For the excited state dynamics of a
specific chromophore in a solvent what are the essential degrees of freedom
(electronic, vibrational, and solvent) that must be included in a model
Hamiltonian?
What determines if the excited state
dynamics is classical, semi-classical, or fully quantum? Under what conditions
does the Born-Oppenheimer approximation break down?
For a specific photochemical reaction what
are the relevant vibrational degrees of freedom? What determines the relative
importance of stretching, torsional, and pyramidal vibrations?
What determines the branching ratio for
passage through a conical intersection? Relevant parameters may be the slope at
the intersection, slanting, size of the wavepacket, and the distance of closest
approach (impact parameter)
What is the interplay of the electronic, vibrational
and solvent degrees of freedom in excited state dynamics?
What determines the relative importance of
the viscosity and the polarity of the solvent for the dynamics? What is the
role of the spatial inhomogeneity of the solvent?
In the presence of a solvent what are
respective criteria for the localization/delocalization of electronic and/or
vibrational excitations over different parts of the chromophore?
What are definitive experimental signatures
of delocalization?
What are definitive experimental signatures
of breakdown of the Born-Oppenheimer approximation?
What is the role of the solvent in
non-adiabatic processes?
I look forward to the follow up post: My answers...
ReplyDelete