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Abstract The X₂MH₆family, consisting of an electropositive cation Xⁿ⁺and a main group metal M octahedrally coordinated by hydrogen, have been identified as promising templates for high‐temperature conventional superconductivity. Herein, we analyze the electronic structure of two members of this family, Mg₂IrH₆and Ca₂IrH₆, showing why the former may possess superconducting properties rivaling those of the cuprates, whereas the latter does not. Within Mg₂IrH₆the vibrations of the anions IrH₆⁴⁻anions are key for the superconducting mechanism, and they induce coupling in the set of orbitals, which are antibonding between the H 1sand the Ir or orbitals. Because calcium possesses low‐lyingd‐orbitals, →Cadback‐donation is preferred, quenching the superconductivity. Our analysis explains why high critical temperatures were only predicted for second or third row X metal atoms, and may provide rules for identifying likely high‐temperature superconductors in other systems where the antibonding anionic states are filled. 

Through laser-heated diamond anvil cell experiments, we synthesize a series of rubidium superhydrides and explore their properties with synchrotron x-ray powder diffraction and Raman spectroscopy measurements, combined with density functional theory calculations. Upon heating rubidium monohydride embedded in ${\mathrm{H}}_2$at a pressure of 18 GPa, we form ${\mathrm{RbH}}_9\text{−}\mathrm{I}$, which is stable upon decompression down to 8.7 GPa, the lowest stability pressure of any known superhydride. At 22 GPa, another polymorph, ${\mathrm{RbH}}_9\text{−}\mathrm{II}$is synthesised at high temperature. Unique to the Rb-H system among binary metal hydrides is that further compression does not promote the formation of polyhydrides with higher hydrogen content. Instead, heating above 87 GPa yields ${\mathrm{RbH}}_5$, which exhibits two polymorphs ( ${\mathrm{RbH}}_5\text{−}\mathrm{I}$and ${\mathrm{RbH}}_5\text{−}\mathrm{II}$). All of the crystal structures comprise a complex network of quasimolecular ${\mathrm{H}}_2$units and ${\mathrm{H}}^{-}$anions, with ${\mathrm{RbH}}_5$providing the first experimental evidence of linear ${\mathrm{H}}_3^{-}$anions. Published by the American Physical Society2025