Generalized master equation for modular exciton density transfer

Abstract

A generalized master equation (GME) governing quantum evolution of modular exciton density (MED) is derived for large scale light harvesting systems composed of weakly interacting modules of multiple chromophores. The GME-MED offers a practical framework to incorporate real time coherent quantum dynamics calculations at small length scales into dynamics over large length scales, without assumptions of time scale separation or specific forms of intra-module quantum dynamics. A test of the GME-MED for four sites of the Fenna-Matthews-Olson complex demonstrates how coherent dynamics of excitonic populations over many coupled chromophores can be accurately described by transitions between subgroups (modules) of delocalized excitons.