Modification of the classical nucleation theory based on molecular simulation data for surface tension, critical nucleus size, and nucleation rate
Modification of the classical nucleation theory based on molecular simulation data for surface tension, critical nucleus size, and nucleation rate
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DOI：
10.1103/physreve.78.011603
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发表时间：
2008-07-01
影响因子：
2.4
通讯作者：
Hasse, Hans
中科院分区：
文献类型：
--
作者：
Horsch, Martin;Vrabec, Jadran;Hasse, Hans
在正则系综中，用两组分子动力学模拟研究了过饱和蒸汽中的成核现象。应用的方法是(a)通过模拟小系统中单个液滴与周围蒸汽的平衡来分析中等过饱和时的临界核；(b)模拟含有10(5)-10(6)个粒子的大体系在冷凝过程中的均匀成核，用于计算高过饱和状态下蒸汽的成核速率。对于截断2.5倍尺寸参数的Lennard-Jones流体，表明经典成核理论低估了成核速率和临界核的大小。提出了一种表面性质修正的理论，以一致地涵盖曲面界面的表面张力，临界核尺寸和成核速率的数据。
Nucleation in supersaturated vapor is investigated with two series of molecular-dynamics simulations in the canonical ensemble. The applied methods are (a) analysis of critical nuclei at moderate supersaturations by simulating equilibria of single droplets with surrounding vapors in small systems; (b) simulation of homogeneous nucleation during condensation with large systems containing 10(5)-10(6) particles for calculating the nucleation rate of vapors at high supersaturations. For the Lennard-Jones fluid, truncated and shifted at 2.5 times the size parameter, it is shown that the classical nucleation theory underestimates both the nucleation rate and the size of the critical nucleus. A surface property corrected modification of this theory is proposed to consistently cover data on the surface tension of the curved interface, the critical nucleus size, and the nucleation rate.