[CPMD-list] convergence problem on iron porphyrin

Yong Zhang zhangymall11 at gmail.com
Sun Jul 30 18:50:38 CEST 2006


Thank you Axel and Pradip,

I tested several options: VDB/MT; LOC=S or not; PCG or not; DUAL=4,5 or 6.
Finally only those options suggested by Pradip work.

Axel is absolutely correct, "LOC=S" does nothing when VDBpp is used and PCG
is essential. (I just want to double check it by my own, please do not mind
 ^_^) But the wavefunction optimization runs using MT (with PCG and LOC=S)
died finally. Does this simply mean that MT is not appropriate for this
calculation or I need to take care of other settings?

Both Dual=5 and Dual=6 work. And dual=5 gave a lower energy after geometry
optimization. I suppose this is good enough.

Thank Axel for the link. I guess the problem is related to the
adiabatic/nonadiabatic dynamics of DFT method. But, to be honest, I do not
know how to prove (or define) that my system is nonadiabatic :-(
I did test the different spin states for my system. For spin=1,3 or 5, all
the wavefunction jobs completed without problem. But in the GEO
optimization, only spin=3 completed with reasonable result. This is
consistent with previous references saying that spin=3 is the stablest state
for this complex. But this is only a static calculation, I do not know what
will happen if I run a dynamics.
For spin=1 or 5, I observed a total energy jump which I believe is caused by
the rapid increase in kinetic energy. But I do not understand why this
happened?

The "jump part" for spin=5 is like this:
###############
  49  6.952E-05   7.506E-06    -286.501141    8.912E-05     16.50
  50  1.485E-04   1.408E-05    -286.500750    3.907E-04     16.50
  51  4.059E-04   3.516E-05    -286.497778    2.972E-03     16.50
  52  1.682E-03   1.557E-04    -286.430725    6.705E-02     16.50
  53  1.276E-02   2.070E-03    -275.098803    1.133E+01     16.50
  54  1.683E-01   1.332E-02       7.105774    2.822E+02     16.46
  55  1.687E-01   1.298E-02       9.960731    2.855E+00     16.46
  56  1.687E-01   1.298E-02       9.937762   -2.297E-02     16.46
  57  1.686E-01   1.298E-02       9.910858   -2.690E-02     16.46
...

 116  1.650E-01   1.352E-02      -2.314784   -6.991E-01     16.46
 117  1.651E-01   1.352E-02      -3.051419   -7.366E-01     16.45
 118  1.651E-01   1.351E-02      -3.826305   -7.749E-01     16.45
 ================================================================
 =              END OF GEOMETRY OPTIMIZATION                    =
 ================================================================

 ################

and the final summary is:

################

 ELECTRONIC GRADIENT:
    MAX. COMPONENT =    1.65130E-01         NORM =    1.35140E-02
 NUCLEAR GRADIENT:
    MAX. COMPONENT =    6.73460E+00         NORM =    1.63507E+00


 TOTAL INTEGRATED ELECTRONIC DENSITY
    IN G-SPACE =                                       128.000000
    IN R-SPACE =                                       128.000000
 TOTAL INTEGRATED SPIN DENSITY                          -4.000000
 TOTAL INTEGRATED ABSOLUTE VALUE OF SPIN DENSITY         9.373111


 VANDERBILT AUGMENTATION CHARGES (MEAN VALUE PER ATOM)
 ATOM TYPE    NR. OF ATOMS        CHARGE
       H          12                .020
       C          20              -1.374
       N           4               -.242
      Fe           1               4.451

 (K+E1+L+N+X)           TOTAL ENERGY =           -3.82630538 A.U.
 (K)                  KINETIC ENERGY =          418.55865163 A.U.
 (E1=A-S+R)     ELECTROSTATIC ENERGY =         -192.60043071 A.U.
 (S)                           ESELF =          228.72690743 A.U.
 (R)                             ESR =            7.52699158 A.U.
 (L)    LOCAL PSEUDOPOTENTIAL ENERGY =         -148.70431024 A.U.
 (N)      N-L PSEUDOPOTENTIAL ENERGY =          -28.39383909 A.U.
 (X)     EXCHANGE-CORRELATION ENERGY =          -52.68637696 A.U.
         GRADIENT CORRECTION ENERGY =            -3.62222815 A.U.

################



the final summary for spin=3 is:

#################

 ELECTRONIC GRADIENT:
    MAX. COMPONENT =    1.06400E-05         NORM =    5.14668E-07
 NUCLEAR GRADIENT:
    MAX. COMPONENT =    5.59494E-02         NORM =    8.90548E-03


 TOTAL INTEGRATED ELECTRONIC DENSITY
    IN G-SPACE =                                       128.000000
    IN R-SPACE =                                       128.000000
 TOTAL INTEGRATED SPIN DENSITY                          -2.000000
 TOTAL INTEGRATED ABSOLUTE VALUE OF SPIN DENSITY         2.335721


 VANDERBILT AUGMENTATION CHARGES (MEAN VALUE PER ATOM)
 ATOM TYPE    NR. OF ATOMS        CHARGE
       H          12                .032
       C          20                .116
       N           4                .296
      Fe           1               9.654

 (K+E1+L+N+X)           TOTAL ENERGY =         -286.52297826 A.U.
 (K)                  KINETIC ENERGY =          105.06259988 A.U.
 (E1=A-S+R)     ELECTROSTATIC ENERGY =         -212.06028870 A.U.
 (S)                           ESELF =          228.72690743 A.U.
 (R)                             ESR =            7.47507791 A.U.
 (L)    LOCAL PSEUDOPOTENTIAL ENERGY =         -156.32548960 A.U.
 (N)      N-L PSEUDOPOTENTIAL ENERGY =           38.68448417 A.U.
 (X)     EXCHANGE-CORRELATION ENERGY =          -61.88428402 A.U.
         GRADIENT CORRECTION ENERGY =            -2.58770500 A.U.

###################

Thank you!



Best wishes

Yong


On 7/28/06, Axel Kohlmeyer <akohlmey at cmm.upenn.edu> wrote:
>
> On 7/28/06, Yong Zhang <zhangymall11 at gmail.com> wrote:
> >
> >  It is working now. Thanks a lot.
> >  I tried both VDB pp and MT pp, both work. So I guess the "LOC=S" for Fe
> is
> > the point.
>
> LOC=S is ignored for VDB. but for the Fe-MT potential essential,
> so you don't have ghost states. PCG and/or PCG MINIMIZE is
> the ticket for systems with tricky electron structures, which is
> truely the case here.


I tested this and


>  By the way, do you have any special reason for using VDB? What is the
> > difference between these PPs? Sorry if this is a naive question. I am a
> very
> > beginner of CMPD. :-p
>
> in that case, you should probably start with a simpler system.
> there are references for both types of pseudopotentials in the manual.
>
> VDB pseudopotentials need a (much) lower plane wave energy cutoff,
> due to not releasing the norm-conservation constraint on the
> pseudopotential.
>
> that has several implications, especially with the VDB implementation in
> CPMD.
> since CPMD does not have a working dual grid for the uspps, you have
> to crank up the density cutoff (best by using DUAL with a value of 5.0
> of even 6.0)
> so you get consistend DFT results and less problems with placing the
> augmentation charges on the grid). also, apart from basic operations like
> MD, geometry optimization, constraints, many advanced features in CPMD
> do not work with ultra-soft pseudopotentials. in the case of iron,
> however,
> the uspps should give a 'better structure' than the MT potential, provided
>
> you take care of the other technical issues.
>
> finally a word of caution. for the kind of system you are dealing with
> certain configurations can be quite tricky and DFT may not always
> give accurate results. please have a look at, e.g., page 18 of
> http://www.vlab.msi.umn.edu/events/download/LDA+U.pdf
> this is done with a different code, and there are other attempts
> to solve this DFT related problem as well, but you should check
> your results carefully.
>
> cheers,
>    axel.
>
> >
> >  Yong
> >
> > On 7/28/06, Pradip Kumar Biswas <p.biswas at csuohio.edu> wrote:
> > > Hi,
> > >
> > > I had a similar problem with convergence; PCG minimize helped.
> However,
> > > this is to mention that I used VDB pp with a w.fn cutoff of 25 Ry,
> dual
> > > 5.0 and for iron I use LMAX=D  LOCAL=S.
> > >
> > > pb.
> >
> >
> > On Jul 28, 2006, at 2:05 PM, Yong Zhang wrote:
> >
> > > Hello CPMDers,
> > >
> > >  I am trying to run some simulation on a Fe-porphyrin complex. The
> > > wavefunction optimation did not tend to converge at all. I took an
> > > optimized structure from MM calculation as the initial input. The
> > > triplet was reported before as the stable state of this complex and
> > > singlet and quintet are also possible. I tried all the three states
> > > but the results are similar.
> > >
>
>
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