[molpro-user] Mixed derivatives in Numerical Hessian

Werner Győrffy gyorffy at theochem.uni-stuttgart.de
Sat Feb 11 11:06:37 CET 2017


Hi Benj,

Not to the best of my knowledge. Until now I have dealt with 
implementing only gradients for closed-shell systems. However, toward 
that end, a PhD student in our group is currently working on the 
implementation of open-shell LMP2 analytical gradients.

Regards,

Werner.

On 02/10/2017 08:18 PM, Benj FitzPatrick wrote:
> Werner,
> Addressing the edge of curiosity, will open-shell CCSD/CCSD(T) also be
> getting analytic gradients?
> Thanks,
> Benj FitzPatrick
>
> On Tue, Feb 7, 2017 at 5:24 PM, Werner Győrffy
> <gyorffy at theochem.uni-stuttgart.de
> <mailto:gyorffy at theochem.uni-stuttgart.de>> wrote:
>
>     Dear Aleksandr,
>
>     I agree that the thresholds must be made tighter: especially for
>     Hartree-Fock, and also for CP-HF in the case of using analytical
>     gradients. One should be careful not to set the thresholds too
>     tight. For example, the suggested "gthresh,orbital=1.0d-10" is
>     equivalent to "{hf;accu,20;}" which seems to be unnecessary low and
>     might cause convergence problems.
>
>     Yes, MP2 and DF-MP2 Hessians are computed by using analytical first
>     derivatives.
>
>     CCSD(T) analytical gradients have been already implemented in the
>     development version of Molpro. It will be hopefully available soon
>     in the next release.
>
>     Regards,
>
>     Werner.
>
>     On 02/06/2017 07:14 PM, sjk wrote:
>
>         I find that tightening the convergence criterion on various
>         evaluations
>         generally solves the low frequency hessian convergence problems (my
>         experience is that anything below about 200 cm-1 should not be
>         considered reliable with the standard parameters).
>         Thus, I generally insert the following line at the top of my
>         input file
>         gthresh,energy=1.0d-10, orbital=1.0d-10, oneint=1.0d-16,
>         twoint=1.0d-16,
>         optgrad=1.0d-6, compress=1.0d-13
>         Best Regards,
>         Stephen
>         On Feb 6, 2017, at 9:12 AM, Leonid Shirkov
>         <leonid.shirkov at gmail.com <mailto:leonid.shirkov at gmail.com>
>         <mailto:leonid.shirkov at gmail.com
>         <mailto:leonid.shirkov at gmail.com>>> wrote:
>
>             Dear Colleagues,
>
>             in some specific cases, the current accuracy of the
>             numerical hessians
>             is not enough, e.g. for very low frequency torsional
>             vibrations (~50cm-1).
>             The CCSD(T) freq analysis gives imaginary values instead of
>             the real ones
>             for the lowest modes.  The solution is to find manually the
>             hessian in
>             the internal coordinates
>             and then find the eigenvalues of the GF matrix, but that is
>             a lot of work.
>
>             If MP2 is used for such cases, then there are no imaginary
>             frequencies.
>             Do I understand correctly, that for MP2 freq analysis the
>             hessians are
>             found
>             by differentiating the analytical MP2 gradients?
>
>             Using the analytical gradients for highly accurate methods like
>             CCSD(T) would probably resolve the problem,
>             but they are not currently available in Molpro.
>
>             Best regards,
>             Leonid
>
>             On Mon, Feb 6, 2017 at 10:18 AM, Werner Győrffy
>             <gyorffy at theochem.uni-stuttgart.de
>             <mailto:gyorffy at theochem.uni-stuttgart.de>
>             <mailto:gyorffy at theochem.uni-stuttgart.de
>             <mailto:gyorffy at theochem.uni-stuttgart.de>>> wrote:
>
>                 Dear Aleksandr,
>
>                 Numerical Hessians in Molpro are computed by using
>                 central finite
>                 differences with a 2-point formula as a default. That is
>                 a "general
>                 formula". That gives accurate results in most of the
>                 cases. There is a
>                 trade-off between accuracy and efficiency: More accurate
>                 finite field
>                 calculations would increase the number of single point
>                 calculations
>                 significantly. If one needs more accurate Hessians, it
>                 can be done
>                 only by
>                 computing that manually by using procedures.
>
>                 Regards,
>
>                 Werner.
>
>
>                 On 02/04/2017 02:04 AM, Aleksandr Lykhin wrote:
>
>
>                     Does anybody know how Molpro calculates mixed
>                     derivatives using central
>                     differences? It seems like it generates only two
>                     mixed displacements
>                     instead of four, so the general formula cannot be
>                     applied directly.
>
>                     --
>                     Kind regards, Aleksandr O. Lykhin.
>
>
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