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Chemical Physics

Effects of bath-induced vibrational transitions on time-resolved resonant light scattering from molecules in condensed phases

Yukiyoshi Ohtsuki, Yuichi Fujimura

Published Jun 1, 1989• 3 citations
Publisher
DOI
10.1016/0301-0104(89)80241-1

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Bath-induced coherence transfer effects on a time- and frequency-resolved resonant light scattering spectrum is theoretically investigated using the Markoff master equation. According to Eberly and Wódkiewicz, a general expression for an experimentally observable spectrum in terms of a molecular response function is derived within the density matrix formalism. To generalize our previous results of the bath-induced coherence transfer which were derived based on a displaced harmonic oscillator model [Y. Ohtsuki and Y. Fujimura, J. Chem. Phys. 91, 3903 (1989)], an eigenstate basis is used to represent a relevant system for investigating characteristics of the transfer. By the present model, we clarify the dependence of the bath-induced coherence transfer on the energy-level structure of the intermediate states associated with the transfer, i.e., energy mismatch effects. It is shown that if the energy mismatch of these states is smaller than dephasing rates, the bath-induced coherence transfer occurs resonantly. In the other cases, the energy mismatch brings about a modulation in the time evolution of the superposition state created by the bath-induced coherence transfer, which strongly diminishes the efficiency of the transfer. The resonance condition is derived analytically and is confirmed by numerical calculations of quantum beats induced by the bath-induced coherence transfer. The possibility of very rapid dephasing of a quantum beat signal which cannot be explained in terms of dephasing rates is also shown, when the transition moments have such values that give π-phase-shifted quantum beats in bath-induced fluorescence.
We consider light scattering from a multilevel system (e.g., a molecule) interacting with several heat baths. The Liouville space approach is employed and weak incident radiation intensity is assumed, whereas the light scattering process is described in the lowest appropriate order in the interaction between the molecule and the incident and emitted photons. The interaction with other radiation field modes as well as with the thermal baths is treated more fully, such as to account for the correct damping terms and their temperature dependence. The formalism is suited for light scattering from an impurity molecule in both gas and dense phases. The thermal baths induce relaxation within the manifold of excited states as well as transitions to nonradiative channels. Damping due to such transitions (as well as radiative damping) corresponds to interactions with zero temperature baths. The physical interpretation of such a bath depends on the nature of the particular damping process. Thermal relaxation within the excited manifold is induced by interaction with the environment represented by a bath of temperature T. Part of this interaction which is diagonal in the molecular space corresponds to the so-called ’’quasielastic collisions’’ and induces modulations of the molecular energy levels and broadening of the relaxed emission. The remainder, nondiagonal part induces actual transitions between the excited molecular energy levels. The formalism yields in a single calculation expressions for the cross section for both the coherent (Raman) scattering process and the relaxed luminescence and enables us to discuss the effects of different factors such as temperature and quenching processes on the relative yields for these processes. The formalism also allows for interference between different levels of the excited manifold due to coupling of several levels to the same bath, and makes it possible to study the effect of thermal relaxation on these interference phenomena.
We study the frequency-resolved density response of a photon Bose-Einstein condensate coupled to a bath of dye molecules by time-periodic driving. By monitoring the photon number dynamics for different drive frequencies, we obtain the spectral response of the condensate in a phase-sensitive way. We find that as the photon number increases, the response of the coupled condensate-bath system transitions from overdamped to resonant behavior, indicating a transition from closed to open system dynamics. Our spectroscopy method paves the way for studies of collective excitations in complex driven-dissipative systems.