State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029, China.
J Chem Phys. 2013 Apr 28;138(16):164704. doi: 10.1063/1.4802633.
A density functional approach is presented to describe the crystal-liquid interfaces and crystal nucleations of Lennard-Jones fluid. Within the theoretical framework, the modified fundamental measure theory is applied to describe the free energy functional of hard sphere repulsion, and the weighted density method based on first order mean spherical approximation is used to describe the free energy contribution arising from the attractive interaction. The liquid-solid equilibria, density profiles within crystal cells and at liquid-solid interfaces, interfacial tensions, nucleation free energy barriers, and critical cluster sizes are calculated for face-centered-cubic and body-centered-cubic nucleus. Some results are in good agreement with available simulation data, indicating that the present model is quantitatively reliable in describing nucleation thermodynamics of Lennard-Jones fluid.
本文提出了一种密度泛函方法来描述 Lennard-Jones 流体的晶体-液体界面和晶体成核。在理论框架内，采用修正的基本测量理论来描述硬球排斥的自由能泛函，而基于一阶平均球近似的加权密度方法则用于描述吸引力相互作用引起的自由能贡献。计算了面心立方和体心立方核的固液平衡、晶体胞内和固液界面处的密度分布、界面张力、成核自由能势垒和临界团簇尺寸。一些结果与现有模拟数据吻合较好，表明该模型在描述 Lennard-Jones 流体成核热力学方面具有定量可靠性。
