Homogeneous ice nucleation rate at negative pressures: The role of the density anomaly

Abstract

Recent experiments suggest a role for pressure fluctuations in nucleation. Homogeneous ice nucleation rates for the ML-mW and mW water models are evaluated at pressures ranging from atmospheric to -1000 atm, using forward flux sampling and constant cooling simulations. Results indicate that the density difference Δνls between water and ice exhibited by these models plays a central role in controlling the change in nucleation rate with pressure. A linear function is found to be a reasonable approximation for lines of constant nucleation rate, which can be useful in making experimental predictions to advance the study of ice nucleation mechanisms.