Classical Nucleation theory predicts the shape of the nucleus in homogeneous solidification

Bingqing Cheng, Michele Ceriotti, Gareth Tribello

Research output: Contribution to journalArticle

Abstract

Macroscopic models of nucleation provide powerful tools for understanding activated phase transition processes. These models do not provide atomistic insights and can thus sometime lack material-specific descriptions. Here we provide a comprehensive framework for constructing a continuum picture from an atomistic simulation of homogeneous nucleation. We use this framework to determine the shape of the equilibrium solid nucleus that forms inside bulk liquid for a Lennard-Jones potential. From this shape, we then extract the anisotropy of the solid-liquid interfacial free energy, by performing a reverse Wulff construction in the space of spherical harmonic expansions. We find that the shape of the nucleus is nearly spherical and that its anisotropy can be perfectly described using classical models.
Original languageEnglish
JournalJournal of Chemical Physics
Publication statusAccepted - 01 Jan 2020

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solidification
Solidification
Nucleation
nucleation
nuclei
Anisotropy
Lennard-Jones potential
anisotropy
Liquids
spherical harmonics
liquids
Free energy
Phase transitions
free energy
continuums
expansion
simulation

Cite this

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Classical Nucleation theory predicts the shape of the nucleus in homogeneous solidification. / Cheng, Bingqing; Ceriotti, Michele; Tribello, Gareth.

In: Journal of Chemical Physics, 01.01.2020.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Classical Nucleation theory predicts the shape of the nucleus in homogeneous solidification

AU - Cheng, Bingqing

AU - Ceriotti, Michele

AU - Tribello, Gareth

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N2 - Macroscopic models of nucleation provide powerful tools for understanding activated phase transition processes. These models do not provide atomistic insights and can thus sometime lack material-specific descriptions. Here we provide a comprehensive framework for constructing a continuum picture from an atomistic simulation of homogeneous nucleation. We use this framework to determine the shape of the equilibrium solid nucleus that forms inside bulk liquid for a Lennard-Jones potential. From this shape, we then extract the anisotropy of the solid-liquid interfacial free energy, by performing a reverse Wulff construction in the space of spherical harmonic expansions. We find that the shape of the nucleus is nearly spherical and that its anisotropy can be perfectly described using classical models.

AB - Macroscopic models of nucleation provide powerful tools for understanding activated phase transition processes. These models do not provide atomistic insights and can thus sometime lack material-specific descriptions. Here we provide a comprehensive framework for constructing a continuum picture from an atomistic simulation of homogeneous nucleation. We use this framework to determine the shape of the equilibrium solid nucleus that forms inside bulk liquid for a Lennard-Jones potential. From this shape, we then extract the anisotropy of the solid-liquid interfacial free energy, by performing a reverse Wulff construction in the space of spherical harmonic expansions. We find that the shape of the nucleus is nearly spherical and that its anisotropy can be perfectly described using classical models.

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JF - Journal of Chemical Physics

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