Theoretical prediction of crystallization kinetics of a supercooled Lennard-Jones fluid
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.
- Authors:
-
- Univ. of Ruhuna, Matara (Sri Lanka). Dept. of Engineering Technology; Ames Lab. and Iowa State Univ., Ames, IA (United States)
- Ames Lab. and Iowa State Univ., Ames, IA (United States). Dept. of Chemistry
- Publication Date:
- Research Org.:
- Ames Lab. and Iowa State Univ., Ames, IA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1459540
- Alternate Identifier(s):
- OSTI ID: 1438283
- Report Number(s):
- IS-J-9695
Journal ID: ISSN 0021-9606; TRN: US1901565
- Grant/Contract Number:
- AC02-07CH11358
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 148; Journal Issue: 20; Journal ID: ISSN 0021-9606
- Publisher:
- American Institute of Physics (AIP)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; heavy fermion systems; crystallography; interfaces; thermodynamic properties; crystallization; density functional theory; gas liquid interfaces; entropy; free energy
Citation Formats
Gunawardana, K. G. S. H., and Song, Xueyu. Theoretical prediction of crystallization kinetics of a supercooled Lennard-Jones fluid. United States: N. p., 2018.
Web. doi:10.1063/1.5021944.
Gunawardana, K. G. S. H., & Song, Xueyu. Theoretical prediction of crystallization kinetics of a supercooled Lennard-Jones fluid. United States. https://doi.org/10.1063/1.5021944
Gunawardana, K. G. S. H., and Song, Xueyu. Tue .
"Theoretical prediction of crystallization kinetics of a supercooled Lennard-Jones fluid". United States. https://doi.org/10.1063/1.5021944. https://www.osti.gov/servlets/purl/1459540.
@article{osti_1459540,
title = {Theoretical prediction of crystallization kinetics of a supercooled Lennard-Jones fluid},
author = {Gunawardana, K. G. S. H. and Song, Xueyu},
abstractNote = {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.},
doi = {10.1063/1.5021944},
journal = {Journal of Chemical Physics},
number = 20,
volume = 148,
place = {United States},
year = {Tue May 22 00:00:00 EDT 2018},
month = {Tue May 22 00:00:00 EDT 2018}
}
Web of Science
Figures / Tables:
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Works referencing / citing this record:
Comment on “Theoretical prediction of crystallization kinetics of a supercooled Lennard-Jones fluid” [J. Chem. Phys. 148, 204506 (2018)]
journal, July 2019
- Tipeev, Azat O.
- The Journal of Chemical Physics, Vol. 151, Issue 1
Response to “Comment on ‘Theoretical prediction of crystallization kinetics of a supercooled Lennard-Jones fluid’” [J. Chem. Phys. 151, 017101 (2019)]
journal, July 2019
- Gunawardana, K. G. S. H.; Song, Xueyu
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Interfacial free energy of a liquid-solid interface: Its change with curvature
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Entropy and the Tolman Parameter in Nucleation Theory
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- Entropy, Vol. 21, Issue 7
Figures / Tables found in this record: