[Q-e-developers] Problems converging anions in vacuum

Oliviero Andreussi oliviero.andreussi at epfl.ch
Wed May 9 15:24:49 CEST 2012


Dear developers,

The title says it all, we have been having problems with calculations of 
organic anions (isolated molecules) with pw.x. The problem arises when 
the cell size is increased above a minimum value, the SCF will almost 
converge, but an error will show up in the diagonalization and the SCF 
will go bananas. The error is quite reproducible, it happens for several 
different organic anions (but also for OH-) and it may be something 
already known to the community. If this is the case, if you know any 
solution it would be very helpful and I apologise for the attachments 
and the rest of the mail.

We tried to play a bit with the standard parameters of pw, in particular 
we tried changing diagonalization scheme (cg vs davidson), changing the 
number of iterations, changing mixing scheme (thomas-fermi, broyden, 
local thomas-fermi), changing mixing parameter (from a starting one of 
0.4 to as low as 0.01), changing the cutoffs, adding a smearing 
(gaussian, with several values of degauss), different functionals (pbe, 
pw91 and lda), we also restarted from a converged density (obtained from 
a calculation in a dielectric environment), but nothing worked. We have 
also tried some combinations of the above variations, probably not all 
of them.

Attached you find an input and an output for an acetate anion (CH3COO-, 
as in figure molecule.png), the output has been obtained with a modified 
version of the code that does noting but printing a cube file of the 
electronic density at each SCF step. This is to show you what happens 
when the SCF goes bananas: in a normal SCF step the density changes 
little and in a smooth way (attachement normal.png, difference between 
the density at step 24 and the density at step 25 of the SCF cycle, 
surfaces plotted at an isovalue of the differential density of 0.00001 
); when the SCF start failing, the difference between two successive 
densities is much larger (attachement critical.png, surfaces plotted at 
an isovalue of 0.00010), it resembles the combination of two pz atomic 
orbitals on the oxygen atoms, and it is highly modulated (in particular 
one can see regular patterns when looking along cell axis, e.g. 
critical_z.png).  Any insight on what is happening would be very 
helpful. Note that calculations with a cell size <= 40 a.u. actually 
converge for this system in a reasonable number of steps (20-30).

Best,

Oliviero Andreussi
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 &CONTROL
   !
   calculation = 'scf'
   restart_mode = 'from_scratch'
   pseudo_dir = '/home/andreuss/PWSCF/pslibrary.0.1/pbe/PSEUDOPOTENTIALS'
   outdir = './'
   prefix = 'c64197'
   tprnfor = .TRUE.
   !
 /
 &SYSTEM
   !
   ecutrho = 300
   ecutwfc = 30
   !
   ibrav = 1
   celldm( 1 ) = 50
   !
   nat = 7
   ntyp = 3
   !
   tot_charge = -1
   !
   assume_isolated = 'makov-payne'
/
 &ELECTRONS
   !
   conv_thr = 5.D-9
   diagonalization = 'cg'
   mixing_beta = 0.4
   electron_maxstep = 200
   !
 /
 &IONS
   !
   ion_dynamics    = 'bfgs'
   !
 /
K_POINTS (automatic)
 1 1 1 0 0 0
ATOMIC_SPECIES  
C   12      C.pbe-rrkjus.UPF
H    1      H.pbe-rrkjus.UPF
O   16      O.pbe-rrkjus.UPF
ATOMIC_POSITIONS (angstrom)
C       -1.301514464   0.322267800  -0.013534662
H       -0.992221776  -0.730771277  -0.017468400
H       -0.953317139   0.822347547  -0.927803089
H       -2.403944997   0.357568238  -0.004148297
C       -0.798965029   0.994835251   1.231555280
O       -0.624449875   2.333980957   1.186305977
O       -0.565657575   0.408425490   2.283827156
-------------- next part --------------

     Program PWSCF v.4.99       starts on  7May2012 at 10:42:54 

     This program is part of the open-source Quantum ESPRESSO suite
     for quantum simulation of materials; please cite
         "P. Giannozzi et al., J. Phys.:Condens. Matter 21 395502 (2009);
          URL http://www.quantum-espresso.org", 
     in publications or presentations arising from this work. More details at
     http://www.quantum-espresso.org/quote.php

     Parallel version (MPI), running on     4 processors
     R & G space division:  proc/pool =    4

     Current dimensions of program PWSCF are:
     Max number of different atomic species (ntypx) = 10
     Max number of k-points (npk) =  40000
     Max angular momentum in pseudopotentials (lmaxx) =  3
     Waiting for input...
     Reading input from standard input

     Subspace diagonalization in iterative solution of the eigenvalue problem:
     a serial algorithm will be used

 
     Parallelization info
     --------------------
     sticks:   dense  smooth     PW     G-vecs:    dense   smooth      PW
     Min       14915    5970   1492              2742228   693699   86741
     Max       14917    5971   1494              2742229   693706   86744
     Sum       59665   23881   5973             10968915  2774807  346971
 


     bravais-lattice index     =            1
     lattice parameter (alat)  =      50.0000  a.u.
     unit-cell volume          =  125000.0000 (a.u.)^3
     number of atoms/cell      =            7
     number of atomic types    =            3
     number of electrons       =        24.00
     number of Kohn-Sham states=           12
     kinetic-energy cutoff     =      30.0000  Ry
     charge density cutoff     =     300.0000  Ry
     convergence threshold     =      5.0E-09
     mixing beta               =       0.4000
     number of iterations used =            8  plain     mixing
     Exchange-correlation      = PBE ( 1 4 3 4 0)
     EXX-fraction              =        0.00
 

     Environ Module
     ==============

     Please cite
         "O. Andreussi, I. Dabo and N. Marzari, J. Chem. Phys. 136, 064102 (2012);"
     in publications or presentations arising from this work.

     compensation onset threshold      =               0.1000E+00 
     switching function adopted        =                     SCCS 
     density limit for vacuum region   =               0.5000E-02 
     density limit for bulk solvent    =               0.1000E-03 
 

     celldm(1)=  50.000000  celldm(2)=   0.000000  celldm(3)=   0.000000
     celldm(4)=   0.000000  celldm(5)=   0.000000  celldm(6)=   0.000000

     crystal axes: (cart. coord. in units of alat)
               a(1) = (   1.000000   0.000000   0.000000 )  
               a(2) = (   0.000000   1.000000   0.000000 )  
               a(3) = (   0.000000   0.000000   1.000000 )  

     reciprocal axes: (cart. coord. in units 2 pi/alat)
               b(1) = (  1.000000  0.000000  0.000000 )  
               b(2) = (  0.000000  1.000000  0.000000 )  
               b(3) = (  0.000000  0.000000  1.000000 )  


     PseudoPot. # 1 for  C read from file:
     /home/andreuss/PWSCF/pslibrary.0.1/pbe/PSEUDOPOTENTIALS/C.pbe-rrkjus.UPF
     MD5 check sum: 95fa12f085d2e18f476bcc6e9c8e426e
     Pseudo is Ultrasoft + core correction, Zval =  4.0
     Generated using "atomic" code by A. Dal Corso  (Quantum ESPRESSO distribution)
     Using radial grid of 1073 points,  4 beta functions with: 
                l(1) =   0
                l(2) =   0
                l(3) =   1
                l(4) =   1
     Q(r) pseudized with 0 coefficients 


     PseudoPot. # 2 for  H read from file:
     /home/andreuss/PWSCF/pslibrary.0.1/pbe/PSEUDOPOTENTIALS/H.pbe-rrkjus.UPF
     MD5 check sum: bfac04b7ccebeaf0326b5278624b3e08
     Pseudo is Ultrasoft, Zval =  1.0
     Generated using "atomic" code by A. Dal Corso  (Quantum ESPRESSO distribution)
     Using radial grid of  929 points,  2 beta functions with: 
                l(1) =   0
                l(2) =   0
     Q(r) pseudized with 0 coefficients 


     PseudoPot. # 3 for  O read from file:
     /home/andreuss/PWSCF/pslibrary.0.1/pbe/PSEUDOPOTENTIALS/O.pbe-rrkjus.UPF
     MD5 check sum: a2d6ea7c9cd2620aae7e5676ca7d6432
     Pseudo is Ultrasoft + core correction, Zval =  6.0
     Generated using "atomic" code by A. Dal Corso  (Quantum ESPRESSO distribution)
     Using radial grid of 1095 points,  4 beta functions with: 
                l(1) =   0
                l(2) =   0
                l(3) =   1
                l(4) =   1
     Q(r) pseudized with 0 coefficients 


     atomic species   valence    mass     pseudopotential
        C              4.00    12.00000      C( 1.00)
        H              1.00     1.00000      H( 1.00)
        O              6.00    16.00000      O( 1.00)

     No symmetry found



   Cartesian axes

     site n.     atom                  positions (alat units)
         1           C   tau(   1) = (  -0.0491901   0.0121800  -0.0005115  )
         2           H   tau(   2) = (  -0.0375005  -0.0276192  -0.0006602  )
         3           H   tau(   3) = (  -0.0360302   0.0310802  -0.0350659  )
         4           H   tau(   4) = (  -0.0908560   0.0135141  -0.0001568  )
         5           C   tau(   5) = (  -0.0301965   0.0375993   0.0465460  )
         6           O   tau(   6) = (  -0.0236008   0.0882117   0.0448359  )
         7           O   tau(   7) = (  -0.0213788   0.0154362   0.0863162  )

     number of k points=     1
                       cart. coord. in units 2pi/alat
        k(    1) = (   0.0000000   0.0000000   0.0000000), wk =   2.0000000

     Dense  grid: 10968915 G-vectors     FFT dimensions: ( 288, 288, 288)

     Smooth grid:  2774807 G-vectors     FFT dimensions: ( 180, 180, 180)

     Largest allocated arrays     est. size (Mb)     dimensions
        Kohn-Sham Wavefunctions        15.88 Mb     (  86742,   12)
        NL pseudopotentials            50.30 Mb     (  86742,   38)
        Each V/rho on FFT grid         91.12 Mb     (5971968)
        Each G-vector array            20.92 Mb     (2742229)
        G-vector shells                 0.12 Mb     (  15831)
     Largest temporary arrays     est. size (Mb)     dimensions
        Each subspace H/S matrix        0.00 Mb     (  12,  12)
        Each <psi_i|beta_j> matrix      0.01 Mb     (     38,   12)
        Arrays for rho mixing         729.00 Mb     (5971968,   8)

     Check: negative/imaginary core charge=   -0.000001    0.000000

     Initial potential from superposition of free atoms
     Check: negative starting charge=   -0.007891

     starting charge   22.99989, renormalised to   24.00000

     negative rho (up, down):  0.823E-02 0.000E+00
     Starting wfc are   19 randomized atomic wfcs

     total cpu time spent up to now is       56.0 secs

     per-process dynamical memory:  1011.2 Mb

     Self-consistent Calculation

     iteration #  1     ecut=    30.00 Ry     beta=0.40
     CG style diagonalization
     ethr =  1.00E-02,  avg # of iterations =  2.8

     negative rho (up, down):  0.677E-02 0.000E+00

     total cpu time spent up to now is      123.6 secs

     total energy              =     -94.38436288 Ry
     Harris-Foulkes estimate   =     -94.56736853 Ry
     estimated scf accuracy    <       0.39995625 Ry

     iteration #  2     ecut=    30.00 Ry     beta=0.40
     CG style diagonalization
     ethr =  1.67E-03,  avg # of iterations =  5.2

     negative rho (up, down):  0.903E-02 0.000E+00

     total cpu time spent up to now is      201.2 secs

     total energy              =     -94.74420127 Ry
     Harris-Foulkes estimate   =     -94.77861381 Ry
     estimated scf accuracy    <       0.12863024 Ry

     iteration #  3     ecut=    30.00 Ry     beta=0.40
     CG style diagonalization
     ethr =  5.36E-04,  avg # of iterations =  3.9

     negative rho (up, down):  0.210E-01 0.000E+00

     add environment contribution to local potential

     total cpu time spent up to now is      298.5 secs

     total energy              =     -94.75927816 Ry
     Harris-Foulkes estimate   =     -94.77532585 Ry
     estimated scf accuracy    <       0.04207723 Ry

     iteration #  4     ecut=    30.00 Ry     beta=0.40
     CG style diagonalization
     ethr =  1.75E-04,  avg # of iterations =  4.1

     negative rho (up, down):  0.103E-01 0.000E+00

     add environment contribution to local potential

     total cpu time spent up to now is      396.1 secs

     total energy              =     -94.76839010 Ry
     Harris-Foulkes estimate   =     -94.77054534 Ry
     estimated scf accuracy    <       0.00493734 Ry

     iteration #  5     ecut=    30.00 Ry     beta=0.40
     CG style diagonalization
     ethr =  2.06E-05,  avg # of iterations =  5.8

     negative rho (up, down):  0.687E-02 0.000E+00

     add environment contribution to local potential

     total cpu time spent up to now is      503.0 secs

     total energy              =     -94.77273727 Ry
     Harris-Foulkes estimate   =     -94.77479229 Ry
     estimated scf accuracy    <       0.00389591 Ry

     iteration #  6     ecut=    30.00 Ry     beta=0.40
     CG style diagonalization
     ethr =  1.62E-05,  avg # of iterations =  4.1

     negative rho (up, down):  0.647E-02 0.000E+00

     add environment contribution to local potential

     total cpu time spent up to now is      602.0 secs

     total energy              =     -94.77379533 Ry
     Harris-Foulkes estimate   =     -94.77389558 Ry
     estimated scf accuracy    <       0.00037473 Ry

     iteration #  7     ecut=    30.00 Ry     beta=0.40
     CG style diagonalization
     ethr =  1.56E-06,  avg # of iterations =  6.4

     negative rho (up, down):  0.595E-02 0.000E+00

     add environment contribution to local potential

     total cpu time spent up to now is      712.4 secs

     total energy              =     -94.77399362 Ry
     Harris-Foulkes estimate   =     -94.77447145 Ry
     estimated scf accuracy    <       0.00075190 Ry

     iteration #  8     ecut=    30.00 Ry     beta=0.40
     CG style diagonalization
     ethr =  1.56E-06,  avg # of iterations =  5.4

     negative rho (up, down):  0.535E-02 0.000E+00

     add environment contribution to local potential

     total cpu time spent up to now is      817.7 secs

     total energy              =     -94.77431193 Ry
     Harris-Foulkes estimate   =     -94.77432019 Ry
     estimated scf accuracy    <       0.00021328 Ry

     iteration #  9     ecut=    30.00 Ry     beta=0.40
     CG style diagonalization
     ethr =  8.89E-07,  avg # of iterations =  4.2

     negative rho (up, down):  0.506E-02 0.000E+00

     add environment contribution to local potential

     total cpu time spent up to now is      916.1 secs

     total energy              =     -94.77425671 Ry
     Harris-Foulkes estimate   =     -94.77438382 Ry
     estimated scf accuracy    <       0.00035173 Ry

     iteration # 10     ecut=    30.00 Ry     beta=0.40
     CG style diagonalization
     ethr =  8.89E-07,  avg # of iterations =  3.2

     negative rho (up, down):  0.494E-02 0.000E+00

     add environment contribution to local potential

     total cpu time spent up to now is     1010.8 secs

     total energy              =     -94.77415401 Ry
     Harris-Foulkes estimate   =     -94.77427252 Ry
     estimated scf accuracy    <       0.00015650 Ry

     iteration # 11     ecut=    30.00 Ry     beta=0.40
     CG style diagonalization
     ethr =  6.52E-07,  avg # of iterations =  4.8

     negative rho (up, down):  0.487E-02 0.000E+00

     add environment contribution to local potential

     total cpu time spent up to now is     1111.7 secs

     total energy              =     -94.77423748 Ry
     Harris-Foulkes estimate   =     -94.77431636 Ry
     estimated scf accuracy    <       0.00016839 Ry

     iteration # 12     ecut=    30.00 Ry     beta=0.40
     CG style diagonalization
     ethr =  6.52E-07,  avg # of iterations =  3.8

     negative rho (up, down):  0.484E-02 0.000E+00

     add environment contribution to local potential

     total cpu time spent up to now is     1207.7 secs

     total energy              =     -94.77427843 Ry
     Harris-Foulkes estimate   =     -94.77429062 Ry
     estimated scf accuracy    <       0.00005597 Ry

     iteration # 13     ecut=    30.00 Ry     beta=0.40
     CG style diagonalization
     ethr =  2.33E-07,  avg # of iterations =  3.6

     negative rho (up, down):  0.482E-02 0.000E+00

     add environment contribution to local potential

     total cpu time spent up to now is     1303.7 secs

     total energy              =     -94.77428316 Ry
     Harris-Foulkes estimate   =     -94.77428611 Ry
     estimated scf accuracy    <       0.00002776 Ry

     iteration # 14     ecut=    30.00 Ry     beta=0.40
     CG style diagonalization
     ethr =  1.16E-07,  avg # of iterations =  3.3

     negative rho (up, down):  0.482E-02 0.000E+00

     add environment contribution to local potential

     total cpu time spent up to now is     1397.9 secs

     total energy              =     -94.77428571 Ry
     Harris-Foulkes estimate   =     -94.77428670 Ry
     estimated scf accuracy    <       0.00001407 Ry

     iteration # 15     ecut=    30.00 Ry     beta=0.40
     CG style diagonalization
     ethr =  5.86E-08,  avg # of iterations =  3.2

     negative rho (up, down):  0.482E-02 0.000E+00

     add environment contribution to local potential

     total cpu time spent up to now is     1492.0 secs

     total energy              =     -94.77428455 Ry
     Harris-Foulkes estimate   =     -94.77428654 Ry
     estimated scf accuracy    <       0.00001239 Ry

     iteration # 16     ecut=    30.00 Ry     beta=0.40
     CG style diagonalization
     ethr =  5.16E-08,  avg # of iterations =  3.3

     negative rho (up, down):  0.483E-02 0.000E+00

     add environment contribution to local potential

     total cpu time spent up to now is     1586.7 secs

     total energy              =     -94.77428730 Ry
     Harris-Foulkes estimate   =     -94.77428631 Ry
     estimated scf accuracy    <       0.00000638 Ry

     iteration # 17     ecut=    30.00 Ry     beta=0.40
     CG style diagonalization
     ethr =  2.66E-08,  avg # of iterations =  3.5

     negative rho (up, down):  0.482E-02 0.000E+00

     add environment contribution to local potential

     total cpu time spent up to now is     1682.8 secs

     total energy              =     -94.77428550 Ry
     Harris-Foulkes estimate   =     -94.77428844 Ry
     estimated scf accuracy    <       0.00000914 Ry

     iteration # 18     ecut=    30.00 Ry     beta=0.40
     CG style diagonalization
     ethr =  2.66E-08,  avg # of iterations =  3.7

     negative rho (up, down):  0.480E-02 0.000E+00

     add environment contribution to local potential

     total cpu time spent up to now is     1778.7 secs

     total energy              =     -94.77428800 Ry
     Harris-Foulkes estimate   =     -94.77428631 Ry
     estimated scf accuracy    <       0.00000292 Ry

     iteration # 19     ecut=    30.00 Ry     beta=0.40
     CG style diagonalization
     ethr =  1.22E-08,  avg # of iterations =  5.1

     negative rho (up, down):  0.477E-02 0.000E+00

     add environment contribution to local potential

     total cpu time spent up to now is     1881.1 secs

     total energy              =     -94.77428948 Ry
     Harris-Foulkes estimate   =     -94.77429044 Ry
     estimated scf accuracy    <       0.00001262 Ry

     iteration # 20     ecut=    30.00 Ry     beta=0.40
     CG style diagonalization
     ethr =  1.22E-08,  avg # of iterations =  3.4

     negative rho (up, down):  0.472E-02 0.000E+00

     add environment contribution to local potential

     total cpu time spent up to now is     1976.8 secs

     total energy              =     -94.77428613 Ry
     Harris-Foulkes estimate   =     -94.77429001 Ry
     estimated scf accuracy    <       0.00000951 Ry

     iteration # 21     ecut=    30.00 Ry     beta=0.40
     CG style diagonalization
     ethr =  1.22E-08,  avg # of iterations =  4.5

     negative rho (up, down):  0.471E-02 0.000E+00

     add environment contribution to local potential

     total cpu time spent up to now is     2077.1 secs

     total energy              =     -94.77428765 Ry
     Harris-Foulkes estimate   =     -94.77428793 Ry
     estimated scf accuracy    <       0.00000106 Ry

     iteration # 22     ecut=    30.00 Ry     beta=0.40
     CG style diagonalization
     ethr =  4.40E-09,  avg # of iterations =  4.4

     negative rho (up, down):  0.470E-02 0.000E+00

     add environment contribution to local potential

     total cpu time spent up to now is     2176.8 secs

     total energy              =     -94.77428822 Ry
     Harris-Foulkes estimate   =     -94.77428837 Ry
     estimated scf accuracy    <       0.00000085 Ry

     iteration # 23     ecut=    30.00 Ry     beta=0.40
     CG style diagonalization
     ethr =  3.53E-09,  avg # of iterations =  3.6

     negative rho (up, down):  0.470E-02 0.000E+00

     add environment contribution to local potential

     total cpu time spent up to now is     2272.5 secs

     total energy              =     -94.77428850 Ry
     Harris-Foulkes estimate   =     -94.77428840 Ry
     estimated scf accuracy    <       0.00000056 Ry

     iteration # 24     ecut=    30.00 Ry     beta=0.40
     CG style diagonalization
     ethr =  2.34E-09,  avg # of iterations =  3.6

     negative rho (up, down):  0.468E-02 0.000E+00

     add environment contribution to local potential

     total cpu time spent up to now is     2367.8 secs

     total energy              =     -94.77428835 Ry
     Harris-Foulkes estimate   =     -94.77428862 Ry
     estimated scf accuracy    <       0.00000074 Ry

     iteration # 25     ecut=    30.00 Ry     beta=0.40
     CG style diagonalization
     ethr =  2.34E-09,  avg # of iterations =  3.2

     negative rho (up, down):  0.466E-02 0.000E+00

     add environment contribution to local potential

     total cpu time spent up to now is     2461.9 secs

     total energy              =     -94.77428832 Ry
     Harris-Foulkes estimate   =     -94.77428840 Ry
     estimated scf accuracy    <       0.00000025 Ry

     iteration # 26     ecut=    30.00 Ry     beta=0.40
     CG style diagonalization
     ethr =  1.04E-09,  avg # of iterations =  5.2

     negative rho (up, down):  0.464E-02 0.000E+00

     add environment contribution to local potential

     total cpu time spent up to now is     2566.3 secs

     total energy              =     -94.77428870 Ry
     Harris-Foulkes estimate   =     -94.77428869 Ry
     estimated scf accuracy    <       0.00000008 Ry

     iteration # 27     ecut=    30.00 Ry     beta=0.40
     CG style diagonalization
     c_bands:  1 eigenvalues not converged
     ethr =  3.22E-10,  avg # of iterations =  6.0

     negative rho (up, down):  0.462E-02 0.000E+00

     add environment contribution to local potential

     total cpu time spent up to now is     2842.4 secs

     total energy              =     -94.77428965 Ry
     Harris-Foulkes estimate   =     -94.77428964 Ry
     estimated scf accuracy    <       0.00000028 Ry

     iteration # 28     ecut=    30.00 Ry     beta=0.40
     CG style diagonalization
     c_bands:  1 eigenvalues not converged
     ethr =  3.22E-10,  avg # of iterations =  5.3

     negative rho (up, down):  0.116E+00 0.000E+00

     total cpu time spent up to now is     2921.7 secs

     total energy              =     -94.78295397 Ry
     Harris-Foulkes estimate   =     -94.77524064 Ry
     estimated scf accuracy    <       1.78307693 Ry

     iteration # 29     ecut=    30.00 Ry     beta=0.40
     CG style diagonalization
     c_bands:  2 eigenvalues not converged
     ethr =  3.22E-10,  avg # of iterations =  8.4

     negative rho (up, down):  0.190E+00 0.000E+00

     total cpu time spent up to now is     3017.1 secs

     total energy              =     -94.79984104 Ry
     Harris-Foulkes estimate   =     -94.79242399 Ry
     estimated scf accuracy    <       1.82610274 Ry

     iteration # 30     ecut=    30.00 Ry     beta=0.40
     CG style diagonalization
     c_bands:  2 eigenvalues not converged
     ethr =  3.22E-10,  avg # of iterations = 10.2

     negative rho (up, down):  0.239E+00 0.000E+00
Ctrl-C caught... cleaning up processes
[press Ctrl-C again to force abort]


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