[CP2K-user] [CP2K:19400] super slow total dipole calculation for Mg2+ compared to Zn2+

Emma Rossi emma.rossi.1 at studenti.unipd.it
Fri Oct 20 09:09:48 UTC 2023


Dear developers and CP2K users,

I'm running AIMD simulations and computing the total dipole moment of a 15 
A cubic box (Berry phase approach) containing water molecules, a phosphate 
chain (-4) and a divalent cation, either Zn2+ or Mg2+. 
For Mg2+, the convergence of the MOs localization process at each step is 
tremendously slower (one/two order of magnitude) compared to the box with 
Zn2+. I cannot figure out the reason of such behaviour. I use the default 
setting for the LOCALIZE section, which employs the JACOBI method.

The -2 net charge of the system is counterbalanced by uniform background. 
600 Ry cutoff for the auxiliary PW expansion of the electron density (500 
or 400 Ry are used in the literature for Zn2+ and Mg2+ respectively) and 
BLYP XC are used. DZVP-MOLOPT-SR-GTH-q10 and DZVP-MOLOPT-SR-GTH-q12 are 
used for Mg2+ and Zn2+ respectively.  

I observe a similar slowdown of the MOs localization speed when I use Na+ 
atoms to counterbalance the -2 charge of the system containing Zn2+.

Here a typical input file follows.

 &GLOBAL
   PRINT_LEVEL  LOW
   PROJECT_NAME MD
   RUN_TYPE  MD
 &END GLOBAL
 &MOTION
   &MD
     ENSEMBLE  NVT
     STEPS  100
     TIMESTEP     0.5 
     TEMPERATURE     3.0000000000000000E+02
     TEMP_TOL     5.0000000000000000E+01
     &THERMOSTAT
       TYPE  CSVR
       &CSVR
         TIMECON     2.4999999999999996E+01
       &END CSVR
     &END THERMOSTAT
   &END MD
 &END MOTION
 &FORCE_EVAL
   METHOD  QS
   &DFT
     BASIS_SET_FILE_NAME BASIS_MOLOPT
     POTENTIAL_FILE_NAME GTH_POTENTIALS
     CHARGE  -2
     &SCF
       MAX_SCF  100
       EPS_SCF     4.9999999999999998E-07
       SCF_GUESS  RESTART
       &OT  T
         MINIMIZER  DIIS
         PRECONDITIONER  FULL_KINETIC
       &END OT
     &END SCF
     &MGRID
       CUTOFF     6.0000000000000000E+02
     &END MGRID
     &XC
       DENSITY_CUTOFF     1.0000000000000000E-10
       GRADIENT_CUTOFF     1.0000000000000000E-10
       TAU_CUTOFF     1.0000000000000000E-10
       &XC_GRID
         XC_SMOOTH_RHO  NN10
         XC_DERIV  SPLINE2_SMOOTH
       &END XC_GRID
       &XC_FUNCTIONAL  NO_SHORTCUT
         &BECKE88  T
         &END BECKE88
         &LYP  T
         &END LYP
       &END XC_FUNCTIONAL
       &VDW_POTENTIAL
         &PAIR_POTENTIAL
           R_CUTOFF     8.0000000000000000E+00
           TYPE  DFTD3(BJ)
           PARAMETER_FILE_NAME dftd3.dat
           REFERENCE_FUNCTIONAL BLYP
           EPS_CN     1.0000000000000000E-02
           CALCULATE_C9_TERM  T
           REFERENCE_C9_TERM  T
           LONG_RANGE_CORRECTION  T
         &END PAIR_POTENTIAL
       &END VDW_POTENTIAL
     &END XC










*     &LOCALIZE  T       &PRINT         &TOTAL_DIPOLE  ON          
 FILENAME =totdipole           PERIODIC  T           &EACH             MD 
 1           &END EACH         &END TOTAL_DIPOLE       &END PRINT     &END 
LOCALIZE*
   &END DFT
   &SUBSYS
     &CELL
       A     1.5460000000000001E+01    0.0000000000000000E+00   
 0.0000000000000000E+00
       B     0.0000000000000000E+00    1.5460000000000001E+01   
 0.0000000000000000E+00
       C     0.0000000000000000E+00    0.0000000000000000E+00   
 1.5460000000000001E+01
       MULTIPLE_UNIT_CELL  1 1 1
     &END CELL
     &KIND O
       BASIS_SET DZVP-MOLOPT-GTH-q6
       POTENTIAL GTH-BLYP-q6
     &END KIND
     &KIND H
       BASIS_SET DZVP-MOLOPT-GTH-q1
       POTENTIAL GTH-BLYP-q1
     &END KIND
     &KIND C
       BASIS_SET DZVP-MOLOPT-GTH-q4
       POTENTIAL GTH-BLYP-q4
     &END KIND
     &KIND P
       BASIS_SET DZVP-MOLOPT-GTH-q5
       POTENTIAL GTH-BLYP-q5
     &END KIND
     &KIND Na
       BASIS_SET DZVP-MOLOPT-SR-GTH-q9
       POTENTIAL GTH-BLYP-q9
     &END KIND
     &KIND Mg
       BASIS_SET DZVP-MOLOPT-SR-GTH-q10
       POTENTIAL GTH-BLYP-q10
     &END KIND
     &TOPOLOGY
       NUMBER_OF_ATOMS  384
       MULTIPLE_UNIT_CELL  1 1 1
     &END TOPOLOGY
   &END SUBSYS
 &END FORCE_EVAL

Here a piece of the *file.out* concerning the *localization* is reported

 ENSEMBLE TYPE                =                                             
 NVT
 STEP NUMBER                  =                                           
 48740
 TIME [fs]                    =                                     
24370.000000
 CONSERVED QUANTITY [hartree] =                             
 -0.234908827385E+04

                                              INSTANTANEOUS             
AVERAGES
 CPU TIME [s]                 =                      220.24               
 29.11
 ENERGY DRIFT PER ATOM [K]    =         -0.274167730955E+04 
 -0.106732023761E+04
 POTENTIAL ENERGY[hartree]    =         -0.235022491736E+04 
 -0.234811418791E+04
 KINETIC ENERGY [hartree]     =          0.530388799833E+00   
0.547854613121E+00
 TEMPERATURE [K]              =                     291.529             
 301.129
 ***************************


 Number of electrons:                                                       
1070
 Number of occupied orbitals:                                               
 535
 Number of molecular orbitals:                                             
  535

 Number of orbital functions:                                               
3012
 Number of independent orbital functions:                                   
3012

 Extrapolation method: ASPC

 SCF WAVEFUNCTION OPTIMIZATION

  ----------------------------------- OT 
---------------------------------------
  Minimizer      : DIIS                : direct inversion
                                         in the iterative subspace
                                         using   7 DIIS vectors
                                         safer DIIS on
  Preconditioner : FULL_KINETIC        : inversion of T + eS
  Precond_solver : DEFAULT
  stepsize       :    0.15000000                  energy_gap     :   
 0.20000000
  eps_taylor     :   0.10000E-15                  max_taylor     :         
    4
  ----------------------------------- OT 
---------------------------------------

  Step     Update method      Time    Convergence         Total energy   
 Change
  
------------------------------------------------------------------------------
     1 OT DIIS     0.15E+00    4.9     0.00001365     -2350.2265786077 
-2.35E+03
     2 OT DIIS     0.15E+00    7.0     0.00000785     -2350.2266129356 
-3.43E-05
     3 OT DIIS     0.15E+00    7.0     0.00000667     -2350.2266281036 
-1.52E-05
     4 OT DIIS     0.15E+00    7.0     0.00000316     -2350.2266318502 
-3.75E-06
     5 OT DIIS     0.15E+00    7.1     0.00000285     -2350.2266340790 
-2.23E-06
     6 OT DIIS     0.15E+00    7.0     0.00000168     -2350.2266355491 
-1.47E-06
     7 OT DIIS     0.15E+00    7.1     0.00000158     -2350.2266365271 
-9.78E-07
     8 OT DIIS     0.15E+00    7.0     0.00000079     -2350.2266370647 
-5.38E-07
     9 OT DIIS     0.15E+00    7.1     0.00000054     -2350.2266374235 
-3.59E-07
    10 OT DIIS     0.15E+00    7.0     0.00000041     -2350.2266374897 
-6.63E-08

  * SCF run converged in    10 steps *


  Electronic density on regular grids:      -1069.9999984366       
 0.0000015634
  Core density on regular grids:             1067.9999999649       
-0.0000000351
  Total charge density on r-space grids:       -1.9999984716
  Total charge density g-space grids:          -1.9999984716

  Overlap energy of the core charge distribution:               
0.00000352123302
  Self energy of the core charge distribution:             
 -6058.29367128599642
  Core Hamiltonian energy:                                   
1758.83041225385932
  Hartree energy:                                           
 2514.80853697306702
  Exchange-correlation energy:                               
-565.57191895188691

  Total energy:                                             
-2350.22663748972354

 LOCALIZE| The spread relative to a set of orbitals is computed
 LOCALIZE| Orbitals to be localized: All orbitals
 LOCALIZE| If fractional occupation, fully occupied MOs are those
           within occupation tolerance of       0.00000001
 LOCALIZE| Spread defined by the Berry phase operator
 LOCALIZE| Optimal unitary transformation generated by Jacobi algorithm
 
  Eigenvalues of the occupied subspace spin            1
 ---------------------------------------------
      -2.77340522     -1.55519360     -1.55401616     -1.55312686
      -0.84401306     -0.81554322     -0.80702571     -0.80237237
      -0.80085752     -0.79902548     -0.79112340     -0.79067760
      -0.78889214     -0.78844561     -0.78745096     -0.78661985
      -0.78594483     -0.78398619     -0.78359896     -0.78223867
      -0.78202387     -0.78089859     -0.77900446     -0.77831838
      -0.77761721     -0.77700210     -0.77677871     -0.77654095
      -0.77610461     -0.77529141     -0.77482833     -0.77403370
[.......]
      -0.09177880     -0.09168157     -0.09118981     -0.09045276
      -0.09027640     -0.08911508     -0.08871380     -0.08817562
      -0.08660485     -0.08624312     -0.08399649     -0.08220911
      -0.07894380     -0.07429071     -0.06779908
 Fermi Energy [eV] :   -1.844907

 LOCALIZATION| Computing localization properties for OCCUPIED ORBITALS. 
Spin:  1
    Spread Functional     sum_in -w_i ln(|z_in|^2)    sum_in w_i(1-|z_in|^2)
    Initial Spread (Berry) :            203183.2008851338   
 34522.9346453651
    Localization by iterative distributed Jacobi rotation
                      Iteration            Functional         Tolerance   
Time
                            100        1035.1444747551       0.7611E-01   
0.145
                            200        1035.1439265702       0.2374E-01   
0.145
                            300        1035.1438285431       0.2086E-01   
0.145
                            400        1035.1437772042       0.1457E-01   
0.155
                            500        1035.1437553092       0.8452E-02   
0.146
                            600        1035.1437479886       0.4565E-02   
0.156
                            700        1035.1437457665       0.2413E-02   
0.144
                            800        1035.1437451192       0.1268E-02   
0.155
                            900        1035.1437449348       0.6661E-03   
0.155
                           1000        1035.1437448830       0.3497E-03   
0.156
                           1100        1035.1437448685       0.1836E-03   
0.169
    Localization  for spin   1 converged in   1195 iterations
    Spread Functional     sum_in -w_i ln(|z_in|^2)    sum_in w_i(1-|z_in|^2)
    Total Spread (Berry) :                1051.8315283360     
1035.1437448646

To check the role of the localization method in such problem, I ran two 
single point calculations, the first using the JACOBI method and the second 
using the CRAZY method to compute the total dipole. The latter makes the 
process even slower.  

I would be very grateful if any of you could give me any insight.

Best regards,
Emma Rossi

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