Phase transition kinetics of superionic H2O ice phases revealed by Megahertz X-ray free-electron laser-heating experiments

H<sub>2</sub>O transforms to two forms of superionic (SI) ice at high pressures and temperatures, which contain highly mobile protons within a solid oxygen sublattice. Yet the stability field of both phases remains debated. Here, we present the results of an ultrafast X-ray heating study utilizing MHz pulse trains produced by the European X-ray Free Electron Laser to create high temperature states of H<sub>2</sub>O, which were probed using X-ray diffraction during dynamic cooling. We confirm an isostructural transition during heating in the 26-69 GPa range, consistent with the formation of SI-bcc. In contrast to prior work, SI-fcc was observed exclusively above ~50 GPa, despite evidence of melting at lower pressures. The absence of SI-fcc in lower pressure runs is attributed to short heating timescales and the pressure-temperature path induced by the pump-probe heating scheme in which H<sub>2</sub>O was heated above its melting temperature before the observation of quenched crystalline states, based on the earlier theoretical prediction that SI-bcc nucleates more readily from the fluid than SI-fcc. Our results may have implications for the stability of SI phases in ice-rich planets, for example during dynamic freezing, where the preferential crystallization of SI-bcc may result in distinct physical properties across mantle ice layers.

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Journal
Nature Communications
Published
2024-09-23
DOI
https://doi.org/10.1038/s41467-024-52505-0
Citations
10
Primary Topic
nanoparticles nucleation surface interactions
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article
Field-Weighted Citation Impact
3.76

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article

Phase transition kinetics of superionic H2O ice phases revealed by Megahertz X-ray free-electron laser-heating experiments

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nanoparticles nucleation surface interactions
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article

Phase transition kinetics of superionic H2O ice phases revealed by Megahertz X-ray free-electron laser-heating experiments

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article en
10 citations

Abstract

H<sub>2</sub>O transforms to two forms of superionic (SI) ice at high pressures and temperatures, which contain highly mobile protons within a solid oxygen sublattice. Yet the stability field of both phases remains debated. Here, we present the results of an ultrafast X-ray heating study utilizing MHz pulse trains produced by the European X-ray Free Electron Laser to create high temperature states of H<sub>2</sub>O, which were probed using X-ray diffraction during dynamic cooling. We confirm an isostructural transition during heating in the 26-69 GPa range, consistent with the formation of SI-bcc. In contrast to prior work, SI-fcc was observed exclusively above ~50 GPa, despite evidence of melting at lower pressures. The absence of SI-fcc in lower pressure runs is attributed to short heating timescales and the pressure-temperature path induced by the pump-probe heating scheme in which H<sub>2</sub>O was heated above its melting temperature before the observation of quenched crystalline states, based on the earlier theoretical prediction that SI-bcc nucleates more readily from the fluid than SI-fcc. Our results may have implications for the stability of SI phases in ice-rich planets, for example during dynamic freezing, where the preferential crystallization of SI-bcc may result in distinct physical properties across mantle ice layers.

Nature CommunicationsVol. 15(1)
Lawrence Livermore National Laboratory (US), University of Freiburg (DE), Jilin University (CN), Carnegie Institution for Science (US), University of Münster (DE), Commissariat à l'Énergie Atomique et aux Énergies Alternatives (FR), Université Paris-Saclay (FR), Helmholtz-Zentrum Dresden-Rossendorf (DE), Deutsches Elektronen-Synchrotron DESY (DE), SLAC National Accelerator Laboratory (US), Diamond Light Source (GB), Gwangju Institute of Science and Technology (KR), Sorbonne Université (FR), University of Oxford (GB), University of Chicago (US), CEA DAM Île-de-France (FR), SpectrumK (Germany) (DE), Institut de minéralogie, de physique des matériaux et de cosmochimie (FR), Yonsei University Health System (KR), Earth and Planets Laboratory, State Key Laboratory of High Pressure and Superhard Materials (CN), University of Bayreuth (DE), University of Milano-Bicocca (IT), European X-Ray Free-Electron Laser (DE), University of Edinburgh (GB)
National Science Foundation, U.S. Department of Energy, Association Sorbonne Université, UK Research and Innovation, Carnegie Institution for Science, Atomic Weapons Establishment, European Commission, Deutsche Forschungsgemeinschaft, Ministry of Science and ICT, South Korea, Sorbonne Université, Horizon 2020 Framework Programme, Engineering and Physical Sciences Research Council, Science and Technology Facilities Council, Deutsches Elektronen-Synchrotron, Division of Chemistry, Lawrence Livermore National Laboratory
Openalex Percentile: Top 6%
nanoparticles nucleation surface interactions
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