Department of Chemistry, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA.
J Chem Phys. 2010 Oct 14;133(14):144107. doi: 10.1063/1.3488136.
Recent experiments on resonance energy transfer (RET) in photosynthetic systems have found evidence of quantum coherence between the donor and the acceptor. Under these conditions, Förster's theory of RET is no longer applicable and no theory of coherent RET advanced to date rivals the intuitive simplicity of Förster's theory. Here, we develop a framework for understanding RET that is based on classical electrodynamics but still captures the essence of the quantum coherence between the molecules. Our theory requires only a knowledge of the complex polarizabilities of the two molecules participating in the transfer as well as the distance between them. We compare our results to quantum mechanical calculations and show that the results agree quantitatively.
最近在光合作用系统中的共振能量转移(RET)实验中发现了供体和受体之间量子相干的证据。在这些条件下,福斯特的 RET 理论不再适用,并且迄今为止没有一种相干 RET 理论能够与福斯特理论的直观简单性相媲美。在这里,我们开发了一种基于经典电动力学但仍能捕捉分子间量子相干本质的 RET 理解框架。我们的理论仅需要参与转移的两个分子的复极化率以及它们之间的距离的知识。我们将我们的结果与量子力学计算进行比较,并表明结果在数量上是一致的。