Hydrogen Reorganization in Hot Dense Ammonia

Abstract: Hydrogen is known to form stable compounds with a variety of simple molecular solids under high pressure. However, ammonia hydride has not been experimentally observed. Here, through a series of laser-heating diamond anvil cell (LHDAC) experiments, we observed the transparent ionic ammonia transformed into an opaque phase above 150 GPa and 1000 K. Raman spectroscopy reveals a pronounced structural change, accompanied by the emergence of two distinct asymmetric H$_2$ vibrons ($ν_1$ and $ν_2$). A new ionic phase produced following thermally induced dissociation and hydrogen reorganization in hot dense ammonia. The combination of experimental results and first-principles calculations identify this phase as the theoretically predicted ionic $P4_12_12$ phase of NH$_7$ , which consists of NH$_4<sup>+$, H$<sup>-$and H$_2$ units. Our results suggest that the formation of ammonia hydrides follows a thermodynamic pathway distinct from those of other H$_2$-containing mixtures, revealing a new ionic transformation pathway driven by hydrogen reorganization in hot dense ammonia.