Supercritical density fluctuations and structural heterogeneity in supercooled water-glycerol microdroplets
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| Format: | Preprint |
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2024
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| author | Berkowicz, Sharon Andronis, Iason Girelli, Anita Filianina, Mariia Bin, Maddalena Nam, Kyeongmin Shin, Myeongsik Kowalewski, Markus Katayama, Tetsuo Giovambattista, Nicolas Kim, Kyung Hwan Perakis, Fivos |
| author_facet | Berkowicz, Sharon Andronis, Iason Girelli, Anita Filianina, Mariia Bin, Maddalena Nam, Kyeongmin Shin, Myeongsik Kowalewski, Markus Katayama, Tetsuo Giovambattista, Nicolas Kim, Kyung Hwan Perakis, Fivos |
| contents | 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 ($χ_g=3.2~\%$ glycerol mole fraction). The combination of rapid evaporative cooling with ultrafast 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, $κ_T$, increases upon cooling. This is confirmed by molecular dynamics simulations, which indicate that the presence of glycerol shifts the temperature of maximum $κ_T$ 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. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2410_08952 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Supercritical density fluctuations and structural heterogeneity in supercooled water-glycerol microdroplets Berkowicz, Sharon Andronis, Iason Girelli, Anita Filianina, Mariia Bin, Maddalena Nam, Kyeongmin Shin, Myeongsik Kowalewski, Markus Katayama, Tetsuo Giovambattista, Nicolas Kim, Kyung Hwan Perakis, Fivos Soft Condensed Matter Statistical Mechanics 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 ($χ_g=3.2~\%$ glycerol mole fraction). The combination of rapid evaporative cooling with ultrafast 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, $κ_T$, increases upon cooling. This is confirmed by molecular dynamics simulations, which indicate that the presence of glycerol shifts the temperature of maximum $κ_T$ 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. |
| title | Supercritical density fluctuations and structural heterogeneity in supercooled water-glycerol microdroplets |
| topic | Soft Condensed Matter Statistical Mechanics |
| url | https://arxiv.org/abs/2410.08952 |