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振动电子耦合量子聚集体上的电子能量转移

Electronic energy transfer on a vibronically coupled quantum aggregate.

作者信息

Roden Jan, Schulz Georg, Eisfeld Alexander, Briggs John

机构信息

Max Planck Institute for the Physics of Complex Systems, Nothnitzer Str. 38, 01187 Dresden, Germany.

出版信息

J Chem Phys. 2009 Jul 28;131(4):044909. doi: 10.1063/1.3176513.

Abstract

We examine the transfer of electronic excitation (an exciton) along a chain of electronically coupled monomers possessing internal vibronic structure and which also interact with degrees of freedom of the surrounding environment. Using a combination of analytical and numerical methods, we calculate the time evolution operator or time-dependent Green's function of the system and thereby isolate the physical parameters influencing the electronic excitation transport. Quite generally, we show that coupling to vibrations slows down and inhibits migration of electronic excitation due to dephasing effects on the coherent transfer present without vibrations. In particular, coupling to a continuous spectrum of environment states leads to a complete halting of transfer, i.e., a trapping of the exciton.

摘要

我们研究了电子激发(激子)沿着具有内部振动结构且还与周围环境自由度相互作用的电子耦合单体链的转移。通过结合解析和数值方法,我们计算了系统的时间演化算符或含时格林函数,从而分离出影响电子激发传输的物理参数。一般来说,我们表明,由于对无振动时存在的相干转移产生的退相效应,与振动的耦合会减慢并抑制电子激发的迁移。特别是,与连续的环境态谱耦合会导致转移完全停止,即激子被俘获。

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