Ephemeral ice-like local environments in classical rigid models of liquid water

Despite great efforts over the past 50 years, the simulation of water still presents significant challenges and open questions. At room temperature and pressure, the collective molecular interactions and dynamics of water molecules may form local structural arrangements that are non-trivial to classify. Here, we employ a data-driven approach built on Smooth Overlap of Atomic Position (SOAP) that allows us to compare and classify how widely used classical models represent liquid water. Macroscopically, the obtained results are rationalized based on water thermodynamic observables. Microscopically, we directly observe how transient ice-like ordered environments may dynamically/statistically form in liquid water, even above freezing temperature, by comparing the SOAP spectra for different ice structures with those of the simulated liquid systems. This confirms recent ab initio-based calculations but also reveals how the emergence of ephemeral local ice-like environments in liquid water at room conditions can be captured by classical water models. Published under an exclusive license by AIP Publishing.

Automated summary

Despite significant efforts, simulating water still poses challenges and questions. By utilizing a data-driven approach, this study reveals that classical models can capture the formation of transient ice-like environments in liquid water, consistent with recent ab initio calculations.