Why are the IR-Active Frequencies Wrong in MOLPRO 2000.1?

Jun Li junli at chemistry.ohio-state.edu
Thu Dec 21 14:47:34 GMT 2000


Dear MOLPRO experts,

I am using MOLPRO 2000.1.  As a test of frequency calculations of
heavy-element systems, I tried to repeat the frequency calculation of UF6
published in J. Chem. Phys. 1998, 109, 3875-3881 (Hay & Martin).  While I
can get the same optimized structure and RHF energy as the literature data,
the calculated frequencies for the IR-active modes are all wrong, but those
for the Raman and other modes are actually the same as in the literature.
I also have this problem for some other molecules.

I am attaching here the input file and some simple output of UF6.  I would
appreciate it very much if any of you could let me know whether this is a
bug of the code or my input file is actually wrong?  Thanks.

Merry Christmas to all,


Jun Li

--------input file-----------------
***, MOLPRO 2000.02 Calculations of UF6
memory 50, m
geomtyp=xyz
geometry={
7  ! Number of Atoms
example of cartesian XYZ coordinate input for MOLPRO
U     0.0   0.0   0.0
F     1.99  0.0   0.0
F    -1.99  0.0   0.0
F     0.0   1.99  0.0
F     0.0  -1.99  0.0
F     0.0   0.0   1.99
F     0.0   0.0  -1.99
}

basis={
! URANIUM LANL2DZ (6S,5P,2D,2F) -> [3S,3P,2D,2F]
s,U,  0.244400000E+01,0.143300000E+01,0.667700000E+00,0.255600000E+00,

0.244400000E+01,0.143300000E+01,0.667700000E+00,0.255600000E+00,0.120000000E
+00,0.400000000E-01
c,1.4,   0.280278000E+00,-0.132311000E+01, 0.139499900E+01, 0.453123000E+00
c,5.9,  -0.837540000E-01,
0.608236000E+00,-0.818433000E+00,-0.905753000E+00, 0.123402000E+01
c,10.10, 0.100000000E+01
p,U,  0.113800000E+01,0.687400000E+00,0.250600000E+00,

0.113800000E+01,0.687400000E+00,0.250600000E+00,0.120000000E+00,0.400000000E-01
c,1.3,  -0.558150000E+00, 0.970172000E+00, 0.541903000E+00
c,4.7,   0.225763000E+00,-0.420469000E+00,-0.545903000E+00, 0.742936000E+00
c,8.8,   0.100000000E+01
d,U ,0.382600000E+00,0.147300000E+00
c,1.1, 0.100000000E+01
c,2.2, 0.100000000E+01
f,U ,0.411300000E+01,0.169700000E+01,0.677400000E+00,0.251000000E+00
c,1.2, 0.218993000E+00, 0.459539000E+00
c,3.4, 0.421699000E+00, 0.179066000E+00

! LANL2DZ  Effective Core Potentials
ECP,u ,78,4;
7; ! g potential
0, 4.51627250,-.22527100;
1, 368.687695,-53.780570;
2, 112.757671,-516.30521;
2, 30.2032915,-202.67382;
2, 10.2978355,-62.564405;
2, 3.49105150,-21.558956;
2, 1.26683910,-1.5390545;
8; ! s-g potential
0, 257.352944,2.61188160;
1, 83.1605428,81.2356657;
2, 29.7200513,353.246536;
2, 6.24821320,311.929223;
2, 4.16346720,-423.55258;
2, 3.00015110,293.216084;
2, 1.56000000,-21.344255;
2,0.870000000,1.66925480;
8; ! p-g potential
0, 288.729825,1.84143880;
1, 76.7838420,75.7054755;
2, 24.8252003,288.460167;
2, 5.12487350,250.728943;
2, 3.76033000,-318.89681;
2, 2.97617060,160.084492;
2, 1.99190170,33.7801891;
2,0.973883200,-2.0699997;
6; ! d-g potential
0, 350.469941,2.90820640;
1, 166.709130,74.3577628;
2, 85.8206119,587.114033;
2, 26.9842255,317.254368;
2, 7.15655920,102.842212;
2, 1.28408550,22.4214278;
7; ! f-g potential
0, 251.267075,3.93503390;
1, 108.010922,64.9434120;
2, 114.802189,265.180478;
2, 39.9112545,389.428409;
2, 11.9039784,153.476722;
2, 3.38507720,12.0807444;
2, 1.26776070,-1.3510138;

spd, F, 6-31g*; c
}

gprint, basis, orbitals
rhf                     
print 3, 0

optg;

frequencies;
thermo  sym=Oh;
print thermo;
---

--------output-----------------

                                   1           2           3           4
       5
 Wavenumbers [cm-1]          217.27      217.27      217.27      260.70
 260.70
 Intensities [km/mol]           .00         .00         .00       26.08
  26.08
 Intensities [relative]         .00         .00         .00        2.82
   2.82
                                   6           7           8           9
      10
 Wavenumbers [cm-1]          260.70      582.65      582.65      760.67
1043.98
 Intensities [km/mol]         26.08         .00         .00         .00
 926.07
 Intensities [relative]        2.82         .00         .00         .00
 100.00
                                  11          12
 Wavenumbers [cm-1]         1043.98     1043.98
 Intensities [km/mol]        926.07      926.07
 Intensities [relative]      100.00      100.00
 
Normal Modes of imaginary frequencies
                                   1           2           3
 Wavenumbers [cm-1]            2.61        2.34        2.05
 Intensities [km/mol]           .00         .00         .00
 Intensities [relative]         .00         .00         .00

Normal Modes of low/zero frequencies
                                   1           2           3           4
       5
 Wavenumbers [cm-1]           22.91       22.91       22.91      157.49
 157.49
 Intensities [km/mol]           .00         .00         .00         .00
    .00
 Intensities [relative]         .00         .00         .00         .00
    .00
                                   6
 Wavenumbers [cm-1]          157.49
 Intensities [km/mol]           .00
 Intensities [relative]         .00



The published Gaussian results are: 157(t2u), 216(t2g), 209(t1u), 702(t1u),
582(eg), 761(a1g), where the T1u modes are IR-active.  The MOLPRO IR
freqeuncies listed above are 261 and 1043 cm-1 (comparing with 209 and 702
cm-1)!
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