Inference of a "Hot Ice" Layer in Nitrogen-Rich Planets: Demixing the Phase Diagram and Phase Composition for Variable Concentration Helium-Nitrogen Mixtures Based on Isothermal Compression.

Van der Waals (vdW) chemistry in simple molecular systems may be important for understanding the structure and properties of the interiors of the outer planets and their satellites, where pressures are high and such components may be abundant. In the current study, Raman spectra and visual observation are employed to investigate the phase separation and composition determination for helium-nitrogen mixtures with helium concentrations from 20 to 95% along the 295 K isothermal compression. Fluid-fluid-solid triple-phase equilibrium and several equilibria of two phases including fluid-fluid and fluid-solid have been observed in different helium-nitrogen mixtures upon loading or unloading pressure. The homogeneous fluid in helium-nitrogen mixtures separates into a helium-rich fluid (F1) and a nitrogen-rich fluid (F2) with increasing pressure. The triple-phase point occurs at 295 K and 8.8 GPa for a solid-phase (N2)11He vdW compound, fluid F1 with around 50% helium, and fluid F2 with 95% helium. Helium concentrations of F1 coexisted with the (N2)11He vdW compound or δ-N2 in helium-nitrogen mixtures with different helium concentrations between 40 and 50% and between 20 and 40%, respectively. In addition, the helium concentration of F2 is the same in helium-nitrogen mixtures with different helium concentrations and decreases upon loading pressure. Pressure-induced nitrogen molecule ordering at 32.6 GPa and a structural phase transition at 110 GPa are observed in (N2)11He. In addition, at 187 GPa, a pressure-induced transition to an amorphous state is identified.