High‐Throughput Study of Ambient‐Pressure High‐Temperature Superconductivity in Ductile Few‐Hydrogen Metal‐Bonded Perovskites

Abstract Several multi‐hydrogen hydrides have exhibited high critical temperature (T_c) superconductivity, but the requirement for ultrahigh pressures limits their applications. Here, high‐throughput calculations are utilized to investigate the superconductivity in few‐hydrogen metal‐bonded (FHMB) perovskites (PVSKs) AHM₃ characterized with perfect ambient‐pressure stability. AHM₃ is classified into two groups, d and sp superconductors, and provide three indicators that accurately describe AHM₃ superconductivity. i) T_c of d superconductors is positively correlated with the number of unpaired d electrons from M atoms; ii) A suitably sized octahedral interstice of H atom is essential for sp superconductors; iii) The introduction of H will further improve the superconductivity, when the M atom has a lower electronegativity than H. ZnHCr₃ and ZnHAl₃, perfectly meeting the requirements aforementioned, exhibit the highest T_c of 30 and 80 K among the d and sp superconductors, respectively. The results are helpful for understanding the electron–phonon coupling (EPC) mechanism in few‐hydrogen metal‐bonded perovskites and facilitate realizations of ambient‐pressure high‐T_c superconductivity in hydrides.