Department of Engineering Technology, Faculty of Technology, University of Ruhuna, Matara, Sri Lanka and Ames Laboratory, Iowa State University, Ames, Iowa 50011, USA.
Ames Laboratory and Department of Chemistry, Iowa State University, Ames, Iowa 50011, USA.
J Chem Phys. 2018 May 28;148(20):204506. doi: 10.1063/1.5021944.
The first order curvature correction to the crystal-liquid interfacial free energy is calculated using a theoretical model based on the interfacial excess thermodynamic properties. The correction parameter (δ), which is analogous to the Tolman length at a liquid-vapor interface, is found to be 0.48 ± 0.05 for a Lennard-Jones (LJ) fluid. We show that this curvature correction is crucial in predicting the nucleation barrier when the size of the crystal nucleus is small. The thermodynamic driving force (Δμ) corresponding to available simulated nucleation conditions is also calculated by combining the simulated data with a classical density functional theory. In this paper, we show that the classical nucleation theory is capable of predicting the nucleation barrier with excellent agreement to the simulated results when the curvature correction to the interfacial free energy is accounted for.
利用基于界面过剩热力学性质的理论模型，计算了晶体-液相界面自由能的一阶曲率修正。对于 Lennard-Jones（LJ）流体，修正参数（δ）为 0.48±0.05，类似于液体-蒸气界面上的 Tolman 长度。我们表明，当晶体核尺寸较小时，这种曲率修正对于预测成核势垒至关重要。通过将模拟数据与经典密度泛函理论相结合，计算了与可用模拟成核条件相对应的热力学驱动力（Δμ）。在本文中，我们表明，当考虑界面自由能的曲率修正时，经典成核理论能够以优异的模拟结果预测成核势垒。
