Homogeneous ice nucleation at moderate supercooling from molecular simulation

Abstract

Among all the freezing transitions, that of water into ice is probably the most relevant to biology, physics, geology or atmospheric science. In this work we investigate homogeneous ice nucleation by means of computer simulations. We evaluate the size of the critical cluster and the nucleation rate for temperatures ranging between 15K and 35K below melting. We use the TIP4P/2005 and the TIP4P/Ice water models. Both give similar results when compared at the same temperature difference with the model's melting temperature. The size of the critical cluster varies from $\sim$8000 molecules (radius$=4$nm) at 15K below melting to $\sim$600 molecules (radius$=1.7$nm) at 35K below melting. We use Classical Nucleation Theory (CNT) to estimate the ice-water interfacial free energy and the nucleation free energy barrier. We obtain an interfacial free energy of 29(3)mN/m from an extrapolation of our results to the melting temperature. This value is in good agreement both with experimental measurements and with previous estimates from computer simulations of TIP4P-like models. Moreover, we obtain estimates of the nucleation rate from simulations of the critical cluster at the barrier top. The values we get for both models agree within statistical error with experimental measurements. At temperatures higher than 20K below melting we get nucleation rates slower than the appearance of a critical cluster in all the water of the hydrosphere in the age of the universe. Therefore, our simulations predict that water freezing above this temperature must necessarily be heterogeneous.

References in corpus (9)

• Canonical sampling through velocity-rescaling
• Accurate determination of crystal structures based on averaged local bond order parameters
• What ice can teach us about water interactions: a critical comparison of the performance of different water models
• The thickness of a liquid layer on the free surface of ice as obtained from computer simulation
• Anomalies in water as obtained from computer simulations of the TIP4P/2005 model: density maxima, and density, isothermal compressibility and heat capacity minima
• Free energy surface of ST2 water near the liquid-liquid phase transition
• Local order parameters for use in driving homogeneous ice nucleation with all-atom models of water
• Absence of superheating for ice Ih with a free surface : a new method of determining the melting point of different water models
• State-of-the-art models for the phase diagram of carbon and diamond nucleation

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