Gas–liquid nucleation in two‐dimensional fluids
Gas–liquid nucleation in two‐dimensional fluids
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DOI：
10.1063/1.470991
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发表时间：
1996-02
影响因子：
4.4
通讯作者：
X. Zeng
中科院分区：
文献类型：
--
作者：
X. Zeng
基于密度泛函（DF）方法，发展了二维Lennard-Jones（LJ）流体气液相变的非经典成核理论.使用Weeks-Chandler-Andersen微扰理论的方法来近似具有温度依赖的硬盘直径和吸引尾的LJ势。所得的自由能泛函然后用于计算成核的自由能势垒。我们发现，2D核的曲率是不重要的成核率（在对比的3D对应）。曲率的影响很容易从经典Becker-Doring理论的成核速率与DF理论的成核速率之比中推断出来。我们的计算表明，经典成核理论实际上对于2D LJ流体在预测成核速率的温度依赖性方面相当有效（而对于3D LJ流体，它严重失败）。
A nonclassical theory of nucleation, based on the density‐functional (DF) approach, is developed for the gas–liquid transitions of two‐dimensional (2D) Lennard‐Jones (LJ) fluids. The methods of Weeks–Chandler–Andersen perturbation theory are used to approximate the LJ potential with a temperature‐dependent hard‐disk diameter plus an attractive tail. The resulting free energy functional is then used to calculate the free energy barrier to nucleation. We find that the curvature of the 2D nucleus is not important to the rate of nucleation (in contrast to the 3D counterpart). The effect of curvature is readily inferred from the ratio of nucleation rate from classical Becker–Doring theory to that from DF theory. Our calculation suggests that classical nucleation theory actually works reasonably well for 2D LJ fluids in predicting the temperature‐dependence of the nucleation rate (whereas for 3D LJ fluids it fails badly).