Water Potential from Adaptive Force Matching for Ice and Liquid with Revised Dispersion Predicts Supercooled Liquid Anomalies in Good Agreement with Two Independent Experimental Fits

Abstract

A revised version of the Water potential from Adaptive force matching for Ice and Liquid (WAIL) was developed by using the previous data set for fitting the WAIL model but with a dispersion term calculated using symmetry adapted perturbation theory (SAPT). The model has no adjustable parameters and relies solely on fitting first-principles information. The new model, named revised WAIL (rWAIL), shows improved predictions of most properties of water when compared to the previously published WAIL model. The rWAIL model also compares favorably to other first-principles-derived water models, such as MB-Pol, at only a fraction of the computational cost. The rWAIL model is used to study the properties of supercooled water. The model shows evidence of a liquid-liquid phase transition (LLPT) in the supercooled regimes with the liquid-liquid critical point (LLCP) at 203 K and 90 MPa. This estimate is in good agreement with a recent polynomial fit to the experimental density of water. Also, the fit to the surface tension of supercooled water based on the rWAIL model shows excellent agreement with the corresponding fit to the experimental data. Consistent with previously published molecular dynamics and experimental data, the surface tension of water exhibits exponential growth in the supercooled regime, which is likely a result of the emergence of a low-density liquid form of water. The simulation thus unites two separate experimental fits with one first-principles-based model, lending strong evidence of an LLPT in real water.