Polariton mediated resonance energy transfer in a fluid

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Abstract

The focus of this work is on a microscopic quantum electrodynamical understanding of cumulative quantum effects in resonance energy transfer occurring in an isotropic and disordered medium. In particular, we consider quantum coherence, defined in terms of interferences between Feynman pathways, and analyze pure-amplitude and phase cross terms that appear in the Fermi golden rule rate equation that results from squaring the matrix element for mediated energy transfer. It is shown that pure-amplitude terms dominate in the near-zone when chromophores are close in proximity to one another (within a few nanometers), and phase cross terms dominate toward the far-zone when phase differences between different Feynman pathways begin to emerge. This can be understood in terms of physical attributes of the mediating photon, whose character becomes more real at long distances, coinciding with vanishing longitudinal components of the field, as transverse components begin to dominate.

Original languageEnglish
Article number034111
JournalThe Journal of Chemical Physics
Volume153
Issue number3
Early online date17 Jul 2020
DOIs
Publication statusPublished - 21 Jul 2020

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