Electron transfer reactions: generalized spin-boson approach
Electron transfer reactions: generalized spin-boson approach
复制标题
DOI：
10.1007/s10910-012-0124-5
复制
发表时间：
2012-08
影响因子：
1.7
通讯作者：
M. Merkli;Gennady P. Berman;Richard T. Sayre
中科院分区：
文献类型：
--
作者：
M. Merkli;Gennady P. Berman;Richard T. Sayre
我们引入了对广义自旋玻色子系统的数学严格分析，用于处理与热量子噪声耦合的供体-受体（反应物-产物）量子系统。供体/受体概率动力学描述了嘈杂环境下化学过程中的传输反应，例如光合作用反应中心的电子转移。除了严谨之外，我们的分析还比以前的分析具有以下优点：（1）我们包括一般的、非节能的系统-环境相互作用，并且（2）我们允许供体或受体由紧密相连的多个能级组成。我们建立了反应速率和效率（最终供体-受体群体差异）的明确表达式。特别是，我们表明多级接受器的速率增加，但效率却没有增加。
We introduce a mathematically rigorous analysis of a generalized spin-boson system for the treatment of a donor–acceptor (reactant-product) quantum system coupled to a thermal quantum noise. The donor/acceptor probability dynamics describes transport reactions in chemical processes in presence of a noisy environment – such as the electron transfer in a photosynthetic reaction center. Besides being rigorous, our analysis has the advantages over previous ones that (1) we include a general,non energy-conserving system-environment interaction, and that (2) we allow for the donor or acceptor to consist ofmultiple energy levelslying closely together. We establish explicit expressions for the rates and the efficiency (final donor–acceptor population difference) of the reaction. In particular, we show that the rate increases for a multi-level acceptor, but the efficiency does not.