Hybrid functional calculation results show large difference with VASP

Xiaoming Wang wxia... at gmail.com
Tue Sep 19 05:44:01 UTC 2017


Hi, Nico,

Thanks for your reply. 
I did tried the case without ADMM_PURIFICATION, but the band gap is only 
0.01 eV smaller. As for the basis set, I don't know whether it would affect 
the HFX electronic structure or not. But for GW calculations, the 
completeness of the basis set plays an important role. I will try the TZVP 
basis to see what happens.

Best,
Xiaoming

On Tuesday, September 19, 2017 at 1:26:43 AM UTC-4, Nico Holmberg wrote:
>
> Hi,
>
> You should try switching off ADMM purification i.e. setting 
> ADMM_PURIFICATION_METHOD NONE. According to the implementation paper, this 
> is the correct way to obtain MO energies. A direct quote from the 
> implementation paper: "In order to use the eigenvalues of the ADMM 
> Kohn-Sham matrix directly as orbital energies, e.g., to calculate the band 
> gaps of a system, an ADMM scheme without purification needs to be 
> employed." 
>
> You can find TZVP-MOLOPT quality basis sets for Ag, Cs, and In in the 
> BASIS_MOLOPT_UCL 
> <https://github.com/cp2k/cp2k/blob/master/cp2k/data/BASIS_MOLOPT_UCL> 
> file distributed with the trunk version of cp2k if you want to test the 
> effect of using larger primary basis sets.
>
>
> BR,
>
> Nico
>
> maanantai 18. syyskuuta 2017 18.31.50 UTC+3 Xiaoming Wang kirjoitti:
>>
>> Hi Marcella,
>>
>> Thanks for your reply. I have checked that parameter. Actually, 
>> eps_schwarz of 1.0e-10 give quite a small improvement of the band gap, 
>> ~0.01 eV. Any other suggestions?
>>
>> Best,
>> Xiaoming 
>>
>> On Monday, September 18, 2017 at 11:18:58 AM UTC-4, Marcella Iannuzzi 
>> wrote:
>>>
>>> Hi, 
>>>
>>> Your eps_schwarz at 1.0e-6 is far too large.
>>> The default is 1.0e-10. 
>>>
>>> Regards
>>> Marcella
>>>
>>> On Monday, September 18, 2017 at 5:07:21 PM UTC+2, Xiaoming Wang wrote:
>>>>
>>>> Hello,
>>>>
>>>> I conducted PBE0 and HSE calculations on a cube of ~10*10*10 
>>>> (perovskite). For comparison, I also did the calculations using VASP (gamma 
>>>> only). However, to my surprise, the band gap obtained by cp2k is about 0.5 
>>>> eV (HSE)  and 0.8 eV(PBE0) smaller than by vasp. The vasp results agree 
>>>> well with literature. For the cp2k calculations, I have checked the 
>>>> convergence of the cutoffs and auxiliary basis sets. Since for my 
>>>> structure, the only available basis sets is DZVP within BASIS_MOLOPT, thus 
>>>> I could not find a way to increase the primary basis size. But I checked 
>>>> the PBE results with DZVP compared with those of VASP. The difference of 
>>>> the band gap is very small, say only 0.02 eV. So I think the DZVP basis set 
>>>> is OK for my system. The inputs of my calculations are as follows. Could 
>>>> anyone give me some suggestions?
>>>>
>>>> HSE input:
>>>> --------------------------------------------------------------------
>>>> &GLOBAL
>>>>  PROJECT_NAME CsInAgCl
>>>>  RUN_TYPE ENERGY
>>>>  PRINT_LEVEL LOW
>>>> &END GLOBAL
>>>>
>>>> &FORCE_EVAL
>>>>  METHOD QS
>>>>   &DFT
>>>>     BASIS_SET_FILE_NAME BASIS_MOLOPT
>>>>     BASIS_SET_FILE_NAME BASIS_ADMM
>>>>     BASIS_SET_FILE_NAME BASIS_ADMM_MOLOPT
>>>>     POTENTIAL_FILE_NAME GTH_POTENTIALS
>>>>     WFN_RESTART_FILE_NAME -PBE.wfn
>>>>     &QS
>>>>      EPS_PGF_ORB 1.0e-6
>>>>     &END
>>>>     &MGRID
>>>>       CUTOFF 250
>>>>       REL_CUTOFF 60
>>>>     &END MGRID
>>>>     &XC
>>>>       &XC_FUNCTIONAL
>>>>        &PBE
>>>>         SCALE_X 0.0
>>>>         SCALE_C 1.0
>>>>        &END PBE
>>>>        &XWPBE
>>>>         SCALE_X -0.25
>>>>         SCALE_X0 1.0
>>>>         OMEGA 0.11
>>>>        &END XWPBE
>>>>       &END XC_FUNCTIONAL
>>>>       &HF
>>>>        FRACTION 0.25
>>>>        &SCREENING
>>>>         EPS_SCHWARZ 1.0e-6
>>>>        &END SCREENING
>>>>        &INTERACTION_POTENTIAL
>>>>         POTENTIAL_TYPE SHORTRANGE
>>>>         OMEGA 0.11
>>>>        &END INTERACTION_POTENTIAL
>>>>        &MEMORY
>>>>         MAX_MEMORY 2400
>>>>         EPS_STORAGE_SCALING 0.1
>>>>        &END MEMORY
>>>>       &END HF
>>>>     &END XC
>>>>     &SCF
>>>>      #ADDED_MOS 2
>>>>       MAX_SCF 100
>>>>       EPS_SCF 1.0e-6
>>>>       CHOLESKY INVERSE
>>>>       SCF_GUESS RESTART
>>>>       &OT
>>>>        PRECONDITIONER FULL_ALL
>>>>        ENERGY_GAP 0.01
>>>>       &END OT
>>>>     &END SCF
>>>>     &AUXILIARY_DENSITY_MATRIX_METHOD
>>>>      METHOD BASIS_PROJECTION
>>>>      ADMM_PURIFICATION_METHOD MO_DIAG
>>>>     &END AUXILIARY_DENSITY_MATRIX_METHOD
>>>>     &PRINT
>>>>      &MO_CUBES
>>>>       WRITE_CUBE F
>>>>       NHOMO 1
>>>>       NLUMO 1
>>>>      &END MO_CUBES
>>>>     &END PRINT
>>>>   &END DFT
>>>>   &SUBSYS
>>>>     &CELL
>>>>       ABC [angstrom] 10.5345 10.5345 10.5345
>>>>       ALPHA_BETA_GAMMA [deg] 90 90 90
>>>>       PERIODIC XYZ
>>>>       SYMMETRY CUBIC
>>>>     &END CELL
>>>>     &COORD
>>>>      ....[I omitted the coors here ]
>>>>       SCALED T
>>>>     &END COORD
>>>>     &KIND Cs
>>>>       ELEMENT Cs
>>>>       BASIS_SET DZVP-MOLOPT-SR-GTH
>>>>       AUX_FIT_BASIS_SET FIT11
>>>>       POTENTIAL GTH-PBE-q9
>>>>     &END KIND
>>>>     &KIND In
>>>>       ELEMENT In
>>>>       BASIS_SET DZVP-MOLOPT-SR-GTH
>>>>       AUX_FIT_BASIS_SET FIT11
>>>>       POTENTIAL GTH-PBE-q13
>>>>     &END KIND
>>>>     &KIND Ag
>>>>       ELEMENT Ag
>>>>       BASIS_SET DZVP-MOLOPT-SR-GTH
>>>>       AUX_FIT_BASIS_SET FIT11
>>>>       POTENTIAL GTH-PBE-q11
>>>>     &END KIND
>>>>     &KIND Cl
>>>>       ELEMENT Cl
>>>>       BASIS_SET DZVP-MOLOPT-SR-GTH
>>>>       AUX_FIT_BASIS_SET FIT3
>>>>       POTENTIAL GTH-PBE-q7
>>>>     &END KIND
>>>>   &END SUBSYS
>>>> &END FORCE_EVAL
>>>>
>>>> -----------------------------------------------------------------------------------------------
>>>>
>>>> PBE0 input
>>>>
>>>>
>>>> --------------------------------------------------------
>>>> &GLOBAL
>>>>  PROJECT_NAME CsInAgCl
>>>>  RUN_TYPE ENERGY
>>>>  PRINT_LEVEL LOW
>>>> &END GLOBAL
>>>> &FORCE_EVAL
>>>>  METHOD QS
>>>>   &DFT
>>>>     BASIS_SET_FILE_NAME BASIS_MOLOPT
>>>>     BASIS_SET_FILE_NAME BASIS_ADMM
>>>>     BASIS_SET_FILE_NAME BASIS_ADMM_MOLOPT
>>>>     POTENTIAL_FILE_NAME GTH_POTENTIALS
>>>>     WFN_RESTART_FILE_NAMEPBE.wfn
>>>>     &QS
>>>>      EPS_PGF_ORB 1.0e-6
>>>>     &END
>>>>     &MGRID
>>>>       CUTOFF 250
>>>>       REL_CUTOFF 60
>>>>     &END MGRID
>>>>     &XC
>>>>       &XC_FUNCTIONAL
>>>>        &PBE
>>>>         SCALE_X 0.75
>>>>         SCALE_C 1.0
>>>>        &END PBE
>>>>        &PBE_HOLE_T_C_LR
>>>>         CUTOFF_RADIUS 5.25
>>>>         SCALE_X 0.25
>>>>        &END PBE_HOLE_T_C_LR
>>>>       &END XC_FUNCTIONAL
>>>>       &HF
>>>>        FRACTION 0.25
>>>>        &SCREENING
>>>>         EPS_SCHWARZ 1.0e-6
>>>>        &END SCREENING
>>>>        &INTERACTION_POTENTIAL
>>>>         POTENTIAL_TYPE TRUNCATED
>>>>         CUTOFF_RADIUS 5.25
>>>>         T_C_G_DATA ./t_c_g.dat
>>>>        &END INTERACTION_POTENTIAL
>>>>        &MEMORY
>>>>         MAX_MEMORY 2400
>>>>         EPS_STORAGE_SCALING 0.1
>>>>        &END MEMORY
>>>>       &END HF
>>>>     &END XC
>>>>     &SCF
>>>>       MAX_SCF 100
>>>>       EPS_SCF 1.0e-6
>>>>       CHOLESKY INVERSE
>>>>       SCF_GUESS RESTART
>>>>       &OT
>>>>        PRECONDITIONER FULL_ALL
>>>>        ENERGY_GAP 0.01
>>>>       &END OT
>>>>     &END SCF
>>>>     &AUXILIARY_DENSITY_MATRIX_METHOD
>>>>      METHOD BASIS_PROJECTION
>>>>      ADMM_PURIFICATION_METHOD MO_DIAG
>>>>     &END AUXILIARY_DENSITY_MATRIX_METHOD
>>>>     &PRINT
>>>>      &MO_CUBES
>>>>       WRITE_CUBE F
>>>>       NHOMO 1
>>>>       NLUMO 1
>>>>      &END MO_CUBES
>>>>     &END PRINT
>>>>   &END DFT
>>>>   &SUBSYS
>>>>     &CELL
>>>>       ABC [angstrom] 10.5345 10.5345 10.5345
>>>>       ALPHA_BETA_GAMMA [deg] 90 90 90
>>>>       PERIODIC XYZ
>>>>       SYMMETRY CUBIC
>>>>     &END CELL
>>>>     &COORD
>>>>        .......
>>>>       SCALED T
>>>>     &END COORD
>>>>     &KIND Cs
>>>>       ELEMENT Cs
>>>>       BASIS_SET DZVP-MOLOPT-SR-GTH
>>>>       AUX_FIT_BASIS_SET FIT11
>>>>       POTENTIAL GTH-PBE-q9
>>>>     &END KIND
>>>>     &KIND In
>>>>       ELEMENT In
>>>>       BASIS_SET DZVP-MOLOPT-SR-GTH
>>>>       AUX_FIT_BASIS_SET FIT11
>>>>       POTENTIAL GTH-PBE-q13
>>>>     &END KIND
>>>>     &KIND Ag
>>>>       ELEMENT Ag
>>>>       BASIS_SET DZVP-MOLOPT-SR-GTH
>>>>       AUX_FIT_BASIS_SET FIT11
>>>>       POTENTIAL GTH-PBE-q11
>>>>     &END KIND
>>>>     &KIND Cl
>>>>       ELEMENT Cl
>>>>       BASIS_SET DZVP-MOLOPT-SR-GTH
>>>>       AUX_FIT_BASIS_SET FIT3
>>>>       POTENTIAL GTH-PBE-q7
>>>>     &END KIND
>>>>   &END SUBSYS
>>>> &END FORCE_EVAL
>>>>
>>>> --------------------------------------
>>>>
>>>>
>>>>
>>>>
>>>> Best,
>>>>
>>>> Xiaoming Wang
>>>>
>>>>
>>>>   
>>>>
>>>
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