Nonmonotonic energy harvesting efficiency in biased exciton chains

TL;DR

This paper models energy harvesting in biased exciton chains, revealing a nonmonotonic efficiency dependence on bias due to a balance between transport enhancement and localization effects.

Contribution

It introduces a theoretical framework combining exciton-phonon interactions and disorder effects to analyze energy harvesting efficiency in biased chains.

Findings

Efficiency peaks at an optimal bias value.

Localization effects reduce efficiency at high bias.

Disorder-induced localization impacts transport dynamics.

Abstract

We theoretically study the efficiency of energy harvesting in linear exciton chains with an energy bias, where the initial excitation is taking place at the high-energy end of the chain and the energy is harvested (trapped) at the other end. The efficiency is characterized by means of the average time for the exciton to be trapped after the initial excitation. The exciton transport is treated as the intraband energy relaxation over the states obtained by numerically diagonalizing the Frenkel Hamiltonian that corresponds to the biased chain. The relevant intraband scattering rates are obtained from a linear exciton-phonon interaction. Numerical solution of the Pauli master equation that describes the relaxation and trapping processes, reveals a complicated interplay of factors that determine the overall harvesting efficiency. Specifically, if the trapping step is slower than or comparable to the intraband relaxation, this efficiency shows a nonmonotonic dependence on the bias: it first increases when introducing a bias, reaches a maximum at an optimal bias value, and then decreases again because of dynamic (Bloch) localization of the exciton states. Effects of on-site (diagonal) disorder, leading to Anderson localization, are addressed as well.