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. 2011 Jul 21;135(3):034105. doi: 10.1063/1.3608914.
The approach of second order time local quantum master equation in the polaron picture, which has been employed for a theory of coherent resonance energy transfer, is extended for general multichromophore systems. Explicit expressions for all the kernel and inhomogeneous terms are derived, which can be calculated by any standard numerical procedure. The theory is then applied to a model of donor-bridge-acceptor system moderately coupled to bosonic bath. The results are compared with those based on the theory of Förster's resonance energy transfer. It is shown that coherently coupled multichromophores can speed up the transfer of energy substantially and in a way insensitive to the disorder.
在极化子图像中,二阶时间局部量子主方程的方法已经被应用于相干共振能量转移的理论中,现在将其扩展到一般的多色团系统。导出了所有核和非均匀项的显式表达式,这些表达式可以通过任何标准的数值程序来计算。然后,该理论被应用于与玻色子浴中度耦合的供体-桥-受体系统的模型。将结果与基于福斯特共振能量转移理论的结果进行了比较。结果表明,相干耦合的多色团可以显著加快能量转移,并且对无序不敏感。