[CP2K:2654] Looking for zero frequencies

Teodoro Laino teodor... at gmail.com
Fri Apr 9 15:37:18 UTC 2010


Dear An,
did you try to use a smaller DX (in the VIB section): the hessian is 
computed numerically and 0.01 may definitely be too large.
Teo

An Ghysels wrote:
> Dear forum users,
>
> I am calculating frequencies in periodic structures, from which I'd
> like to derive thermodynamic quantities like the entropy etc.
> Therefore I use the VIBRATIONAL_ANALYSIS keyword, where I have put the
> FULLY_PERIODIC keyword to True, such that rotational motions are not
> projected out.
>
> In principle, the second derivatives matrix should have 3 zero
> eigenvalues (even in non-optimized systems), because the system is
> translational invariant. However, this is not the case in my
> calculations. Even in a small test case like diamond with a cubic cell
> containing 8 atoms, the "zero" frequencies deviate largely from zero.
>
> (Between brackets: I'm much bothered by this bad performance, because
> it signals that the numerical accuracy of the frequencies is poor. I
> aim at studying larger unit cells (eg with 100 to 200 QM atoms) where
> I surely will encounter floppy modes, which are even more sensible to
> numerical errors. And those floppy modes play an essential role in the
> partition function/thermodynamics. Therefore, I wish to improve the
> accuracy of the calculated frequencies.)
>
> So my questions are mainly: why is the accuracy so bad? Is this
> directly related to the eggbox effect, and if so, how to remedy it? Is
> it something with interpolation grids? And what to do to improve it?
>
> I tried decreasing the EPS_DEFAULT (down to 10e-16), increasing the
> E_CUTOFF (up to 1400 Rydberg), increasing the REL_CUTOFF accordingly,
> adding the keyword COMMENSURATE, changing the interpolation grid (to
> spline3), but the improvements still do not get me close to "zero"
> frequencies (still of the order -70 to 50 cm-1).
>
> Looking forward to your comments and remarks,
>
> An
>
> Below: Information on version, input geometry optimization, input
> frequency run, snippets of output
> =====
> Version:
>  CP2K| version string:                  CP2K version 2.0.1
> (Development Version)
>  CP2K| is freely available from                          http://cp2k.berlios.de/
>  CP2K| Program compiled at
> Wed_Sep__9_15:48:59_CEST_2009
>  CP2K| Program compiled
> on                                               gengar1
>  CP2K| Program compiled for                                   Linux-
> x86-64-intel
> =====
> Input geomery optimization
> &GLOBAL
>   PRINT_LEVEL high
>   PROJECT_NAME vib
>   RUN_TYPE GEO_OPT
>   PREFERRED_FFT_LIBRARY FFTW
> &END GLOBAL
>
> &MOTION
>   &GEO_OPT
>     OPTIMIZER BFGS
>     MAX_ITER 300
>   &END GEO_OPT
> &END MOTION
>
> &VIBRATIONAL_ANALYSIS
>     FULLY_PERIODIC T
> &END VIBRATIONAL_ANALYSIS
>
> &FORCE_EVAL
>
>   METHOD QS
>   &DFT
>     BASIS_SET_FILE_NAME GTH_BASIS_SETS
>     POTENTIAL_FILE_NAME GTH_POTENTIALS
>     &MGRID
>       CUTOFF 100
>       REL_CUTOFF 23
>       COMMENSURATE
>     &END MGRID
>     &QS
>      EPS_DEFAULT 1.0E-10
>     &END QS
>     &SCF
>       EPS_SCF 1.0E-5
>       MAX_SCF 100
>       SCF_GUESS RESTART
>       &OUTER_SCF
>         EPS_SCF 1.0E-5
>         MAX_SCF 20
>       &END
>       &OT
>         ALGORITHM IRAC
>         MINIMIZER CG
>         PRECONDITIONER FULL_ALL
>         ENERGY_GAP 0.001
>       &END OT
>       &PRINT
>         &RESTART
>          BACKUP_COPIES 0
>         &END RESTART
>       &END PRINT
>     &END SCF
>     &XC
>       &XC_FUNCTIONAL PBE
>       &END XC_FUNCTIONAL
>     &END XC
>     &POISSON
>      POISSON_SOLVER PERIODIC
>      PERIODIC XYZ
>      &EWALD
>        EWALD_TYPE EWALD
>        ALPHA 0.3
>        GMAX 11
>        O_SPLINE 6
>      &END EWALD
>    &END POISSON
>   &PRINT
>   &END PRINT
>   &END DFT
>
>   &SUBSYS
>     &CELL
>       ABC 3.567 3.567 3.567
>       PERIODIC XYZ
>     &END CELL
>     &COORD
> C  -0.066491  -0.063731  -0.038851
> C   0.019572   1.759040   1.767428
> C   1.756129   0.023158   1.769616
> C   1.767376   1.770784   0.004363
> C   0.841267   0.843123   0.828198
> C   2.663349   0.903043   2.661920
> C   0.899007   2.665284   2.661387
> C   2.644659   2.648722   0.926362
>   &END COORD
>     &TOPOLOGY
>       &GENERATE
>         CREATE_MOLECULES
>       &END GENERATE
>     &END TOPOLOGY
>
>       &KIND C
>       BASIS_SET DZVP-GTH
>       POTENTIAL GTH-PBE-q4
>     &END KIND
>
>   &END SUBSYS
> &END FORCE_EVAL
> =====
> Input Frequency run
> &GLOBAL
>   PRINT_LEVEL high
>   PROJECT_NAME vib
>   RUN_TYPE VIBRATIONAL_ANALYSIS
>   PREFERRED_FFT_LIBRARY FFTW
> &END GLOBAL
>
> &MOTION
>   &GEO_OPT
>     OPTIMIZER BFGS
>     MAX_ITER 300
>   &END GEO_OPT
> &END MOTION
>
> &VIBRATIONAL_ANALYSIS
>     FULLY_PERIODIC T
> &END VIBRATIONAL_ANALYSIS
>
> &FORCE_EVAL
>
>   METHOD QS
>   &DFT
>     BASIS_SET_FILE_NAME GTH_BASIS_SETS
>     POTENTIAL_FILE_NAME GTH_POTENTIALS
>     &MGRID
>       CUTOFF 100
>       REL_CUTOFF 23
>       COMMENSURATE
>     &END MGRID
>     &QS
>      EPS_DEFAULT 1.0E-10
>     &END QS
>     &SCF
>       EPS_SCF 1.0E-5
>       MAX_SCF 100
>       SCF_GUESS RESTART
>       &OUTER_SCF
>         EPS_SCF 1.0E-5
>         MAX_SCF 20
>       &END
>       &OT
>         ALGORITHM IRAC
>         MINIMIZER CG
>         PRECONDITIONER FULL_ALL
>         ENERGY_GAP 0.001
>       &END OT
>       &PRINT
>         &RESTART
>          BACKUP_COPIES 0
>         &END RESTART
>       &END PRINT
>     &END SCF
>     &XC
>       &XC_FUNCTIONAL PBE
>       &END XC_FUNCTIONAL
>     &END XC
>     &POISSON
>      POISSON_SOLVER PERIODIC
>      PERIODIC XYZ
>      &EWALD
>        EWALD_TYPE EWALD
>        ALPHA 0.3
>        GMAX 11
>        O_SPLINE 6
>      &END EWALD
>    &END POISSON
>   &PRINT
>   &END PRINT
>   &END DFT
>   &SUBSYS
>     &CELL
>       ABC 3.567 3.567 3.567
>       PERIODIC XYZ
>     &END CELL
>     &COORD
>   C        -0.0393192769       -0.0522499977       -0.0007602780
>   C         0.0299677090        1.7769206120        1.7824574256
>   C         1.7642084626        0.0471181783        1.7911208859
>   C         1.7938452241        1.7853211459        0.0053883203
>   C         0.8664406756        0.8762954420        0.8435833733
>   C         2.6939879368        0.9029246308        2.6806928814
>   C         0.9092781460        2.6785011492        2.6771532650
>   C         2.6481574040        2.6661172907        0.9483093511
>   &END COORD
>     &TOPOLOGY
>       &GENERATE
>         CREATE_MOLECULES
>       &END GENERATE
>     &END TOPOLOGY
>
>       &KIND C
>       BASIS_SET DZVP-GTH
>       POTENTIAL GTH-PBE-q4
>     &END KIND
>
>   &END SUBSYS
> &END FORCE_EVAL
> =====
> Snippet output frequency run:
> If I look at the values with the lowest absolute value and I convert
> them to cm-1, it is poor accuracy:
>
>  VIB| Cartesian Low frequencies ----0.44072    -0.10876E-01
> 0.12458     0.69806
>  VIB| Cartesian Low frequencies --- 0.71490      1.4715
> 2.0898      3.8120
>  VIB| Cartesian Low frequencies ---  5.8007
>  VIB| Frequencies after removal of the rotations and translations
>  VIB| Internal  Low frequencies ----0.14095     0.50894
> 1.4072      2.0559
>  VIB| Internal  Low frequencies ---  3.6794      5.7900
> 25.027      25.504
>  VIB| Internal  Low frequencies ---  25.855      25.997
> 26.180      26.684
>  VIB| Internal  Low frequencies ---  26.818      26.970
> 27.202      27.461
>  VIB| Internal  Low frequencies ---  27.643      28.937
> 54.059      54.351
>  VIB| Internal  Low frequencies ---  54.817
>
>  VIB|                        NORMAL MODES - CARTESIAN DISPLACEMENTS
>  VIB|
>  VIB|                         1
> 2                    3
>  VIB|Frequency (cm^-1)   -82.399299           156.573040
> 260.352529
> ...
>  
> -------------------------------------------------------------------------------
>  ----                             MULTIGRID
> INFO                            ----
>  
> -------------------------------------------------------------------------------
>  count for grid        1:            868          cutoff
> [a.u.]           50.00
>  count for grid        2:            276          cutoff
> [a.u.]           12.50
>  count for grid        3:             80          cutoff
> [a.u.]            3.12
>  count for grid        4:              0          cutoff
> [a.u.]            0.78
>  total gridlevel count  :           1224
>
>   




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