Nuclear spin coupling crossover in dense molecular hydrogen

• 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 H-2 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 123GPa at room temperature. While our measurements confirm the presence of ortho-hydrogen at low pressures, above 70GPa, 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. Solid hydrogen has increasingly hindered rotation under high pressure, but the effect on spin isomer populations had not been directly probed. Here the authors measure NMR spectra of solid hydrogen up to the megabar, and observe the crossover to a spin 1/2 dipolar system above 70GPa where distinction between ortho and para spin isomers is lost.

Subject headings

NATURVETENSKAP  -- Fysik -- Den kondenserade materiens fysik (hsv//swe)

NATURAL SCIENCES  -- Physical Sciences -- Condensed Matter Physics (hsv//eng)

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