Ultrafast Yttrium Hydride Chemistry at High Pressures via Non-equilibrium States Induced by an X-ray Free Electron Laser
Controlling the formation and stoichiometric content of the desired phases of materials has become of central interest for a variety of fields. The possibility of accessing metastable states by initiating reactions by X-ray-triggered mechanisms over ultrashort time scales has been enabled by the development of X-ray free electron lasers (XFELs). Utilizing the exceptionally high-brilliance X-ray pulses from the EuXFEL, we report the synthesis of a previously unobserved yttrium hydride under high pressure, along with nonstoichiometric changes in hydrogen content as probed at a repetition rate of 4.5 MHz using time-resolved X-ray diffraction. Exploiting non-equilibrium pathways, we synthesize and characterize a hydride in a Weaire-Phelan structure type at pressures as low as 125 GPa, predicted using a crystal structure search, with a hydrogen content of 4.0-5.75 hydrogens per cation, that is enthalpically metastable on the convex hull.
Authors
- Stephan Kuschel (ORCID: https://orcid.org/0000-0001-5159-525X)
- Dean F. Smith (ORCID: https://orcid.org/0000-0001-5491-747X)
- Chris J. Pickard (ORCID: https://orcid.org/0000-0002-9684-5432)
- Zuzana Konôpková
- Sylvain Petitgirard (ORCID: https://orcid.org/0000-0001-9838-1742)
- Sergio Villa-Cortes
- M. Nakatsutsumi (ORCID: https://orcid.org/0000-0003-0868-4745)
- Torsten Laurus (ORCID: https://orcid.org/0000-0002-2258-2123)
- 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)
- Lewis J. Conway (ORCID: https://orcid.org/0000-0001-7039-6045)
- Carsten Baehtz (ORCID: https://orcid.org/0000-0003-1480-511X)
- Emily Siska (ORCID: https://orcid.org/0000-0002-2348-201X)
- S. M. A. Hosseini‐Saber (ORCID: https://orcid.org/0000-0001-7594-555X)
- G. Alexander Smith (ORCID: https://orcid.org/0000-0001-9701-1328)
- V. Bouffetier (ORCID: https://orcid.org/0000-0001-6079-1260)
- Ashkan Salamat (ORCID: https://orcid.org/0000-0001-6556-7532)
- U. Zastrau (ORCID: https://orcid.org/0000-0002-3575-4449)
- Tais Gorkhover (ORCID: https://orcid.org/0009-0001-8804-1186)
- Keith V. Lawler (ORCID: https://orcid.org/0000-0003-1087-5815)
- Valerio Cerantola (ORCID: https://orcid.org/0000-0002-2808-2963)
- Joshua Van Cleave
- Craig P. Schwartz (ORCID: https://orcid.org/0000-0002-4149-2684)
- J. Sztuk-Dambietz
- Sebastian Göde
Institutions
- University of Nevada, Las Vegas (US)
- Universität Hamburg (DE)
- Tohoku University (JP)
- University of Cambridge (GB)
- Deutsches Elektronen-Synchrotron DESY (DE)
- ETH Zurich (CH)
- University of Milano-Bicocca (IT)
- European X-Ray Free-Electron Laser (DE)
Publication Details
- Journal
- The Journal of Physical Chemistry Letters
- Published
- 2024-09-20
- DOI
- https://doi.org/10.1021/acs.jpclett.4c02134
- Citations
- 11
- Primary Topic
- High-pressure geophysics and materials
- Type
- article
- Field-Weighted Citation Impact
- 5.34
Funders
- Gordon and Betty Moore Foundation
- Engineering and Physical Sciences Research Council
- Science and Technology Facilities Council
- Basic Energy Sciences