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Nuclear spin coupling crossover in dense molecular hydrogen

Thomas Meier (), Dominique Laniel, Miriam Pena-Alvarez, Florian Trybel, Saiana Khandarkhaeva, Alena Krupp, Jeroen Jacobs, Natalia Dubrovinskaia and Leonid Dubrovinsky
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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

Nature Communications, 2020, vol. 11, issue 1, 1-7

Abstract: 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.

Date: 2020
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DOI: 10.1038/s41467-020-19927-y

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