Liquid-Liquid Phase Transition in Simulated Supercooled Water Nanodroplets

Abstract

Using simulations, we demonstrate how a liquid-liquid phase transition (LLPT) manifests in supercooled water nanodroplets. Selecting an interaction potential for which a LLPT occurs in the bulk liquid, we conduct simulations of supercooled water nanodroplets having between 1000 and 80000 molecules. We show that as the droplet size decreases, the Laplace pressure grows large enough to drive the droplets through the transition from the low-density to the high-density liquid phase, and that all droplets in this size range are large enough to have cores exhibiting the structure and properties of bulk water. To guide experiments, we estimate the range of values for the critical pressure of the LLPT in real water that can be observed using nanodroplets, and propose structural and dynamical measures by which the LLPT in nanodroplets can be detected. Published by the American Physical Society 2025