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存在偏压时的体相介导表面输运。

Bulk-mediated surface transport in the presence of bias.

机构信息

Section on Molecular Transport, Eunice Kennedy Shriver National Institute of Child Health and Human Development, National Institutes of Health, Bethesda, Maryland 20892, USA.

出版信息

J Chem Phys. 2017 Jul 7;147(1):014103. doi: 10.1063/1.4991730.

Abstract

Surface transport, when the particle is allowed to leave the surface, travel in the bulk for some time, and then return to the surface, is referred to as bulk-mediated surface transport. Recently, we proposed a formalism that significantly simplifies analysis of bulk-mediated surface diffusion [A. M. Berezhkovskii, L. Dagdug, and S. M. Bezrukov, J. Chem. Phys. 143, 084103 (2015)]. Here this formalism is extended to bulk-mediated surface transport in the presence of bias, i.e., when the particle has arbitrary drift velocities on the surface and in the bulk. A key advantage of our approach is that the transport problem reduces to that of a two-state problem of the particle transitions between the surface and the bulk. The latter can be solved with relative ease. The formalism is used to find the Laplace transforms of the first two moments of the particle displacement over the surface in time t at arbitrary values of the particle drift velocities and diffusivities on the surface and in the bulk. This allows us to analyze in detail the time dependence of the effective drift velocity of the particle on the surface, which can be highly nontrivial.

摘要

当允许粒子离开表面后在体相中传输一段时间,然后再回到表面时,这种过程被称为体相介导的表面输运。最近,我们提出了一种形式理论,该理论极大地简化了体相介导的表面扩散的分析[A. M. Berezhkovskii、L. Dagdug 和 S. M. Bezrukov,J. Chem. Phys. 143, 084103 (2015)]。在这里,该形式理论被扩展到存在偏置的体相介导的表面输运中,即粒子在表面和体相中有任意的漂移速度。我们方法的一个关键优势在于,输运问题可以简化为粒子在表面和体相之间的两个状态之间的跃迁问题。后一个问题可以相对容易地解决。该形式理论用于在任意表面和体相中的粒子漂移速度和扩散系数下,找到粒子在表面上的位移的前两个矩的拉普拉斯变换在时间 t 上的时间依赖关系。这使我们能够详细分析粒子在表面上的有效漂移速度的时间依赖性,这可能非常复杂。

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