Energy transfer and interference by collective electromagnetic coupling

TL;DR

This paper investigates how collective electromagnetic coupling influences energy transfer and interference in molecular assemblies near metal interfaces, combining experimental and theoretical approaches to reveal spatial modulation effects.

Contribution

It introduces a simple framework to analyze cooperative optical responses and predicts interference phenomena in excitation energy transfer involving molecular aggregates.

Findings

Spatial modulations of collective decay rates observed experimentally.

Intermolecular correlations cause interference effects.

Predicted similar phenomena in excitation energy transfer.

Abstract

The physics of collective optical response of molecular assemblies, pioneered by Dicke in 1954, has long been at the center of theoretical and experimental scrutiny. The influence of the environment on such phenomena is also of great interest due to various important applications in e.g. energy conversion devices. In this manuscript we demonstrate both experimentally and theoretically the spatial modulations of the collective decay rates of molecules placed in proximity to a metal interface. We show in a very simple framework how the cooperative optical response can be analyzed in terms of intermolecular correlations causing interference between the response of different molecules and the polarization induced on a nearby metallic boundary and predict similar collective interference phenomena in excitation energy transfer between molecular aggregates.