Chenu Aurélia, Scholes Gregory D
Department of Chemistry, University of Toronto, Toronto, Ontario M5S 3H6, Canada.
Annu Rev Phys Chem. 2015 Apr;66:69-96. doi: 10.1146/annurev-physchem-040214-121713. Epub 2014 Dec 1.
Ultrafast energy transfer is used to transmit electronic excitation among the many molecules in photosynthetic antenna complexes. Recent experiments and theories have highlighted the role of coherent transfer in femtosecond studies of these proteins, suggesting the need for accurate dynamical models to capture the subtle characteristics of energy transfer mechanisms. Here we discuss how to think about coherence in light harvesting and electronic energy transfer. We review the various fundamental concepts of coherence, spanning from classical phenomena to the quantum superposition, and define coherence in electronic energy transfer. We describe the current status of experimental studies on light-harvesting complexes. Insights into the microscopic process are presented to highlight how and why this is a challenging problem to elucidate. We present an overview of the applicable dynamical theories to model energy transfer in the intermediate coupling regime.
超快能量转移用于在光合天线复合体中的众多分子之间传递电子激发。最近的实验和理论突出了相干转移在这些蛋白质飞秒研究中的作用,这表明需要精确的动力学模型来捕捉能量转移机制的微妙特征。在这里,我们讨论如何思考光捕获和电子能量转移中的相干性。我们回顾了从经典现象到量子叠加的各种相干基本概念,并定义了电子能量转移中的相干性。我们描述了光捕获复合体实验研究的现状。对微观过程的见解旨在突出这为何是一个具有挑战性的待阐明问题以及如何具有挑战性。我们概述了适用于模拟中间耦合 regime 中能量转移的动力学理论。