Liquid-liquid phase separation in supercooled water from ultrafast heating of low-density amorphous ice

Katrin Amann-Winkel, Kyung Hwan Kim, Nicolas Giovambattista, Marjorie Ladd-Parada, Alexander Späh, Fivos Perakis, Harshad Pathak, Cheolhee Yang, Tobias Eklund, Thomas J. Lane, Seonju You, Sangmin Jeong, Jae Hyuk Lee, Intae Eom, Minseok Kim, Jaeku Park, Sae Hwan Chun, Peter H. Poole () and Anders Nilsson ()
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Katrin Amann-Winkel: Stockholm University
Kyung Hwan Kim: Department of Chemistry, POSTECH
Nicolas Giovambattista: Brooklyn College of the City University of New York
Marjorie Ladd-Parada: Stockholm University
Alexander Späh: Stockholm University
Fivos Perakis: Stockholm University
Harshad Pathak: Stockholm University
Cheolhee Yang: Department of Chemistry, POSTECH
Tobias Eklund: Stockholm University
Thomas J. Lane: SLAC National Accelerator Laboratory
Seonju You: Department of Chemistry, POSTECH
Sangmin Jeong: Department of Chemistry, POSTECH
Jae Hyuk Lee: Pohang Accelerator Laboratory
Intae Eom: Pohang Accelerator Laboratory
Minseok Kim: Pohang Accelerator Laboratory
Jaeku Park: Pohang Accelerator Laboratory
Sae Hwan Chun: Pohang Accelerator Laboratory
Peter H. Poole: St. Francis Xavier University
Anders Nilsson: Stockholm University

Nature Communications, 2023, vol. 14, issue 1, 1-8

Abstract: Abstract Recent experiments continue to find evidence for a liquid-liquid phase transition (LLPT) in supercooled water, which would unify our understanding of the anomalous properties of liquid water and amorphous ice. These experiments are challenging because the proposed LLPT occurs under extreme metastable conditions where the liquid freezes to a crystal on a very short time scale. Here, we analyze models for the LLPT to show that coexistence of distinct high-density and low-density liquid phases may be observed by subjecting low-density amorphous (LDA) ice to ultrafast heating. We then describe experiments in which we heat LDA ice to near the predicted critical point of the LLPT by an ultrafast infrared laser pulse, following which we measure the structure factor using femtosecond x-ray laser pulses. Consistent with our predictions, we observe a LLPT occurring on a time scale 1 μs.

Date: 2023
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DOI: 10.1038/s41467-023-36091-1

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