Generalized master equation for modular exciton density transfer

TL;DR

This paper introduces a generalized master equation for modeling quantum exciton transfer in large modular light-harvesting systems, enabling scalable simulations that incorporate detailed quantum dynamics without simplifying assumptions.

Contribution

The paper develops a novel generalized master equation framework that bridges small-scale quantum calculations with large-scale exciton transfer modeling in complex systems.

Findings

Accurately describes exciton population dynamics across multiple chromophore modules.

Demonstrates effectiveness on Fenna-Matthews-Olson complex data.

Provides a scalable approach for quantum dynamics in large systems.

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.