Vibration-Assisted and Vibration-Hampered Excitonic Quantum Transport

TL;DR

This study theoretically investigates how global and local vibrations influence exciton transport in light-harvesting complexes, revealing that vibrations can either enhance or hinder transfer efficiency through interference and resonance effects, with temperature effects counterintuitively increasing these phenomena.

Contribution

The paper introduces a theoretical model distinguishing global and local vibrational effects on exciton transport, highlighting their contrasting impacts and temperature dependence.

Findings

Global vibrations cause anti-resonances via exciton-polaron interference.

Local vibrations induce tunneling resonances at vibration energy multiples.

Both effects intensify with increasing temperature.

Abstract

The interplay between exctions and vibrations is considered to be a key factor in determining the exciton transfer properties in light-harvesting exciton transfer complexes. Here we study this interplay theoretically in a model for exciton transport, composed of two chromophores coupled to an exciton source and sink in the presence of vibrations. We consider two cases, that show qualitatively distinct transport features. In the first, the vibrations are global and affect the two chromophores simultaneously. In the second case, the vibrations are localized on each chromophore. For global vibrations, the current exhibits {\sl anti-resonances} as a function of the chromophore energy difference, which are due to exciton-polaron interference. For local vibrations, on the other hand, the currents shows tunneling {\sl resonances} at multiples of the vibration energy. Counter-intuitively, both effects increase with increasing temperature. Our results demonstrate that an environment can either assist or hamper exciton transport, and are in accord with current understanding of energy transfer in natural exciton transfer complexes.