Multiple freezing–melting pathways of high-density ice through ice XXI phase at room temperature
Various metastable ice phases and their complicated transition pathways have been found by pressurization at low temperatures at which slow kinetics and high metastability are easily achieved. By contrast, such diversity is less expected at room or elevated temperatures. Here, using a combination of a dynamic diamond anvil cell and X-ray free electron laser techniques, we demonstrate that supercompressed water transforms into ice VI through multiple freezing-melting pathways at room temperature, hidden within the pressure region of ice VI. These multiple transition pathways occur via a metastable ice (more specifically, ice XXI with body-centred tetragonal structure ( <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:mrow><mml:mi>I</mml:mi> <mml:mover><mml:mn>4</mml:mn> <mml:mo>¯</mml:mo></mml:mover> <mml:mn>2</mml:mn> <mml:mi>d</mml:mi></mml:mrow> </mml:math> )) discovered in this study and a metastable ice VII that exists within the pressure range of ice VI. We find that supercompressed water structurally evolves from high-density water to very-high-density water, causing multiple transition pathways. These findings provide an insight to find more metastable ice phases and their transition pathways at elevated temperatures.
Authors
- Yong-Jae Kim (ORCID: https://orcid.org/0000-0002-1839-332X)
- Anshuman Mondal (ORCID: https://orcid.org/0000-0002-3424-5693)
- Geun Woo Lee (ORCID: https://orcid.org/0000-0003-3681-1641)
- Earl F. O’Bannon (ORCID: https://orcid.org/0000-0002-9341-5090)
- Tobias Eklund (ORCID: https://orcid.org/0000-0002-5851-3939)
- Choong‐Shik Yoo
- Minxue Tang (ORCID: https://orcid.org/0000-0002-3923-0677)
- Katrin Amann‐Winkel (ORCID: https://orcid.org/0000-0002-7319-7807)
- Zuzana Konôpková
- Lisa Katharina Mohrbach
- Torsten Laurus (ORCID: https://orcid.org/0000-0002-2258-2123)
- Khachiwan Buakor (ORCID: https://orcid.org/0000-0003-0257-2822)
- Anand Dwivedi (ORCID: https://orcid.org/0009-0008-7497-0444)
- C. Strohm (ORCID: https://orcid.org/0000-0001-6384-0259)
- Karen Appel (ORCID: https://orcid.org/0000-0002-2902-2102)
- Rachel J. Husband (ORCID: https://orcid.org/0000-0002-7666-401X)
- Lisa Randolph (ORCID: https://orcid.org/0000-0001-9587-404X)
- Carsten Baehtz (ORCID: https://orcid.org/0000-0003-1480-511X)
- Emma Ehrenreich-Petersen
- Oliver Humphries (ORCID: https://orcid.org/0000-0001-6748-0422)
- Hauke Marquardt (ORCID: https://orcid.org/0000-0003-1784-6515)
- H. Graafsma (ORCID: https://orcid.org/0000-0003-2304-667X)
- Yong Chan Cho (ORCID: https://orcid.org/0000-0003-3976-8343)
- Robert P. C. Bauer (ORCID: https://orcid.org/0000-0002-2932-6683)
- Hanns‐Peter Liermann (ORCID: https://orcid.org/0000-0001-5039-1183)
- Hiroki Nada (ORCID: https://orcid.org/0000-0002-1744-2759)
- U. Zastrau (ORCID: https://orcid.org/0000-0002-3575-4449)
- Felix Lehmkühler (ORCID: https://orcid.org/0000-0003-1289-995X)
- Konstantin V. Glazyrin (ORCID: https://orcid.org/0000-0002-5296-9265)
- Jin Kyun Kim (ORCID: https://orcid.org/0000-0003-2650-9879)
- Minju Kim (ORCID: https://orcid.org/0000-0003-1999-7392)
- Yunhee Lee (ORCID: https://orcid.org/0000-0002-9177-2553)
- Jolanta Sztuck-Dambietz
Institutions
- Lawrence Livermore National Laboratory (US)
- Johannes Gutenberg University Mainz (DE)
- University of Münster (DE)
- Korea Research Institute of Standards and Science (KR)
- Helmholtz-Zentrum Dresden-Rossendorf (DE)
- Deutsches Elektronen-Synchrotron DESY (DE)
- University of Oxford (GB)
- Max Planck Institute for Polymer Research (DE)
- Freiberger Compound Materials (Germany) (DE)
- Max Planck Institute for the Structure and Dynamics of Matter (DE)
- Hamburg Centre for Ultrafast Imaging
- Tottori University (JP)
- TU Bergakademie Freiberg (DE)
- Washington State University (US)
- Korea University of Science and Technology (KR)
- European X-Ray Free-Electron Laser (DE)
Publication Details
- Journal
- Nature Materials
- Published
- 2025-10-10
- DOI
- https://doi.org/10.1038/s41563-025-02364-x
- Citations
- 5
- Primary Topic
- Material Dynamics and Properties
- Type
- article
- Field-Weighted Citation Impact
- 2.59
Funders
- U.S. Department of Energy
- UK Research and Innovation
- Deutsche Forschungsgemeinschaft
- Korea Research Institute of Standards and Science
- University of Tokyo
- National Research Council of Science and Technology
- Science and Technology Facilities Council
- Deutsches Elektronen-Synchrotron
- Japan Society for the Promotion of Science
- Laboratory Directed Research and Development
- Lawrence Livermore National Laboratory