Ji, Cheng
; Li, Bing
; Luo, Jie
; ... - Nature (London)
The structural evolution of molecular hydrogen H
2 under multi-megabar compression and its relation to atomic metallic hydrogen is a key unsolved problem in condensed-matter physics. Although dozens of crystal structures have been proposed by theory, only one, the simple hexagonal-close-packed (hcp) structure of only spherical disordered H
2, has been previously confirmed in experiments. Through advancing nano-focused synchrotron X-ray probes, here we report the observation of the transition from hcp H
2 to a post-hcp structure with a six-fold larger supercell at pressures above 212 GPa, indicating the change of spherical H
2 to various ordered configurations. Theoretical calculations based on our XRD
more » results found a time-averaged structure model in the space group $$P\bar{6}2c$$ with alternating layers of spherically disordered H2 and new graphene-like layers consisting of H2 trimers (H6) formed by the association of three H2 molecules. Here, this supercell has not been reported by any previous theoretical study for the post-hcp phase, but is close to a number of theoretical models with mixed-layer structures. The evidence of a structural transition beyond hcp establishes the trend of H2 molecular association towards polymerization at extreme pressures, giving clues about the nature of the molecular-to-atomic transition of metallic hydrogen. Considering the spectroscopic behaviours that show strong vibrational and bending peaks of H2 up to 400 GPa, it would be prudent to speculate the continuation of hydrogen molecular polymerization up to its metallization.« less