Polyhydride CeH9 with an atomic-like hydrogen clathrate structure

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.