[CP2K-user] Spin contamination in condensed molecular liquid system

Tom H tom.... at gmail.com
Mon May 31 12:06:16 UTC 2021


Hi all, 

I am investigating a molecular liquid system, namely liquid-Se. It is 
formed of short chains of Se (down to only 2 Se atoms), which may show 
partially occupied electronic states, especially in the low pressure 
regime, in which molecules are well separated. I am slightly confused about 
how to model such a system using CP2K. 

I have started running unrestricted Kohn-Sham MD calculations, starting 
from an amorphous configuration of Se8 molecules in a chain configuration. 
I do have an even number of electrons, but I am suspecting spin 
polarization due to the reasons mentioned above. I've been checking for 
spin contamination in the CP2K output, and obtained the following for the 
first 100 steps of dynamics: 

  Ideal and single determinant S**2 :                    0.000000      
 0.000000
  Ideal and single determinant S**2 :                    0.000000      
 0.000000
  Ideal and single determinant S**2 :                    0.000000      
 0.000000
  Ideal and single determinant S**2 :                    0.000000      
 0.000000
  Ideal and single determinant S**2 :                    0.000000      
-0.000000
  Ideal and single determinant S**2 :                    0.000000      
-0.000000
  Ideal and single determinant S**2 :                    0.000000      
 0.000000
  Ideal and single determinant S**2 :                    0.000000      
-0.000000
  Ideal and single determinant S**2 :                    0.000000      
-0.000000
  Ideal and single determinant S**2 :                    0.000000      
-0.000000
  Ideal and single determinant S**2 :                    0.000000      
-0.000000
  Ideal and single determinant S**2 :                    0.000000      
-0.000000
  Ideal and single determinant S**2 :                    0.000000      
 0.000000
  Ideal and single determinant S**2 :                    0.000000      
-0.000000
  Ideal and single determinant S**2 :                    0.000000      
 0.000000
  Ideal and single determinant S**2 :                    0.000000      
 0.000000
  Ideal and single determinant S**2 :                    0.000000      
 0.000000
  Ideal and single determinant S**2 :                    0.000000      
 0.000000
  Ideal and single determinant S**2 :                    0.000000      
 0.000000
  Ideal and single determinant S**2 :                    0.000000      
 0.000000
  Ideal and single determinant S**2 :                    0.000000      
 0.000000
  Ideal and single determinant S**2 :                    0.000000      
 0.000000
  Ideal and single determinant S**2 :                    0.000000      
 0.000002
  Ideal and single determinant S**2 :                    0.000000      
 0.000018
  Ideal and single determinant S**2 :                    0.000000      
 0.000152
  Ideal and single determinant S**2 :                    0.000000      
 0.001315
  Ideal and single determinant S**2 :                    0.000000      
 0.012071
  Ideal and single determinant S**2 :                    0.000000      
 0.108839
  Ideal and single determinant S**2 :                    0.000000      
 1.570334
  Ideal and single determinant S**2 :                    0.000000      
 8.075949
  Ideal and single determinant S**2 :                    0.000000      
12.475536
  Ideal and single determinant S**2 :                    0.000000      
14.594641
  Ideal and single determinant S**2 :                    0.000000      
15.297790
  Ideal and single determinant S**2 :                    0.000000      
16.214178
  Ideal and single determinant S**2 :                    0.000000      
16.323013
  Ideal and single determinant S**2 :                    0.000000      
16.129883
  Ideal and single determinant S**2 :                    0.000000      
15.688840
  Ideal and single determinant S**2 :                    0.000000      
15.961233
  Ideal and single determinant S**2 :                    0.000000      
15.596193
  Ideal and single determinant S**2 :                    0.000000      
15.578972
  Ideal and single determinant S**2 :                    0.000000      
15.859515
  Ideal and single determinant S**2 :                    0.000000      
15.810544
  Ideal and single determinant S**2 :                    0.000000      
14.870891
  Ideal and single determinant S**2 :                    0.000000      
14.549977
  Ideal and single determinant S**2 :                    0.000000      
14.490598
  Ideal and single determinant S**2 :                    0.000000      
14.477700
  Ideal and single determinant S**2 :                    0.000000      
14.251470
  Ideal and single determinant S**2 :                    0.000000      
14.256963
  Ideal and single determinant S**2 :                    0.000000      
14.245575
  Ideal and single determinant S**2 :                    0.000000      
14.657994
  Ideal and single determinant S**2 :                    0.000000      
14.097974
  Ideal and single determinant S**2 :                    0.000000      
14.181373
  Ideal and single determinant S**2 :                    0.000000      
14.265038
  Ideal and single determinant S**2 :                    0.000000      
14.134708
  Ideal and single determinant S**2 :                    0.000000      
14.176089
  Ideal and single determinant S**2 :                    0.000000      
14.011084
  Ideal and single determinant S**2 :                    0.000000      
14.038357
  Ideal and single determinant S**2 :                    0.000000      
14.313602
  Ideal and single determinant S**2 :                    0.000000      
14.458239
  Ideal and single determinant S**2 :                    0.000000      
14.474756
  Ideal and single determinant S**2 :                    0.000000      
15.064850
  Ideal and single determinant S**2 :                    0.000000      
15.349064
  Ideal and single determinant S**2 :                    0.000000      
15.697990
  Ideal and single determinant S**2 :                    0.000000      
15.740888
  Ideal and single determinant S**2 :                    0.000000      
15.605483
  Ideal and single determinant S**2 :                    0.000000      
15.619671
  Ideal and single determinant S**2 :                    0.000000      
16.146289
  Ideal and single determinant S**2 :                    0.000000      
16.571982
  Ideal and single determinant S**2 :                    0.000000      
16.791026
  Ideal and single determinant S**2 :                    0.000000      
16.182009
  Ideal and single determinant S**2 :                    0.000000      
16.201162
  Ideal and single determinant S**2 :                    0.000000      
16.799011
  Ideal and single determinant S**2 :                    0.000000      
17.191503
  Ideal and single determinant S**2 :                    0.000000      
16.657538
  Ideal and single determinant S**2 :                    0.000000      
16.398196
  Ideal and single determinant S**2 :                    0.000000      
16.685182
  Ideal and single determinant S**2 :                    0.000000      
17.269278
  Ideal and single determinant S**2 :                    0.000000      
17.420976
  Ideal and single determinant S**2 :                    0.000000      
17.327620
  Ideal and single determinant S**2 :                    0.000000      
17.123223
  Ideal and single determinant S**2 :                    0.000000      
17.213689
  Ideal and single determinant S**2 :                    0.000000      
17.264376
  Ideal and single determinant S**2 :                    0.000000      
17.123970
  Ideal and single determinant S**2 :                    0.000000      
16.758495
  Ideal and single determinant S**2 :                    0.000000      
16.487501
  Ideal and single determinant S**2 :                    0.000000      
16.738201
  Ideal and single determinant S**2 :                    0.000000      
16.527679
  Ideal and single determinant S**2 :                    0.000000      
16.042440
  Ideal and single determinant S**2 :                    0.000000      
15.726199
  Ideal and single determinant S**2 :                    0.000000      
15.538890
  Ideal and single determinant S**2 :                    0.000000      
15.731163
  Ideal and single determinant S**2 :                    0.000000      
15.596686
  Ideal and single determinant S**2 :                    0.000000      
15.086832
  Ideal and single determinant S**2 :                    0.000000      
15.170306
  Ideal and single determinant S**2 :                    0.000000      
14.774768
  Ideal and single determinant S**2 :                    0.000000      
14.358169
  Ideal and single determinant S**2 :                    0.000000      
14.818519
  Ideal and single determinant S**2 :                    0.000000      
15.032944
  Ideal and single determinant S**2 :                    0.000000      
14.517417
  Ideal and single determinant S**2 :                    0.000000      
14.088642

Should I be bothered? Over this short MD run, some Se8 chains already break 
into smaller chunks - so I'm expecting more singly-occupied electronic 
states than at the beginning. I'm having a hard time understanding the 
connection between spin polarization in the "isolated, single molecule" 
formalism of CP2K and spin polarization in condensed molecular systems. 

One last question : any tips on accelerating SCF convergence of UKS related 
to the OT method? 

thank you, 
Tom


-------------- next part --------------
An HTML attachment was scrubbed...
URL: <https://lists.cp2k.org/archives/cp2k-user/attachments/20210531/8fa88cf8/attachment.htm>


More information about the CP2K-user mailing list