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Free energy landscapes for homogeneous nucleation of ice for a monatomic model of water

Aleks Reinhardt and Jonathan P.K. Doye

J. Chem. Phys. 136, 054501 (2012)

Abstract

We simulate the homogeneous nucleation of ice from supercooled liquid water at 220K in the isobaric-isothermal ensemble using the MW monatomic water potential. Monte Carlo simulations using umbrella sampling are performed in order to determine the nucleation free energy barrier. We find the Gibbs energy profile to be relatively consistent with that predicted by classical nucleation theory; the free energy barrier to nucleation was determined to be 18kT and the critical nucleus comprised ~80 ice particles. Growth from the supercooled liquid gives clusters that are predominantly cubic, whilst starting with a pre-formed subcritical nucleus of cubic or hexagonal ice results in the growth of predominantly that phase of ice only.


The full paper is available from The Journal of Chemical Physics and arXiv.org.