Finding the differences: Classical nucleation perspective on homogeneous melting and freezing of hard spheres

By employing brute-force molecular dynamics, umbrella sampling, and seeding simulations, we investigate homogeneous nucleation during melting and freezing of hard spheres. We provide insights into these opposing phase transitions from the standpoint of classical nucleation theory. We observe that me...

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Bibliographic Details
Published in:The Journal of chemical physics 2024-04, Vol.160 (14)
Main Authors: Gispen, Willem, Dijkstra, Marjolein
Format: Article
Language:English
Subjects:
Freezing
Interface stability
Melting
Molecular dynamics
Nucleation
Phase transitions
Strain energy
Surface tension
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Summary:By employing brute-force molecular dynamics, umbrella sampling, and seeding simulations, we investigate homogeneous nucleation during melting and freezing of hard spheres. We provide insights into these opposing phase transitions from the standpoint of classical nucleation theory. We observe that melting has both a lower driving force and a lower interfacial tension than freezing. The lower driving force arises from the vicinity of a spinodal instability in the solid and from a strain energy. The lower interfacial tension implies that the Tolman lengths associated with melting and freezing have opposite signs, a phenomenon that we interpret with Turnbull’s rule. Despite these asymmetries, the nucleation rates for freezing and melting are found to be comparable.
ISSN:0021-9606
1089-7690
DOI:10.1063/5.0201629