Dear Dan,
I have noticed similar problems.  Mulliken charges depend on the atomic basis 
set used.  In Siesta the cutoff radius (of H) seems to be the critical 
parameter.  I suggest that you check the dipol moment of an isolated water 
molecule (10 Angstrom box).  It should have the correct magnitude and sign for 
the basis set settings you use.

Regards, Ulrich.


 From:   Dan Gil <[email protected]> 
 To:   <[email protected]> 
 Sent:   06.10.2017 16:13 
 Subject:   [SIESTA-L] Mulliken Charges on Water 


Hi,


I am using Siesta 3.2 and ran into a strange problem.


I simulate a water molecule and the Mulliken charges are wrong. It shows that 
the oxygen atom is positively charged and the two hydrogens are negatively 
charged. The Hirshfeld and Voronoi populations are fine. Did I run into a bug?


input.fdf

NumberOfAtoms       3
NumberOfSpecies     4


%block ChemicalSpeciesLabel 
 1  13 Al
 2  14 Si
 3   8 O
 4   1 H
%endblock ChemicalSpeciesLabel


PAO.BasisType     nodes


%block PAO.BasisSizes
Al DZP
Si DZP
O  DZP
H  DZP
%endblock PAO.BasisSizes


XC.functional GGA
XC.authors    PBE


# SCF options
MaxSCFIterations      200
DM.MixingWeight       0.25         # New DM amount for next SCF cycle
DM.Tolerance          1.d-6         # Tolerance in maximum difference
SolutionMethod        diagon        # OrderN or Diagon
MeshCutoff  400 Ry
DM.Require.Energy.Convergence    .true.
DM.Energy.Tolerance              1.d-6 eV


MD.TypeOfRun          CG
MD.NumCGsteps         100
MD.InitialTemperature 300.0 K
MD.TargetTemperature  300.0 K


WriteHirshfeldPop .true.
WriteVoronoiPop     .true.
WriteMullikenPop    1


LatticeConstant 1   Ang


%block LatticeVectors
 9.5160000000  0.0000000000  0.0000000000
-4.7580000000  8.2411000000  0.0000000000
 0.0000000000  0.0000000000 48.2792733630
%endblock LatticeVectors


WarningMinimumAtiomicDistance 1.0 Ang
AtomicCoordinatesFormat  NotScaledCartesianAng
%block AtomicCoordinatesAndAtomicSpecies < Coord.fdf


Coord.fdf

5.265981 -1.943725 -6.378528 3
4.222545 -1.943725 -6.378528 4
5.612381 -0.997652 -6.378528 4


Output (excerpts)

mulliken: Mulliken Atomic and Orbital Populations:

Species: O                   
Atom  Qatom  Qorb
               2s      2s      2py     2pz     2px     2py     2pz     2px     
               2Pdxy   2Pdyz   2Pdz2   2Pdxz   2Pdx2-y2
   1  5.764   1.436  -0.027   1.363   1.793   1.235  -0.023  -0.003  -0.034
              0.003   0.002   0.005   0.001   0.014


Species: H                   
Atom  Qatom  Qorb
               1s      1s      1Ppy    1Ppz    1Ppx    
   2  1.118   0.845   0.036   0.063   0.104   0.070


   3  1.118   0.845   0.036   0.091   0.104   0.042


Hirshfeld Net Atomic Populations:
Atom #    Qatom  Species
     1   -0.234  O                   
     2    0.117  H                   
     3    0.117  H                   


Voronoi Net Atomic Populations:
Atom #    Qatom  Species
     1   -0.171  O                   
     2    0.086  H                   
     3    0.085  H          


Best Regards,


Dan




 

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