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

R. J. Husband (), H. P. Liermann, J. D. McHardy, R. S. McWilliams, A. F. Goncharov, V. B. Prakapenka, E. Edmund, S. Chariton, Z. Konôpková, C. Strohm, C. Sanchez-Valle, M. Frost, L. Andriambariarijaona, K. Appel, C. Baehtz, O. B. Ball, R. Briggs, J. Buchen, V. Cerantola, J. Choi, A. L. Coleman, H. Cynn, A. Dwivedi, H. Graafsma, H. Hwang, E. Koemets, T. Laurus, Y. Lee, X. Li, H. Marquardt, A. Mondal, M. Nakatsutsumi, S. Ninet, E. Pace, C. Pepin, C. Prescher, S. Stern, J. Sztuk-Dambietz, U. Zastrau and M. I. McMahon ()
Additional contact information
R. J. Husband: Deutsches Elektronen-Synchrotron DESY
H. P. Liermann: Deutsches Elektronen-Synchrotron DESY
J. D. McHardy: The University of Edinburgh
R. S. McWilliams: The University of Edinburgh
A. F. Goncharov: Earth and Planets Laboratory
V. B. Prakapenka: Center for Advanced Radiation Sources
E. Edmund: Earth and Planets Laboratory
S. Chariton: Center for Advanced Radiation Sources
Z. Konôpková: European XFEL
C. Strohm: Deutsches Elektronen-Synchrotron DESY
C. Sanchez-Valle: Institut für Mineralogie, Corrensstraße 24
M. Frost: SLAC National Accelerator Laboratory
L. Andriambariarijaona: Sorbonne Université
K. Appel: European XFEL
C. Baehtz: Helmholtz-Zentrum Dresden-Rossendorf, Bautzner Landstraße 400
O. B. Ball: The University of Edinburgh
R. Briggs: Lawrence Livermore National Laboratory
J. Buchen: University of Oxford
V. Cerantola: European XFEL
J. Choi: Yonsei University
A. L. Coleman: Lawrence Livermore National Laboratory
H. Cynn: Lawrence Livermore National Laboratory
A. Dwivedi: European XFEL
H. Graafsma: Deutsches Elektronen-Synchrotron DESY
H. Hwang: Deutsches Elektronen-Synchrotron DESY
E. Koemets: University of Oxford
T. Laurus: Deutsches Elektronen-Synchrotron DESY
Y. Lee: Yonsei University
X. Li: Deutsches Elektronen-Synchrotron DESY
H. Marquardt: University of Oxford
A. Mondal: Institut für Mineralogie, Corrensstraße 24
M. Nakatsutsumi: European XFEL
S. Ninet: Sorbonne Université
E. Pace: The University of Edinburgh
C. Pepin: Laboratoire Matière en Conditions Extrêmes
C. Prescher: University of Freiburg
S. Stern: Deutsches Elektronen-Synchrotron DESY
J. Sztuk-Dambietz: European XFEL
U. Zastrau: European XFEL
M. I. McMahon: The University of Edinburgh

Nature Communications, 2024, vol. 15, issue 1, 1-13

Abstract: Abstract H2O 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 H2O, 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 H2O 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.

Date: 2024
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DOI: 10.1038/s41467-024-52505-0

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