! Now we compute the average for each block - if (fourthorder) then + if (thermo%fourthorder) then f0 = lo_mean(ediff(istart:iend, 4)) buf(1, j) = f0 buf(2, j) = lo_mean((ediff(istart:iend, 3) - f0)**2) - else if (thirdorder) then + else if (thermo%thirdorder) then f0 = lo_mean(ediff(istart:iend, 3)) buf(1, j) = f0 buf(2, j) = lo_mean((ediff(istart:iend, 3) - f0)**2) @@ -342,17 +333,13 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, stochastic, t end if ! And the stress - if (fourthorder .or. thirdorder) then - do a=1, 3 - do b=1, 3 - buf_stress(a, b, j) = lo_mean(sdiff(istart:iend, a, b, 2)) - end do + if (thermo%fourthorder .or. thermo%thirdorder) then + do a=1, 6 + bufstress(a, j) = lo_mean(sdiff(istart:iend, a, 2)) end do else - do a=1, 3 - do b=1, 3 - buf_stress(a, b, j) = lo_mean(sdiff(istart:iend, a, b, 1)) - end do + do a=1, 6 + bufstress(a, j) = lo_mean(sdiff(istart:iend, a, 1)) end do end if end do @@ -363,22 +350,21 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, stochastic, t ! Then the ! And the stress - do a=1, 3 - do b=1, 3 - stress(a, b, 1) = lo_mean(buf_stress(a, b, :)) - stress(a, b, 2) = sqrt(lo_mean((buf_stress(a, b, :) - stress(a, b, 1))**2)) - end do + do a=1, 6 + stress_voigt(a, 1) = lo_mean(bufstress(a, :)) + stress_voigt(a, 2) = lo_stddev(bufstress(a, :)) * sqnm1 end do thermo%first_order%F = U0 - thermo%first_order%stress = thermo%first_order%stress + stress + thermo%first_order%stress(:, :, 1) = thermo%first_order%stress(:, :, 1) + lo_voigt_to_full_33(stress_voigt(:, 1)) + thermo%first_order%stress(:, :, 2) = thermo%first_order%stress(:, :, 2) + lo_voigt_to_full_33(stress_voigt(:, 2)) else call mem%allocate(buf, [2, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) call mem%allocate(bufcv, [2, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) - call mem%allocate(buf_stress, [3, 3, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) + call mem%allocate(bufstress, [6, nblocks], persistent=.false., scalable=.false., file=__FILE__, line=__LINE__) buf = 0.0_r8 bufcv = 0.0_r8 - buf_stress = 0.0_r8 + bufstress = 0.0_r8 do j=1, nblocks ! Index for the block istart = ceiling(blocksize*(j-1) + 1) @@ -393,33 +379,35 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, stochastic, t ! This is to get the correction to the heat capacity bufcv(1, j) = lo_mean((ediff(istart:iend, 1) - f1) * (ediff(istart:iend, 2) - f0)) ! And the stress - do a=1, 3 - do b=1, 3 - buf_stress(a, b, j) = lo_mean(sdiff(istart:iend, a, b, 1)) - end do + do a=1, 6 + bufstress(a, j) = lo_mean(sdiff(istart:iend, a, 1)) end do end do + ! Something to normalize the block averaging + if (nblocks .eq. 1) then + sqnm1 = 1.0_r8 + else + sqnm1 = 1.0_r8 / sqrt(real(nblocks, r8) - 1.0_r8) + end if ! First we get the U0 term U0(1) = lo_mean(buf(1, :)) - U0(2) = sqrt(lo_mean((buf(1, :) - U0(1))**2)) + U0(2) = lo_stddev(buf(1, :)) * sqnm1 U0 = U0 / sim%na ! Now we need the entropy correction S(1) = lo_mean(buf(2, :)) - S(2) = sqrt(lo_mean((buf(2, :) - S(1))**2)) + S(2) = lo_stddev(buf(2, :)) * sqnm1 S = 0.5_r8 * lo_kb_Hartree * S * inverse_kbt**2 / sim%na ! And the heat capacity correction Cv(1) = lo_mean(bufcv(1, :)) - Cv(2) = sqrt(lo_mean((bufcv(1, :) - Cv(1))**2)) + Cv(2) = lo_stddev(bufcv(1, :)) * sqnm1 Cv = Cv * inverse_kbt**2 * lo_kb_Hartree / sim%na ! And the stress - do a=1, 3 - do b=1, 3 - stress(a, b, 1) = lo_mean(buf_stress(a, b, :)) - stress(a, b, 2) = sqrt(lo_mean((buf_stress(a, b, :) - stress(a, b, 1))**2)) - end do + do a=1, 6 + stress_voigt(a, 1) = lo_mean(bufstress(a, :)) + stress_voigt(a, 2) = lo_stddev(bufstress(a, :)) * sqnm1 end do ! And we store the results @@ -429,7 +417,8 @@ subroutine compute_realspace_thermo(pot, ss, sim, thermo, nblocks, stochastic, t thermo%first_order%U = U0 thermo%second_order%S = S thermo%second_order%Cv = Cv - thermo%first_order%stress = stress + thermo%first_order%stress(:,: , 1) = lo_voigt_to_full_33(stress_voigt(:, 1)) + thermo%first_order%stress(:,: , 2) = lo_voigt_to_full_33(stress_voigt(:, 2)) end if end block averaging end subroutine diff --git a/src/anharmonic_free_energy/lo_thermodynamic_helpers.f90 b/src/anharmonic_free_energy/lo_thermodynamic_helpers.f90 index 0d5df52e..8550867e 100644 --- a/src/anharmonic_free_energy/lo_thermodynamic_helpers.f90 +++ b/src/anharmonic_free_energy/lo_thermodynamic_helpers.f90 @@ -10,6 +10,8 @@ module lo_thermodynamic_helpers public :: lo_thermodynamics public :: lo_symmetrize_stress public :: lo_full_to_voigt +public :: lo_full_to_voigt_33 +public :: lo_voigt_to_full_33 type lo_thermodynamic_contribution ! The different contributions. First dimension is the result, second one the uncertainty @@ -32,6 +34,12 @@ module lo_thermodynamic_helpers type(lo_thermodynamic_contribution) :: fourphonon !> The thermal expansion real(r8), dimension(3, 3) :: alpha + !> Is it a stochastic simulation ? + logical :: stochastic = .false. + !> Do we have third order ? + logical :: thirdorder = .false. + !> Do we have fourth order ? + logical :: fourthorder = .false. end type contains @@ -73,4 +81,45 @@ function lo_full_to_voigt(i, j) result(k) if (d(1) .eq. 1 .and. d(2) .eq. 3) k = 5 if (d(1) .eq. 2 .and. d(2) .eq. 3) k = 4 end function + +!> Transform a 3x3 tensor in full representation into its Voigt representation +function lo_full_to_voigt_33(mi) result(mo) + !> The input tensor in full notation + real(r8), dimension(3, 3), intent(in) :: mi + !> The output vector in Voigt notation + real(r8), dimension(6) :: mo + + integer :: i, j + + mo = 0.0_r8 + do i=1, 3 + do j=i, 3 + if (i .eq. j) then + mo = mi(i, j) + else + mo = 0.5_r8 * (mi(i, j) + mi(j, i)) + end if + end do + end do +end function + +!> Transform a vector in Voigt notation into it's 3x3 full representation +function lo_voigt_to_full_33(mi) result(mo) + !> The input tensor in full notation + real(r8), dimension(6), intent(in) :: mi + !> The output vector in Voigt notation + real(r8), dimension(3, 3) :: mo + + integer :: i, j, k + + mo = 0.0_r8 + do i=1, 3 + do j=i, 3 + k = lo_full_to_voigt(i, j) + mo(i, j) = mi(k) + mo(j, i) = mi(k) + end do + end do +end function + end module diff --git a/src/anharmonic_free_energy/main.f90 b/src/anharmonic_free_energy/main.f90 index 2c590d06..2f44ab71 100644 --- a/src/anharmonic_free_energy/main.f90 +++ b/src/anharmonic_free_energy/main.f90 @@ -93,6 +93,9 @@ program anharmonic_free_energy timer_init = walltime() - timer_init thermo%temperature = opts%temperature + thermo%stochastic = opts%stochastic + thermo%thirdorder = opts%thirdorder + thermo%fourthorder = opts%fourthorder end block init latdyn: block @@ -209,8 +212,7 @@ program anharmonic_free_energy write(*, *) end if - call pot%compute_realspace_thermo(ss, sim, thermo, opts%nblocks, & - opts%stochastic, opts%thirdorder, opts%fourthorder, mw, mem) + call pot%compute_realspace_thermo(ss, sim, thermo, opts%nblocks, mw, mem) ! We also need to symmetrize the stress tensor call lo_symmetrize_stress(thermo%first_order%stress(:, :, 1), uc) call lo_symmetrize_stress(thermo%first_order%stress(:, :, 2), uc) From 8a47a5bc12595a9be0c2f1756eb95c9ecbf6701a Mon Sep 17 00:00:00 2001 From: Ethan Meitz <54505069+ejmeitz@users.noreply.github.com> Date: Fri, 20 Mar 2026 13:06:57 -0400 Subject: [PATCH 17/28] fix bugs --- src/anharmonic_free_energy/fourthorder.f90 | 2 +- src/anharmonic_free_energy/main.f90 | 218 ++++++--------------- src/anharmonic_free_energy/options.f90 | 19 -- src/anharmonic_free_energy/thirdorder.f90 | 10 +- 4 files changed, 68 insertions(+), 181 deletions(-) diff --git a/src/anharmonic_free_energy/fourthorder.f90 b/src/anharmonic_free_energy/fourthorder.f90 index 88cfd337..812aece5 100644 --- a/src/anharmonic_free_energy/fourthorder.f90 +++ b/src/anharmonic_free_energy/fourthorder.f90 @@ -106,7 +106,7 @@ subroutine free_energy_fourthorder(uc, fcf, qp, dr, temperature, df4, s4, cv4, q ddn1 = lo_planck_secondderiv(temperature, om1) ddn2 = lo_planck_secondderiv(temperature, om2) ! The free energy - f0 = (2.0_r8 * n1 + 1.0_r8) * (2.0_r8 * n2 + 1.0_r8) * psisq * prefactor / 32.0_r8 + f0 = (2.0_r8 * n1 + 1.0_r8) * (2.0_r8 * n2 + 1.0_r8) / 32.0_r8 ! The entropy df0 = 2.0_r8 * dn1 * (2.0_r8 * n2 + 1.0_r8) + (2.0_r8 * n1 + 1.0_r8) * 2.0_r8 * dn2 df0 = df0 / 32.0_r8 diff --git a/src/anharmonic_free_energy/main.f90 b/src/anharmonic_free_energy/main.f90 index 2f44ab71..da42f71a 100644 --- a/src/anharmonic_free_energy/main.f90 +++ b/src/anharmonic_free_energy/main.f90 @@ -1,8 +1,7 @@ program anharmonic_free_energy !!{!src/anharmonic_free_energy/manual.md!} -use konstanter, only: r8, lo_Hartree_to_eV, lo_kb_Hartree, lo_pressure_HartreeBohr_to_GPa, & - lo_tol, lo_status -use gottochblandat, only: open_file, walltime, tochar, lo_does_file_exist, open_file, lo_trace +use konstanter, only: r8, lo_Hartree_to_eV, lo_kb_Hartree, lo_pressure_HartreeBohr_to_GPa, lo_status +use gottochblandat, only: open_file, walltime, lo_trace use mpi_wrappers, only: lo_mpi_helper use lo_memtracker, only: lo_mem_helper use lo_timetracker, only: lo_timer @@ -10,16 +9,13 @@ program anharmonic_free_energy use type_forceconstant_secondorder, only: lo_forceconstant_secondorder use type_forceconstant_thirdorder, only: lo_forceconstant_thirdorder use type_forceconstant_fourthorder, only: lo_forceconstant_fourthorder -use type_mdsim, only: lo_mdsim use type_qpointmesh, only: lo_qpoint_mesh, lo_generate_qmesh use type_phonon_dispersions, only: lo_phonon_dispersions -use lo_phonon_bandstructure_on_path, only: lo_phonon_bandstructure use options, only: lo_opts use thirdorder, only: free_energy_thirdorder, elastic_thirdorder -use fourthorder, only: free_energy_fourthorder, free_energy_fourthorder_secondorder -use epot, only: lo_energy_differences -use lo_thermodynamic_helpers, only: lo_thermodynamics, lo_symmetrize_stress, lo_full_to_voigt +use fourthorder, only: free_energy_fourthorder +use lo_thermodynamic_helpers, only: lo_thermodynamics, lo_symmetrize_stress implicit none @@ -33,11 +29,8 @@ program anharmonic_free_energy type(lo_timer) :: tmr type(lo_thermodynamics) :: thermo -real(r8), dimension(3, 5) :: cumulant, cumulant_var -real(r8), dimension(3, 3, 5) :: stress_pot, stress_potvar real(r8) :: timer_init, timer_total -real(r8) :: U0, U1, energy_unit_factor -logical :: havehighorder, havesim +logical :: havehighorder ! Init MPI, timers and options call mw%init() @@ -57,9 +50,7 @@ program anharmonic_free_energy write(*, *) 'Recap of the parameters governing the calculation' write(*, *) '' write(*, '(1X,A40,F20.12)') 'Temperature ', opts%temperature - write(*, '(1X,A40,I4)') 'Number of blocks ', opts%nblocks write(*, '(1X,A40,L3)') 'Quantum limit ', opts%quantum - write(*, '(1X,A40,L3)') 'Stochastic sampling ', opts%stochastic write(*, '(1X,A40,I4,I4,I4)') 'Q-point grid Harmonic ', opts%qgrid write(*, '(1X,A40,I4,I4,I4)') 'Third order q-point grid ', opts%qg3ph write(*, '(1X,A40,I4,I4,I4)') 'Fourth order q-point grid ', opts%qg4ph @@ -93,7 +84,6 @@ program anharmonic_free_energy timer_init = walltime() - timer_init thermo%temperature = opts%temperature - thermo%stochastic = opts%stochastic thermo%thirdorder = opts%thirdorder thermo%fourthorder = opts%fourthorder end block init @@ -161,72 +151,11 @@ program anharmonic_free_energy ! Now we symmetrize call lo_symmetrize_stress(thermo%threephonon%stress(:, :, 1), uc) call lo_symmetrize_stress(thermo%alpha, uc) - if (opts%stochastic) thermo%first_order%stress = thermo%threephonon%stress end if call tmr%tock('harmonic properties') end block latdyn -calcepot: block - !> The simulation - type(lo_mdsim) :: sim - !> The potentiel energy helper - type(lo_energy_differences) :: pot - !> The supercell - type(lo_crystalstructure) :: ss - - if (mw%talk) write(*, *) '' - if (lo_does_file_exist('infile.sim.hdf5') .or. lo_does_file_exist('infile.meta')) then - havesim = .true. - - if (mw%talk) write(*, *) 'REAL-SPACE ENERGY CORRECTIONS' - - if (mw%talk) write(*, *) '... reading simulation files' - ! Read the supercell - call ss%readfromfile('infile.ssposcar') - call ss%classify('supercell', uc) - ! Setup the ifc with the potential - if (mw%talk) write(*, *) '... preparing potential energy differences' - call pot%setup(uc, ss, fc, fct, fcf, mw, opts%verbosity+1) - - ! We fetch the simulation data - if (lo_does_file_exist('infile.sim.hdf5')) then - call sim%read_from_hdf5('infile.sim.hdf5', verbosity=-1, stride=-1) - else - call sim%read_from_file(verbosity=-1, stride=1, magnetic=.false., dielectric=.false., nrand=-1, mw=mw) - end if - - ! Let's recap info on the simulation - if (mw%talk) then - write (*, *) '... short summary of simulation:' - write (*, *) ' number of atoms: ', tochar(sim%na) - write (*, *) ' number of configurations: ', tochar(sim%nt) - write (*, *) ' thermostat set to (K): ', tochar(sim%temperature_thermostat) - end if - - if (abs(opts%temperature - sim%temperature_thermostat) .gt. lo_tol .and. mw%talk) then - write(*, *) - write(*, *) 'WARNING: input and simulation temperatures do not match' - write(*, '(1X,A24,F24.12)') 'Input temperature', opts%temperature - write(*, '(1X,A24,F24.12)') 'Simulation temperature', sim%temperature_thermostat - write(*, *) 'Results might be garbage !' - write(*, *) - end if - - call pot%compute_realspace_thermo(ss, sim, thermo, opts%nblocks, mw, mem) - ! We also need to symmetrize the stress tensor - call lo_symmetrize_stress(thermo%first_order%stress(:, :, 1), uc) - call lo_symmetrize_stress(thermo%first_order%stress(:, :, 2), uc) - call lo_symmetrize_stress(thermo%second_order%stress(:, :, 1), uc) - call lo_symmetrize_stress(thermo%second_order%stress(:, :, 2), uc) - - call tmr%tock('simulation') - else - havesim = .false. - if (mw%talk) then - write(*, *) 'No simulation found, skipping computation of cumulant correction' - end if - end if -end block calcepot +! Skipping cumulant/real-space corrections - only computing phonon contributions latdyn3ph: block @@ -255,14 +184,6 @@ program anharmonic_free_energy thermo%threephonon%S(1) = s3 thermo%threephonon%U(1) = (fe3 + opts%temperature * s3) thermo%threephonon%Cv(1) = cv3 - ! If we are in the stochastic mode, we have to add it to the result - ! It's a second order correction - if (opts%stochastic) then - thermo%second_order%F(1) = thermo%second_order%F(1) +thermo%threephonon%F(1) - thermo%second_order%S(1) = thermo%second_order%S(1) +thermo%threephonon%S(1) - thermo%second_order%U(1) = thermo%second_order%U(1) +thermo%threephonon%U(1) - thermo%second_order%Cv(1) = thermo%second_order%Cv(1) + thermo%threephonon%Cv(1) - end if end if call tmr%tock('three-phonon') @@ -289,21 +210,10 @@ program anharmonic_free_energy call dr%generate(qp, fc, uc, mw=mw, mem=mem, verbosity=opts%verbosity) call free_energy_fourthorder(uc, fcf, qp, dr, opts%temperature, fe4, s4, cv4, opts%quantum, mw, mem) - thermo%fourphonon%F = fe4 - thermo%fourphonon%S = s4 - thermo%fourphonon%U = (fe4 + opts%temperature * s4) - thermo%fourphonon%Cv = cv4 - ! If we are in the stochastic mode, we have to add it to the result - ! It's a first order correction - if (opts%stochastic) then - thermo%first_order%F(1) = thermo%first_order%F(1) + thermo%fourphonon%F(1) - thermo%first_order%U(1) = thermo%first_order%U(1) + thermo%fourphonon%U(1) - thermo%first_order%S(1) = thermo%first_order%S(1) + thermo%fourphonon%S(1) - thermo%first_order%Cv(1) = thermo%first_order%Cv(1) + thermo%fourphonon%Cv(1) - end if - - ! TODO set fourthorder, second order cumulant its own qpoint grid density, too expensive otherwise -! call free_energy_fourthorder_secondorder(uc, fcf, qp, dr, opts%temperature, fe4, s4, cv4, opts%quantum, mw, mem) + thermo%fourphonon%F(1) = fe4 + thermo%fourphonon%S(1) = s4 + thermo%fourphonon%U(1) = (fe4 + opts%temperature * s4) + thermo%fourphonon%Cv(1) = cv4 end if call tmr%tock('four-phonon') end block latdyn4ph @@ -312,15 +222,13 @@ program anharmonic_free_energy !> Unit conversion factor real(r8) :: f_unit, e_unit, s_unit, c_unit, p_unit !> Buffer for the stress tensor - real(r8), dimension(3, 3, 2) :: sigma + real(r8), dimension(3, 3) :: sigma !> Some buffer to print the results - real(r8), dimension(4) :: buf, var + real(r8), dimension(4) :: buf, buf3, buf4 !> The pressure - real(r8), dimension(2) :: pressure + real(r8) :: pressure !> To have a pretty logfile character(len=1000) :: opfc, opff, opfs - !> A tolerance to clean-up stress results - real(r8) :: stol !> Some integers integer :: i, u @@ -330,11 +238,9 @@ program anharmonic_free_energy c_unit = 1.0 / lo_kb_Hartree p_unit = lo_pressure_HartreeBohr_to_GPa - ! Get the stress tensor - sigma = (thermo%harmonic%stress + thermo%first_order%stress + thermo%second_order%stress) * p_unit - ! And the pressure - pressure(1) = lo_trace(sigma(:, :, 1)) / 3.0_r8 - pressure(2) = lo_trace(sigma(:, :, 2)) / 3.0_r8 + ! Get the stress tensor (harmonic + threephonon only) + sigma = (thermo%harmonic%stress(:, :, 1) + thermo%threephonon%stress(:, :, 1)) * p_unit + pressure = lo_trace(sigma) / 3.0_r8 if (mw%talk) then u = open_file('out', 'outfile.anharmonic_free_energy') @@ -343,74 +249,72 @@ program anharmonic_free_energy opfc = '(4(1X,A24))' opff = '(4(1X,F24.12))' opfs = '(3(1X,F24.12))' + + ! Harmonic contribution buf(1) = thermo%harmonic%F(1) * f_unit buf(2) = thermo%harmonic%U(1) * e_unit buf(3) = thermo%harmonic%S(1) * s_unit buf(4) = thermo%harmonic%Cv(1) * c_unit - var = 0.0_r8 write(*, *) '' write(*, *) 'SUMMARY OF RESULTS' write(*, *) '' - write(*, *) 'Effective harmonic contribution: F = F_harm' - write(*, opfc) 'Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' - write(*, opff) buf - write(*, opff) var - write(u, *) '# Effective harmonic contribution: F = F_harm' - write(u, opfc) '# Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' - write(u, opff) buf - write(u, opff) var - - ! Update the values - buf(1) = buf(1) + thermo%first_order%F(1) * f_unit - buf(2) = buf(2) + thermo%first_order%U(1) * e_unit - buf(3) = buf(3) + thermo%first_order%S(1) * s_unit - buf(4) = buf(4) + thermo%first_order%Cv(1) * c_unit - ! And the uncertainty - var(1) = var(1) + thermo%first_order%F(2) * f_unit - var(2) = var(2) + thermo%first_order%U(2) * e_unit - var(3) = var(3) + thermo%first_order%S(2) * s_unit - var(4) = var(4) + thermo%first_order%Cv(2) * c_unit - write(*, *) '' - write(*, *) 'Gibbs-Bogoliubov approximation: F = F_harm + ' + write(*, *) 'Harmonic contribution' write(*, opfc) 'Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' write(*, opff) buf - write(*, opff) var - write(u, *) '# Gibbs-Bogoliubov approximation: F = F_harm + ' + write(u, *) '# Harmonic contribution' write(u, opfc) '# Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' write(u, opff) buf - write(u, opff) var - - ! Update the values - buf(1) = buf(1) + thermo%second_order%F(1) * f_unit - buf(2) = buf(2) + thermo%second_order%U(1) * e_unit - buf(3) = buf(3) + thermo%second_order%S(1) * s_unit - buf(4) = buf(4) + thermo%second_order%Cv(1) * c_unit - ! And the uncertainty - var(1) = var(1) + thermo%second_order%F(2) * f_unit - var(2) = var(2) + thermo%second_order%U(2) * e_unit - var(3) = var(3) + thermo%second_order%S(2) * s_unit - var(4) = var(4) + thermo%second_order%Cv(2) * c_unit + + ! Third order (three-phonon) contribution + if (opts%thirdorder) then + buf3(1) = thermo%threephonon%F(1) * f_unit + buf3(2) = thermo%threephonon%U(1) * e_unit + buf3(3) = thermo%threephonon%S(1) * s_unit + buf3(4) = thermo%threephonon%Cv(1) * c_unit + write(*, *) '' + write(*, *) 'Third order contribution (F3)' + write(*, opfc) 'Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' + write(*, opff) buf3 + write(u, *) '# Third order contribution (F3)' + write(u, opfc) '# Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' + write(u, opff) buf3 + end if + + ! Fourth order (four-phonon) contribution + if (opts%fourthorder) then + buf4(1) = thermo%fourphonon%F(1) * f_unit + buf4(2) = thermo%fourphonon%U(1) * e_unit + buf4(3) = thermo%fourphonon%S(1) * s_unit + buf4(4) = thermo%fourphonon%Cv(1) * c_unit + write(*, *) '' + write(*, *) 'Fourth order contribution (F4)' + write(*, opfc) 'Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' + write(*, opff) buf4 + write(u, *) '# Fourth order contribution (F4)' + write(u, opfc) '# Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' + write(u, opff) buf4 + end if + + ! Total anharmonic free energy write(*, *) '' - write(*, *) 'Second order cumulant approximation to the free energy' + write(*, *) 'Total: F = F_harm + F3 + F4' + buf(1) = buf(1) + thermo%threephonon%F(1) * f_unit + thermo%fourphonon%F(1) * f_unit + buf(2) = buf(2) + thermo%threephonon%U(1) * e_unit + thermo%fourphonon%U(1) * e_unit + buf(3) = buf(3) + thermo%threephonon%S(1) * s_unit + thermo%fourphonon%S(1) * s_unit + buf(4) = buf(4) + thermo%threephonon%Cv(1) * c_unit + thermo%fourphonon%Cv(1) * c_unit write(*, opfc) 'Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' write(*, opff) buf - write(*, opff) var - write(u, *) '# Second order cumulant approximation to the free energy' + write(u, *) '# Total: F = F_harm + F3 + F4' write(u, opfc) '# Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' write(u, opff) buf - write(u, opff) var write(*, *) '' write(*, *) 'Elastic properties' - write(*, '(2(1X,A24))') 'Pressure [GPa]', 'Uncertainty [GPa]' - write(*, '(2(1X,F24.12))') -pressure(1), pressure(2) + write(*, '(1X,A24)') 'Pressure [GPa]' + write(*, '(1X,F24.12)') -pressure write(*, *) 'Stress tensor [GPa]' do i=1, 3 - write(*, opfs) sigma(i, :, 1) - end do - write(*, *) 'Uncertainty [GPa]' - do i=1, 3 - write(*, opfs) sigma(i, :, 2) + write(*, opfs) sigma(i, :) end do close(u) end if diff --git a/src/anharmonic_free_energy/options.f90 b/src/anharmonic_free_energy/options.f90 index c2e6383a..0512a2bc 100644 --- a/src/anharmonic_free_energy/options.f90 +++ b/src/anharmonic_free_energy/options.f90 @@ -12,9 +12,7 @@ module options integer, dimension(3) :: qgrid, qg3ph, qg4ph integer :: integrationtype integer :: verbosity - integer :: nblocks logical :: quantum = .false. - logical :: stochastic = .false. logical :: thirdorder = .false. logical :: fourthorder = .false. contains @@ -61,10 +59,6 @@ subroutine parse(opts) help='Use Bose-Einstein occupations to compute the free energy', & required=.false., act='store_true', def='.false.', error=lo_status) if (lo_status .ne. 0) stop - call cli%add(switch='--stochastic', & - help='Add second order cumulant contribution to the free energy with a minus sign for self-consistent sampling', & - required=.false., act='store_true', def='.false.', error=lo_status) - if (lo_status .ne. 0) stop call cli%add(switch='--thirdorder', & help='Compute third order anharmonic correction to the free energy', & required=.false., act='store_true', def='.false.', error=lo_status) @@ -73,10 +67,6 @@ subroutine parse(opts) help='Compute fourth order anharmonic correction to the free energy', & required=.false., act='store_true', def='.false.', error=lo_status) if (lo_status .ne. 0) stop - call cli%add(switch='--nblocks', & - help='Number of blocks used to compute uncertainty', & - required=.false., act='store', def='10', error=lo_status) - if (lo_status .ne. 0) stop cli_manpage cli_verbose @@ -99,22 +89,13 @@ subroutine parse(opts) call cli%get(switch='--temperature', val=opts%temperature, error=lo_status); errctr = errctr + lo_status call cli%get(switch='--qpoint_grid', val=opts%qgrid, error=lo_status); errctr = errctr + lo_status call cli%get(switch='--quantum', val=opts%quantum, error=lo_status); errctr = errctr + lo_status - call cli%get(switch='--stochastic', val=opts%stochastic, error=lo_status); errctr = errctr + lo_status call cli%get(switch='--thirdorder', val=opts%thirdorder, error=lo_status); errctr = errctr + lo_status call cli%get(switch='--fourthorder', val=opts%fourthorder, error=lo_status); errctr = errctr + lo_status - call cli%get(switch='--nblocks', val=opts%nblocks, error=lo_status); errctr = errctr + lo_status call cli%get(switch='--qpoint_grid3ph', val=opts%qg3ph, error=lo_status); errctr = errctr + lo_status call cli%get(switch='--qpoint_grid4ph', val=opts%qg4ph, error=lo_status); errctr = errctr + lo_status - call cli%get(switch='--nblocks', val=opts%nblocks, error=lo_status); errctr = errctr + lo_status if (errctr .ne. 0) call lo_stop_gracefully(['Failed parsing the command line options'], lo_exitcode_baddim) - ! If we have MD data, makes no sense to use the high order correction - if (.not. opts%stochastic .and. (opts%thirdorder .or. opts%fourthorder)) then - write(*, *) 'Makes no sense to use higher order IFC if the configurations are not from a stochastic sampling' - stop - end if - ! We have to enable thirdorder to use the qg3ph flag if (maxval(opts%qg3ph) .gt. 0 .and. .not. opts%thirdorder) then write(*, *) 'You have to enable thirdorder to use a three-phonon q-grid, stopping calculation.' diff --git a/src/anharmonic_free_energy/thirdorder.f90 b/src/anharmonic_free_energy/thirdorder.f90 index bf9900bd..9a833248 100644 --- a/src/anharmonic_free_energy/thirdorder.f90 +++ b/src/anharmonic_free_energy/thirdorder.f90 @@ -210,6 +210,7 @@ subroutine free_energy_thirdorder(uc, fct, qp, dr, temperature, fe3, s3, cv3, qu end select fe3 = 0.0_r8 + s3 = 0.0_r8 cv3 = 0.0_r8 ! First we compute the broadening parameter for each modes @@ -286,15 +287,16 @@ subroutine free_energy_thirdorder(uc, fct, qp, dr, temperature, fe3, s3, cv3, qu ! This are the formula to get the free energy f1 = (n1 + 1.0_r8)*(n2 + n3 + 1.0_r8) + n2*n3 - f2 = n1*n2 + n1*n3 - n2*n3 + 1.0_r8 + f2 = n3*(n1 + n2 + 1.0_r8) - n1*n2 ! Here is for the entropy df1 = dn1 * (n2 + n3 + 1.0_r8) + (n1 + 1.0_r8) * (dn2 + dn3) + dn2 * n3 + n2 * dn3 - df2 = dn1 * n2 + n1 * dn2 + dn1 * n3 + n1 * dn3 - dn2 * n3 - n2 * dn3 + df2 = dn3 * (n1 + n2 + 1.0_r8) + dn1 * (n3 - n2) + dn2 * (n3 - n1) ! And the heat capacity ddf1 = ddn1 * (n2 + n3 + 1.0_r8) + 2.0_r8 * dn1 * (dn2 + dn3) + (n1 + 1.0_r8) * (ddn2 + ddn3) + & ddn2 * n3 + n2 * ddn3 + 2.0_r8 * dn2 * dn3 - ddf2 = ddn1 * n2 + n1 * ddn2 + 2.0_r8 * dn1 * dn2 + ddn1 * n3 + n1 * ddn3 + 2.0_r8 * dn1 * dn3 - & - ddn2 * n3 - n2 * ddn3 - 2.0_r8 * dn2 * dn3 + ddf2 = ddn3 * (n1 + n2 + 1.0_r8) + dn3 * (dn1 + dn2) + & + ddn1 * (n3 - n2) + dn1 * (dn3 - dn2) + & + ddn2 * (n3 - n1) + dn2 * (dn3 - dn1) ! Compute the principal values f1 = f1*real(1.0_r8/(om1 + om2 + om3 + lo_imag*sigma), r8) From b9b53b9d814208d367d5929188be9009e58d6f31 Mon Sep 17 00:00:00 2001 From: ejmeitz Date: Fri, 20 Mar 2026 14:48:21 -0400 Subject: [PATCH 18/28] remove unneeded options, check build --- src/anharmonic_free_energy/main.f90 | 80 +++++++++----------------- src/anharmonic_free_energy/options.f90 | 48 +++++++--------- 2 files changed, 48 insertions(+), 80 deletions(-) diff --git a/src/anharmonic_free_energy/main.f90 b/src/anharmonic_free_energy/main.f90 index da42f71a..0a11842a 100644 --- a/src/anharmonic_free_energy/main.f90 +++ b/src/anharmonic_free_energy/main.f90 @@ -30,7 +30,6 @@ program anharmonic_free_energy type(lo_thermodynamics) :: thermo real(r8) :: timer_init, timer_total -logical :: havehighorder ! Init MPI, timers and options call mw%init() @@ -51,7 +50,7 @@ program anharmonic_free_energy write(*, *) '' write(*, '(1X,A40,F20.12)') 'Temperature ', opts%temperature write(*, '(1X,A40,L3)') 'Quantum limit ', opts%quantum - write(*, '(1X,A40,I4,I4,I4)') 'Q-point grid Harmonic ', opts%qgrid + write(*, '(1X,A40,I4,I4,I4)') 'Q-point grid Harmonic ', opts%qgh write(*, '(1X,A40,I4,I4,I4)') 'Third order q-point grid ', opts%qg3ph write(*, '(1X,A40,I4,I4,I4)') 'Fourth order q-point grid ', opts%qg4ph write(*, *) '' @@ -68,24 +67,22 @@ program anharmonic_free_energy call fc%readfromfile(uc, 'infile.forceconstant', mem, verbosity=-1) if (mw%talk) write (*, *) '... read second order forceconstant' - if (opts%thirdorder) then + if (.not. opts%nothirdorder) then call fct%readfromfile(uc, 'infile.forceconstant_thirdorder') if (mw%talk) write (*, *) '... read third order forceconstant' end if - if (opts%fourthorder) then + if (.not. opts%nofourthorder) then call fcf%readfromfile(uc, 'infile.forceconstant_fourthorder') if (mw%talk) write (*, *) '... read fourth order forceconstant' end if - havehighorder = .false. - if (opts%thirdorder .or. opts%fourthorder) havehighorder = .true. call tmr%tock('reading input') timer_init = walltime() - timer_init thermo%temperature = opts%temperature - thermo%thirdorder = opts%thirdorder - thermo%fourthorder = opts%fourthorder + thermo%thirdorder = .not. opts%nothirdorder + thermo%fourthorder = .not. opts%nofourthorder end block init latdyn: block @@ -104,7 +101,7 @@ program anharmonic_free_energy end if if (mw%talk) write(*, *) '... generating q-mesh' - call lo_generate_qmesh(qp, uc, opts%qgrid, 'fft', timereversal=.true., & + call lo_generate_qmesh(qp, uc, opts%qgh, 'fft', timereversal=.true., & headrankonly=.false., mw=mw, mem=mem, verbosity=opts%verbosity) if (mw%talk) write(*, *) '... generating harmonic dispersion' call dr%generate(qp, fc, uc, mw=mw, mem=mem, verbosity=opts%verbosity) @@ -128,30 +125,30 @@ program anharmonic_free_energy thermo%harmonic%S(1) = dr%phonon_entropy(temperature) thermo%harmonic%U(1) = thermo%harmonic%F(1) + temperature * thermo%harmonic%S(1) thermo%harmonic%Cv(1) = dr%phonon_cv(temperature) - call dr%phonon_kinetic_stress(qp, uc, temperature, thermo%harmonic%stress(:, :, 1)) + ! call dr%phonon_kinetic_stress(qp, uc, temperature, thermo%harmonic%stress(:, :, 1)) else thermo%harmonic%F(1) = dr%phonon_free_energy_classical(temperature) thermo%harmonic%U(1) = 3.0_r8 * lo_kb_Hartree * temperature thermo%harmonic%S(1) = (thermo%harmonic%U(1) - thermo%harmonic%F(1)) / temperature thermo%harmonic%Cv(1) = 3.0_r8 * lo_kb_Hartree thermo%harmonic%stress = 0.0_r8 - do i=1, 3 - thermo%harmonic%stress(i, i, 1) = lo_kb_Hartree * temperature * uc%na / uc%volume - end do + ! do i=1, 3 + ! thermo%harmonic%stress(i, i, 1) = lo_kb_Hartree * temperature * uc%na / uc%volume + ! end do end if ! Usually not needed here, but always a good idea to clean - call lo_symmetrize_stress(thermo%harmonic%stress(:, :, 1), uc) + ! call lo_symmetrize_stress(thermo%harmonic%stress(:, :, 1), uc) ! If we have third order IFC, might as well compute elastic things - if (opts%thirdorder) then - if (mw%talk) write(*, *) '... computing third order contribution to elastic properties' - - call elastic_thirdorder(uc, fc, fct, qp, dr, opts%temperature, thermo%threephonon%stress(:, :, 1), & - thermo%alpha, opts%quantum, mw, mem) - ! Now we symmetrize - call lo_symmetrize_stress(thermo%threephonon%stress(:, :, 1), uc) - call lo_symmetrize_stress(thermo%alpha, uc) - end if + ! if (opts%thirdorder) then + ! if (mw%talk) write(*, *) '... computing third order contribution to elastic properties' + + ! call elastic_thirdorder(uc, fc, fct, qp, dr, opts%temperature, thermo%threephonon%stress(:, :, 1), & + ! thermo%alpha, opts%quantum, mw, mem) + ! ! Now we symmetrize + ! call lo_symmetrize_stress(thermo%threephonon%stress(:, :, 1), uc) + ! call lo_symmetrize_stress(thermo%alpha, uc) + ! end if call tmr%tock('harmonic properties') end block latdyn @@ -167,7 +164,7 @@ program anharmonic_free_energy real(r8) :: fe3, s3, cv3 - if (opts%thirdorder) then + if (.not. opts%nothirdorder) then if (mw%talk) then write(*, *) '' write(*, *) 'THREE PHONONS CONTRIBUTION' @@ -197,7 +194,7 @@ program anharmonic_free_energy !> The third order contribution real(r8) :: fe4, s4, cv4 - if (opts%fourthorder) then + if (.not. opts%nofourthorder) then if (mw%talk) then write(*, *) '' write(*, *) 'FOUR PHONONS CONTRIBUTION' @@ -236,14 +233,14 @@ program anharmonic_free_energy e_unit = lo_Hartree_to_eV s_unit = 1.0 / lo_kb_Hartree c_unit = 1.0 / lo_kb_Hartree - p_unit = lo_pressure_HartreeBohr_to_GPa + ! p_unit = lo_pressure_HartreeBohr_to_GPa ! Get the stress tensor (harmonic + threephonon only) - sigma = (thermo%harmonic%stress(:, :, 1) + thermo%threephonon%stress(:, :, 1)) * p_unit - pressure = lo_trace(sigma) / 3.0_r8 + ! sigma = (thermo%harmonic%stress(:, :, 1) + thermo%threephonon%stress(:, :, 1)) * p_unit + ! pressure = lo_trace(sigma) / 3.0_r8 if (mw%talk) then - u = open_file('out', 'outfile.anharmonic_free_energy') + u = open_file('out', 'outfile.anharmonic_thermodynamics') write(u, '(A2,A12,8X,E20.12)') '# ', 'Temperature:', opts%temperature opfc = '(4(1X,A24))' @@ -266,7 +263,7 @@ program anharmonic_free_energy write(u, opff) buf ! Third order (three-phonon) contribution - if (opts%thirdorder) then + if (.not. opts%nothirdorder) then buf3(1) = thermo%threephonon%F(1) * f_unit buf3(2) = thermo%threephonon%U(1) * e_unit buf3(3) = thermo%threephonon%S(1) * s_unit @@ -281,7 +278,7 @@ program anharmonic_free_energy end if ! Fourth order (four-phonon) contribution - if (opts%fourthorder) then + if (.not. opts%nofourthorder) then buf4(1) = thermo%fourphonon%F(1) * f_unit buf4(2) = thermo%fourphonon%U(1) * e_unit buf4(3) = thermo%fourphonon%S(1) * s_unit @@ -295,27 +292,6 @@ program anharmonic_free_energy write(u, opff) buf4 end if - ! Total anharmonic free energy - write(*, *) '' - write(*, *) 'Total: F = F_harm + F3 + F4' - buf(1) = buf(1) + thermo%threephonon%F(1) * f_unit + thermo%fourphonon%F(1) * f_unit - buf(2) = buf(2) + thermo%threephonon%U(1) * e_unit + thermo%fourphonon%U(1) * e_unit - buf(3) = buf(3) + thermo%threephonon%S(1) * s_unit + thermo%fourphonon%S(1) * s_unit - buf(4) = buf(4) + thermo%threephonon%Cv(1) * c_unit + thermo%fourphonon%Cv(1) * c_unit - write(*, opfc) 'Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' - write(*, opff) buf - write(u, *) '# Total: F = F_harm + F3 + F4' - write(u, opfc) '# Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' - write(u, opff) buf - - write(*, *) '' - write(*, *) 'Elastic properties' - write(*, '(1X,A24)') 'Pressure [GPa]' - write(*, '(1X,F24.12)') -pressure - write(*, *) 'Stress tensor [GPa]' - do i=1, 3 - write(*, opfs) sigma(i, :) - end do close(u) end if diff --git a/src/anharmonic_free_energy/options.f90 b/src/anharmonic_free_energy/options.f90 index 0512a2bc..c95699b0 100644 --- a/src/anharmonic_free_energy/options.f90 +++ b/src/anharmonic_free_energy/options.f90 @@ -9,12 +9,12 @@ module options type lo_opts real(r8) :: temperature - integer, dimension(3) :: qgrid, qg3ph, qg4ph + integer, dimension(3) :: qgh, qg3ph, qg4ph integer :: integrationtype integer :: verbosity logical :: quantum = .false. - logical :: thirdorder = .false. - logical :: fourthorder = .false. + logical :: nothirdorder = .false. + logical :: nofourthorder = .false. contains procedure :: parse end type @@ -42,14 +42,17 @@ subroutine parse(opts) epilog=new_line('a')//"...") ! Specify some options - cli_qpoint_grid + call cli%add(switch='--qpoint_harmonic', switch_ab='-qgh', & + help='Dimension of the q-grid for harmonic contributions', & + nargs='3', required=.false., act='store', def='25 25 25', error=lo_status) + if (lo_status .ne. 0) stop call cli%add(switch='--qpoint_grid3ph', switch_ab='-qg3ph', & help='Dimension of the q-grid for three phonon contribution', & - nargs='3', required=.false., act='store', def='-1 -1 -1', error=lo_status) + nargs='3', required=.false., act='store', def='20 20 20', error=lo_status) if (lo_status .ne. 0) stop call cli%add(switch='--qpoint_grid4ph', switch_ab='-qg4ph', & help='Dimension of the q-grid for four phonon contribution', & - nargs='3', required=.false., act='store', def='-1 -1 -1', error=lo_status) + nargs='3', required=.false., act='store', def='20 20 20', error=lo_status) if (lo_status .ne. 0) stop call cli%add(switch='--temperature', & help='The temperature at which the thermodynamic properties are computed', & @@ -59,12 +62,12 @@ subroutine parse(opts) help='Use Bose-Einstein occupations to compute the free energy', & required=.false., act='store_true', def='.false.', error=lo_status) if (lo_status .ne. 0) stop - call cli%add(switch='--thirdorder', & - help='Compute third order anharmonic correction to the free energy', & + call cli%add(switch='--nothirdorder', & + help='Do NOT compute third order anharmonic correction to the free energy', & required=.false., act='store_true', def='.false.', error=lo_status) if (lo_status .ne. 0) stop - call cli%add(switch='--fourthorder', & - help='Compute fourth order anharmonic correction to the free energy', & + call cli%add(switch='--nofourthorder', & + help='Do NOT compute fourth order anharmonic correction to the free energy', & required=.false., act='store_true', def='.false.', error=lo_status) if (lo_status .ne. 0) stop cli_manpage @@ -87,33 +90,22 @@ subroutine parse(opts) ! get real options call cli%get(switch='--temperature', val=opts%temperature, error=lo_status); errctr = errctr + lo_status - call cli%get(switch='--qpoint_grid', val=opts%qgrid, error=lo_status); errctr = errctr + lo_status call cli%get(switch='--quantum', val=opts%quantum, error=lo_status); errctr = errctr + lo_status - call cli%get(switch='--thirdorder', val=opts%thirdorder, error=lo_status); errctr = errctr + lo_status - call cli%get(switch='--fourthorder', val=opts%fourthorder, error=lo_status); errctr = errctr + lo_status + call cli%get(switch='--nothirdorder', val=opts%nothirdorder, error=lo_status); errctr = errctr + lo_status + call cli%get(switch='--nofourthorder', val=opts%nofourthorder, error=lo_status); errctr = errctr + lo_status call cli%get(switch='--qpoint_grid3ph', val=opts%qg3ph, error=lo_status); errctr = errctr + lo_status call cli%get(switch='--qpoint_grid4ph', val=opts%qg4ph, error=lo_status); errctr = errctr + lo_status if (errctr .ne. 0) call lo_stop_gracefully(['Failed parsing the command line options'], lo_exitcode_baddim) - ! We have to enable thirdorder to use the qg3ph flag - if (maxval(opts%qg3ph) .gt. 0 .and. .not. opts%thirdorder) then - write(*, *) 'You have to enable thirdorder to use a three-phonon q-grid, stopping calculation.' - stop - end if - if (minval(opts%qg3ph) .le. 0 .and. opts%thirdorder) then - opts%qg3ph = opts%qgrid + if (maxval(opts%qg3ph) .gt. 0 .and. opts%nothirdorder) then + write(*, *) 'WARNING: You turned off thirdorder but still specified a three-phonon q-grid.' end if - ! We have to enable fourthorder to use the qg4ph flag - if (maxval(opts%qg4ph) .gt. 0 .and. .not. opts%fourthorder) then - write(*, *) 'You have to enable fourthorder to use a four-phonon q-grid, stopping calculation.' - stop - end if - if (minval(opts%qg4ph) .le. 0 .and. opts%fourthorder) then - write(*, *) opts%qg4ph - opts%qg4ph = opts%qgrid + if (maxval(opts%qg4ph) .gt. 0 .and. opts%nofourthorder) then + write(*, *) 'WARNING: You turned off fourthorder but still specified a four-phonon q-grid.' end if + end subroutine end module From 56f049c8c2b0ab2261c039203c602e52ad03693c Mon Sep 17 00:00:00 2001 From: ejmeitz Date: Fri, 20 Mar 2026 17:13:46 -0400 Subject: [PATCH 19/28] seems mostly right now --- src/anharmonic_free_energy/options.f90 | 1 + src/anharmonic_free_energy/thirdorder.f90 | 13 +++---------- 2 files changed, 4 insertions(+), 10 deletions(-) diff --git a/src/anharmonic_free_energy/options.f90 b/src/anharmonic_free_energy/options.f90 index c95699b0..d125d112 100644 --- a/src/anharmonic_free_energy/options.f90 +++ b/src/anharmonic_free_energy/options.f90 @@ -93,6 +93,7 @@ subroutine parse(opts) call cli%get(switch='--quantum', val=opts%quantum, error=lo_status); errctr = errctr + lo_status call cli%get(switch='--nothirdorder', val=opts%nothirdorder, error=lo_status); errctr = errctr + lo_status call cli%get(switch='--nofourthorder', val=opts%nofourthorder, error=lo_status); errctr = errctr + lo_status + call cli%get(switch='--qpoint_harmonic', val=opts%qgh, error=lo_status); errctr = errctr + lo_status call cli%get(switch='--qpoint_grid3ph', val=opts%qg3ph, error=lo_status); errctr = errctr + lo_status call cli%get(switch='--qpoint_grid4ph', val=opts%qg4ph, error=lo_status); errctr = errctr + lo_status diff --git a/src/anharmonic_free_energy/thirdorder.f90 b/src/anharmonic_free_energy/thirdorder.f90 index 9a833248..7fee5fe1 100644 --- a/src/anharmonic_free_energy/thirdorder.f90 +++ b/src/anharmonic_free_energy/thirdorder.f90 @@ -183,7 +183,7 @@ subroutine free_energy_thirdorder(uc, fct, qp, dr, temperature, fe3, s3, cv3, qu !> Frequencies, bose-einstein occupation and scattering strength and some other buffer real(r8) :: sigma, om1, om2, om3, n2, n3, psisq, f0, f1, plf0, plf1, perm, f2, n1, pref, t0, prefactor !> - real(r8) :: sig1, sig2, sig3, mult, dn1, dn2, dn3, ddn1, ddn2, ddn3, df1, df2, ddf1, ddf2, df0, ddf0 + real(r8) :: sig1, sig2, sig3, dn1, dn2, dn3, ddn1, ddn2, ddn3, df1, df2, ddf1, ddf2, df0, ddf0 !> The complex threephonon matrix element complex(r8) :: c0 !> Integers for do loops and counting @@ -227,16 +227,9 @@ subroutine free_energy_thirdorder(uc, fct, qp, dr, temperature, fe3, s3, cv3, qu ctr = ctr + 1 if (mod(ctr, mw%n) .ne. mw%r) cycle q3 = fft_third_grid_index(qp%ip(q1)%full_index, q2, dims) - if (q3 .lt. q2) cycle + - ! The prefactor to take into account what we are skipping - if (q2 .eq. q3) then - mult = 1.0_r8 - else - mult = 2.0_r8 - end if - - prefactor = qp%ip(q1)%integration_weight*qp%ap(q2)%integration_weight*mult/uc%na + prefactor = qp%ip(q1)%integration_weight*qp%ap(q2)%integration_weight/uc%na ! pre-transform the matrix element call pretransform_phi3(fct, qp%ap(q2)%r, qp%ap(q3)%r, ptf) From abbeb76055d03d6ec5de1a604cfefac3639797bf Mon Sep 17 00:00:00 2001 From: ejmeitz Date: Tue, 24 Mar 2026 14:18:40 -0400 Subject: [PATCH 20/28] add tests, update manual --- src/anharmonic_free_energy/main.f90 | 34 +- src/anharmonic_free_energy/manual.md | 4 +- src/anharmonic_free_energy/options.f90 | 2 +- .../Argon_80K_classical/infile.forceconstant | 399 + .../infile.forceconstant_fourthorder | 43928 +++++++++++++ .../infile.forceconstant_thirdorder | 44028 +++++++++++++ .../Argon_80K_classical/infile.ssposcar | 264 + .../Argon_80K_classical/infile.ucposcar | 9 + tests/anharmonic_free_energy/Makefile | 4 +- .../Neon_14K_quantum/infile.forceconstant | 279 + .../infile.forceconstant_fourthorder | 14738 +++++ .../infile.forceconstant_thirdorder | 21348 +++++++ .../Neon_14K_quantum/infile.ssposcar | 264 + .../Neon_14K_quantum/infile.ucposcar | 9 + .../infile.forceconstant | 175 + .../infile.forceconstant_fourthorder | 53274 ++++++++++++++++ .../infile.forceconstant_thirdorder | 3994 ++ .../Silicon_1600K_classical/infile.ssposcar | 224 + .../Silicon_1600K_classical/infile.ucposcar | 11 + .../infile.forceconstant | 1 - .../infile.forceconstant_thirdorder | 1 - tests/anharmonic_free_energy/infile.forces | 1 - tests/anharmonic_free_energy/infile.meta | 1 - tests/anharmonic_free_energy/infile.positions | 1 - tests/anharmonic_free_energy/infile.ssposcar | 1 - tests/anharmonic_free_energy/infile.stat | 1 - tests/anharmonic_free_energy/infile.ucposcar | 1 - .../reference/Argon_80K_classical_reference | 6 + .../reference/Neon_14K_quantum_reference | 6 + .../Silicon_1600K_classical_reference | 6 + .../reference/outfile.anharmonic_free_energy | 5 - .../test_anharmonic_free_energy.py | 34 +- 32 files changed, 183013 insertions(+), 40 deletions(-) create mode 100644 tests/anharmonic_free_energy/Argon_80K_classical/infile.forceconstant create mode 100644 tests/anharmonic_free_energy/Argon_80K_classical/infile.forceconstant_fourthorder create mode 100644 tests/anharmonic_free_energy/Argon_80K_classical/infile.forceconstant_thirdorder create mode 100644 tests/anharmonic_free_energy/Argon_80K_classical/infile.ssposcar create mode 100644 tests/anharmonic_free_energy/Argon_80K_classical/infile.ucposcar create mode 100644 tests/anharmonic_free_energy/Neon_14K_quantum/infile.forceconstant create mode 100644 tests/anharmonic_free_energy/Neon_14K_quantum/infile.forceconstant_fourthorder create mode 100644 tests/anharmonic_free_energy/Neon_14K_quantum/infile.forceconstant_thirdorder create mode 100644 tests/anharmonic_free_energy/Neon_14K_quantum/infile.ssposcar create mode 100644 tests/anharmonic_free_energy/Neon_14K_quantum/infile.ucposcar create mode 100644 tests/anharmonic_free_energy/Silicon_1600K_classical/infile.forceconstant create mode 100644 tests/anharmonic_free_energy/Silicon_1600K_classical/infile.forceconstant_fourthorder create mode 100644 tests/anharmonic_free_energy/Silicon_1600K_classical/infile.forceconstant_thirdorder create mode 100644 tests/anharmonic_free_energy/Silicon_1600K_classical/infile.ssposcar create mode 100644 tests/anharmonic_free_energy/Silicon_1600K_classical/infile.ucposcar delete mode 120000 tests/anharmonic_free_energy/infile.forceconstant delete mode 120000 tests/anharmonic_free_energy/infile.forceconstant_thirdorder delete mode 120000 tests/anharmonic_free_energy/infile.forces delete mode 120000 tests/anharmonic_free_energy/infile.meta delete mode 120000 tests/anharmonic_free_energy/infile.positions delete mode 120000 tests/anharmonic_free_energy/infile.ssposcar delete mode 120000 tests/anharmonic_free_energy/infile.stat delete mode 120000 tests/anharmonic_free_energy/infile.ucposcar create mode 100644 tests/anharmonic_free_energy/reference/Argon_80K_classical_reference create mode 100644 tests/anharmonic_free_energy/reference/Neon_14K_quantum_reference create mode 100644 tests/anharmonic_free_energy/reference/Silicon_1600K_classical_reference delete mode 100644 tests/anharmonic_free_energy/reference/outfile.anharmonic_free_energy diff --git a/src/anharmonic_free_energy/main.f90 b/src/anharmonic_free_energy/main.f90 index 0a11842a..99f8b92f 100644 --- a/src/anharmonic_free_energy/main.f90 +++ b/src/anharmonic_free_energy/main.f90 @@ -262,21 +262,6 @@ program anharmonic_free_energy write(u, opfc) '# Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' write(u, opff) buf - ! Third order (three-phonon) contribution - if (.not. opts%nothirdorder) then - buf3(1) = thermo%threephonon%F(1) * f_unit - buf3(2) = thermo%threephonon%U(1) * e_unit - buf3(3) = thermo%threephonon%S(1) * s_unit - buf3(4) = thermo%threephonon%Cv(1) * c_unit - write(*, *) '' - write(*, *) 'Third order contribution (F3)' - write(*, opfc) 'Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' - write(*, opff) buf3 - write(u, *) '# Third order contribution (F3)' - write(u, opfc) '# Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' - write(u, opff) buf3 - end if - ! Fourth order (four-phonon) contribution if (.not. opts%nofourthorder) then buf4(1) = thermo%fourphonon%F(1) * f_unit @@ -284,14 +269,29 @@ program anharmonic_free_energy buf4(3) = thermo%fourphonon%S(1) * s_unit buf4(4) = thermo%fourphonon%Cv(1) * c_unit write(*, *) '' - write(*, *) 'Fourth order contribution (F4)' + write(*, *) 'First Cumulant Contribution' write(*, opfc) 'Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' write(*, opff) buf4 - write(u, *) '# Fourth order contribution (F4)' + write(u, *) '# First Cumulant Contribution' write(u, opfc) '# Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' write(u, opff) buf4 end if + ! Third order (three-phonon) contribution + if (.not. opts%nothirdorder) then + buf3(1) = thermo%threephonon%F(1) * f_unit + buf3(2) = thermo%threephonon%U(1) * e_unit + buf3(3) = thermo%threephonon%S(1) * s_unit + buf3(4) = thermo%threephonon%Cv(1) * c_unit + write(*, *) '' + write(*, *) 'Second Cumulant Contribution' + write(*, opfc) 'Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' + write(*, opff) buf3 + write(u, *) '# Second Cumulant Contribution' + write(u, opfc) '# Free energy [eV/at]', 'Internal energy [eV/at]', 'Entropy [kB]', 'Heat capacity [kB]' + write(u, opff) buf3 + end if + close(u) end if diff --git a/src/anharmonic_free_energy/manual.md b/src/anharmonic_free_energy/manual.md index 5ba7e953..0b269dda 100644 --- a/src/anharmonic_free_energy/manual.md +++ b/src/anharmonic_free_energy/manual.md @@ -1,5 +1,7 @@ -This code calculates the anharmonic Helmholtz free energy. It includes the contributions from baseline shifts, renormalized phonons and higher order terms. +This code calculates the anharmonic Helmholtz free energy, internal energy, entropy and heat capacity. It includes the contributions from baseline shifts, renormalized phonons and higher order terms. This program must use force constants from sTDEP/SSCHA (self-consistent phonons). Force cosntants fit to MD/PIMD data are incompatible with this theory. + +Only the first and second-cumulant corrections are computed by this code. The constant corrections (i.e., $U_0$ and its derivatives) must be implemented elsewhere as it requires interfacing with a force-calculator like LAMMPS. Please refer to CITATION and a reference implementation [here](https://github.com/ejmeitz/CumulantAnalysis.jl). ### Longer summary diff --git a/src/anharmonic_free_energy/options.f90 b/src/anharmonic_free_energy/options.f90 index d125d112..0c1ed528 100644 --- a/src/anharmonic_free_energy/options.f90 +++ b/src/anharmonic_free_energy/options.f90 @@ -37,7 +37,7 @@ subroutine parse(opts) version=lo_version, & license=lo_licence, & help='Usage: ', & - description='Calculates the anharmonic free energy.', & + description='Calculates the anharmonic free energy given sTDEP force constants.', & examples=["mpirun anharmonic_free_energy"], & epilog=new_line('a')//"...") diff --git a/tests/anharmonic_free_energy/Argon_80K_classical/infile.forceconstant b/tests/anharmonic_free_energy/Argon_80K_classical/infile.forceconstant new file mode 100644 index 00000000..e6b58490 --- /dev/null +++ b/tests/anharmonic_free_energy/Argon_80K_classical/infile.forceconstant @@ -0,0 +1,399 @@ + 1 How many atoms per unit cell + 8.295919213738646 Realspace cutoff (A) + 79 How many neighbours does atom 1 have + 1 In the unit cell, what is the index of neighbour 1 of atom 1 + 0.0000000000000000 0.0000000000000000 0.0000000000000000 + 0.44889178211100261 0.0000000000000000 0.0000000000000000 + 0.0000000000000000 0.44889178211100256 0.0000000000000000 + 0.0000000000000000 0.0000000000000000 0.44889178211100261 + 1 In the unit cell, what is the index of neighbour 2 of atom 1 + -1.0000000000000000 1.0000000000000000 0.0000000000000000 + -5.9723718853086610E-002 0.0000000000000000 6.3253514816645873E-002 + 0.0000000000000000 3.8307737422309911E-003 0.0000000000000000 + 6.3253514816645873E-002 0.0000000000000000 -5.9723718853086610E-002 + 1 In the unit cell, what is the index of neighbour 3 of atom 1 + 1.0000000000000000 -1.0000000000000000 0.0000000000000000 + -5.9723718853086610E-002 0.0000000000000000 6.3253514816645873E-002 + 0.0000000000000000 3.8307737422309911E-003 0.0000000000000000 + 6.3253514816645873E-002 0.0000000000000000 -5.9723718853086610E-002 + 1 In the unit cell, what is the index of neighbour 4 of atom 1 + 0.0000000000000000 0.0000000000000000 1.0000000000000000 + -5.9723718853086610E-002 0.0000000000000000 -6.3253514816645873E-002 + 0.0000000000000000 3.8307737422309911E-003 0.0000000000000000 + -6.3253514816645873E-002 0.0000000000000000 -5.9723718853086610E-002 + 1 In the unit cell, what is the index of neighbour 5 of atom 1 + -1.0000000000000000 0.0000000000000000 1.0000000000000000 + 3.8307737422309911E-003 0.0000000000000000 0.0000000000000000 + 0.0000000000000000 -5.9723718853086610E-002 6.3253514816645873E-002 + 0.0000000000000000 6.3253514816645873E-002 -5.9723718853086610E-002 + 1 In the unit cell, what is the index of neighbour 6 of atom 1 + -1.0000000000000000 0.0000000000000000 0.0000000000000000 + -5.9723718853086610E-002 -6.3253514816645873E-002 0.0000000000000000 + -6.3253514816645873E-002 -5.9723718853086610E-002 0.0000000000000000 + 0.0000000000000000 0.0000000000000000 3.8307737422309911E-003 + 1 In the unit cell, what is the index of neighbour 7 of atom 1 + 0.0000000000000000 1.0000000000000000 -1.0000000000000000 + -5.9723718853086610E-002 6.3253514816645873E-002 0.0000000000000000 + 6.3253514816645873E-002 -5.9723718853086610E-002 0.0000000000000000 + 0.0000000000000000 0.0000000000000000 3.8307737422309911E-003 + 1 In the unit cell, what is the index of neighbour 8 of atom 1 + 0.0000000000000000 1.0000000000000000 0.0000000000000000 + 3.8307737422309911E-003 0.0000000000000000 0.0000000000000000 + 0.0000000000000000 -5.9723718853086610E-002 -6.3253514816645873E-002 + 0.0000000000000000 -6.3253514816645873E-002 -5.9723718853086610E-002 + 1 In the unit cell, what is the index of neighbour 9 of atom 1 + 0.0000000000000000 -1.0000000000000000 0.0000000000000000 + 3.8307737422309911E-003 0.0000000000000000 0.0000000000000000 + 0.0000000000000000 -5.9723718853086610E-002 -6.3253514816645873E-002 + 0.0000000000000000 -6.3253514816645873E-002 -5.9723718853086610E-002 + 1 In the unit cell, what is the index of neighbour 10 of atom 1 + 0.0000000000000000 -1.0000000000000000 1.0000000000000000 + -5.9723718853086610E-002 6.3253514816645873E-002 0.0000000000000000 + 6.3253514816645873E-002 -5.9723718853086610E-002 0.0000000000000000 + 0.0000000000000000 0.0000000000000000 3.8307737422309911E-003 + 1 In the unit cell, what is the index of neighbour 11 of atom 1 + 1.0000000000000000 0.0000000000000000 0.0000000000000000 + -5.9723718853086610E-002 -6.3253514816645873E-002 0.0000000000000000 + -6.3253514816645873E-002 -5.9723718853086610E-002 0.0000000000000000 + 0.0000000000000000 0.0000000000000000 3.8307737422309911E-003 + 1 In the unit cell, what is the index of neighbour 12 of atom 1 + 1.0000000000000000 0.0000000000000000 -1.0000000000000000 + 3.8307737422309911E-003 0.0000000000000000 0.0000000000000000 + 0.0000000000000000 -5.9723718853086610E-002 6.3253514816645873E-002 + 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5.8429860388881907E-004 -3.0927235457822169E-004 -3.0927235457822169E-004 + -3.0927235457822169E-004 -9.4905718066452856E-005 9.6529816339358481E-005 + -3.0927235457822169E-004 9.6529816339358481E-005 -9.4905718066452856E-005 + 1 In the unit cell, what is the index of neighbour 42 of atom 1 + -2.0000000000000000 1.0000000000000000 0.0000000000000000 + 5.8429860388881907E-004 3.0927235457822169E-004 -3.0927235457822169E-004 + 3.0927235457822169E-004 -9.4905718066452856E-005 -9.6529816339358481E-005 + -3.0927235457822169E-004 -9.6529816339358481E-005 -9.4905718066452856E-005 + 1 In the unit cell, what is the index of neighbour 43 of atom 1 + -2.0000000000000000 1.0000000000000000 1.0000000000000000 + -9.4905718066452856E-005 9.6529816339358481E-005 -3.0927235457822169E-004 + 9.6529816339358481E-005 -9.4905718066452856E-005 -3.0927235457822169E-004 + -3.0927235457822169E-004 -3.0927235457822169E-004 5.8429860388881907E-004 + 1 In the unit cell, what is the index of neighbour 44 of atom 1 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0.875000000000000 0.875000000000000 diff --git a/tests/anharmonic_free_energy/Argon_80K_classical/infile.ucposcar b/tests/anharmonic_free_energy/Argon_80K_classical/infile.ucposcar new file mode 100644 index 00000000..a3217e46 --- /dev/null +++ b/tests/anharmonic_free_energy/Argon_80K_classical/infile.ucposcar @@ -0,0 +1,9 @@ +Ar FCC +5.2468 +0.500000000000 0.500000000000 0.000000000000 +0.000000000000 0.500000000000 0.500000000000 +0.500000000000 0.000000000000 0.500000000000 +Ar +1 +direct coordinates +0.000000000000 0.000000000000 0.000000000000 diff --git a/tests/anharmonic_free_energy/Makefile b/tests/anharmonic_free_energy/Makefile index e6c734df..0e14a355 100644 --- a/tests/anharmonic_free_energy/Makefile +++ b/tests/anharmonic_free_energy/Makefile @@ -1,2 +1,4 @@ testfiles: - anharmonic_free_energy --thirdorder -qg 4 4 4 + cd ./Argon_80K_classical | anharmonic_free_energy --temperature 80 -qg3ph 10 10 10 -qg4ph 10 10 10 -qgh 30 30 30 + cd ../Silicon_1600K_classical | anharmonic_free_energy --temperature 1600 -qg3ph 10 10 10 -qg4ph 10 10 10 -qgh 30 30 30 + cd ../Neon_14K_quantum | anharmonic_free_energy --temperature 14 --quantum -qg3ph 10 10 10 -qg4ph 10 10 10 -qgh 30 30 30 \ No newline at end of file diff --git a/tests/anharmonic_free_energy/Neon_14K_quantum/infile.forceconstant b/tests/anharmonic_free_energy/Neon_14K_quantum/infile.forceconstant new file mode 100644 index 00000000..c2423f59 --- /dev/null +++ b/tests/anharmonic_free_energy/Neon_14K_quantum/infile.forceconstant @@ -0,0 +1,279 @@ + 1 How many atoms per unit cell + 6.331974629739952 Realspace cutoff (A) + 55 How many neighbours does atom 1 have + 1 In the unit cell, what is the index of neighbour 1 of atom 1 + 0.0000000000000000 0.0000000000000000 0.0000000000000000 + 0.12761135226416648 0.0000000000000000 0.0000000000000000 + 0.0000000000000000 0.12761135226416648 0.0000000000000000 + 0.0000000000000000 0.0000000000000000 0.12761135226416648 + 1 In the unit cell, what is the index of neighbour 2 of atom 1 + -1.0000000000000000 0.0000000000000000 1.0000000000000000 + 6.6794254861375017E-004 0.0000000000000000 0.0000000000000000 + 0.0000000000000000 -1.6825940836041040E-002 1.7552120374330335E-002 + 0.0000000000000000 1.7552120374330335E-002 -1.6825940836041040E-002 + 1 In the unit cell, what is the index of neighbour 3 of atom 1 + -1.0000000000000000 1.0000000000000000 0.0000000000000000 + -1.6825940836041040E-002 0.0000000000000000 1.7552120374330335E-002 + 0.0000000000000000 6.6794254861375017E-004 0.0000000000000000 + 1.7552120374330335E-002 0.0000000000000000 -1.6825940836041040E-002 + 1 In the unit cell, what is the index of neighbour 4 of atom 1 + 0.0000000000000000 -1.0000000000000000 0.0000000000000000 + 6.6794254861375017E-004 0.0000000000000000 0.0000000000000000 + 0.0000000000000000 -1.6825940836041040E-002 -1.7552120374330335E-002 + 0.0000000000000000 -1.7552120374330335E-002 -1.6825940836041040E-002 + 1 In the unit cell, what is the index of neighbour 5 of atom 1 + 0.0000000000000000 -1.0000000000000000 1.0000000000000000 + -1.6825940836041040E-002 1.7552120374330335E-002 0.0000000000000000 + 1.7552120374330335E-002 -1.6825940836041040E-002 0.0000000000000000 + 0.0000000000000000 0.0000000000000000 6.6794254861375017E-004 + 1 In the unit cell, what is the index of neighbour 6 of atom 1 + 0.0000000000000000 0.0000000000000000 -1.0000000000000000 + -1.6825940836041040E-002 0.0000000000000000 -1.7552120374330335E-002 + 0.0000000000000000 6.6794254861375017E-004 0.0000000000000000 + -1.7552120374330335E-002 0.0000000000000000 -1.6825940836041040E-002 + 1 In the unit cell, what is the index of neighbour 7 of atom 1 + 0.0000000000000000 0.0000000000000000 1.0000000000000000 + -1.6825940836041040E-002 0.0000000000000000 -1.7552120374330335E-002 + 0.0000000000000000 6.6794254861375017E-004 0.0000000000000000 + -1.7552120374330335E-002 0.0000000000000000 -1.6825940836041040E-002 + 1 In the unit cell, what is the index of neighbour 8 of atom 1 + 0.0000000000000000 1.0000000000000000 -1.0000000000000000 + -1.6825940836041040E-002 1.7552120374330335E-002 0.0000000000000000 + 1.7552120374330335E-002 -1.6825940836041040E-002 0.0000000000000000 + 0.0000000000000000 0.0000000000000000 6.6794254861375017E-004 + 1 In the unit cell, what is the index of neighbour 9 of atom 1 + 0.0000000000000000 1.0000000000000000 0.0000000000000000 + 6.6794254861375017E-004 0.0000000000000000 0.0000000000000000 + 0.0000000000000000 -1.6825940836041040E-002 -1.7552120374330335E-002 + 0.0000000000000000 -1.7552120374330335E-002 -1.6825940836041040E-002 + 1 In the unit cell, what is the index of neighbour 10 of atom 1 + 1.0000000000000000 -1.0000000000000000 0.0000000000000000 + -1.6825940836041040E-002 0.0000000000000000 1.7552120374330335E-002 + 0.0000000000000000 6.6794254861375017E-004 0.0000000000000000 + 1.7552120374330335E-002 0.0000000000000000 -1.6825940836041040E-002 + 1 In the unit cell, what is the index of neighbour 11 of atom 1 + 1.0000000000000000 0.0000000000000000 -1.0000000000000000 + 6.6794254861375017E-004 0.0000000000000000 0.0000000000000000 + 0.0000000000000000 -1.6825940836041040E-002 1.7552120374330335E-002 + 0.0000000000000000 1.7552120374330335E-002 -1.6825940836041040E-002 + 1 In the unit cell, what is the index of neighbour 12 of atom 1 + 1.0000000000000000 0.0000000000000000 0.0000000000000000 + -1.6825940836041040E-002 -1.7552120374330335E-002 0.0000000000000000 + -1.7552120374330335E-002 -1.6825940836041040E-002 0.0000000000000000 + 0.0000000000000000 0.0000000000000000 6.6794254861375017E-004 + 1 In the unit cell, what is the index of neighbour 13 of atom 1 + -1.0000000000000000 0.0000000000000000 0.0000000000000000 + -1.6825940836041040E-002 -1.7552120374330335E-002 0.0000000000000000 + -1.7552120374330335E-002 -1.6825940836041040E-002 0.0000000000000000 + 0.0000000000000000 0.0000000000000000 6.6794254861375017E-004 + 1 In the unit cell, what is the index of neighbour 14 of atom 1 + 1.0000000000000000 -1.0000000000000000 1.0000000000000000 + 1.3052250315195696E-003 0.0000000000000000 0.0000000000000000 + 0.0000000000000000 -2.0979874022088686E-004 0.0000000000000000 + 0.0000000000000000 0.0000000000000000 -2.0979874022088686E-004 + 1 In the unit cell, what is the index of neighbour 15 of atom 1 + 1.0000000000000000 -1.0000000000000000 -1.0000000000000000 + -2.0979874022088686E-004 0.0000000000000000 0.0000000000000000 + 0.0000000000000000 -2.0979874022088686E-004 0.0000000000000000 + 0.0000000000000000 0.0000000000000000 1.3052250315195696E-003 + 1 In the unit cell, what is the index of neighbour 16 of atom 1 + -1.0000000000000000 -1.0000000000000000 1.0000000000000000 + -2.0979874022088686E-004 0.0000000000000000 0.0000000000000000 + 0.0000000000000000 1.3052250315195696E-003 0.0000000000000000 + 0.0000000000000000 0.0000000000000000 -2.0979874022088686E-004 + 1 In the unit cell, what is the index of neighbour 17 of atom 1 + 1.0000000000000000 1.0000000000000000 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-2.8006966538707362E-005 -1.1821289833230045E-004 -1.2077363531637089E-004 + -1.1821289833230045E-004 2.5728241544663603E-004 1.1821289833230045E-004 + -1.2077363531637089E-004 1.1821289833230045E-004 -2.8006966538707362E-005 + 1 In the unit cell, what is the index of neighbour 21 of atom 1 + 0.0000000000000000 1.0000000000000000 1.0000000000000000 + -2.8006966538707362E-005 1.2077363531637089E-004 1.1821289833230045E-004 + 1.2077363531637089E-004 -2.8006966538707362E-005 1.1821289833230045E-004 + 1.1821289833230045E-004 1.1821289833230045E-004 2.5728241544663603E-004 + 1 In the unit cell, what is the index of neighbour 22 of atom 1 + -2.0000000000000000 1.0000000000000000 1.0000000000000000 + -2.8006966538707362E-005 1.2077363531637089E-004 -1.1821289833230045E-004 + 1.2077363531637089E-004 -2.8006966538707362E-005 -1.1821289833230045E-004 + -1.1821289833230045E-004 -1.1821289833230045E-004 2.5728241544663603E-004 + 1 In the unit cell, what is the index of neighbour 23 of atom 1 + 2.0000000000000000 0.0000000000000000 -1.0000000000000000 + -2.8006966538707362E-005 1.1821289833230045E-004 -1.2077363531637089E-004 + 1.1821289833230045E-004 2.5728241544663603E-004 -1.1821289833230045E-004 + -1.2077363531637089E-004 -1.1821289833230045E-004 -2.8006966538707362E-005 + 1 In the unit cell, what is the index of neighbour 24 of atom 1 + 0.0000000000000000 1.0000000000000000 -2.0000000000000000 + 2.5728241544663603E-004 -1.1821289833230045E-004 1.1821289833230045E-004 + -1.1821289833230045E-004 -2.8006966538707362E-005 -1.2077363531637089E-004 + 1.1821289833230045E-004 -1.2077363531637089E-004 -2.8006966538707362E-005 + 1 In the unit cell, what is the index of neighbour 25 of atom 1 + 1.0000000000000000 0.0000000000000000 1.0000000000000000 + 2.5728241544663603E-004 1.1821289833230045E-004 1.1821289833230045E-004 + 1.1821289833230045E-004 -2.8006966538707362E-005 1.2077363531637089E-004 + 1.1821289833230045E-004 1.2077363531637089E-004 -2.8006966538707362E-005 + 1 In the unit cell, what is the index of neighbour 26 of atom 1 + -2.0000000000000000 0.0000000000000000 1.0000000000000000 + -2.8006966538707362E-005 1.1821289833230045E-004 -1.2077363531637089E-004 + 1.1821289833230045E-004 2.5728241544663603E-004 -1.1821289833230045E-004 + -1.2077363531637089E-004 -1.1821289833230045E-004 -2.8006966538707362E-005 + 1 In the unit cell, what is the index of neighbour 27 of atom 1 + 1.0000000000000000 0.0000000000000000 -2.0000000000000000 + -2.8006966538707362E-005 -1.2077363531637089E-004 1.1821289833230045E-004 + -1.2077363531637089E-004 -2.8006966538707362E-005 -1.1821289833230045E-004 + 1.1821289833230045E-004 -1.1821289833230045E-004 2.5728241544663603E-004 + 1 In the unit cell, what is the index of neighbour 28 of atom 1 + -2.0000000000000000 1.0000000000000000 0.0000000000000000 + 2.5728241544663603E-004 1.1821289833230045E-004 -1.1821289833230045E-004 + 1.1821289833230045E-004 -2.8006966538707362E-005 -1.2077363531637089E-004 + -1.1821289833230045E-004 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1.1821289833230045E-004 -1.1821289833230045E-004 + 1.1821289833230045E-004 -2.8006966538707362E-005 -1.2077363531637089E-004 + -1.1821289833230045E-004 -1.2077363531637089E-004 -2.8006966538707362E-005 + 1 In the unit cell, what is the index of neighbour 35 of atom 1 + 0.0000000000000000 -2.0000000000000000 1.0000000000000000 + -2.8006966538707362E-005 -1.1821289833230045E-004 -1.2077363531637089E-004 + -1.1821289833230045E-004 2.5728241544663603E-004 1.1821289833230045E-004 + -1.2077363531637089E-004 1.1821289833230045E-004 -2.8006966538707362E-005 + 1 In the unit cell, what is the index of neighbour 36 of atom 1 + -1.0000000000000000 2.0000000000000000 0.0000000000000000 + -2.8006966538707362E-005 -1.2077363531637089E-004 -1.1821289833230045E-004 + -1.2077363531637089E-004 -2.8006966538707362E-005 1.1821289833230045E-004 + -1.1821289833230045E-004 1.1821289833230045E-004 2.5728241544663603E-004 + 1 In the unit cell, what is the index of neighbour 37 of atom 1 + -1.0000000000000000 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what is the index of neighbour 40 of atom 1 + 0.0000000000000000 -1.0000000000000000 2.0000000000000000 + 2.5728241544663603E-004 -1.1821289833230045E-004 1.1821289833230045E-004 + -1.1821289833230045E-004 -2.8006966538707362E-005 -1.2077363531637089E-004 + 1.1821289833230045E-004 -1.2077363531637089E-004 -2.8006966538707362E-005 + 1 In the unit cell, what is the index of neighbour 41 of atom 1 + 2.0000000000000000 -1.0000000000000000 -1.0000000000000000 + -2.8006966538707362E-005 1.2077363531637089E-004 -1.1821289833230045E-004 + 1.2077363531637089E-004 -2.8006966538707362E-005 -1.1821289833230045E-004 + -1.1821289833230045E-004 -1.1821289833230045E-004 2.5728241544663603E-004 + 1 In the unit cell, what is the index of neighbour 42 of atom 1 + 1.0000000000000000 1.0000000000000000 0.0000000000000000 + -2.8006966538707362E-005 1.1821289833230045E-004 1.2077363531637089E-004 + 1.1821289833230045E-004 2.5728241544663603E-004 1.1821289833230045E-004 + 1.2077363531637089E-004 1.1821289833230045E-004 -2.8006966538707362E-005 + 1 In the unit cell, what is the index of neighbour 43 of atom 1 + -1.0000000000000000 -1.0000000000000000 0.0000000000000000 + -2.8006966538707362E-005 1.1821289833230045E-004 1.2077363531637089E-004 + 1.1821289833230045E-004 2.5728241544663603E-004 1.1821289833230045E-004 + 1.2077363531637089E-004 1.1821289833230045E-004 -2.8006966538707362E-005 + 1 In the unit cell, what is the index of neighbour 44 of atom 1 + 2.0000000000000000 0.0000000000000000 0.0000000000000000 + 1.1132448247350010E-004 8.6456849125589585E-005 0.0000000000000000 + 8.6456849125589585E-005 1.1132448247350010E-004 0.0000000000000000 + 0.0000000000000000 0.0000000000000000 1.3101352202344419E-005 + 1 In the unit cell, what is the index of neighbour 45 of atom 1 + 2.0000000000000000 -2.0000000000000000 0.0000000000000000 + 1.1132448247350010E-004 0.0000000000000000 -8.6456849125589585E-005 + 0.0000000000000000 1.3101352202344419E-005 0.0000000000000000 + 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a/tests/anharmonic_free_energy/Neon_14K_quantum/infile.ucposcar b/tests/anharmonic_free_energy/Neon_14K_quantum/infile.ucposcar new file mode 100644 index 00000000..a4c55880 --- /dev/null +++ b/tests/anharmonic_free_energy/Neon_14K_quantum/infile.ucposcar @@ -0,0 +1,9 @@ +POSCAR +4.4773821989528795 +0.500000000000 0.500000000000 0.000000000000 +0.000000000000 0.500000000000 0.500000000000 +0.500000000000 0.000000000000 0.500000000000 +Ne +1 +Direct +0.000000000000000 0.000000000000000 0.000000000000000 diff --git a/tests/anharmonic_free_energy/Silicon_1600K_classical/infile.forceconstant b/tests/anharmonic_free_energy/Silicon_1600K_classical/infile.forceconstant new file mode 100644 index 00000000..3480354c --- /dev/null +++ b/tests/anharmonic_free_energy/Silicon_1600K_classical/infile.forceconstant @@ -0,0 +1,175 @@ + 2 How many atoms per unit cell + 3.839589821895871 Realspace cutoff (A) + 17 How many neighbours does atom 1 have + 1 In the unit cell, what is the index of neighbour 1 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-0.10919224582373405 + 4.9423266512913018E-002 -4.9576827118800064E-002 0.10919224582373405 + 0.10919224582373405 -0.10919224582373405 0.24746210671238913 + 1 In the unit cell, what is the index of neighbour 8 of atom 1 + 0.0000000000000000 1.0000000000000000 0.0000000000000000 + 0.24746210671238913 0.10919224582373405 0.10919224582373405 + -0.10919224582373405 -4.9576827118800064E-002 -4.9423266512913018E-002 + -0.10919224582373405 -4.9423266512913018E-002 -4.9576827118800064E-002 + 1 In the unit cell, what is the index of neighbour 9 of atom 1 + 1.0000000000000000 -1.0000000000000000 0.0000000000000000 + -4.9576827118800064E-002 0.10919224582373405 4.9423266512913018E-002 + -0.10919224582373405 0.24746210671238913 0.10919224582373405 + 4.9423266512913018E-002 -0.10919224582373405 -4.9576827118800064E-002 + 1 In the unit cell, what is the index of neighbour 10 of atom 1 + 1.0000000000000000 0.0000000000000000 -1.0000000000000000 + 0.24746210671238913 -0.10919224582373405 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0.750000000000000 0.916666666666667 +0.916666666666667 0.916666666666667 0.750000000000000 diff --git a/tests/anharmonic_free_energy/Silicon_1600K_classical/infile.ucposcar b/tests/anharmonic_free_energy/Silicon_1600K_classical/infile.ucposcar new file mode 100644 index 00000000..3c904cb8 --- /dev/null +++ b/tests/anharmonic_free_energy/Silicon_1600K_classical/infile.ucposcar @@ -0,0 +1,11 @@ +Si Diamond +5.43 +0.500000000000 0.500000000000 0.000000000000 +0.000000000000 0.500000000000 0.500000000000 +0.500000000000 0.000000000000 0.500000000000 +Si +2 +direct coordinates +0.000000000000 0.000000000000 0.000000000000 +0.250000000000 0.250000000000 0.250000000000 + diff --git a/tests/anharmonic_free_energy/infile.forceconstant b/tests/anharmonic_free_energy/infile.forceconstant deleted file mode 120000 index 4b261f83..00000000 --- a/tests/anharmonic_free_energy/infile.forceconstant +++ /dev/null @@ -1 +0,0 @@ -../infiles/infile.forceconstant \ No newline at end of file diff --git a/tests/anharmonic_free_energy/infile.forceconstant_thirdorder b/tests/anharmonic_free_energy/infile.forceconstant_thirdorder deleted file mode 120000 index f544ade8..00000000 --- a/tests/anharmonic_free_energy/infile.forceconstant_thirdorder +++ /dev/null @@ -1 +0,0 @@ -../infiles/infile.forceconstant_thirdorder \ No newline at end of file diff --git a/tests/anharmonic_free_energy/infile.forces b/tests/anharmonic_free_energy/infile.forces deleted file mode 120000 index 347ec060..00000000 --- a/tests/anharmonic_free_energy/infile.forces +++ /dev/null @@ -1 +0,0 @@ -../infiles/infile.forces \ No newline at end of file diff --git a/tests/anharmonic_free_energy/infile.meta b/tests/anharmonic_free_energy/infile.meta deleted file mode 120000 index ef14956c..00000000 --- a/tests/anharmonic_free_energy/infile.meta +++ /dev/null @@ -1 +0,0 @@ -../infiles/infile.meta \ No newline at end of file diff --git a/tests/anharmonic_free_energy/infile.positions b/tests/anharmonic_free_energy/infile.positions deleted file mode 120000 index fcce51a5..00000000 --- a/tests/anharmonic_free_energy/infile.positions +++ /dev/null @@ -1 +0,0 @@ -../infiles/infile.positions \ No newline at end of file diff --git a/tests/anharmonic_free_energy/infile.ssposcar b/tests/anharmonic_free_energy/infile.ssposcar deleted file mode 120000 index 1cfa068d..00000000 --- a/tests/anharmonic_free_energy/infile.ssposcar +++ /dev/null @@ -1 +0,0 @@ -../infiles/infile.ssposcar \ No newline at end of file diff --git a/tests/anharmonic_free_energy/infile.stat b/tests/anharmonic_free_energy/infile.stat deleted file mode 120000 index 3e9aa633..00000000 --- a/tests/anharmonic_free_energy/infile.stat +++ /dev/null @@ -1 +0,0 @@ -../infiles/infile.stat \ No newline at end of file diff --git a/tests/anharmonic_free_energy/infile.ucposcar b/tests/anharmonic_free_energy/infile.ucposcar deleted file mode 120000 index b943f946..00000000 --- a/tests/anharmonic_free_energy/infile.ucposcar +++ /dev/null @@ -1 +0,0 @@ -../infiles/infile.ucposcar \ No newline at end of file diff --git a/tests/anharmonic_free_energy/reference/Argon_80K_classical_reference b/tests/anharmonic_free_energy/reference/Argon_80K_classical_reference new file mode 100644 index 00000000..bcf0ffb3 --- /dev/null +++ b/tests/anharmonic_free_energy/reference/Argon_80K_classical_reference @@ -0,0 +1,6 @@ +# Harmonic (F,U,S,Cv) +-0.0021623 0.0206808 3.3135466 3.0000 +# First-Cumulant Part (F,U,S,Cv) +0.0000557 -0.0000557 -0.0161597 -0.0161597 +# Second-Cumulant Part (F,U,S,Cv) +-0.0007879 0.0007879 0.2285819 0.2285819 diff --git a/tests/anharmonic_free_energy/reference/Neon_14K_quantum_reference b/tests/anharmonic_free_energy/reference/Neon_14K_quantum_reference new file mode 100644 index 00000000..e06a44a5 --- /dev/null +++ b/tests/anharmonic_free_energy/reference/Neon_14K_quantum_reference @@ -0,0 +1,6 @@ +# Harmonic (F,U,S,Cv) +0.0072576 0.0077620 0.4181343 0.9870306 +# First-Cumulant Part (F,U,S,Cv) +-0.0002033 0.0000628 -0.0105287 -0.0262279 +# Second-Cumulant Part (F,U,S,Cv) +0.0000755 -0.0000349 0.1395437 0.2610684 diff --git a/tests/anharmonic_free_energy/reference/Silicon_1600K_classical_reference b/tests/anharmonic_free_energy/reference/Silicon_1600K_classical_reference new file mode 100644 index 00000000..53aad0d9 --- /dev/null +++ b/tests/anharmonic_free_energy/reference/Silicon_1600K_classical_reference @@ -0,0 +1,6 @@ +# Harmonic (F,U,S,Cv) +-0.5152258 0.4136242 6.7367855 3.0000 +# First-Cumulant Part (F,U,S,Cv) +-0.0005732 0.0005732 0.0083149 0.0083149 +# Second-Cumulant Part (F,U,S,Cv) +-0.0025352 0.0025352 0.0367748 0.0367748 diff --git a/tests/anharmonic_free_energy/reference/outfile.anharmonic_free_energy b/tests/anharmonic_free_energy/reference/outfile.anharmonic_free_energy deleted file mode 100644 index df17a2d4..00000000 --- a/tests/anharmonic_free_energy/reference/outfile.anharmonic_free_energy +++ /dev/null @@ -1,5 +0,0 @@ - # Free energy at -314.16 K, unit : eV/atom - # Lowest order (1st order cumulant, 2nd order cumulant) - -3744.84683 -3744.84683 - # Third order anharmonic corrections (1st order cumulant, 2nd order cumulant) - -3744.84770 -3744.84770 diff --git a/tests/anharmonic_free_energy/test_anharmonic_free_energy.py b/tests/anharmonic_free_energy/test_anharmonic_free_energy.py index a749cb70..e4c204e7 100644 --- a/tests/anharmonic_free_energy/test_anharmonic_free_energy.py +++ b/tests/anharmonic_free_energy/test_anharmonic_free_energy.py @@ -1,21 +1,41 @@ import numpy as np +import pytest from pathlib import Path parent = Path(__file__).parent folder = parent / "reference" +cases = [ + "Argon_80K_classical", + "Silicon_1600K_classical", + "Neon_14K_quantum", +] +output_file = "outfile.anharmoinc_thermodynamics" def _read_file(file): - data = np.loadtxt(file) - return data + values = [] + with open(file, encoding="utf-8") as f: + for line in f: + stripped = line.strip() + if not stripped or stripped.startswith("#"): + continue + row = np.fromstring(stripped, sep=" ") + if row.size: + values.extend(row.tolist()) + return np.asarray(values, dtype=float) -def test_output(file="outfile.anharmonic_free_energy"): - data_ref = _read_file(folder / file) - data_new = _read_file(parent / file) +@pytest.mark.parametrize("case", cases) +def test_output(case): + file_ref = folder / f"{case}_reference" + file_new = parent / case / output_file + data_ref = _read_file(file_ref) + data_new = _read_file(file_new) - np.testing.assert_allclose(data_ref, data_new, err_msg=(parent / file).absolute()) + assert data_ref.shape == data_new.shape, file_new.absolute() + np.testing.assert_allclose(data_ref, data_new, err_msg=file_new.absolute()) if __name__ == "__main__": - test_output() + for case in cases: + test_output(case) From 7eebac6f7f3e202bee5ede408be8f87c04688ccc Mon Sep 17 00:00:00 2001 From: ejmeitz Date: Tue, 24 Mar 2026 14:30:15 -0400 Subject: [PATCH 21/28] fix makefile, remove argon test --- tests/anharmonic_free_energy/Makefile | 5 ++--- 1 file changed, 2 insertions(+), 3 deletions(-) diff --git a/tests/anharmonic_free_energy/Makefile b/tests/anharmonic_free_energy/Makefile index 0e14a355..25628cf9 100644 --- a/tests/anharmonic_free_energy/Makefile +++ b/tests/anharmonic_free_energy/Makefile @@ -1,4 +1,3 @@ testfiles: - cd ./Argon_80K_classical | anharmonic_free_energy --temperature 80 -qg3ph 10 10 10 -qg4ph 10 10 10 -qgh 30 30 30 - cd ../Silicon_1600K_classical | anharmonic_free_energy --temperature 1600 -qg3ph 10 10 10 -qg4ph 10 10 10 -qgh 30 30 30 - cd ../Neon_14K_quantum | anharmonic_free_energy --temperature 14 --quantum -qg3ph 10 10 10 -qg4ph 10 10 10 -qgh 30 30 30 \ No newline at end of file + cd ./Silicon_1600K_classical && anharmonic_free_energy --temperature 1600 -qg3ph 10 10 10 -qg4ph 10 10 10 -qgh 30 30 30 + cd ./Neon_14K_quantum && anharmonic_free_energy --temperature 14 --quantum -qg3ph 10 10 10 -qg4ph 10 10 10 -qgh 30 30 30 From 99681e6486905ccccc2a5a35b37c6d23b68f7b77 Mon Sep 17 00:00:00 2001 From: ejmeitz Date: Tue, 24 Mar 2026 14:39:34 -0400 Subject: [PATCH 22/28] typo.... --- tests/anharmonic_free_energy/test_anharmonic_free_energy.py | 3 +-- 1 file changed, 1 insertion(+), 2 deletions(-) diff --git a/tests/anharmonic_free_energy/test_anharmonic_free_energy.py b/tests/anharmonic_free_energy/test_anharmonic_free_energy.py index e4c204e7..54316c5a 100644 --- a/tests/anharmonic_free_energy/test_anharmonic_free_energy.py +++ b/tests/anharmonic_free_energy/test_anharmonic_free_energy.py @@ -5,11 +5,10 @@ parent = Path(__file__).parent folder = parent / "reference" cases = [ - "Argon_80K_classical", "Silicon_1600K_classical", "Neon_14K_quantum", ] -output_file = "outfile.anharmoinc_thermodynamics" +output_file = "outfile.anharmonic_thermodynamics" def _read_file(file): From 250e0bf448ab46ee7faa08438e6ed9fbead15d0e Mon Sep 17 00:00:00 2001 From: ejmeitz Date: Tue, 24 Mar 2026 14:48:35 -0400 Subject: [PATCH 23/28] round parsed values to 7 sig-figs --- .../anharmonic_free_energy/test_anharmonic_free_energy.py | 7 ++++++- 1 file changed, 6 insertions(+), 1 deletion(-) diff --git a/tests/anharmonic_free_energy/test_anharmonic_free_energy.py b/tests/anharmonic_free_energy/test_anharmonic_free_energy.py index 54316c5a..ca42c1b4 100644 --- a/tests/anharmonic_free_energy/test_anharmonic_free_energy.py +++ b/tests/anharmonic_free_energy/test_anharmonic_free_energy.py @@ -9,6 +9,7 @@ "Neon_14K_quantum", ] output_file = "outfile.anharmonic_thermodynamics" +decimals = 7 # my ground-truth data just has this many decimals def _read_file(file): @@ -32,7 +33,11 @@ def test_output(case): data_new = _read_file(file_new) assert data_ref.shape == data_new.shape, file_new.absolute() - np.testing.assert_allclose(data_ref, data_new, err_msg=file_new.absolute()) + np.testing.assert_array_equal( + np.round(data_ref, decimals=decimals), + np.round(data_new, decimals=decimals), + err_msg=file_new.absolute(), + ) if __name__ == "__main__": From 58030d92928af5f1975fe6b81ae031db410b6041 Mon Sep 17 00:00:00 2001 From: ejmeitz Date: Tue, 24 Mar 2026 15:50:15 -0400 Subject: [PATCH 24/28] typo in reference --- .../reference/Neon_14K_quantum_reference | 4 ++-- 1 file changed, 2 insertions(+), 2 deletions(-) diff --git a/tests/anharmonic_free_energy/reference/Neon_14K_quantum_reference b/tests/anharmonic_free_energy/reference/Neon_14K_quantum_reference index e06a44a5..8a0be869 100644 --- a/tests/anharmonic_free_energy/reference/Neon_14K_quantum_reference +++ b/tests/anharmonic_free_energy/reference/Neon_14K_quantum_reference @@ -1,6 +1,6 @@ # Harmonic (F,U,S,Cv) 0.0072576 0.0077620 0.4181343 0.9870306 # First-Cumulant Part (F,U,S,Cv) --0.0002033 0.0000628 -0.0105287 -0.0262279 +0.0000755 0.0000628 -0.0105287 -0.0262279 # Second-Cumulant Part (F,U,S,Cv) -0.0000755 -0.0000349 0.1395437 0.2610684 +-0.0002033 -0.0000349 0.1395437 0.2610684 From 845b1f3def479ded3b10cf6f49ce68b5246b778b Mon Sep 17 00:00:00 2001 From: ejmeitz Date: Thu, 26 Mar 2026 17:54:43 -0400 Subject: [PATCH 25/28] update reference data --- src/anharmonic_free_energy/thirdorder.f90 | 12 ++++++------ .../reference/Argon_80K_classical_reference | 16 ++++++++++------ .../reference/Neon_14K_quantum_reference | 16 ++++++++++------ .../reference/Silicon_1600K_classical_reference | 16 ++++++++++------ 4 files changed, 36 insertions(+), 24 deletions(-) diff --git a/src/anharmonic_free_energy/thirdorder.f90 b/src/anharmonic_free_energy/thirdorder.f90 index 7fee5fe1..9a9e8bfa 100644 --- a/src/anharmonic_free_energy/thirdorder.f90 +++ b/src/anharmonic_free_energy/thirdorder.f90 @@ -282,20 +282,20 @@ subroutine free_energy_thirdorder(uc, fct, qp, dr, temperature, fe3, s3, cv3, qu f1 = (n1 + 1.0_r8)*(n2 + n3 + 1.0_r8) + n2*n3 f2 = n3*(n1 + n2 + 1.0_r8) - n1*n2 ! Here is for the entropy - df1 = dn1 * (n2 + n3 + 1.0_r8) + (n1 + 1.0_r8) * (dn2 + dn3) + dn2 * n3 + n2 * dn3 - df2 = dn3 * (n1 + n2 + 1.0_r8) + dn1 * (n3 - n2) + dn2 * (n3 - n1) + df1 = dn1 * (n2 + n3 + 1.0_r8) + (n1 + 1.0_r8) * (dn2 + dn3) + (dn2 * n3) + (n2 * dn3) + df2 = dn3 * (n1 + n2 + 1.0_r8) + (dn1 * (n3 - n2)) + (dn2 * (n3 - n1)) ! And the heat capacity ddf1 = ddn1 * (n2 + n3 + 1.0_r8) + 2.0_r8 * dn1 * (dn2 + dn3) + (n1 + 1.0_r8) * (ddn2 + ddn3) + & ddn2 * n3 + n2 * ddn3 + 2.0_r8 * dn2 * dn3 - ddf2 = ddn3 * (n1 + n2 + 1.0_r8) + dn3 * (dn1 + dn2) + & - ddn1 * (n3 - n2) + dn1 * (dn3 - dn2) + & - ddn2 * (n3 - n1) + dn2 * (dn3 - dn1) + ddf2 = (ddn3 * (n1 + n2 + 1.0_r8)) + (dn3 * (dn1 + dn2)) + & + (ddn1 * (n3 - n2)) + (dn1 * (dn3 - dn2)) + & + (ddn2 * (n3 - n1)) + (dn2 * (dn3 - dn1)) ! Compute the principal values f1 = f1*real(1.0_r8/(om1 + om2 + om3 + lo_imag*sigma), r8) df1 = df1*real(1.0_r8/(om1 + om2 + om3 + lo_imag*sigma), r8) ddf1 = ddf1*real(1.0_r8/(om1 + om2 + om3 + lo_imag*sigma), r8) - f2 = 3*f2*real(1.0/(om1 + om2 - om3 + lo_imag*sigma), r8) + f2 = 3.0_r8*f2*real(1.0/(om1 + om2 - om3 + lo_imag*sigma), r8) df2 = 3.0_r8 * df2 * real(1.0/(om1 + om2 - om3 + lo_imag*sigma), r8) ddf2 = 3.0_r8 * ddf2 * real(1.0/(om1 + om2 - om3 + lo_imag*sigma), r8) diff --git a/tests/anharmonic_free_energy/reference/Argon_80K_classical_reference b/tests/anharmonic_free_energy/reference/Argon_80K_classical_reference index bcf0ffb3..89594adc 100644 --- a/tests/anharmonic_free_energy/reference/Argon_80K_classical_reference +++ b/tests/anharmonic_free_energy/reference/Argon_80K_classical_reference @@ -1,6 +1,10 @@ -# Harmonic (F,U,S,Cv) --0.0021623 0.0206808 3.3135466 3.0000 -# First-Cumulant Part (F,U,S,Cv) -0.0000557 -0.0000557 -0.0161597 -0.0161597 -# Second-Cumulant Part (F,U,S,Cv) --0.0007879 0.0007879 0.2285819 0.2285819 +# Temperature: 0.800000000000E+02 + # Harmonic contribution + # Free energy [eV/at] Internal energy [eV/at] Entropy [kB] Heat capacity [kB] + -0.002161720125 0.020681592720 3.313571612390 3.000000000000 + # First Cumulant Contribution + # Free energy [eV/at] Internal energy [eV/at] Entropy [kB] Heat capacity [kB] + 0.000055701287 -0.000055701287 -0.016159670355 -0.016159670355 + # Second Cumulant Contribution + # Free energy [eV/at] Internal energy [eV/at] Entropy [kB] Heat capacity [kB] + -0.000786700801 0.000786700801 0.228232171055 0.228232171055 diff --git a/tests/anharmonic_free_energy/reference/Neon_14K_quantum_reference b/tests/anharmonic_free_energy/reference/Neon_14K_quantum_reference index 8a0be869..d813d622 100644 --- a/tests/anharmonic_free_energy/reference/Neon_14K_quantum_reference +++ b/tests/anharmonic_free_energy/reference/Neon_14K_quantum_reference @@ -1,6 +1,10 @@ -# Harmonic (F,U,S,Cv) -0.0072576 0.0077620 0.4181343 0.9870306 -# First-Cumulant Part (F,U,S,Cv) -0.0000755 0.0000628 -0.0105287 -0.0262279 -# Second-Cumulant Part (F,U,S,Cv) --0.0002033 -0.0000349 0.1395437 0.2610684 +# Temperature: 0.140000000000E+02 + # Harmonic contribution + # Free energy [eV/at] Internal energy [eV/at] Entropy [kB] Heat capacity [kB] + 0.007257533994 0.007761992603 0.418142934371 0.987045346630 + # First Cumulant Contribution + # Free energy [eV/at] Internal energy [eV/at] Entropy [kB] Heat capacity [kB] + 0.000075474136 0.000062771925 -0.010528792426 -0.026228049607 + # Second Cumulant Contribution + # Free energy [eV/at] Internal energy [eV/at] Entropy [kB] Heat capacity [kB] + -0.000204142906 -0.000033607872 0.141355540918 0.264402508187 diff --git a/tests/anharmonic_free_energy/reference/Silicon_1600K_classical_reference b/tests/anharmonic_free_energy/reference/Silicon_1600K_classical_reference index 53aad0d9..bdf251de 100644 --- a/tests/anharmonic_free_energy/reference/Silicon_1600K_classical_reference +++ b/tests/anharmonic_free_energy/reference/Silicon_1600K_classical_reference @@ -1,6 +1,10 @@ -# Harmonic (F,U,S,Cv) --0.5152258 0.4136242 6.7367855 3.0000 -# First-Cumulant Part (F,U,S,Cv) --0.0005732 0.0005732 0.0083149 0.0083149 -# Second-Cumulant Part (F,U,S,Cv) --0.0025352 0.0025352 0.0367748 0.0367748 +# Temperature: 0.160000000000E+04 + # Harmonic contribution + # Free energy [eV/at] Internal energy [eV/at] Entropy [kB] Heat capacity [kB] + -0.515229485446 0.413631854400 6.736869972408 3.000000000000 + # First Cumulant Contribution + # Free energy [eV/at] Internal energy [eV/at] Entropy [kB] Heat capacity [kB] + -0.000573215900 0.000573215900 0.008314870736 0.008314870736 + # Second Cumulant Contribution + # Free energy [eV/at] Internal energy [eV/at] Entropy [kB] Heat capacity [kB] + -0.002541038722 0.002541038722 0.036859425048 0.036859425048 From 9636b30d16b1e3b7f9d7617c797e7ebbef4cce7b Mon Sep 17 00:00:00 2001 From: ejmeitz Date: Mon, 30 Mar 2026 14:56:18 -0400 Subject: [PATCH 26/28] try rtol, atol --- .../test_anharmonic_free_energy.py | 14 +++++++++----- 1 file changed, 9 insertions(+), 5 deletions(-) diff --git a/tests/anharmonic_free_energy/test_anharmonic_free_energy.py b/tests/anharmonic_free_energy/test_anharmonic_free_energy.py index ca42c1b4..94479b83 100644 --- a/tests/anharmonic_free_energy/test_anharmonic_free_energy.py +++ b/tests/anharmonic_free_energy/test_anharmonic_free_energy.py @@ -9,7 +9,9 @@ "Neon_14K_quantum", ] output_file = "outfile.anharmonic_thermodynamics" -decimals = 7 # my ground-truth data just has this many decimals +# Seems to be some noise due to ordering of sums. +rtol = 1e-6 +atol = 1e-8 def _read_file(file): @@ -33,10 +35,12 @@ def test_output(case): data_new = _read_file(file_new) assert data_ref.shape == data_new.shape, file_new.absolute() - np.testing.assert_array_equal( - np.round(data_ref, decimals=decimals), - np.round(data_new, decimals=decimals), - err_msg=file_new.absolute(), + np.testing.assert_allclose( + data_ref, + data_new, + rtol=rtol, + atol=atol, + err_msg=str(file_new.absolute()), ) From 7617cdaefae976ec00b8b13205353fd3902b17c8 Mon Sep 17 00:00:00 2001 From: ejmeitz Date: Mon, 30 Mar 2026 15:03:10 -0400 Subject: [PATCH 27/28] calculate ref data withou MPI --- .../reference/Argon_80K_classical_reference | 2 +- .../anharmonic_free_energy/reference/Neon_14K_quantum_reference | 2 +- .../reference/Silicon_1600K_classical_reference | 2 +- 3 files changed, 3 insertions(+), 3 deletions(-) diff --git a/tests/anharmonic_free_energy/reference/Argon_80K_classical_reference b/tests/anharmonic_free_energy/reference/Argon_80K_classical_reference index 89594adc..54d125c0 100644 --- a/tests/anharmonic_free_energy/reference/Argon_80K_classical_reference +++ b/tests/anharmonic_free_energy/reference/Argon_80K_classical_reference @@ -7,4 +7,4 @@ 0.000055701287 -0.000055701287 -0.016159670355 -0.016159670355 # Second Cumulant Contribution # Free energy [eV/at] Internal energy [eV/at] Entropy [kB] Heat capacity [kB] - -0.000786700801 0.000786700801 0.228232171055 0.228232171055 + -0.000787906127 0.000787906127 0.228581851748 0.228581851748 diff --git a/tests/anharmonic_free_energy/reference/Neon_14K_quantum_reference b/tests/anharmonic_free_energy/reference/Neon_14K_quantum_reference index d813d622..0077caec 100644 --- a/tests/anharmonic_free_energy/reference/Neon_14K_quantum_reference +++ b/tests/anharmonic_free_energy/reference/Neon_14K_quantum_reference @@ -7,4 +7,4 @@ 0.000075474136 0.000062771925 -0.010528792426 -0.026228049607 # Second Cumulant Contribution # Free energy [eV/at] Internal energy [eV/at] Entropy [kB] Heat capacity [kB] - -0.000204142906 -0.000033607872 0.141355540918 0.264402508187 + -0.000203876181 -0.000033689528 0.141066770144 0.264442999555 diff --git a/tests/anharmonic_free_energy/reference/Silicon_1600K_classical_reference b/tests/anharmonic_free_energy/reference/Silicon_1600K_classical_reference index bdf251de..a9dd3cfd 100644 --- a/tests/anharmonic_free_energy/reference/Silicon_1600K_classical_reference +++ b/tests/anharmonic_free_energy/reference/Silicon_1600K_classical_reference @@ -7,4 +7,4 @@ -0.000573215900 0.000573215900 0.008314870736 0.008314870736 # Second Cumulant Contribution # Free energy [eV/at] Internal energy [eV/at] Entropy [kB] Heat capacity [kB] - -0.002541038722 0.002541038722 0.036859425048 0.036859425048 + -0.002535207816 0.002535207816 0.036774843951 0.036774843951 From cd5674f783d9f4fa8512ae3b938775572cd50dae Mon Sep 17 00:00:00 2001 From: ejmeitz Date: Fri, 3 Apr 2026 10:51:11 -0400 Subject: [PATCH 28/28] update manual eqns, make tests use smaller q-grid --- src/anharmonic_free_energy/manual.md | 31 ++++--------------- tests/anharmonic_free_energy/Makefile | 4 +-- .../reference/Argon_80K_classical_reference | 4 +-- .../reference/Neon_14K_quantum_reference | 4 +-- .../Silicon_1600K_classical_reference | 4 +-- 5 files changed, 14 insertions(+), 33 deletions(-) diff --git a/src/anharmonic_free_energy/manual.md b/src/anharmonic_free_energy/manual.md index 0b269dda..534d7d9e 100644 --- a/src/anharmonic_free_energy/manual.md +++ b/src/anharmonic_free_energy/manual.md @@ -1,5 +1,5 @@ -This code calculates the anharmonic Helmholtz free energy, internal energy, entropy and heat capacity. It includes the contributions from baseline shifts, renormalized phonons and higher order terms. This program must use force constants from sTDEP/SSCHA (self-consistent phonons). Force cosntants fit to MD/PIMD data are incompatible with this theory. +This code calculates the anharmonic part of the Helmholtz free energy, internal energy, entropy and heat capacity. It includes the contributions from baseline shifts, renormalized phonons and higher order terms. This program must use force constants from sTDEP/SSCHA (self-consistent phonons). Force cosntants fit to MD/PIMD data are incompatible with this theory. Only the first and second-cumulant corrections are computed by this code. The constant corrections (i.e., $U_0$ and its derivatives) must be implemented elsewhere as it requires interfacing with a force-calculator like LAMMPS. Please refer to CITATION and a reference implementation [here](https://github.com/ejmeitz/CumulantAnalysis.jl). @@ -40,7 +40,7 @@ $$ \end{equation} $$ -where $F_{\textrm{ph}}$ is the usual phonon free energy and $U_0$ the renormalized baseline free energy given by +where $F_{\textrm{ph}}$ is the phonon free energy and $U_0$ the renormalized baseline free energy. However, since the derivations of $\Delta F^{3\mathrm{ph}}$ and $\Delta F^{4\mathrm{ph}}$ assume self-consistent phonons the average is with respect to harmonic dynamics (i.e., $\langle \cdot \rangle_\mathrm{H}$). The expression is given by $$ \begin{equation} @@ -59,7 +59,7 @@ u_i^\alpha u_j^\beta u_k^\gamma - }} \Phi_{ijkl}^{\alpha\beta\gamma\delta} u_i^\alpha u_j^\beta u_k^\gamma u_l^\delta - \right\rangle + \right\rangle_\mathrm{H} \end{equation} $$ @@ -67,26 +67,8 @@ Here it is important to note that we have to subtract the long-ranged polar inte $$ \begin{equation}%\label{eq:deltaF3} - \Delta F^{3\textrm{ph}} = - -6 - \sum_{\lambda\lambda'\lambda''} - \left| - \Phi_{\lambda\lambda'\lambda''} - \right|^2 - % - \left( - %\Bigg{\{} - \frac{3n_{\lambda} n_{\lambda'} + 3n_{\lambda} + 1} - {(\omega_{\lambda}+\omega_{\lambda'}+\omega_{\lambda''})_p} - + - \frac{ 6n_{\lambda} n_{\lambda''} - 3 n_{\lambda} n_{\lambda'} + 3n_{\lambda''}} - {(\omega_{\lambda}+\omega_{\lambda'}-\omega_{\lambda''})_p} - \right) - %\Bigg{\}} - % - +9\Phi_{\lambda\bar{\lambda}\lambda''}\Phi_{\lambda'\bar{\lambda}'\bar{\lambda}''} - \frac{4 n_{\lambda}( n_{\lambda'}+1)+1} - {(\omega_{\lambda''})_p}\,, + \Delta F^{3\textrm{ph}} = -\frac{\hbar^2}{48N}\sum_{\substack{\bm k\bm k^\prime \bm k^{\prime\prime} \\ \lambda\lambda^\prime\lambda^{\prime\prime}}}\frac{\left|\Phi_{\lambda \lambda^\prime \lambda^{\prime\prime}} ^ {\bm k \bm k^\prime \bm k^{\prime\prime}}\right|^2}{\omega\omega^\prime\omega^{\prime\prime}} \left[\frac{(n+1)(n^\prime + n^{\prime\prime} + 1) + n^\prime n^{\prime\prime}}{\omega + \omega^\prime + \omega^{\prime\prime}} + + 3\frac{n^{\prime\prime}(n+n^\prime+1)-nn^\prime}{\omega + \omega^\prime - \omega^{\prime\prime}}\right] \end{equation} $$ @@ -95,8 +77,7 @@ and $$ \begin{equation}%\label{eq:deltaF4} \Delta F^{4\textrm{ph}} = - 3\sum_{\lambda\lambda'} - \Phi_{\lambda\bar{\lambda}\lambda'\bar{\lambda}'}(2n_{\lambda}+1)(2n_{\lambda'}+1) + \frac{\hbar^2}{8N}\sum_{\bm k\ \bm k^\prime \lambda\lambda^\prime}\frac{\Phi_{\lambda\lambda\lambda^\prime\lambda^\prime}^{\bm k,-\bm k,\bm k^\prime,-\bm k^\prime}}{\omega\omega^{\prime}}\left(n+\frac{1}{2}\right)\left(n^\prime + \frac{1}{2}\right) \end{equation} $$ diff --git a/tests/anharmonic_free_energy/Makefile b/tests/anharmonic_free_energy/Makefile index 25628cf9..f85c538d 100644 --- a/tests/anharmonic_free_energy/Makefile +++ b/tests/anharmonic_free_energy/Makefile @@ -1,3 +1,3 @@ testfiles: - cd ./Silicon_1600K_classical && anharmonic_free_energy --temperature 1600 -qg3ph 10 10 10 -qg4ph 10 10 10 -qgh 30 30 30 - cd ./Neon_14K_quantum && anharmonic_free_energy --temperature 14 --quantum -qg3ph 10 10 10 -qg4ph 10 10 10 -qgh 30 30 30 + cd ./Silicon_1600K_classical && anharmonic_free_energy --temperature 1600 -qg3ph 5 5 5 -qg4ph 5 5 5 -qgh 30 30 30 + cd ./Neon_14K_quantum && anharmonic_free_energy --temperature 14 --quantum -qg3ph 5 5 5 -qg4ph 5 5 5 -qgh 30 30 30 diff --git a/tests/anharmonic_free_energy/reference/Argon_80K_classical_reference b/tests/anharmonic_free_energy/reference/Argon_80K_classical_reference index 54d125c0..9ed342af 100644 --- a/tests/anharmonic_free_energy/reference/Argon_80K_classical_reference +++ b/tests/anharmonic_free_energy/reference/Argon_80K_classical_reference @@ -4,7 +4,7 @@ -0.002161720125 0.020681592720 3.313571612390 3.000000000000 # First Cumulant Contribution # Free energy [eV/at] Internal energy [eV/at] Entropy [kB] Heat capacity [kB] - 0.000055701287 -0.000055701287 -0.016159670355 -0.016159670355 + 0.000052542238 -0.000052542238 -0.015243188956 -0.015243188956 # Second Cumulant Contribution # Free energy [eV/at] Internal energy [eV/at] Entropy [kB] Heat capacity [kB] - -0.000787906127 0.000787906127 0.228581851748 0.228581851748 + -0.000757328812 0.000757328812 0.219710973722 0.219710973722 diff --git a/tests/anharmonic_free_energy/reference/Neon_14K_quantum_reference b/tests/anharmonic_free_energy/reference/Neon_14K_quantum_reference index 0077caec..7b44cffe 100644 --- a/tests/anharmonic_free_energy/reference/Neon_14K_quantum_reference +++ b/tests/anharmonic_free_energy/reference/Neon_14K_quantum_reference @@ -4,7 +4,7 @@ 0.007257533994 0.007761992603 0.418142934371 0.987045346630 # First Cumulant Contribution # Free energy [eV/at] Internal energy [eV/at] Entropy [kB] Heat capacity [kB] - 0.000075474136 0.000062771925 -0.010528792426 -0.026228049607 + 0.000070677388 0.000063045856 -0.006325734499 -0.023459532844 # Second Cumulant Contribution # Free energy [eV/at] Internal energy [eV/at] Entropy [kB] Heat capacity [kB] - -0.000203876181 -0.000033689528 0.141066770144 0.264442999555 + -0.000195310263 -0.000040784905 0.128085209130 0.242479458040 diff --git a/tests/anharmonic_free_energy/reference/Silicon_1600K_classical_reference b/tests/anharmonic_free_energy/reference/Silicon_1600K_classical_reference index a9dd3cfd..b87c6fc2 100644 --- a/tests/anharmonic_free_energy/reference/Silicon_1600K_classical_reference +++ b/tests/anharmonic_free_energy/reference/Silicon_1600K_classical_reference @@ -4,7 +4,7 @@ -0.515229485446 0.413631854400 6.736869972408 3.000000000000 # First Cumulant Contribution # Free energy [eV/at] Internal energy [eV/at] Entropy [kB] Heat capacity [kB] - -0.000573215900 0.000573215900 0.008314870736 0.008314870736 + -0.000543896863 0.000543896863 0.007889578969 0.007889578969 # Second Cumulant Contribution # Free energy [eV/at] Internal energy [eV/at] Entropy [kB] Heat capacity [kB] - -0.002535207816 0.002535207816 0.036774843951 0.036774843951 + -0.002515013780 0.002515013780 0.036481916272 0.036481916272