Kinetics and Mechanisms of Pressure-induced Ice Amorphization and Polyamorphic Transitions in a Machine-learned Coarse-Grained Water Model

18 January 2023, Version 1
This content is a preprint and has not undergone peer review at the time of posting.


Water glasses have attracted considerable attention due to their potential connection to a liquid-liquid transition in supercooled water. Here we use molecular simulations to investigate the formation and phase behavior of water glasses using the ML-BOP water model. We produce glasses through hyperquenching of water, pressure-induced amorphization (PIA) of ice, and pressure-induced polyamorphic transformations. Our simulations show that PIA of polycrystalline ice occurs at a lower pressure than for mono-crystalline ice, and through a different mechanism. The temperature dependence of the amorphization pressure of polycrystalline ice for ML-BOP agrees with experiments. We also find that ML-BOP accurately reproduces the density, coordination number, and struc-tural features of LDA, HDA and VHDA water glasses. We examine the kinetics and mechanism of the transformation between low-density and high-density glasses, and find that the sharp nature of these transitions in ML-BOP is similar to that in experiments and all-atom water models with a liquid-liquid transition. Transitions between ML-BOP glasses occur through a spinodal-like mechanism, similar to ice crystallization from LDA. Both glass-to-glass and glass-to-ice transformations have Avrami-Kolmogorov kinetics with exponent n=1.5±0.2 in experiments and simulations. Importantly, ML-BOP reproduces the competition between crystallization and HDA→LDA transition above the glass transition temperature Tg, and separation of their time scales below Tg, observed also in experi-ments. These findings demonstrate the ability of ML-BOP to accurately reproduce water properties across various regimes, making it a promising model for addressing the competition between polyamorphic transitions and crystallization in water and solutions.


glassy water
liquid-liquid transition

Supplementary materials

Supporting Information
contains supporting figures


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