[Wien] Mixer surprise when using PBE0 hybrid on-site functional

Xavier Rocquefelte xavier.rocquefelte at univ-rennes1.fr
Sat Jan 21 08:28:47 CET 2017


Dear Laurence

Thank you so much for your detailled replies.

I agree that something curious happens here. In particular, my surprise 
is why the convergency is fast and leads to a ferromagnetic solution in 
GGA+U and not in PBE0 on-site hybrid. These two schemes must be quite 
similar in the way they correct the GGA eigenvalues. I will continue to 
test the different options of mixer. Just one question, I didn't know 
the :MV keyword. Where should I find it?

Best Regards

Xavier

Le 20/01/2017 à 22:16, Laurence Marks a écrit :
> I can provide some partial responses, although there are also some 
> things that I don't understand. Some of this (maybe most) is not the 
> mixer but in other parts of Wien2k.
>
> First, the old (2008) version is there if you use MSEC1, but I have 
> not tested it and it may fail. Better is to use MSEC3 which is almost 
> the old version. For some classes of problems this is more stable than 
> MSR1, and works better. If you are talking about the pre-multisecant 
> version (BROYD) that vanished some time ago.
>
> Second, there is a nasty "feature" particularly for +U (eece) cases, 
> which is partially discussed in the mixer Readme. There is no 
> guarantee that a solution exists -- the KS theorem is for densities 
> but U is an orbital term. It is very possible to have cases where 
> there is no fixed-point solution. The older MSEC1 (maybe BROYD) could 
> find a fake solution where the density was consistent but the orbital 
> potential was not. The latest version is much better in avoiding them 
> and going for "real" solutions rather than being trapped. For orbital 
> potentials it is very important to look at :MV to check that one 
> really has a self-consistent orbital potential.
>
> Third, there are cases where PBE (and all the GGA's in Wien2k that I 
> have tested) give unphysical results when applied to isolated d or f 
> electrons as done for -eece. I guess that the GGA functionals were not 
> designed for the densities of just high L orbitals. This leads to very 
> bad behavior of the mixing. I know of no way to solve this in the 
> mixer, it is a structural problem. It goes away if LDA is used as the 
> form for VXC in -eece.
>
> Fourth, larger problem with low symmetry (P1 in particular) can 
> certainly behave badly. Part of this might be "somewhere" in Wien2k 
> coding, part of it is generic to a low symmetry problem. In many cases 
> these have small eigenvalues in the mixing Jacobian which are removed 
> when symmetry is imposed. All one can do is use MSEC3 or some of the 
> additional flags (see the mixer README) such as "SLOW".
>
> Fifth...probably exists, but I can't think of it immediately.
>
> On Fri, Jan 20, 2017 at 2:03 PM, Xavier Rocquefelte 
> <xavier.rocquefelte at univ-rennes1.fr 
> <mailto:xavier.rocquefelte at univ-rennes1.fr>> wrote:
>
>     Dear Colleagues
>
>     I did recently a calculation which has been published long time ago
>     using a old WIEN2k version (in 2008).
>
>     It corresponds to a spin-polarized calculation for the compound
>     CuO. The
>     symmetry is removed and the idea is to estimate the total energies for
>     different magnetic orders to extract magnetic couplings from a mapping
>     analysis. Such calculations were converging fastly without any trouble
>     in 2008.
>
>     Here I have started from the scratch with a case.cif file to generate
>     the case.struct file and initializing the calculation in a
>     standard manner.
>
>     Then I wanted to have the energy related to a ferromagnetic situation
>     (not the more stable). I have 8 copper sites in the unit cell I am
>     using.
>
>     When this calculation is done using PBE+U everything goes fine.
>     However
>     when PBE0 hybrid on-site functional is used we observed
>     oscillations and
>     the magnetic moment disappear, which is definitely not correct. It
>     should be mentionned that the convergency is really bad. If we do a
>     similar calculation on the cristallographic unit cell (2 copper sites
>     only) the calculations converge both in PBE+U and PBE0.
>
>     The convergency problems only arises for low-symmetry and high
>     number of
>     magnetic elements. I didn't have such problems before and I wonder
>     if we
>     could still use old mixer scheme in such situations. Looking at the
>     userguide, it seems that the mixer does not allow to do as before and
>     PRATT mixer is too slow.
>
>     Did you encounter similar difficulties (which were not in older WIEN2k
>     versions)?
>
>     Best Regards
>
>     Xavier
>
>     Here is the case.struct:
>
>     blebleble
>     P   LATTICE,NONEQUIV.ATOMS: 16 1_P1
>     MODE OF CALC=RELA unit=bohr
>       14.167163  6.467777 11.993298 90.000000 95.267000 90.000000
>     ATOM  -1: X=0.87500000 Y=0.75000000 Z=0.87500000
>                MULT= 1          ISPLIT= 8
>     Cu         NPT=  781  R0=0.00005000 RMT=    1.9700   Z: 29.0
>     LOCAL ROT MATRIX:    1.0000000 0.0000000 0.0000000
>                           0.0000000 1.0000000 0.0000000
>                           0.0000000 0.0000000 1.0000000
>     ATOM  -2: X=0.12500000 Y=0.25000000 Z=0.62500000
>                MULT= 1          ISPLIT= 8
>     Cu         NPT=  781  R0=0.00005000 RMT=    1.9700   Z: 29.0
>     LOCAL ROT MATRIX:    1.0000000 0.0000000 0.0000000
>                           0.0000000 1.0000000 0.0000000
>                           0.0000000 0.0000000 1.0000000
>     ATOM  -3: X=0.12500000 Y=0.25000000 Z=0.12500000
>                MULT= 1          ISPLIT= 8
>     Cu         NPT=  781  R0=0.00005000 RMT=    1.9700   Z: 29.0
>     LOCAL ROT MATRIX:    1.0000000 0.0000000 0.0000000
>                           0.0000000 1.0000000 0.0000000
>                           0.0000000 0.0000000 1.0000000
>     ATOM  -4: X=0.87500000 Y=0.75000000 Z=0.37500000
>                MULT= 1          ISPLIT= 8
>     Cu         NPT=  781  R0=0.00005000 RMT=    1.9700   Z: 29.0
>     LOCAL ROT MATRIX:    1.0000000 0.0000000 0.0000000
>                           0.0000000 1.0000000 0.0000000
>                           0.0000000 0.0000000 1.0000000
>     ATOM  -5: X=0.62500000 Y=0.25000000 Z=0.62500000
>                MULT= 1          ISPLIT= 8
>     Cu         NPT=  781  R0=0.00005000 RMT=    1.9700   Z: 29.0
>     LOCAL ROT MATRIX:    1.0000000 0.0000000 0.0000000
>                           0.0000000 1.0000000 0.0000000
>                           0.0000000 0.0000000 1.0000000
>     ATOM  -6: X=0.37500000 Y=0.75000000 Z=0.87500000
>                MULT= 1          ISPLIT= 8
>     Cu         NPT=  781  R0=0.00005000 RMT=    1.9700   Z: 29.0
>     LOCAL ROT MATRIX:    1.0000000 0.0000000 0.0000000
>                           0.0000000 1.0000000 0.0000000
>                           0.0000000 0.0000000 1.0000000
>     ATOM  -7: X=0.37500000 Y=0.75000000 Z=0.37500000
>                MULT= 1          ISPLIT= 8
>     Cu         NPT=  781  R0=0.00005000 RMT=    1.9700   Z: 29.0
>     LOCAL ROT MATRIX:    1.0000000 0.0000000 0.0000000
>                           0.0000000 1.0000000 0.0000000
>                           0.0000000 0.0000000 1.0000000
>     ATOM  -8: X=0.62500000 Y=0.25000000 Z=0.12500000
>                MULT= 1          ISPLIT= 8
>     Cu         NPT=  781  R0=0.00005000 RMT=    1.9700   Z: 29.0
>     LOCAL ROT MATRIX:    1.0000000 0.0000000 0.0000000
>                           0.0000000 1.0000000 0.0000000
>                           0.0000000 0.0000000 1.0000000
>     ATOM  -9: X=0.87500000 Y=0.41840000 Z=0.62500000
>                MULT= 1          ISPLIT= 8
>     O          NPT=  781  R0=0.00010000 RMT=    1.6900   Z: 8.0
>     LOCAL ROT MATRIX:    1.0000000 0.0000000 0.0000000
>                           0.0000000 1.0000000 0.0000000
>                           0.0000000 0.0000000 1.0000000
>     ATOM -10: X=0.12500000 Y=0.91840000 Z=0.87500000
>                MULT= 1          ISPLIT= 8
>     O          NPT=  781  R0=0.00010000 RMT=    1.6900   Z: 8.0
>     LOCAL ROT MATRIX:    1.0000000 0.0000000 0.0000000
>                           0.0000000 1.0000000 0.0000000
>                           0.0000000 0.0000000 1.0000000
>     ATOM -11: X=0.12500000 Y=0.58160000 Z=0.37500000
>                MULT= 1          ISPLIT= 8
>     O          NPT=  781  R0=0.00010000 RMT=    1.6900   Z: 8.0
>     LOCAL ROT MATRIX:    1.0000000 0.0000000 0.0000000
>                           0.0000000 1.0000000 0.0000000
>                           0.0000000 0.0000000 1.0000000
>     ATOM -12: X=0.87500000 Y=0.08160000 Z=0.12500000
>                MULT= 1          ISPLIT= 8
>     O          NPT=  781  R0=0.00010000 RMT=    1.6900   Z: 8.0
>     LOCAL ROT MATRIX:    1.0000000 0.0000000 0.0000000
>                           0.0000000 1.0000000 0.0000000
>                           0.0000000 0.0000000 1.0000000
>     ATOM -13: X=0.62500000 Y=0.58160000 Z=0.87500000
>                MULT= 1          ISPLIT= 8
>     O          NPT=  781  R0=0.00010000 RMT=    1.6900   Z: 8.0
>     LOCAL ROT MATRIX:    1.0000000 0.0000000 0.0000000
>                           0.0000000 1.0000000 0.0000000
>                           0.0000000 0.0000000 1.0000000
>     ATOM -14: X=0.37500000 Y=0.08160000 Z=0.62500000
>                MULT= 1          ISPLIT= 8
>     O          NPT=  781  R0=0.00010000 RMT=    1.6900   Z: 8.0
>     LOCAL ROT MATRIX:    1.0000000 0.0000000 0.0000000
>                           0.0000000 1.0000000 0.0000000
>                           0.0000000 0.0000000 1.0000000
>     ATOM -15: X=0.37500000 Y=0.41840000 Z=0.12500000
>                MULT= 1          ISPLIT= 8
>     O          NPT=  781  R0=0.00010000 RMT=    1.6900   Z: 8.0
>     LOCAL ROT MATRIX:    1.0000000 0.0000000 0.0000000
>                           0.0000000 1.0000000 0.0000000
>                           0.0000000 0.0000000 1.0000000
>     ATOM -16: X=0.62500000 Y=0.91840000 Z=0.37500000
>                MULT= 1          ISPLIT= 8
>     O          NPT=  781  R0=0.00010000 RMT=    1.6900   Z: 8.0
>     LOCAL ROT MATRIX:    1.0000000 0.0000000 0.0000000
>                           0.0000000 1.0000000 0.0000000
>                           0.0000000 0.0000000 1.0000000
>         1      NUMBER OF SYMMETRY OPERATIONS
>       1 0 0 0.00000000
>       0 1 0 0.00000000
>       0 0 1 0.00000000
>             1
>
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>
> -- 
> Professor Laurence Marks
> "Research is to see what everybody else has seen, and to think what 
> nobody else has thought", Albert Szent-Gyorgi
> www.numis.northwestern.edu <http://www.numis.northwestern.edu> ; 
> Corrosion in 4D: MURI4D.numis.northwestern.edu 
> <http://MURI4D.numis.northwestern.edu>
> Partner of the CFW 100% program for gender equity, 
> www.cfw.org/100-percent <http://www.cfw.org/100-percent>
> Co-Editor, Acta Cryst A
>
>
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