Efficient estimation of energy transfer efficiency in light-harvesting complexes

TL;DR

This paper develops and validates an efficient method based on the TC2 master equation to accurately estimate energy transfer efficiency in light-harvesting complexes, especially under non-Markovian conditions.

Contribution

It derives a non-perturbative TC2 equation and provides a constructive error analysis to reliably simulate exciton dynamics in biological environments.

Findings

TC2 equation performs well in weak and intermediate regimes

Energy transfer efficiency is optimal and robust in FMO complex

Method enables efficient simulation of complex biological energy transfer

Abstract

The fundamental physical mechanisms of energy transfer in photosynthetic complexes is not yet fully understood. In particular, the degree of efficiency or sensitivity of these systems for energy transfer is not known given their non-perturbative and non-Markovian interactions with proteins backbone and surrounding photonic and phononic environments. One major problem in studying light-harvesting complexes has been the lack of an efficient method for simulation of their dynamics in biological environments. To this end, here we revisit the second-order time-convolution (TC2) master equation and examine its reliability beyond extreme Markovian and perturbative limits. In particular, we present a derivation of TC2 without making the usual weak system-bath coupling assumption. Using this equation, we explore the long time behaviour of exciton dynamics of Fenna-Matthews-Olson (FMO) protein complex. Moreover, we introduce a constructive error analysis to estimate the accuracy of TC2 equation in calculating energy transfer efficiency, exhibiting reliable performance for environments with weak and intermediate memory and strength. Furthermore, we numerically show that energy transfer efficiency is optimal and robust for the FMO protein complex of green sulphur bacteria with respect to variations in reorganization energy and bath correlation time-scales.