Molecular dynamics simulation of the ice nucleation and growth process leading to water freezing

Masakazu Matsumoto, Shinji Saito, Iwao Ohmine

Research output: Contribution to journalArticlepeer-review

619 Citations (Scopus)

Abstract

Upon cooling, water freezes to ice. This familiar phase transition occurs widely in nature, yet unlike the freezing of simple liquids, it has never been successfully simulated on a computer. The difficulty lies with the fact that hydrogen bonding between individual water molecules yields a disordered threedimensional hydrogen-bond network whose rugged and complex global potential energy surface permits a large number of possible network configurations. As a result, it is very challenging to reproduce the freezing of 'real' water into a solid with a unique crystalline structure. For systems with a limited number of possible disordered hydrogen-bond network structures, such as confined water, it is relatively easy to locate a pathway from a liquid state to a crystalline structure. For pure and spatially unconfined water, however, molecular dynamics simulations of freezing are severely hampered by the large number of possible network configurations that exist. Here we present a molecular dynamics trajectory that captures the molecular processes involved in the freezing of pure water. We find that ice nucleation occurs once a sufficient number of relatively long-lived hydrogen bonds develop spontaneously at the same location to form a fairly compact initial nucleus. The initial nucleus then slowly changes shape and size until it reaches a stage that allows rapid expansion, resulting in crystallization of the entire system.

Original languageEnglish
Pages (from-to)409-413
Number of pages5
JournalNature
Volume416
Issue number6879
DOIs
Publication statusPublished - Mar 28 2002
Externally publishedYes

ASJC Scopus subject areas

  • General

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