Glassy Arrest Behind the Apparent Second Liquid in Water

Abstract

The origin of water's anomalous behavior remains a central open problem in the physical sciences and is often attributed to a liquid-liquid transition (LLT) between high- and low-density liquid states deep in the supercooled regime. Experimental access to this region has been challenging due to rapid crystallization, leaving atomistic simulations as a major source of supporting evidence. Using extensive machine-learning-accelerated first-principles simulations in direct comparison with spectroscopic, structural, and dynamical experimental measurements, we show that features commonly interpreted as signatures of two-liquid behavior emerge at the onset of dynamical arrest. Specifically, we find that two-state fluctuations previously associated with an LLT reflect a transformation from a high-density liquid to a kinetically arrested low-density glass. By mapping equilibrium dynamics across pressure and temperature, our results suggest a reassessment of water's metastable landscape, in which apparent two-state behavior may reflect a relatively high glass-transition temperature of ambient-pressure low-density water, 189$\pm$8 K -- remarkably close to the temperature previously associated with the LLT.