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The high-pressure phases of solid hydrogen are of fundamental interest andrelevant to the interior of giant planets; however, knowledge of these phasesis far from complete. Particle swarm optimization (PSO) techniques were appliedto a structural search, yielding hitherto unexpected high-pressure phases ofsolid hydrogen at pressures up to 5 TPa. An exotic quasi-molecular mC24structure (space group C2/c, stable at 0.47-0.59 TPa) with two types ofintramolecular bonds was predicted, providing a deeper understanding ofmolecular dissociation in solid hydrogen, which has been a mystery for decades.We further predicted the existence of two atomic phases: (i) the oC12 structure(space group Cmcm, stable at > 2.1 TPa), consisting of planar H3 clusters, and(ii) the cI16 structure, previously observed in lithium and sodium, stableabove 3.5 TPa upon consideration of the zero-point energy. This work clearlyrevised the known zero-temperature and high-pressure (>0.47 TPa) phase diagramfor solid hydrogen and has implications for the constituent structures of giantplanets.

Quasi-molecular and atomic phases of dense solid hydrogen