Correlated Fluctuations of Structural Indicators Close to the Liquid-Liquid Transition in Supercooled Water

Abstract

Multiple numerical studies have unambiguously shown the existence of a liquid-liquid critical point in supercooled states for different numerical models of water, and various structural indicators have been put forward to describe the transformation associated with this phase transition. Here we analyze numerical simulations of near-critical supercooled water to compare the behavior of several of such indicators with critical density fluctuations. We show that close to the critical point most indicators are strongly correlated to density, and some of them even display identical distributions of fluctuations. These indicators probe the exact same free energy landscape, therefore providing a thermodynamic description of critical supercooled water which is identical to that provided by the density order parameter. This implies that close to the critical point, there is a tight coupling between many, only apparently distinct, structural degrees of freedom.