Electron transfer rates in bridged molecular systems: A phenomenological approach to relaxation

被引:173
作者
Davis, WB
Wasielewski, MR
Ratner, MA
Mujica, V
Nitzan, A
机构
[1] ARGONNE NATL LAB, DIV CHEM, ARGONNE, IL 60439 USA
[2] CENT UNIV VENEZUELA, FAC CIENCIAS, ESCUELA QUIM, CARACAS 1020A, VENEZUELA
[3] TEL AVIV UNIV, SCH CHEM, IL-69978 TEL AVIV, ISRAEL
关键词
D O I
10.1021/jp970909c
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
A model for bridge-assisted, long-range electron transfer in a molecule interacting with a dissipative external bath is presented. The effects of the system-bath interaction are included phenomenologically in the evolution of the system density matrix as energy dephasings on the bridge sites. When the bridge dephasings are small, the steady state ET rate in this model is found to be the sum of two competing terms; the first is a McConnell-type rate arising from direct tunneling from donor to acceptor, and the second is a dephasing dependent, length-independent scattering channel through the bridge sites. In the limit of large dephasings, an incoherent channel dominates the dynamics and leads to ET rates that can become only weakly dependent (k(ET) proportional to 1/N) on the number of bridge sites in the system, for multisite bridges.
引用
收藏
页码:6158 / 6164
页数:7
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