Light-harvesting enhanced by quantum ratchet states

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.

20 pages, 15 figures

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• Optical signatures of coherence in molecular dimers
• Design Principles for Enhanced Quantum Transport with Site-Dependent Noise