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Supercritical density fluctuations and structural heterogeneity in supercooled water-glycerol microdroplets

Author

Listed:
  • Sharon Berkowicz

    (AlbaNova University Center, Stockholm University)

  • Iason Andronis

    (AlbaNova University Center, Stockholm University)

  • Anita Girelli

    (AlbaNova University Center, Stockholm University)

  • Mariia Filianina

    (AlbaNova University Center, Stockholm University)

  • Maddalena Bin

    (AlbaNova University Center, Stockholm University)

  • Kyeongmin Nam

    (Pohang University of Science and Technology (POSTECH))

  • Myeongsik Shin

    (Pohang University of Science and Technology (POSTECH))

  • Markus Kowalewski

    (AlbaNova University Center, Stockholm University)

  • Tetsuo Katayama

    (Japan Synchrotron Radiation Research Institute
    RIKEN SPring-8 Center)

  • Nicolas Giovambattista

    (Brooklyn College of the City University of New York
    The Graduate Center of the City University of New York)

  • Kyung Hwan Kim

    (Pohang University of Science and Technology (POSTECH))

  • Fivos Perakis

    (AlbaNova University Center, Stockholm University)

Abstract

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.

Suggested Citation

  • Sharon Berkowicz & Iason Andronis & Anita Girelli & Mariia Filianina & Maddalena Bin & Kyeongmin Nam & Myeongsik Shin & Markus Kowalewski & Tetsuo Katayama & Nicolas Giovambattista & Kyung Hwan Kim & , 2024. "Supercritical density fluctuations and structural heterogeneity in supercooled water-glycerol microdroplets," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-54890-y
    DOI: 10.1038/s41467-024-54890-y
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    References listed on IDEAS

    as
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