Glassy Arrest Behind the Apparent Second Liquid in Water
Florian Pabst, Ali Hassanali

TL;DR
This study uses advanced simulations and experimental data to argue that water's two-liquid signatures are actually due to a transition into a glassy state, challenging the traditional liquid-liquid transition hypothesis.
Contribution
It provides a reinterpretation of water's anomalous behavior, linking two-state fluctuations to glass formation rather than a liquid-liquid transition.
Findings
Features of two-liquid behavior emerge at dynamical arrest onset.
Two-state fluctuations reflect a transition to a kinetically arrested glass.
Estimated glass-transition temperature of low-density water is 189±8 K.
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…
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