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Nuclear spin coupling crossover in dense molecular hydrogen

Author

Listed:
  • Thomas Meier

    (Bayerisches Geoinstitut, University of Bayreuth)

  • Dominique Laniel

    (Material Physics and Technology at Extreme Conditions, Laboratory of Crystallography, University of Bayreuth)

  • Miriam Pena-Alvarez

    (Centre for Science at Extreme Conditions and School of Physics and Astronomy, University of Edinburgh)

  • Florian Trybel

    (Bayerisches Geoinstitut, University of Bayreuth)

  • Saiana Khandarkhaeva

    (Bayerisches Geoinstitut, University of Bayreuth)

  • Alena Krupp

    (Bayerisches Geoinstitut, University of Bayreuth)

  • Jeroen Jacobs

    (European Synchrotron Radiation Facility (ESRF))

  • Natalia Dubrovinskaia

    (Material Physics and Technology at Extreme Conditions, Laboratory of Crystallography, University of Bayreuth)

  • Leonid Dubrovinsky

    (Bayerisches Geoinstitut, University of Bayreuth)

Abstract

One of the most striking properties of molecular hydrogen is the coupling between molecular rotational properties and nuclear spin orientations, giving rise to the spin isomers ortho- and para-hydrogen. At high pressure, as intermolecular interactions increase significantly, the free rotation of H2 molecules is increasingly hindered, and consequently a modification of the coupling between molecular rotational properties and the nuclear spin system can be anticipated. To date, high-pressure experimental methods have not been able to observe nuclear spin states at pressures approaching 100 GPa (Meier, Annu. Rep. NMR Spectrosc. 94:1–74, 2017; Meier, Prog. Nucl. Magn. Reson. Spectrosc. 106–107:26–36, 2018) and consequently the effect of high pressure on the nuclear spin statistics could not be directly measured. Here, we present in-situ high-pressure nuclear magnetic resonance data on molecular hydrogen in its hexagonal phase I up to 123 GPa at room temperature. While our measurements confirm the presence of ortho-hydrogen at low pressures, above 70 GPa, we observe a crossover in the nuclear spin statistics from a spin-1 quadrupolar to a spin-1/2 dipolar system, evidencing the loss of spin isomer distinction. These observations represent a unique case of a nuclear spin crossover phenomenon in quantum solids.

Suggested Citation

  • Thomas Meier & Dominique Laniel & Miriam Pena-Alvarez & Florian Trybel & Saiana Khandarkhaeva & Alena Krupp & Jeroen Jacobs & Natalia Dubrovinskaia & Leonid Dubrovinsky, 2020. "Nuclear spin coupling crossover in dense molecular hydrogen," Nature Communications, Nature, vol. 11(1), pages 1-7, December.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-19927-y
    DOI: 10.1038/s41467-020-19927-y
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    Cited by:

    1. Dominique Laniel & Florian Trybel & Bjoern Winkler & Florian Knoop & Timofey Fedotenko & Saiana Khandarkhaeva & Alena Aslandukova & Thomas Meier & Stella Chariton & Konstantin Glazyrin & Victor Milman, 2022. "High-pressure synthesis of seven lanthanum hydrides with a significant variability of hydrogen content," Nature Communications, Nature, vol. 13(1), pages 1-9, December.

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