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ANALYTICAL KINETIC THEORY OF SINGLE-PARTICLE AND COLLECTIVE SURFACE DIFFUSION

机译:单粒子和集体表面扩散的分析动力学理论

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This paper generalizes the results of a recently developed kinetic theory of surface diffusion conceptually different both from the popular transition state hopping model and from the Fokker-Plank kinetic model (or its equivalent Generalized Langevin approach). Following the first principles of statistical mechanics, the theory is based on the evolution of the particle's probability density, and takes into account the possibility of a finite change in adparticle energy due to its interaction with the substrate excitations. We show how, in this general way under some simplifying assumptions, one can reach a relatively simple, analytical description of surface diffusion that goes far beyond the abilities of the TST model. Examples are given by the occurrence of long jumps and "anomalous" pre-exponential factors of the diffusion coefficient in the low-density limit. Moreover, the theory allows, for the first time, kinetic treatment of surface diffusion at inite occupancy, resulting in a new sight on mechanisms determining the density dependence of collective diffusivity. Some puzzling aspects of surface cluster diffusion (gliding) can also be elucidated.
机译:本文概括表面扩散无论是从流行的过渡态跃迁模型,并从福克 - 普朗克动力学模型(或等值广义朗之万的做法)概念不同的最近开发的动力学理论的结果。以下统计力学的基本原理,理论是基于粒子的概率密度的演变,并考虑到在adparticle能量有限变化的可能性,因为它与基底激励作用。我们将展示如何在在一些简化的假设这种普遍的方式,可以达到表面扩散的一个比较简单的,分析的描述是远远超出了TST模型的能力。实例由长的跳跃和“异常的”在低密度极限的扩散系数的预指数因子的发生给定。此外,理论允许,对于第一次,在inite占用表面扩散,从而产生一个新的视线上确定集体扩散的密度依赖性机制的动力学治疗。表面簇扩散(滑行)的一些令人费解的各方面也可以阐明。

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