Coherent multidimensional spectroscopy in polariton systems
arxiv(2024)
Abstract
The fast dynamics of molecular polaritonics is scrutinized theoretically
through the implementation of two-dimensional spectroscopy protocols. We derive
conceptually simple and computationally efficient formulas to calculate
two-dimensional spectra for molecules, each of them modeled as a system of two
electronic states including vibrational relaxation, immersed in an optical
cavity, thus coupled to quantized radiation. Cavity photon losses and molecular
relaxation are incorporated into the Hamiltonian dynamics to form an open
quantum system that is solved through a master equation. In the collective
case, the relaxation dynamics into dark states reveals to be the crucial factor
to explain the asymmetries in both the diagonal and cross peaks of
two-dimensional spectra for long waiting times between excitation and
detection, a feature shown by recent experiments. Our theoretical method
provides a deeper insight in those processes that yield relevant signals in
multidimensional molecular spectroscopy.
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