Response to “Comment on ‘Theoretical prediction of crystallization kinetics of a supercooled Lennard-Jones fluid’” [J.Chem.Phys. 151, 017101 (2019)]
The Classical Nucleation Theory (CNT) describes the Gibbs free energy cost to create a crystallite of N atoms out of a metastable phase as follows:
ΔG = −N|Δμ| + γA. (1)
The first term gives the Gibbs free energy cost to create a crystallite of N atoms in its bulk phase. The term Δμ = μc − μl is the thermodynamic driving force, where μc and μl are the chemical potentials of bulk crystal and liquid phases. The second part is the contribution from the solid-liquid interface, where γ is the solid-liquid interfacial free energy and A is the area of the interface. The driving force is estimated with bulk properties of liquid and crystal phases. The interfacial free energy γ = γ0 is often estimated from its planar interface value γ0, the capillarity approximation. These independently estimated quantities lead to a nucleation profile, where the critical nucleus locates at the maximum of the profile and the resulting nucleation barrier can be used to estimate the nucleation rate. It has been a long standing goal of the classical nucleation theory to be able to predict accurate nucleation rate from these independently estimated thermodynamical properties.
This letter to the editor is published as Gunawardana, K.G.S.H., and Xueyu Song, Response to “Comment on ‘Theoretical prediction of crystallization kinetics of a supercooled Lennard-Jones fluid’” [J.Chem.Phys. 151, 017101 (2019)], Journal of Chemical Physics 151 (2019): 017102. DOI: 10.1063/1.5108755. Posted with permission.