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Supercritical density fluctuations and structural heterogeneity in supercooled water-glycerol microdroplets
Stockholm University, Faculty of Science, Department of Physics.ORCID iD: 0000-0001-5754-9334
Stockholm University, Faculty of Science, Department of Physics.
Stockholm University, Faculty of Science, Department of Physics.
Stockholm University, Faculty of Science, Department of Physics.ORCID iD: 0000-0002-1366-7360
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Number of Authors: 122024 (English)In: Nature Communications, E-ISSN 2041-1723, Vol. 15, no 1, article id 10610Article in journal (Refereed) Published
Abstract [en]

Recent experiments and theoretical studies strongly indicate that water exhibits a liquid-liquid phase transition (LLPT) in the supercooled domain. An open question is how the LLPT of water can affect the properties of aqueous solutions. Here, we study the structural and thermodynamic properties of supercooled glycerol-water microdroplets at dilute conditions (χg = 3.2% glycerol mole fraction). The combination of rapid evaporative cooling with femtosecond X-ray scattering allows us to outrun crystallization and gain access to the deeply supercooled regime down to T = 229.3 K. We find that the density fluctuations of the glycerol-water solution or, equivalently, its isothermal compressibility, κT, increases upon cooling. This is confirmed by molecular dynamics simulations, which indicate that the presence of glycerol shifts the temperature of maximum κT from T = 230 K in pure water down to T = 223 K in the solution. Our findings elucidate the interplay between the complex behavior of water, including its LLPT, and the properties of aqueous solutions at low temperatures, which can have practical consequences in cryogenic biological applications and cryopreservation techniques.

Place, publisher, year, edition, pages
2024. Vol. 15, no 1, article id 10610
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Subatomic Physics
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URN: urn:nbn:se:su:diva-240718DOI: 10.1038/s41467-024-54890-yISI: 001372601000038PubMedID: 39638810Scopus ID: 2-s2.0-85211391583OAI: oai:DiVA.org:su-240718DiVA, id: diva2:1944493
Available from: 2025-03-14 Created: 2025-03-14 Last updated: 2025-03-14Bibliographically approved

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Berkowicz, SharonFilianina, MariiaBin, MaddalenaKowalewski, MarkusPerakis, Fivos

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