A Quantum Electrodynamics Description of Quantum Coherence and Damping in Condensed-Phase Energy Transfer

摘要

Quantum coherence in condensed-phase electronic resonance energy transfer (RET) is described within the context of quantum electrodynamics (QED) theory. Mediating dressed virtual photons (polaritons) are explicitly incorporated into the treatment, and coherence is understood within the context of interfering Feynman pathways connecting the initial and final states for the RET process. The model investigated is that of an oriented three-body donor, acceptor, and mediator RET system embedded within a dispersive and absorbing polarizable medium. We show how quantum coherence can significantly enhance the rate of RET and give a rigorous picture for subsequent decoherence that is driven by both phase and amplitude damping. Energy-conserving phase damping occurs as a result of geometric and dispersive effects and is associated with destructive interference between Feynman pathways. Dissipative amplitude damping, on the other hand, is attributed to vibronic relaxation and absorptivity of the medium and can be understood as virtual photons (polaritons) leaking into the environment. This model offers insights into the emergence of coherence and subsequent decoherence for energy transfer in photosynthetic systems.