Homogeneous ice nucleation evaluated for several water models

JR Espinosa and E Sanz and C Valeriani and C Vega, JOURNAL OF CHEMICAL PHYSICS, 141, 18C529 (2014).

DOI: 10.1063/1.4897524

In this work, we evaluate by means of computer simulations the rate for ice homogeneous nucleation for several water models such as TIP4P, TIP4P/2005, TIP4P/ICE, and mW (following the same procedure as in Sanz et al. J. Am. Chem. Soc. 135, 15008 (2013)) in a broad temperature range. We estimate the ice-liquid interfacial free-energy, and conclude that for all water models gamma decreases as the temperature decreases. Extrapolating our results to the melting temperature, we obtain a value of the interfacial free-energy between 25 and 32 mN/m in reasonable agreement with the reported experimental values. Moreover, we observe that the values of gamma depend on the chosen water model and this is a key factor when numerically evaluating nucleation rates, given that the kinetic prefactor is quite similar for all water models with the exception of the mW (due to the absence of hydrogens). Somewhat surprisingly the estimates of the nucleation rates found in this work for TIP4P/2005 are slightly higher than those of the mW model, even though the former has explicit hydrogens. Our results suggest that it may be possible to observe in computer simulations spontaneous crystallization of TIP4P/2005 at about 60 K below the melting point. (C) 2014 AIP Publishing LLC.

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