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

Several multi‐hydrogen hydrides have exhibited high critical temperature (Tc) 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) Tc 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 Tc 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‐Tc superconductivity in hydrides. Contrary to the conventional design strategy of multi‐hydrogen covalent hydride superconductors at ultrahigh pressure about several hundred GPa, the novel few‐hydrogen metal‐bonded perovskite high‐Tc superconductors are designed at ambient pressure, of which ZnHAl3 perovskite is the only new Al‐based superconductor with both better ductility than multi‐hydrogen, cuprate and iron‐based superconductors and high Tc at 80 K above liquid‐nitrogen temperature.