Light-harvesting enhanced by quantum ratchet states

TL;DR

This paper investigates bio-inspired ring systems as photovoltaic circuits, demonstrating how optical ratcheting and excitonic protection can enhance light-harvesting efficiency, with performance depending on system geometry, extraction method, and vibrational interactions.

Contribution

It introduces the concept of optical ratcheting in ring systems and analyzes how system size, extraction mechanisms, and vibrational coupling influence performance improvements.

Findings

Performance improves with certain geometries and extraction mechanisms.

Strong vibrational coupling can enhance or hinder efficiency.

Optimal conditions depend on a complex interplay of factors.

Abstract

We consider bio-inspired ring systems as photovoltaic circuits to explore the advantage of `optical ratcheting', a process whereby the arrangement of coupled optical dipoles enables delocalised excitonic states that are protected against radiative decay whilst permitting the absorption of further photons. We explore how the performance of a ratcheting antenna scales with system size when excitons are incoherently or coherently extracted from the antenna to an associated trap site. In both instances we also move to the polaron frame in order to more closely model realistic systems where the coupling to vibrational modes can generally be assumed to be strong. We find a multifaceted and nuanced dependence of the predicted performance on an interplay between geometrical arrangement, extraction mechanism, and vibrational coupling strength. Certain regimes support substantial performance improvements in the power extracted per site.