Stable Solid Molecular Hydrogen above 900 K from a Machine-Learned Potential Trained with Diffusion Quantum Monte Carlo

We survey the phase diagram of high-pressure molecular hydrogen with path integral molecular dynamics using a machine-learned interatomic potential trained with quantum Monte Carlo forces and energies. Besides the HCP and C2/c-24 phases, we find two new stable phases both with molecular centers in the Fmmm-4 structure, separated by a molecular orientation transition with temperature. The high temperature isotropic Fmmm-4 phase has a reentrant melting line with a maximum at higher temperature (1450 K at 150 GPa) than previously estimated and crosses the liquid-liquid transition line around 1200 K and 200 GPa.

Automated summary

We investigate the phase diagram of high-pressure molecular hydrogen using molecular dynamics and machine learning techniques. Our results reveal two new stable phases with a Fmmm-4 structure, and we observe a molecular orientation transition with temperature. The isotropic Fmmm-4 phase exhibits a reentrant melting line with a maximum temperature (1450 K at 150 GPa) higher than previously estimated, and it also crosses the liquid-liquid transition line around 1200 K and 200 GPa.