Nanosecond Freezing of Water at High Pressures: Nucleation and Growth near the Metastability Limit

Abstract

The fundamental study of phase transition kinetics has motivated experimental methods toward achieving the largest degree of undercooling possible, more recently culminating in the technique of rapid, quasi-isentropic compression. This approach has been demonstrated to freeze water into the high-pressure ice VII phase on nanosecond time scales, with some experiments undergoing heterogeneous nucleation while others, in apparent contradiction, suggesting a homogeneous nucleation mode. In this study, we show through a combination of theory, simulation, and analysis of experiments that these seemingly contradictory results are in agreement when viewed from the perspective of classical nucleation theory. We find that, perhaps surprisingly, classical nucleation theory is capable of accurately predicting the solidification kinetics of ice VII formation under an extremely high driving force (|∆µ/k B T | ≈ 1), but only if amended by two important considerations: 1) transient nucleation and 2) separate liquid and solid temperatures. This is the first demonstration of a model that is able to reproduce the experimentally observed rapid freezing kinetics.

Melting and refreezing of zirconium observed using ultrafast x-ray diffraction

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Super Rapid Crystal Growth and Quench of Monoclinic Bi-II* During Dynamic Compression

“…Rapid grain growth on the order of 100 m/s has been studied experimentally [67] and theoretically [68], but with a caveat: the pure metal must be supercooled. Advanced equipment has been developed to achieve this in static experiments, but in shockwave studies it is common for liquids to become supercooled before solidifying [69]. µm in length before ambient pressure was reached.…”