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关于扩散动力学中独立对的近似:三体系统中距离的相关性

On the approximation of independent pairs in diffusion kinetics: correlation of distances in a three-body system.

作者信息

Al-Samra Eyad H, Green Nicholas J B

机构信息

Physical & Theoretical Chemistry Laboratory, University of Oxford, UK.

出版信息

Phys Chem Chem Phys. 2018 Jan 24;20(4):2872-2879. doi: 10.1039/c7cp06929d.

Abstract

This study investigates the problem of diffusion kinetics in a three-body system, motivated by the theory of radiation chemical kinetics. The backward diffusion equation for the joint density of the distances is formulated, and an explicit formula for the infinitesimal covariance of two diffusing distances is derived. The Clifford-Green theorem is used to show how the infinitesimal covariance of two distances is linked to the covariance of the corresponding two squared distances as time evolves. In addition, computer simulations for the problem are presented, which indicate that hitting probabilities are also correlated. While the results indicate that more work is needed before a usable correction to the independence approximation is possible, clear progress has been made.

摘要

本研究受辐射化学动力学理论的启发,探讨了三体系统中的扩散动力学问题。推导了距离联合密度的反向扩散方程,并得出了两个扩散距离的无穷小协方差的显式公式。利用克利福德 - 格林定理展示了随着时间的演化,两个距离的无穷小协方差如何与相应两个距离平方的协方差相关联。此外,还给出了该问题的计算机模拟结果,结果表明命中概率也是相关的。虽然结果表明在对独立性近似进行可用修正之前还需要做更多工作,但已经取得了明显进展。

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