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Title: The thermodynamics of a liquid-solid interface at extreme conditions: A model close-packed system up to 100 GPa

Abstract

The first experimental insight into the nature of the liquid-solid interface occurred with the pioneering experiments of Turnbull, which simultaneously demonstrated both that metals could be deeply undercooled (and therefore had relatively large barriers to nucleation) and that the inferred interfacial free energy γ was linearly proportional to the enthalpy of fusion [D. Turnbull, J. Appl. Phys. 21, 1022 (1950)]. By an atomistic simulation of a model face-centered cubic system via adiabatic free energy dynamics, we extend Turnbull’s result to the realm of high pressure and demonstrate that the interfacial free energy, evaluated along the melting curve, remains linear with the bulk enthalpy of fusion, even up to 100 GPa. This linear dependence of γ on pressure is shown to be a consequence of the entropy dominating the free energy of the interface in conjunction with the fact that the entropy of fusion does not vary greatly along the melting curve for simple monoatomic metals. Here, based on this observation, it appears that large undercoolings in liquid metals can be achieved even at very high pressure. Therefore, nucleation rates at high pressure are expected to be non-negligible, resulting in observable solidification kinetics.

Authors:
 [1]; ORCiD logo [1]
  1. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Publication Date:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1502047
Alternate Identifier(s):
OSTI ID: 1474009
Report Number(s):
LLNL-JRNL-755173
Journal ID: ISSN 0021-9606; 942049
Grant/Contract Number:  
AC52-07NA27344
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 149; Journal Issue: 12; 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; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS

Citation Formats

Samanta, Amit, and Belof, Jonathan L. The thermodynamics of a liquid-solid interface at extreme conditions: A model close-packed system up to 100 GPa. United States: N. p., 2018. Web. doi:10.1063/1.5028268.
Samanta, Amit, & Belof, Jonathan L. The thermodynamics of a liquid-solid interface at extreme conditions: A model close-packed system up to 100 GPa. United States. doi:10.1063/1.5028268.
Samanta, Amit, and Belof, Jonathan L. Wed . "The thermodynamics of a liquid-solid interface at extreme conditions: A model close-packed system up to 100 GPa". United States. doi:10.1063/1.5028268. https://www.osti.gov/servlets/purl/1502047.
@article{osti_1502047,
title = {The thermodynamics of a liquid-solid interface at extreme conditions: A model close-packed system up to 100 GPa},
author = {Samanta, Amit and Belof, Jonathan L.},
abstractNote = {The first experimental insight into the nature of the liquid-solid interface occurred with the pioneering experiments of Turnbull, which simultaneously demonstrated both that metals could be deeply undercooled (and therefore had relatively large barriers to nucleation) and that the inferred interfacial free energy γ was linearly proportional to the enthalpy of fusion [D. Turnbull, J. Appl. Phys. 21, 1022 (1950)]. By an atomistic simulation of a model face-centered cubic system via adiabatic free energy dynamics, we extend Turnbull’s result to the realm of high pressure and demonstrate that the interfacial free energy, evaluated along the melting curve, remains linear with the bulk enthalpy of fusion, even up to 100 GPa. This linear dependence of γ on pressure is shown to be a consequence of the entropy dominating the free energy of the interface in conjunction with the fact that the entropy of fusion does not vary greatly along the melting curve for simple monoatomic metals. Here, based on this observation, it appears that large undercoolings in liquid metals can be achieved even at very high pressure. Therefore, nucleation rates at high pressure are expected to be non-negligible, resulting in observable solidification kinetics.},
doi = {10.1063/1.5028268},
journal = {Journal of Chemical Physics},
number = 12,
volume = 149,
place = {United States},
year = {2018},
month = {9}
}

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