Manifestations of metastable criticality in the long-range structure of model water glasses

Thomas E. Gartner, Salvatore Torquato, Roberto Car and Pablo G. Debenedetti ()
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Thomas E. Gartner: Princeton University
Salvatore Torquato: Princeton University
Roberto Car: Princeton University
Pablo G. Debenedetti: Princeton University

Nature Communications, 2021, vol. 12, issue 1, 1-9

Abstract: Abstract Much attention has been devoted to water’s metastable phase behavior, including polyamorphism (multiple amorphous solid phases), and the hypothesized liquid-liquid transition and associated critical point. However, the possible relationship between these phenomena remains incompletely understood. Using molecular dynamics simulations of the realistic TIP4P/2005 model, we found a striking signature of the liquid-liquid critical point in the structure of water glasses, manifested as a pronounced increase in long-range density fluctuations at pressures proximate to the critical pressure. By contrast, these signatures were absent in glasses of two model systems that lack a critical point. We also characterized the departure from equilibrium upon vitrification via the non-equilibrium index; water-like systems exhibited a strong pressure dependence in this metric, whereas simple liquids did not. These results reflect a surprising relationship between the metastable equilibrium phenomenon of liquid-liquid criticality and the non-equilibrium structure of glassy water, with implications for our understanding of water phase behavior and glass physics. Our calculations suggest a possible experimental route to probing the existence of the liquid-liquid transition in water and other fluids.

Date: 2021
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DOI: 10.1038/s41467-021-23639-2

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