Stability and Metastability of Liquid Water in a Machine-Learned Coarse- Grained Model with Short-Range Interactions

D Dhabal and SKRS Sankaranarayanan and V Molinero, JOURNAL OF PHYSICAL CHEMISTRY B, 126, 9881-9892 (2022).

DOI: 10.1021/acs.jpcb.2c06246

Coarse-grained water models are similar to 100 times more efficient than all-atom models, enabling simulations of supercooled water and crystallization. The machine-learned monatomic model ML-BOP reproduces the experimental equation of state (EOS) and ice- liquid thermodynamics at 0.1 MPa on par with the all-atom TIP4P/2005 and TIP4P/Ice models. These all-atom models were parametrized using high-pressure experimental data and are either accurate for water's EOS (TIP4P/2005) or ice-liquid equilibrium (TIP4P/Ice). ML-BOP was parametrized from temperature- dependent ice and liquid experimental densities and melting data at 0.1 MPa; its only pressure training is from compression of TIP4P/2005 ice at 0 K. Here we investigate whether ML-BOP replicates the experimental EOS and ice-water thermodynamics along all pressures of ice I. We find that ML-BOP reproduces the temperature, enthalpy, entropy, and volume of melting of hexagonal ice up to 400 MPa and the EOS of water along the melting line with an accuracy that rivals that of both TIP4P/2005 and TIP4P/Ice. We interpret that the accuracy of ML-BOP originates from its ability to capture the shift between compact and open local structures to changes in pressure and temperature. ML-BOP reproduces the sharpening of the tetrahedral peak of the pair distribution function of water upon supercooling, and its pressure dependence. We characterize the region of metastability of liquid ML-BOP with respect to crystallization and cavitation. The accessibility of ice crystallization to simulations of ML-BOP, together with its accurate representation of the thermodynamics of water, makes it promising for investigating the interplay between anomalies, glass transition, and crystallization under conditions challenging to access through experiments.

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