Tomasi Stefano, Kassal Ivan
School of Chemistry and University of Sydney Nano Institute, University of Sydney, Sydney, NSW 2006, Australia.
J Phys Chem Lett. 2020 Mar 19;11(6):2348-2355. doi: 10.1021/acs.jpclett.9b03490. Epub 2020 Mar 9.
Several kinds of coherence have recently been shown to affect the performance of light-harvesting systems, in some cases significantly improving their efficiency. Here, we classify the possible mechanisms of coherent efficiency enhancements, based on the types of coherence that can characterize a light-harvesting system and the types of processes these coherences can affect. We show that enhancements are possible only when coherences and dissipative effects are best described in different bases of states. Our classification allows us to predict a previously unreported coherent enhancement mechanism, where coherence between delocalized eigenstates can be used to localize excitons away from dissipation, thus reducing the rate of recombination and increasing efficiency.
最近已证明几种相干性会影响光捕获系统的性能，在某些情况下会显著提高其效率。在此，我们根据可表征光捕获系统的相干性类型以及这些相干性可影响的过程类型，对相干效率增强的可能机制进行分类。我们表明，只有当相干性和耗散效应在不同的态基中得到最佳描述时，增强才有可能。我们的分类使我们能够预测一种先前未报道的相干增强机制，其中离域本征态之间的相干性可用于将激子定位在远离耗散的位置，从而降低复合率并提高效率。
