[molpro-user] Bug in spin-orbit calculation

ZOUWL qcband at gmail.com
Mon Nov 30 16:11:16 CET 2015


Thanks, Alexander. I tried your method, but the results are exactly the
same.

By the way, I found a typo in my first input: hlsmat,ecpls should be
hlsmat,ecp. But it doesn't change the results.

Wenli

On Sat, Nov 28, 2015 at 5:34 PM, Alexander Mitrushchenkov <
Alexander.Mitrushchenkov at u-pem.fr> wrote:

> Hi,
>
> The error seem to be numerical, probably due to small symmetry problem in
> orbitals/integrals; but might be a bug as well. Before looking in detail,
> could you please try the same calculation with much tighter thresholds for
> integrals, orbitals, and CI coefficients?
>
> Best,
>
> Alexander
>
>
> Le 26/11/2015 02:49, ZOUWL a écrit :
>
> Dear developers,
>
> There may be a bug in the following spin-orbit calculation. The low-lying
> 1D, 3P, 3F, and 5F states of Ta+ are calculated at the CASSCF(4,6) level,
> where the 5d6s orbitals are active. Group symmery used here is Ci, but the
> results and errors are the same if D2h is used. All the calculations are
> performed using the 2010 version. Input:
>
> ***,Ta+, SOC with ECP
> memory,100,m
>
> symmetry,xyz
>
> geometry={Ta}
>
> basis=vtz-pp
>
> {multi;natorb,ci;
> frozen,0;closed,1,3;occ,7,3;
> wf,12,1,0;state,5;   ! 1D
> wf,12,1,2;state,10;  ! 3P, 3F
> wf,12,1,4;state,7;   ! 5F
> }
>
> {ci;noexc;wf,12,1,0;state,5;
> save,4201.3;}
> {ci;noexc;wf,12,1,2;state,10;
> save,4221.3;}
> {ci;noexc;wf,12,1,4;state,7;
> save,4241.3;}
>
> ! SOC: singlet and triplet states
> {ci;hlsmat,ecpls,4201.3,4221.3;}
> ! SOC: triplet and quintet states
> {ci;hlsmat,ecpls,4221.3,4241.3;}
> ! SOC: singlet and quintet states
> {ci;hlsmat,ecpls,4201.3,4241.3;}
> ---
>
> The CASSCF energies of L-S states are degenerate (normal):
> 1D: -56.47502225 (x 5)
> 3P: -56.49919112 (x 3)
> 3F: -56.48533379 (x 7)
> 5F: -56.52492675 (x 7)
>
> In the first (singlet + triplet) and the third (singlet + quintet) SOC
> calculations, the energies of atomic J terms are degenerate (normal):
>
>    Nr  Sym         E             E-E0         E-E0           E-E(1)
>  E-E(1)      E-E(1)
>                  (au)            (au)        (cm-1)           (au)
> (cm-1)        (eV)
>    1   1    -56.51000193     -0.01081081    -2372.70      0.00000000
>  0.00      0.0000
>    2   1    -56.50459652     -0.00540540    -1186.35      0.00540540
> 1186.35      0.1471
>    3   1    -56.50459652     -0.00540540    -1186.35      0.00540540
> 1186.35      0.1471
>    4   1    -56.50459652     -0.00540540    -1186.35      0.00540540
> 1186.35      0.1471
>    5   1    -56.50158234     -0.00239123     -524.81      0.00841958
> 1847.88      0.2291
>    6   1    -56.50158234     -0.00239123     -524.81      0.00841958
> 1847.88      0.2291
>    7   1    -56.50158234     -0.00239123     -524.81      0.00841958
> 1847.88      0.2291
>    8   1    -56.50158234     -0.00239123     -524.81      0.00841958
> 1847.88      0.2291
>    9   1    -56.50158234     -0.00239123     -524.81      0.00841958
> 1847.88      0.2291
>   10   1    -56.49671921      0.00247191      542.52      0.01328272
> 2915.22      0.3614
>   11   1    -56.49671921      0.00247191      542.52      0.01328272
> 2915.22      0.3614
>   12   1    -56.49671921      0.00247191      542.52      0.01328272
> 2915.22      0.3614
>   13   1    -56.49671921      0.00247191      542.52      0.01328272
> 2915.22      0.3614
>   14   1    -56.49671921      0.00247191      542.52      0.01328272
> 2915.22      0.3614
> ...
>    Nr         E             E-E0         E-E0           E-E(1)      E-E(1)
>      E-E(1)
>             (au)            (au)        (cm-1)           (au)       (cm-1)
>        (eV)
>    1   -56.54141852    -0.01649177    -3619.53      0.00000000        0.00
>      0.0000
>    2   -56.54141852    -0.01649177    -3619.53      0.00000000        0.00
>      0.0000
>    3   -56.54141852    -0.01649177    -3619.53      0.00000000        0.00
>      0.0000
>    4   -56.53729558    -0.01236883    -2714.64      0.00412294      904.88
>      0.1122
>    5   -56.53729558    -0.01236883    -2714.64      0.00412294      904.88
>      0.1122
>    6   -56.53729558    -0.01236883    -2714.64      0.00412294      904.88
>      0.1122
>    7   -56.53729558    -0.01236883    -2714.64      0.00412294      904.88
>      0.1122
>    8   -56.53729558    -0.01236883    -2714.64      0.00412294      904.88
>      0.1122
>    9   -56.53111117    -0.00618441    -1357.32      0.01030736     2262.20
>      0.2805
>   10   -56.53111117    -0.00618441    -1357.32      0.01030736     2262.20
>      0.2805
>   11   -56.53111117    -0.00618441    -1357.32      0.01030736     2262.20
>      0.2805
>   12   -56.53111117    -0.00618441    -1357.32      0.01030736     2262.20
>      0.2805
>   13   -56.53111117    -0.00618441    -1357.32      0.01030736     2262.20
>      0.2805
>   14   -56.53111117    -0.00618441    -1357.32      0.01030736     2262.20
>      0.2805
>   15   -56.53111117    -0.00618441    -1357.32      0.01030736     2262.20
>      0.2805
> ...
>
> However, in the second SOC calculation (triplet + quintet), spherical
> degeneracy (degeneracy = J * 2 + 1) is broken because of unknown reasons:
>
>    Nr         E             E-E0         E-E0           E-E(1)      E-E(1)
>      E-E(1)
>             (au)            (au)        (cm-1)           (au)       (cm-1)
>        (eV)
>    1   -56.54145102    -0.01652427    -3626.66      0.00000000        0.00
>      0.0000
>    2   -56.54145075    -0.01652400    -3626.60      0.00000027        0.06
>      0.0000
>    3   -56.54144331    -0.01651655    -3624.96      0.00000771        1.69
>      0.0002
>    4   -56.53734340    -0.01241665    -2725.14      0.00410762      901.52
>      0.1118
>    5   -56.53734093    -0.01241418    -2724.60      0.00411009      902.06
>      0.1118
>    6   -56.53731961    -0.01239286    -2719.92      0.00413141      906.74
>      0.1124
>    7   -56.53730864    -0.01238189    -2717.51      0.00414238      909.15
>      0.1127
>    8   -56.53730809    -0.01238134    -2717.39      0.00414293      909.27
>      0.1127
>    9   -56.53118445    -0.00625770    -1373.41      0.01026657     2253.25
>      0.2794
>   10   -56.53117231    -0.00624555    -1370.74      0.01027871     2255.92
>      0.2797
>   11   -56.53116127    -0.00623451    -1368.32      0.01028975     2258.34
>      0.2800
>   12   -56.53114109    -0.00621434    -1363.89      0.01030993     2262.77
>      0.2805
>   13   -56.53113027    -0.00620352    -1361.52      0.01032075     2265.14
>      0.2808
>   14   -56.53112879    -0.00620203    -1361.19      0.01032223     2265.47
>      0.2809
>   15   -56.53112337    -0.00619661    -1360.00      0.01032765     2266.66
>      0.2810
> ...
>
> There is no such a problem in the following all-electron calculation, so
> the error may be related to the ECPLS option.
>
> ***,Ta+, SOC with A.E.
> memory,100,m
>
> symmetry,xyz
>
> geometry={Ta}
>
> basis=vtz-dk
>
> set dkroll=1
>
> {hf;occ,21,19;wf,80,1,0}
>
> {multi;natorb,ci;
> ! 4f5s5p are inactive
> frozen,14,9;closed,15,19;occ,21,19;
> wf,72,1,0;state,5;   ! 1D
> wf,72,1,2;state,10;  ! 3P, 3F
> wf,72,1,4;state,7;   ! 5F
> }
>
> {ci;noexc;wf,72,1,0;state,5;
> save,4201.3;}
> {ci;noexc;wf,72,1,2;state,10;
> save,4221.3;}
> {ci;noexc;wf,72,1,4;state,7;
> save,4241.3;}
>
> lsint
> {ci;hlsmat,ls,4201.3,4221.3;}
> {ci;hlsmat,ls,4221.3,4241.3;}
> {ci;hlsmat,ls,4201.3,4241.3;}
> ---
>
> Best wishes,
> Wenli
>
>
>
> _______________________________________________
> Molpro-user mailing listMolpro-user at molpro.nethttp://www.molpro.net/mailman/listinfo/molpro-user
>
>
>
> --
> Dr. Alexander Mitrushchenkov, IGR
> Laboratoire de Modélisation et Simulation Multi Echelle
> UMR 8208 CNRS
> Université Paris-Est Marne-la-Vallée
> 5 Bd Descartes
> 77454 Marne la Vallée, Cedex 2, France
>
> Phone:    +33(0)160957316
> Fax:      +33(0)160957320
> e-mail:   Alexander.Mitrushchenkov at u-pem.fr
>
>
-------------- next part --------------
An HTML attachment was scrubbed...
URL: <http://www.molpro.net/pipermail/molpro-user/attachments/20151130/22b24367/attachment.html>


More information about the Molpro-user mailing list