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General remarks
- The phrase non-local in the discussion of density
functionals does not mean that non-local potentials are involved.
The
potentials are perfectly local, but when you go beyond LDA and include gradient
corrections,
the value of the density functional potential in a point r is
evaluated not only from the local value
of the charge density, but also from
the gradient of the charge density.
- The Stoll formula is considered to be a correlation correction to the Local Density Approximation.
It is conceptually not
correct to use the Stoll correction and apply non-local gradient (GGA)
corrections to the correlation.
It is the user's responsibility, in general
and also here, to avoid using options that are not solidly justified
theoretically.
- It is questionable to apply gradient corrections to the
correlation, while not doing so at the
same time for the exchange.
Therefore the program will check this and stop with an error message.
This check can be overruled with the key allow.
- The issue of the 'best' density functional is a subject
of extensive and widespread research.
It is generally recognized that applying
gradient corrections to the simplest Local Density Approximation
usually
gives better results for comparison with experimental data, especially
as regards bond energies
and the spectra computed from one-electron energies.
- The incorporation of gradient corrections during
the SCF significantly increases the computing effort.
In this
respect it makes no difference which specific GGA formula is applied.
The Energy (PostSCF) feature is therefore an
alternative worthwhile considering:
it saves a lot of time and the effects of
this approximation are often small as regards the SCF solution,
so the
non-self-consistent aspect hardly shows up in the computed bond energy.
In Geometry
Optimizations, however, the Post-SCF option implies that the
energy gradients are computed from
the LDA energy expression and hence the
resulting optimized geometry corresponds to the LDA functional.
In such a
case, including the GGA term may make a substantial difference to the computed
equilibrium geometry.
    
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