Dynamics of electrochemical electron-transfer reactions

虽然电化学电子转移反应的理论研究已经深入了50年，但仍然有几个重要的问题是悬而未决的。在这个项目中，我们想解决两个相关的问题：(1)电子转移速率如何依赖于反应物之间的相互作用？(2)与溶剂浴的相互作用和伴随的耗散对反应动力学有什么影响？在这项研究中，我们希望利用量子系统中耗散理论的最新进展；此外，我们计划对模型系统进行计算机模拟。我们期望，我们的结果不仅应该与电化学系统相关，而且应该与电子转移耦合到镀液的其他情况相关；特别是，我们计划将它们应用于半导体中的电子注入。我们的长期目标是建立生物系统中远程电子转移的理论，这项工作应该是一个重要的垫脚石。

Although the theory of electrochemical electron transfer reactions has been the subject of intensive research for five decades, there are still several important questions open. In this project we want to address two related problems: (1) How does the rate of electron transfer depend on the interaction between the reactants? (2) What effect does the interaction with the solvent bath and the concomitant dissipation have on the reaction dynamics? For the investigation we want to draw on recent progress in the theory of dissipation in quantum systems; in addition, we plan to perform computer simulations for model systems. We expect, that our results should not only be relevant to electrochemical systems, but also to other cases in which electron transfer is coupled to a bath; in particular, we plan to apply them to electron injection into semiconductors. Our long-term goal is a theory for long-range electron transfer in biological systems, to which this work should be an important stepping stone.