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Abstract Many planets in the solar system and across the Galaxy have hydrogen-rich atmospheres overlying more heavy element-rich interiors with which they interact for billions of years. Atmosphere–interior interactions are thus crucial to understanding the formation and evolution of these bodies. However, this understanding is still lacking in part because the relevant pressure–temperature conditions are extreme. We conduct molecular dynamics simulations based on density functional theory to investigate how hydrogen and water interact over a wide range of pressure and temperature, encompassing the interiors of Neptune-sized and smaller planets. We determine the critical curve at which a single homogeneous phase exsolves into two separate hydrogen-rich and water-rich phases, finding good agreement with existing experimental data. We find that the temperature along the critical curve increases with increasing pressure and shows the influence of a change in fluid structure from molecular to atomic near 30 GPa and 3000 K, which may impact magnetic field generation. The internal temperatures of many exoplanets, including TOI-270 d and K2-18 b, may lie entirely above the critical curve: the envelope is expected to consist of a single homogeneous hydrogen–water fluid, which is much less susceptible to atmospheric loss as compared with a pure hydrogen envelope. As planets cool, they cross the critical curve, leading to rainout of water-rich fluid and an increase in internal luminosity. Compositions of the resulting outer, hydrogen-rich and inner, water-rich envelopes depend on age and instellation and are governed by thermodynamics. Rainout of water may be occurring in Uranus and Neptune at present. 

Abstract We investigate the consequences of nonideal chemical interaction between silicate and overlying hydrogen-rich envelopes for rocky planets using basic tenets of phase equilibria. Based on our current understanding of the temperature and pressure conditions for complete miscibility of silicate and hydrogen, we find that the silicate-hydrogen binary solvus will dictate the nature of atmospheres and internal layering in rocky planets that garnered H₂-rich primary atmospheres. The temperatures at the surfaces of supercritical magma oceans will correspond to the silicate-hydrogen solvus. As a result, the radial positions of supercritical magma ocean–atmosphere interfaces, rather than their temperatures and pressures, should reflect the thermal states of these planets. The conditions prescribed by the solvus influence the structure of the atmosphere, and thus the transit radii of sub-Neptunes. Separation of iron-rich metal to form metal cores in sub-Neptunes and super-Earths is not assured due to prospects for neutral buoyancy of metal in silicate melt induced by dissolution of H, Si, and O in the metal at high temperatures.