[QE-users] DOS Calculation for a Molecule of Water

Giuseppe Mattioli giuseppe.mattioli at ism.cnr.it
Fri Dec 7 10:53:46 CET 2018


Dear Dan

When you compare experimental results and DFT-based results you must  
be very careful and you must know very well the limits of theory  
itself and the limits of the specitic exchange-correlation functional  
you apply. In your case:

1) you are comparing Kohn-Sham orbitals, a single-particle auxiliary  
basis having no strict relationship with physical quantities, with an  
intrinsically many-body excitation or ionization process.

2) your PBE functional suffers a strong delocalization error. So even  
if you trust in the assignment of binding energies to Kophn-Sham  
orbitals (which is not entirely correct), you are strongly  
overestimating orbitals energies.

You can recover an acceptable description of small isolated systems  
such as molecules by using, for example, the  CAM-B3LYP functional,  
which is unfortunately not available in plane-wave codes like QE. For  
a decent description you should use a PBE0 or B3LYP functional  
together with the assume_isolated='mt' option which decouples the  
electrostatic interaction of the water dipole with its periodicaly  
repeated images.
HTH
Giuseppe

Dan Gil <dan.gil9973 at gmail.com> ha scritto:

> Hi,
>
> I am trying out a DOS calculation for a molecule of water, however, my
> results are very inaccurate compared to literature (
> http://www1.lsbu.ac.uk/water/water_methods.html). I was wondering if you
> could give me some advice on improving my results. I am expecting states at
> -14, -15, -19, and -37 eV. Instead, I am getting states at -7, -9, -13, and
> -25 eV.
>
> I am first carrying out an SCF calculation of a water molecule (pw.x) and
> then obtaining the density of states (dos.x). The structure of water is
> already relaxed.
>
> The relevant files are contained below.
>
> - - - - - -water.pw.in
> &control
>     calculation='scf',
>     wf_collect = .true. ,
>     outdir = 'water' ,
>     restart_mode = 'from_scratch' ,
>     pseudo_dir = 'pseudo' ,
>     disk_io = 'low' ,
>     verbosity = 'low' ,
>     max_seconds = 68000 ,
>  /
>  &system
>     ibrav = 4,
>     celldm(1)=19.174,
>     celldm(3)=1,
>     nat = 3 ,
>     ntyp = 2 ,
>     ecutwfc = 70.0,
>     ecutrho = 560.0,
>     smearing='gaussian',
>     occupations='fixed',
>  /
>  &electrons
>     diagonalization='david',
>     mixing_mode = 'local-TF',
>  /
>  &ions
>  /
> ATOMIC_SPECIES
> O    15.999   O.pbe-n-rrkjus_psl.1.0.0.UPF
> H    1.00794  H.pbe-rrkjus_psl.1.0.0.UPF
> ATOMIC_POSITIONS crystal
> H        0.003478196   0.090739324   0.224999603
> H        0.090739324   0.003478196   0.224999603
> O        0.105782480   0.105782480   0.225000794
> K_POINTS gamma
> - - - - - -
>
> - - - - - - get.dos.in
>  &dos
>                       outdir = 'water' ,
>                      DeltaE  = .1
>  /
> - - - - - -
>
> - - - - - - pwscf.dos
> #  E (eV)   dos(E)     Int dos(E) EFermi =   0.000 eV
>  -25.473  0.1393E-02  0.1393E-03
>  -25.373  0.2067E+00  0.2081E-01
>  -25.273  0.4151E+01  0.4359E+00
>  -25.173  0.1128E+02  0.1564E+01
>  -25.073  0.4151E+01  0.1979E+01
>  -24.973  0.2067E+00  0.2000E+01
>  -24.873  0.1393E-02  0.2000E+01
>  -24.773  0.1270E-05  0.2000E+01
>  -24.673  0.1567E-09  0.2000E+01
>  -24.573  0.2617E-14  0.2000E+01
>  -24.473  0.5916E-20  0.2000E+01
>  -24.373  0.1810E-26  0.2000E+01
>  -24.273  0.7492E-34  0.2000E+01
>  -24.173  0.4198E-42  0.2000E+01
>  -24.073  0.3183E-51  0.2000E+01
>  -23.973  0.3266E-61  0.2000E+01
>  -23.873  0.4536E-72  0.2000E+01
>  -23.773  0.8994E-84  0.2000E+01
>  -23.673  0.6246E-85  0.2000E+01
>  -23.573  0.6246E-85  0.2000E+01
>  -23.473  0.6246E-85  0.2000E+01
>  -23.373  0.6246E-85  0.2000E+01
>  -23.273  0.6246E-85  0.2000E+01
>  -23.173  0.6246E-85  0.2000E+01
>  -23.073  0.6246E-85  0.2000E+01
>  -22.973  0.6246E-85  0.2000E+01
>  -22.873  0.6246E-85  0.2000E+01
>  -22.773  0.6246E-85  0.2000E+01
>  -22.673  0.6246E-85  0.2000E+01
>  -22.573  0.6246E-85  0.2000E+01
>  -22.473  0.6246E-85  0.2000E+01
>  -22.373  0.6246E-85  0.2000E+01
>  -22.273  0.6246E-85  0.2000E+01
>  -22.173  0.6246E-85  0.2000E+01
>  -22.073  0.6246E-85  0.2000E+01
>  -21.973  0.6246E-85  0.2000E+01
>  -21.873  0.6246E-85  0.2000E+01
>  -21.773  0.6246E-85  0.2000E+01
>  -21.673  0.6246E-85  0.2000E+01
>  -21.573  0.6246E-85  0.2000E+01
>  -21.473  0.6246E-85  0.2000E+01
>  -21.373  0.6246E-85  0.2000E+01
>  -21.273  0.6246E-85  0.2000E+01
>  -21.173  0.6246E-85  0.2000E+01
>  -21.073  0.6246E-85  0.2000E+01
>  -20.973  0.6246E-85  0.2000E+01
>  -20.873  0.6246E-85  0.2000E+01
>  -20.773  0.6246E-85  0.2000E+01
>  -20.673  0.6246E-85  0.2000E+01
>  -20.573  0.6246E-85  0.2000E+01
>  -20.473  0.6246E-85  0.2000E+01
>  -20.373  0.6246E-85  0.2000E+01
>  -20.273  0.6246E-85  0.2000E+01
>  -20.173  0.6246E-85  0.2000E+01
>  -20.073  0.6246E-85  0.2000E+01
>  -19.973  0.6246E-85  0.2000E+01
>  -19.873  0.6246E-85  0.2000E+01
>  -19.773  0.6246E-85  0.2000E+01
>  -19.673  0.6246E-85  0.2000E+01
>  -19.573  0.6246E-85  0.2000E+01
>  -19.473  0.6246E-85  0.2000E+01
>  -19.373  0.6246E-85  0.2000E+01
>  -19.273  0.6246E-85  0.2000E+01
>  -19.173  0.6246E-85  0.2000E+01
>  -19.073  0.6246E-85  0.2000E+01
>  -18.973  0.6246E-85  0.2000E+01
>  -18.873  0.6246E-85  0.2000E+01
>  -18.773  0.6246E-85  0.2000E+01
>  -18.673  0.6246E-85  0.2000E+01
>  -18.573  0.6246E-85  0.2000E+01
>  -18.473  0.6246E-85  0.2000E+01
>  -18.373  0.6246E-85  0.2000E+01
>  -18.273  0.6246E-85  0.2000E+01
>  -18.173  0.6246E-85  0.2000E+01
>  -18.073  0.6246E-85  0.2000E+01
>  -17.973  0.6246E-85  0.2000E+01
>  -17.873  0.6246E-85  0.2000E+01
>  -17.773  0.6246E-85  0.2000E+01
>  -17.673  0.6246E-85  0.2000E+01
>  -17.573  0.6246E-85  0.2000E+01
>  -17.473  0.6246E-85  0.2000E+01
>  -17.373  0.6246E-85  0.2000E+01
>  -17.273  0.6246E-85  0.2000E+01
>  -17.173  0.6246E-85  0.2000E+01
>  -17.073  0.6246E-85  0.2000E+01
>  -16.973  0.6246E-85  0.2000E+01
>  -16.873  0.6246E-85  0.2000E+01
>  -16.773  0.6246E-85  0.2000E+01
>  -16.673  0.6246E-85  0.2000E+01
>  -16.573  0.6246E-85  0.2000E+01
>  -16.473  0.6246E-85  0.2000E+01
>  -16.373  0.6246E-85  0.2000E+01
>  -16.273  0.6246E-85  0.2000E+01
>  -16.173  0.6246E-85  0.2000E+01
>  -16.073  0.6246E-85  0.2000E+01
>  -15.973  0.6246E-85  0.2000E+01
>  -15.873  0.6246E-85  0.2000E+01
>  -15.773  0.6246E-85  0.2000E+01
>  -15.673  0.6246E-85  0.2000E+01
>  -15.573  0.6246E-85  0.2000E+01
>  -15.473  0.6246E-85  0.2000E+01
>  -15.373  0.6246E-85  0.2000E+01
>  -15.273  0.6246E-85  0.2000E+01
>  -15.173  0.6246E-85  0.2000E+01
>  -15.073  0.6246E-85  0.2000E+01
>  -14.973  0.6246E-85  0.2000E+01
>  -14.873  0.6246E-85  0.2000E+01
>  -14.773  0.6246E-85  0.2000E+01
>  -14.673  0.6246E-85  0.2000E+01
>  -14.573  0.6246E-85  0.2000E+01
>  -14.473  0.6246E-85  0.2000E+01
>  -14.373  0.6326E-85  0.2000E+01
>  -14.273  0.1156E-73  0.2000E+01
>  -14.173  0.1102E-62  0.2000E+01
>  -14.073  0.1422E-52  0.2000E+01
>  -13.973  0.2484E-43  0.2000E+01
>  -13.873  0.5870E-35  0.2000E+01
>  -13.773  0.1878E-27  0.2000E+01
>  -13.673  0.8127E-21  0.2000E+01
>  -13.573  0.4761E-15  0.2000E+01
>  -13.473  0.3775E-10  0.2000E+01
>  -13.373  0.4050E-06  0.2000E+01
>  -13.273  0.5881E-03  0.2000E+01
>  -13.173  0.1156E+00  0.2012E+01
>  -13.073  0.3074E+01  0.2319E+01
>  -12.973  0.1106E+02  0.3426E+01
>  -12.873  0.5389E+01  0.3964E+01
>  -12.773  0.3553E+00  0.4000E+01
>  -12.673  0.3170E-02  0.4000E+01
>  -12.573  0.3827E-05  0.4000E+01
>  -12.473  0.6255E-09  0.4000E+01
>  -12.373  0.1383E-13  0.4000E+01
>  -12.273  0.4140E-19  0.4000E+01
>  -12.173  0.1677E-25  0.4000E+01
>  -12.073  0.9192E-33  0.4000E+01
>  -11.973  0.6820E-41  0.4000E+01
>  -11.873  0.6847E-50  0.4000E+01
>  -11.773  0.9304E-60  0.4000E+01
>  -11.673  0.1711E-70  0.4000E+01
>  -11.573  0.4263E-82  0.4000E+01
>  -11.473  0.6246E-85  0.4000E+01
>  -11.373  0.6246E-85  0.4000E+01
>  -11.273  0.6246E-85  0.4000E+01
>  -11.173  0.6246E-85  0.4000E+01
>  -11.073  0.6246E-85  0.4000E+01
>  -10.973  0.6246E-85  0.4000E+01
>  -10.873  0.6246E-85  0.4000E+01
>  -10.773  0.6246E-85  0.4000E+01
>  -10.673  0.6246E-85  0.4000E+01
>  -10.573  0.8307E-84  0.4000E+01
>  -10.473  0.4196E-72  0.4000E+01
>  -10.373  0.3039E-61  0.4000E+01
>  -10.273  0.2979E-51  0.4000E+01
>  -10.173  0.3953E-42  0.4000E+01
>  -10.073  0.7098E-34  0.4000E+01
>   -9.973  0.1725E-26  0.4000E+01
>   -9.873  0.5672E-20  0.4000E+01
>   -9.773  0.2525E-14  0.4000E+01
>   -9.673  0.1521E-09  0.4000E+01
>   -9.573  0.1240E-05  0.4000E+01
>   -9.473  0.1368E-02  0.4000E+01
>   -9.373  0.2042E+00  0.4021E+01
>   -9.273  0.4126E+01  0.4434E+01
>   -9.173  0.1128E+02  0.5562E+01
>   -9.073  0.4176E+01  0.5979E+01
>   -8.973  0.2092E+00  0.6000E+01
>   -8.873  0.1418E-02  0.6001E+01
>   -8.773  0.1301E-05  0.6001E+01
>   -8.673  0.1615E-09  0.6001E+01
>   -8.573  0.2713E-14  0.6001E+01
>   -8.473  0.6170E-20  0.6001E+01
>   -8.373  0.1899E-26  0.6001E+01
>   -8.273  0.7908E-34  0.6001E+01
>   -8.173  0.4457E-42  0.6001E+01
>   -8.073  0.1524E-39  0.6001E+01
>   -7.973  0.1495E-31  0.6001E+01
>   -7.873  0.1985E-24  0.6001E+01
>   -7.773  0.3567E-18  0.6001E+01
>   -7.673  0.8674E-13  0.6001E+01
>   -7.573  0.2855E-08  0.6001E+01
>   -7.473  0.1272E-04  0.6001E+01
>   -7.373  0.7666E-02  0.6001E+01
>   -7.273  0.6254E+00  0.6064E+01
>   -7.173  0.6905E+01  0.6754E+01
>   -7.073  0.1032E+02  0.7786E+01
>   -6.973  0.2086E+01  0.7995E+01
>   -6.873  0.5710E-01  0.8000E+01
> - - - - - -
>
> Best Regards,
>
> Dan Gil
> PhD Candidate
> Department of Chemical and Biomolecular Engineering
> Case Western Reserve University



GIUSEPPE MATTIOLI
CNR - ISTITUTO DI STRUTTURA DELLA MATERIA
Via Salaria Km 29,300 - C.P. 10
I-00015 - Monterotondo Scalo (RM)
Mob (*preferred*) +39 373 7305625
Tel + 39 06 90672342 - Fax +39 06 90672316
E-mail: <giuseppe.mattioli at ism.cnr.it>



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