Coherent and controllable enhancement of light-harvesting efficiency

Abstract

Spectroscopic experiments have identified long-lived coherences in several light-harvesting systems, suggesting that coherent effects may be relevant to their performance. However, there is limited experimental evidence of coherence enhancing light-harvesting efficiency, largely due to the difficulty of turning coherences on and off to create an experimental control. Here, we show that coherence can indeed enhance light harvesting, and that this effect can be controlled. We construct a model system in which initial coherence can be controlled using the incident light, and which is significantly more efficient under coherent, rather than incoherent, excitation. Our proposal would allow for the first unambiguous demonstration of light harvesting enhanced by intermolecular coherence, as well as demonstrate the potential for coherent control of excitonic energy transfer.