H 2 Chemical Bond in a High-Pressure Crystalline Environment.
Miriam MarquésMiriam Peña-AlvarezMiguel Martínez-CanalesGraeme J AcklandPublished in: The journal of physical chemistry. C, Nanomaterials and interfaces (2023)
We show that the hydrogen in metal superhydride compounds can adopt two distinct states-atomic and molecular. At low pressures, the maximum number of atomic hydrogens is typically equal to the valency of the cation; additional hydrogens pair to form molecules with electronic states far below the Fermi energy causing low-symmetry structures with large unit cells. At high pressures, molecules become unstable, and all hydrogens become atomic. This study uses density functional theory, adopting BaH 4 as a reference compound, which is compared with other stoichiometries and other cations. Increased temperature and zero-point motion also favor high-symmetry atomic states, and picosecond-timescale breaking and remaking of the bond permutations via intermediate H 3 - units.