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

Sharon Berkowicz, Iason Andronis, Anita Girelli, Mariia Filianina, Maddalena Bin, Kyeongmin Nam, Myeongsik Shin, Markus Kowalewski, Tetsuo Katayama, Nicolas Giovambattista, Kyung Hwan Kim and Fivos Perakis ()
Additional contact information
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
Nicolas Giovambattista: Brooklyn College of the City University of New York
Kyung Hwan Kim: Pohang University of Science and Technology (POSTECH)
Fivos Perakis: AlbaNova University Center, Stockholm University

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: 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.

Date: 2024
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DOI: 10.1038/s41467-024-54890-y

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