Anomalous Behavior in the Nucleation of Ice at Negative Pressures

Abstract

Ice nucleation is a phenomenon that, despite the relevant implications for life, atmospheric sciences, and technological applications, is far from being completely understood, especially under extreme thermodynamic conditions. In this work we present a computational investigation of the homogeneous ice nucleation at negative pressures. By means of the seeding technique we estimate the size of the ice critical nucleus Nc for the TIP4P/Ice water model. This is done along the isotherms 230, 240, and 250 K, from positive to negative pressures until reaching the liquid-gas kinetic stability limit (where cavitation cannot be avoided). We find that Nc is nonmonotonic upon depressurization, reaching a minimum at negative pressures in the doubly metastable region of water. According to classical nucleation theory we establish the nucleation rate J and the surface tension gamma, revealing a retracing behavior of both when the liquid-gas kinetic stability limit is approached. We also predict a reentrant behavior of the homogeneous nucleation line. The reentrance of these properties is related to the reentrance of the coexistence line at negative pressure, revealing new anomalies of water. The results of this work suggest the possibility of having metastable samples of liquid water for long times at negative pressure provided that heterogeneous nucleation is suppressed.

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Cited by in corpus (4)

• The kinetics of the ice-water interface from ab initio machine learning simulations
• Homogeneous nucleation rate of carbon dioxide hydrate formation under experimental condition from Seeding simulations
• Rotationally invariant local bond order parameters for accurate determination of hydrate structures
• Can molecular simulations reliably compare homogeneous and heterogeneous ice nucleation?