Response to “Comment on ‘Theoretical prediction of crystallization kinetics of a supercooled Lennard-Jones fluid’” [J.Chem.Phys. 151, 017101 (2019)]

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2019-07-03
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Gunawardana, K. G. S. H.
Song, Xueyu
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Ames National Laboratory

Ames National Laboratory is a government-owned, contractor-operated national laboratory of the U.S. Department of Energy (DOE), operated by and located on the campus of Iowa State University in Ames, Iowa.

For more than 70 years, the Ames National Laboratory has successfully partnered with Iowa State University, and is unique among the 17 DOE laboratories in that it is physically located on the campus of a major research university. Many of the scientists and administrators at the Laboratory also hold faculty positions at the University and the Laboratory has access to both undergraduate and graduate student talent.

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Chemistry

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The Department of Chemistry was founded in 1880.

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Ames National LaboratoryChemistry
Abstract

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.

Comments

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.

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Tue Jan 01 00:00:00 UTC 2019
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