Vibrational response functions for multidimensional electronic
spectroscopy in the adiabatic regime: a coherent-state approach
- URL: http://arxiv.org/abs/2204.01415v4
- Date: Mon, 25 Jul 2022 07:44:08 GMT
- Title: Vibrational response functions for multidimensional electronic
spectroscopy in the adiabatic regime: a coherent-state approach
- Authors: Frank Ernesto Quintela Rodriguez and Filippo Troiani
- Abstract summary: We present a coherent state representation of the vibronic dynamics and of the resulting response functions.
Results are generalized to the case of M-th order response functions, with arbitrary M.
Non-Hermitian Hamiltonian approach is used to include in the above expressions the effect of vibrational relaxation.
- Score: 0.0
- License: http://arxiv.org/licenses/nonexclusive-distrib/1.0/
- Abstract: Multi-dimensional spectroscopy represents a particularly insightful tool for
investigating the interplay of nuclear and electronic dynamics, which plays an
important role in a number of photophysical processes and photochemical
reactions. Here we present a coherent state representation of the vibronic
dynamics and of the resulting response functions for the widely used linearly
displaced oscillator model. Analytical expressions are initially derived for
the case of third-order response functions in an N-level system, with ground
state initialization of the oscillator (zero-temperature limit). The results
are then generalized to the case of M-th order response functions, with
arbitrary M. The formal derivation is translated into a simple recipe, whereby
the explicit analytical expressions of the response functions can be derived
directly from the Feynman diagrams. We further generalize to the whole set of
initial coherent states, which form an overcomplete basis. This allows one in
principle to derive the dependence of the response functions on arbitrary
initial states of the vibrational modes and is here applied to the case of
thermal states. Finally, a non-Hermitian Hamiltonian approach is used to
include in the above expressions the effect of vibrational relaxation.
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