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Conference on Lasers and Electro-Optics

Non-Radiative Energy Transfer via Hybrid Light-Matter States

Xiaolan Zhong, Thibault Chervy, Shaojun Wang, Jino George, Anoop Thomas, James Andell Hutchison, Éloïse Devaux, Cyriaque Genet, Thomas W. Ebbesen

Published Jan 1, 2016• 1 citation
Publisher

Abstract

Direct evidence of enhanced non-radiative energy transfer between two molecules strongly coupled to the cavity vacuum field form light-matter hybrid states. Excitation spectroscopy and femtosecond pump-probe measurements show that the energy transfer is highly efficient.
DOI
10.1364/cleo_si.2016.sth4q.5

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Nonlinear spectroscopy is widely used to study the transient dynamics of molecules under strong light-matter coupling, though it remains unclear to what extent uncoupled intracavity molecules obscure signals from the strongly-coupled species of interest. Pump or probe fields resonant in the strongly-coupled spectral region will preferentially interact with cavity-coupled molecules, but can exhibit severe optical artifacts due to wave interference in the cavity. On the other hand, non-resonant pump or probe fields having wavelengths at which the cavity mirrors are highly transmissive propagate as traveling waves along the cavity axis, interacting with both coupled and uncoupled intracavity molecules. Here, we quantify the contributions of signals from strongly-coupled and uncoupled populations in simulated experiments with different resonant and non-resonant pump-probe configurations. We find that while resonant schemes maximize selectivity for the signals of strongly-coupled molecules, non-resonant schemes retain surprisingly high sensitivity to these signals while remaining less susceptible to optical artifacts.
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An empirical framework for studying the way vacuum fluctuations in a Fabry–Perot cavity produce collective light–matter hybrid states (polariton states) is reported. The reason that the Tavis–Cummings model, where a single mode of the radiation field couples to all the molecules, succeeds is discussed in terms of the strong phase correlation of the vacuum fluctuations in the cavity, which produces a single effective cavity mode (ECM). The model is used to study the onset of the collective state, or “superradiant phase”, for ensembles of molecules with significant disorder in their transition energies, as a function of cavity strength factor, from low Q cavities to high Q cavities. A key result is the quantification of the coherence of the ensemble of the lowest energy eigenstate. This is assessed, primarily, using an entropy distance measure. The statistical model provides a physical intuition for the formation of coherence of polariton states when the collective coupling is strong enough that they dominate over the tail of the dark-state density-of-states.