Jang Seogjoo, Cheng Yuan-Chung, Reichman David R, Eaves Joel D
Department of Chemistry and Biochemistry, Queens College of the City University of New York, 65-30 Kissena Boulevard, Flushing, New York 11367, USA.
J Chem Phys. 2008 Sep 14;129(10):101104. doi: 10.1063/1.2977974.
A theory of coherent resonance energy transfer is developed combining the polaron transformation and a time-local quantum master equation formulation, which is valid for arbitrary spectral densities including common modes. The theory contains inhomogeneous terms accounting for nonequilibrium initial preparation effects and elucidates how quantum coherence and nonequilibrium effects manifest themselves in the coherent energy transfer dynamics beyond the weak resonance coupling limit of the Forster and Dexter (FD) theory. Numerical tests show that quantum coherence can cause significant changes in steady state donor/acceptor populations from those predicted by the FD theory and illustrate delicate cooperation of nonequilibrium and quantum coherence effects on the transient population dynamics.
结合极化子变换和时间局部量子主方程公式，发展了一种相干共振能量转移理论，该理论适用于包括共同模式在内的任意谱密度。该理论包含了非齐次项，用于解释非平衡初始制备效应，并阐明了量子相干和非平衡效应如何在超越福斯特和德克斯特（FD）理论的弱共振耦合极限的相干能量转移动力学中表现出来。数值测试表明，量子相干会导致稳态供体/受体种群与FD理论预测的种群有显著变化，并说明了非平衡和量子相干效应在瞬态种群动力学中的微妙协同作用。
