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

Author(s): Gartner, Thomas E; Torquato, Salvatore; Car, Roberto; Debenedetti, Pablo G

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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.
Publication Date: 7-Jun-2021
Electronic Publication Date: 7-Jun-2021
Citation: Gartner, Thomas E, Torquato, Salvatore, Car, Roberto, Debenedetti, Pablo G. (Manifestations of metastable criticality in the long-range structure of model water glasses. Nature Communications, 12 (1), 10.1038/s41467-021-23639-2
DOI: doi:10.1038/s41467-021-23639-2
EISSN: 2041-1723
Language: en
Type of Material: Journal Article
Journal/Proceeding Title: Nature Communications
Version: Final published version. This is an open access article.

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