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arXiv 1208.6499math-phmath.MPphysics.chem-phquant-ph
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电子转移反应:广义自旋玻色子方法

Electron Transfer Reactions: Generalized Spin-Boson Approach

Marco Merkli, Gennady Berman, Richard Sayre

摘要:

我们介绍了一个数学上严格的分析广义自旋玻色子系统的施主-受主(反应产物)量子系统耦合到热量子噪声的治疗。供体/受体概率动力学描述了在噪声环境中化学过程中的传输反应,例如光合反应中心的电子转移。除了严格之外,我们的分析与以前的分析相比还有以下优点:(1)我们包括了一个一般的、非能量守恒的系统-环境相互作用;(2)我们允许施主或受主由多个紧密相连的能级组成。我们建立明确的反应速率和效率(最终供体-受体群体差异)的表达式。特别是,我们表明,率增加了多层次的受体,但效率没有。

英文摘要:

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 of multiple energy levels lying 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.

机构、总结、中文摘要均由AI分析而来,可能存在错误,请以论文正文为准。

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