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超越确定性极限的成核理论。I. 成核阶段。

Nucleation theory beyond the deterministic limit. I. The nucleation stage.

机构信息

St. Petersburg Academic University, Khlopina 8/3, 194021 St. Petersburg, Russia.

出版信息

J Chem Phys. 2010 Mar 21;132(11):114507. doi: 10.1063/1.3354118.

Abstract

This work addresses theory of nucleation and condensation based on the continuous Fokker-Plank type kinetic equation for the distribution of supercritical embryos over sizes beyond the deterministic limit, i.e., keeping the second derivative with respect to size. The first part of the work treats the nucleation stage. It is shown that the size spectrum should be generally obtained by the convolution of the initial distribution with the Gaussian-like Green function with spreading dispersion. It is then demonstrated that the fluctuation-induced effects can be safely neglected at the nucleation stage, where the spectrum broadening due to the nonlinear boundary condition is much larger than the fluctuational one. The crossover between the known triangular and double exponential distributions under different conditions of material influx into the system is demonstrated. Some examples of size distributions at the nucleation stage in different regimes of material influx are also presented.

摘要

这项工作基于连续的福克-普朗克型统计动力方程,解决了过饱和度下的临界核胚胎的尺寸分布的成核和凝结理论,该方程超越了尺寸的确定性极限,即保留了对尺寸的二阶导数。工作的第一部分处理成核阶段。结果表明,尺寸谱通常应该通过初始分布与具有扩展分散的类高斯格林函数的卷积来获得。然后证明,在成核阶段,由于非线性边界条件引起的谱展宽远大于波动引起的谱展宽,因此可以安全地忽略波动诱导的影响。在不同的物质流入系统的条件下,展示了已知的三角形和双指数分布之间的交叉。还给出了在不同物质流入模式下成核阶段的一些尺寸分布实例。

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