Abstract
Compression of hydrogen-rich hydrides has been proposed as an alternative way to attain the atomic metallic hydrogen state or high-temperature superconductors. However, it remains a challenge to get access to these states by synthesizing novel polyhydrides with unusually high hydrogen-to-metal ratios. Here we synthesize a series of cerium (Ce) polyhydrides by a direct reaction of Ce and H2 at high pressures. We discover that cerium polyhydride CeH9, formed above 100 GPa, presents a three-dimensional hydrogen network composed of clathrate H29 cages. The electron localization function together with band structure calculations elucidate the weak electron localization between H-H atoms and confirm its metallic character. By means of Ce atom doping, metallic hydrogen structure can be realized via the existence of CeH9. Particularly, Ce atoms play a positive role to stabilize the sublattice of hydrogen cages similar to the recently discovered near-room-temperature lanthanum hydride superconductors.
Highlights
Compression of hydrogen-rich hydrides has been proposed as an alternative way to attain the atomic metallic hydrogen state or high-temperature superconductors
FeH5 prepared from a laser-heated diamond anvil cell (DAC) above 130 GPa have been proposed as a layered structure built of atomic hydrogen only[19]
The surprising high Tc near room temperature in lanthanum hydride is mainly attributed to an intriguing H clathrate structure with large H-derived electron density of states at Fermi level and the strong electron–phonon coupling related to H cages[21]
Summary
Compression of hydrogen-rich hydrides has been proposed as an alternative way to attain the atomic metallic hydrogen state or high-temperature superconductors. Metallization of solid hydrogen at 495 GPa has been reported, but such high pressure is a challenge for further experimental exploration[7]. At 3 GPa, just after the target sample loading into DAC, the diffraction pattern reveals that the sample crystallizes in a facecentered cubic (fcc) structure with the most possible space group Fm-3m (Supplementary Fig. 3).
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