Spatially Inhomogeneous Bimodal Inherent Structure in Simulated Liquid Water

TL;DR

This study uses large-scale molecular dynamics simulations to reveal that liquid water exhibits a spatially inhomogeneous bimodal structure across a wide temperature range, linking supercooled and ambient states.

Contribution

It demonstrates a consistent bimodal potential energy surface in water, connecting supercooled and ambient conditions, and aligns with recent experimental data.

Findings

Water molecules are either LDL- or HDL-like with a 3:1 ratio at ambient conditions.

The Widom line corresponds to a 1:1 distribution of LDL- and HDL-like molecules.

The results unify the understanding of water's structure from supercooled to ambient states.

Abstract

In the supercooled regime at elevated pressure two forms of liquid water, high-density (HDL) and low-density (LDL), have been proposed to be separated by a coexistence line ending at a critical point, but a connection to ambient conditions has been lacking. Here we perform large-scale molecular dynamics simulations and demonstrate that the underlying potential energy surface gives a strictly bimodal characterization of the molecules at all temperatures as spatially inhomogeneous either LDL- or HDL-like with a 3:1 predominance for HDL at ambient conditions. The Widom line, indicating maximum fluctuations, coincides with a 1:1 distribution. Our results indicate a unified description of liquid water covering supercooled to ambient conditions in agreement with recent x-ray spectroscopy and scattering data.