[QE-users] non-convergent scf calculation on organometal perovskite structure

Julien Barbaud julien_barbaud at sjtu.edu.cn
Fri Feb 22 07:49:55 CET 2019


Dear Fabrizio,

Thank you for your very quick answer and your suggestions. To answer 
your question, I did not inlcude smearing in my most general attempts 
(the "by default" input file), because it was my understanding that 
semiconductors /should/ not require it. Indeed, the charge density 
already decays smoothly to 0 around the band gap, so it should not pose 
the numerical problems that metals do. Am I mistaken ?


However, as mentionned, I did experiment with a fix where I include some 
additional empty bands to see if that solves the problem (as suggested 
in: https://www.quantum-espresso.org/Doc/pw_user_guide/node21.html 
section5.0.0.21). In this case, I used a Methfessel-Paxton smearing 
(m-p). I tried 30 bands (instead of 25 by default) with several values 
of broadening, but this does not appear to solve the problem.

As shown in the figure attached (reporting the evolution of estimated 
accuracy at each scf iteration), there is no obvious advantage in 
raising the value of degauss. The curve still stalls after a cetain 
number of iterations.

I also attached the input file used for this test.


Julien


Le 21/02/2019 à 12:53, Fabrizio Cossu a écrit :
>    Dear Julien,
> what smearing did you have in mind? Have you tried raising the broadening?
>
>    Cheers,
>    Fabrizio
>
> On Thu, 21 Feb 2019 at 12:19, Julien Barbaud 
> <julien_barbaud at sjtu.edu.cn <mailto:julien_barbaud at sjtu.edu.cn>> wrote:
>
>     Dear users,
>
>
>     I am new to QE, and trying to run a simple scf calculation on a
>     CH3NH3PbI3 crystal (semi-conducting material). I am using
>     ultrasoft pseudopotentials based on the exchange-correlation
>     functionnal PBEsol.
>
>     I set up a first input, with values of parameters inspired from
>     literature on the subject. However, I could not reach convergence
>     after 100 iterations. The estimated error was actually "exploding"
>     to very high values, indicating a serious problem. I tried several
>     changes but was unsuccessful:
>
>       *  varying plane-wave cutoff energy does not solve the problem
>         (cf attached ecut.png, giving the estimated error as a
>         function of the number of iterations. It is shown here only on
>         the first 15 iterations as the results pretty much only stall
>         from there)
>       *  varying cutoff energy for charge (cf ecutrho.png)
>       * taking larger k-point sampling (not shown)
>       *  I also read that for metallic or "close to metallic
>         conductors", there might be problems with the first unoccupied
>         states that can be solved by adding a few empty bands. My
>         system being a semi-conductor, I tried adding additional bands
>         using a m-p smearing but no improvement was found (not shown)
>
>
>     The only change that I found effective was to reduce the
>     mixing_beta factor.
>
>
>     It effectively prevents the error from diverging to very large
>     values, but I still do not reach convergence, even after longer
>     iterations. I tried much smaller values of mixing beta which
>     improves the final value of the error, but I still cannot reach
>     convergence on 100 iterations. As shown in the mixbeta2_zoom.png,
>     the error reduces to smaller values around ~1e-5~1e-6, but it
>     keeps stalling after a while. I do not observe a well-converging
>     behaviour for any value.
>
>
>     I attached the "default version" of my script on which the various
>     modifications described above have been independently performed. I
>     obtained the geometry from a CIF file in literature and checked it
>     with visualization software; it seems perfectly ok as far as I can
>     tell.
>
>
>     Any insight on what I did wrong would be really helpful. I suspect
>     a shameful beginner mistake, but can not find it out.
>
>
>     Thanks in advance,
>
>     Julien barbaud
>
>
>     P.S: this is my first time posting on this user list. Please let
>     me know if my question is not suitable for it, or can be improved
>     either in its content or presentation. I will gladly take any
>     recommandation into account in order not to negatively impact the
>     quality of this user list !
>
>     _______________________________________________
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>     <mailto:users at lists.quantum-espresso.org>
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>
>
>
> -- 
> *Fabrizio Cossu
> postdoctoral fellow at APCTP (Asia Pacific Center for Theoretical 
> Physics)*,
> Hogil Kim Memorial Building #501
> POSTECH, 67 Cheongam-Ro, Nam-Gu,
> Pohang-si, Gyeongsangbuk-do,
> 790-784 (37673), Republic of Korea
>                         |
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>
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&CONTROL
  pseudo_dir = "/home/julien_barbaud/QUANTUM_ESPRESSO/Program/qe-6.3/pseudo"
  calculation = 'scf'
  outdir= "./out"
  tstress=.TRUE.
  tprnfor=.TRUE.
/
 
&SYSTEM
  nat= 12
  ntyp= 5
  ibrav= 0
  ecutwfc= 30, ecutrho = 300
  nbnd= 30
  occupations= 'smearing', smearing = 'm-p', degauss = 0.1
/
 
&ELECTRONS
  mixing_beta = 0.00075
  conv_thr =  1.0d-8
  electron_maxstep = 70
/
 
&IONS
/
 
&CELL
/
 
ATOMIC_SPECIES
C   12.011  C.pbesol-n-rrkjus_ps1.1.0.0.UPF
N   14.007  N.pbesol-n-rrkjus_ps1.1.0.0.UPF
H    1.008  H.pbesol-rrkjus_ps1.0.1.UPF
Pb   207.2  Pb.pbesol-dn-rrkjus_ps1.1.0.0.UPF
I   126.90  I.pbesol-n-rrkjus_ps1.1.0.0.UPF
 
CELL_PARAMETERS angstrom
      6.28880000        0.00000000        0.00000000
      0.00154263        6.22876981        0.00000000
      0.13973295       -0.00036613        6.37255819
 
ATOMIC_POSITIONS angstrom
C         5.68762816        6.22746232        2.91755469
N         0.76248596       -0.00015695        3.49068983
H         5.76522586        6.22643528        1.82113056
H         5.15723272        0.90114080        3.25657478
H         5.15968675        5.32511200        3.25829538
H         1.30458379        0.84536565        3.19592078
H         1.30663813        5.38278144        3.19763499
H         0.76813187        0.00090438        4.53227809
Pb        2.93516392        3.11390239        6.22995946
I         2.64234654        3.11409882        3.02788916
I         2.51578467        6.22849954        0.15080022
I         5.99299067        3.11401602        5.87855111

K_POINTS automatic
4 4 4 0 0 0


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