Homogeneous ice nucleation evaluated for several water models

TL;DR

This study uses computer simulations to evaluate ice homogeneous nucleation rates across various water models, estimating interfacial free-energy and analyzing how model differences influence nucleation behavior.

Contribution

It provides a comparative analysis of nucleation rates and interfacial free-energy for multiple water models, highlighting the impact of model choice on nucleation predictions.

Findings

Interfacial free-energy decreases with temperature for all models.

Estimated interfacial free-energy aligns with experimental values.

Nucleation rates vary depending on the water model used.

Abstract

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.