Chemistry, Ames Laboratory
Letter to the Editor
Journal or Book Title
Journal of Chemical Physics
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.
Gunawardana, K. G. S. H. and Song, Xueyu, "Response to “Comment on ‘Theoretical prediction of crystallization kinetics of a supercooled Lennard-Jones fluid’” [J.Chem.Phys. 151, 017101 (2019)]" (2019). Chemistry Publications. 1153.
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