[QE-users] Questions related to vibrational analysis (for both molecule and adsorbate)--update

Shen, Ziheng zshen83 at gatech.edu
Fri Mar 13 04:22:07 CET 2020


Dear QE users,

Greetings! Last week I posted a problem related to vibration analysis (https://www.mail-archive.com/users@lists.quantum-espresso.org/msg37294.html), unfortunately I didn’t get responses. In the past week I did several trials and got some new results. But I still cannot completely figure out my confusions. I would really appreciate it if some one could give me some advice and instructions.

Basically my question is:
1) When doing frequency analysis for molecules, I expected to get zero or extremely small value for the first six frequencies (i.e. translational & rotational modes). According to suggestions from those previously posted problems, I tried to apply more restrict convergence thresholds and ASR. It seems that ASR help a lot to reduce the number. But I still got frequencies at ~50 level. Is it possible to completely remove those small values? Or are those values small enough to be neglected?
Following are the I/O file of ph.x:
=======================================phonon input=======================================
phonons of CH4
 &inputph
 tr2_ph=1.0d-16,
 prefix='ch4_cell2',
 amass(1)=12.011,
 amass(2)=1.0,
 alpha_mix(1)=0.1,
 asr=.true.
 outdir='./ts/tmp/',
 fildyn='CH4_cell3.dynG'
 /
 0.0 0.0 0.0

The calculated frequencies are:
=======================================phonon output=======================================
 freq (    1) = -0.507756 [THz] =     -16.936932 [cm-1]
     freq (    2) = -0.459728 [THz] =     -15.334860 [cm-1]
     freq (    3) = -0.271000 [THz] = -9.039597 [cm-1]
     freq (    4) =   1.535467 [THz] = 51.217660 [cm-1]
     freq (    5) =   1.705940 [THz] = 56.904033 [cm-1]
     freq (    6) =   1.741249 [THz] = 58.081818 [cm-1]
     freq (    7) = 38.593830 [THz] =    1287.351595 [cm-1]
     freq (    8) = 38.610060 [THz] =    1287.892987 [cm-1]
     freq (    9) = 38.618418 [THz] =    1288.171751 [cm-1]
     freq (   10) = 45.381162 [THz] =    1513.752629 [cm-1]
     freq (   11) = 45.388200 [THz] =    1513.987398 [cm-1]
     freq (   12) = 89.406470 [THz] =    2982.278836 [cm-1]
     freq (   13) = 92.546906 [THz] =    3087.032485 [cm-1]
     freq (   14) = 92.772395 [THz] =    3094.554013 [cm-1]
     freq (   15) = 92.773975 [THz] =    3094.606712 [cm-1]


2) My ultimate goal is to perform frequency analysis for adsorbate so that I can both determine transition state structures and apply ZPE corrections. I tried to use “nat_todo” to fix the surface atoms and only did calculation for adsorbate (CH in my case). I got crazy result (~10000 cm-1) when using large tr2_ph, and got improved results when I decrease the threshold. But I still got fairly large translational & rotational frequencies like below:

  freq (    1) =     -25.618746 [THz] =    -854.549399 [cm-1]
     freq (    2) =      -7.333895 [THz] =    -244.632409 [cm-1]
     freq (    3) =      -6.696884 [THz] =    -223.383991 [cm-1]
     freq (    4) =      -6.248674 [THz] =    -208.433322 [cm-1]
     freq (    5) =      -4.947831 [THz] =    -165.041892 [cm-1]
     freq (    6) =      -2.014699 [THz] =     -67.203109 [cm-1]
     freq (   37) =       0.571458 [THz] =      19.061786 [cm-1]
     freq (   38) =       5.754719 [THz] =     191.956759 [cm-1]
     freq (   39) =      16.488930 [THz] =     550.011494 [cm-1]
     freq (   40) =      16.563150 [THz] =     552.487199 [cm-1]
     freq (   41) =      18.255969 [THz] =     608.953585 [cm-1]
     freq (   42) =      56.121326 [THz] =    1872.005923 [cm-1]

What does negative translational frequencies indicate, is it possible to eliminate these imaginary numbers (like using more restrict threshold)?
And does my result indicate that my structure is most probably not a transition state since all the other frequencies are positive?

I’m attaching the input file of pw.x &ph.x below:
=========================scf input, structure obtained from neb.x========================
&CONTROL
  Calculation='scf',
  restart_mode='from_scratch',
  prefix         = "Ni_ch_ts"
  outdir         = "./ts/tmp",
  pseudo_dir     = "./pseudo",
  tstress        = .true.
  verbosity      = 'high'
  tefield      = .true.
  dipfield     = .true.
/
&SYSTEM
  ibrav                  = 0,
  nat                    = 14,
  ntyp                   = 3,
  ecutwfc                = 65,
  ecutrho                = 650,
  Occupations='smearing',
  smearing='mp',
  degauss=0.01,
  nspin=2,
  starting_magnetization(1)=0.2,
  eamp        = 0.0
  edir        = 3
  emaxpos     = 0.95
  eopreg      = 0.05
/
&ELECTRONS
  electron_maxstep=250,
  conv_thr    = 1.D-10,
  mixing_beta = 0.1,
/

ATOMIC_SPECIES
Ni 58.69 ni_pbe_v1.4.uspp.F.UPF
C  12    C.pbe-n-kjpaw_psl.1.0.0.UPF
H  1     H.pbe-kjpaw_psl.1.0.0.UPF
CELL_PARAMETERS { angstrom }

        4.9667177200         0.0000000000         0.0000000000
        2.4833588600         4.3013037190         0.0000000000
        0.0000000000         0.0000000000         20.000000000

ATOMIC_POSITIONS { angstrom }
Ni    0.0000000000    0.0000000000    7.9723500000
Ni    1.2416800000    2.1506500000    7.9723500000
Ni    2.4833600000    0.0000000000    7.9723500000
Ni    3.7250400000    2.1506500000    7.9723500000
Ni    2.4833600000    1.4337700000   10.0000000000
Ni    3.7250400000    3.5844200000   10.0000000000
Ni    4.9667200000    1.4337700000   10.0000000000
Ni    6.2084000000    3.5844200000   10.0000000000
Ni    1.2281125212    0.7413038538   12.1124602290
Ni    2.4833613443    2.9495126082   12.0722664849
Ni    3.7386101535    0.7413040204   12.1124604793
Ni    4.9667205066    2.8946406480   11.9560276983
 C    2.4833610952    1.4972020489   13.1166864267
 H    2.4833559794    3.1940064219   13.5465576823

K_POINTS { automatic }
6 6 1 0 0 0

=======================================ph.x input=======================================
phonons of CH on metal Ni at Gamma
 &inputph
 tr2_ph=1.0d-16,
 prefix='Ni_ch_ts',
 epsil=.false.,
 amass(1)=58.69,
 amass(2)=12.011,
 amass(3)=1.0,
 alpha_mix(1)=0.1,
 outdir='./tmp/',
 fildyn='CH.dynG',
 nat_todo= 2,
 /
 0.0 0.0 0.0
 13 14


Thanks in advance for anyone that could give suggestions to me!

Best regards
Ziheng Shen
PhD student @ Georgia Institute of Technology
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