Title
Theoretical prediction of crystallization kinetics of a supercooled Lennard-Jones fluid
Publication Date
5-22-2018
Department
Ames Laboratory; Chemistry
Campus Units
Chemistry, Ames Laboratory
Report Number
IS-J 9695
DOI
10.1063/1.5021944
Journal Title
Journal of Chemical Physics
Volume Number
148
First Page
204506
Abstract
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.
Language
en
Department of Energy Subject Categories
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Publisher
Iowa State University Digital Repository, Ames IA (United States)
