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克莱默斯反应速率理论的最新进展

Recent Developments in Kramers' Theory of Reaction Rates.

作者信息

Pollak Eli, Miret-Artés Salvador

机构信息

Chemical and Biological Physics Department, Weizmann Institute of Science, 76100, Rehovoth, Israel.

Instituto de Física Fundamental, Consejo, Superior de Investigaciones Científicas, Serrano 123, 28006, Madrid, Spain.

出版信息

Chemphyschem. 2023 Aug 15;24(16):e202300272. doi: 10.1002/cphc.202300272. Epub 2023 Aug 3.

Abstract

In this short review, we provide an update of recent developments in Kramers' theory of reaction rates. After a brief introduction stressing the importance of this theory initially developed for chemical reactions, we briefly present the main theoretical formalism starting from the generalized Langevin equation and continue by showing the main points of the modern Pollak, Grabert and Hänggi theory. Kramers' theory is then sketched for quantum and classical surface diffusion. As an illustration the surface diffusion of Na atoms on a Cu(110) surface is discussed showing escape rates, jump distributions and diffusion coefficients as a function of reduced friction. Finally, some very recent applications of turnover theory to different fields such as nanoparticle levitation, microcavity polariton dynamics and simulation of reaction in liquids are presented. We end with several open problems and future challenges faced up by Kramers turnover theory.

摘要

在这篇简短的综述中,我们提供了克莱默斯反应速率理论近期进展的最新情况。在简要介绍强调最初为化学反应发展的该理论的重要性之后,我们从广义朗之万方程开始简要介绍主要的理论形式,接着阐述现代波拉克、格拉伯特和亨吉理论的要点。然后勾勒了克莱默斯理论在量子和经典表面扩散方面的情况。作为例证,讨论了钠原子在铜(110)表面的表面扩散,展示了逃逸率、跳跃分布和扩散系数作为约化摩擦力的函数。最后,介绍了周转理论在纳米颗粒悬浮、微腔极化激元动力学和液体中反应模拟等不同领域的一些最新应用。我们以克莱默斯周转理论面临的几个未解决问题和未来挑战作为结尾。

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