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

Author

Listed:
  • Katrin Amann-Winkel

    (Stockholm University
    Max Planck Institute for Polymer Research and Johannes Gutenberg University)

  • Kyung Hwan Kim

    (Department of Chemistry, POSTECH)

  • Nicolas Giovambattista

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

  • Marjorie Ladd-Parada

    (Stockholm University
    AlbaNova University Center)

  • 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)

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.

Suggested Citation

  • 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 & S, 2023. "Liquid-liquid phase separation in supercooled water from ultrafast heating of low-density amorphous ice," Nature Communications, Nature, vol. 14(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-36091-1
    DOI: 10.1038/s41467-023-36091-1
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    References listed on IDEAS

    as
    1. Osamu Mishima & H. Eugene Stanley, 1998. "Decompression-induced melting of ice IV and the liquid–liquid transition in water," Nature, Nature, vol. 392(6672), pages 164-168, March.
    2. Osamu Mishima & H. Eugene Stanley, 1998. "The relationship between liquid, supercooled and glassy water," Nature, Nature, vol. 396(6709), pages 329-335, November.
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