Density-functional study of perovskite-type hydride LiNiH and its synthesis; Mechanism for formation of metallic perovskite

Takagi, Shigeyuki*; Saito, Hiroyuki; Endo, Naruki; Sato, Ryutaro*; Ikeshoji, Tamio*; Matsuo, Motoaki*; Miwa, Kazutoshi*; Aoki, Katsutoshi; Orimo, Shinichi*

A metallic perovskite-type hydride LiNiH was synthesized based on first-principles prediction. We theoretically examined its electronic structure and found that half of the Ni-H derived antibonding states are occupied and that the modest thermodynamic stability depends on a delicate balance between (1) destabilization and (2) alleviation of compression frustration in corner-sharing octahedra, both of which arise from occupation of antibonding states. Through density-functional analyses of the electronic structure and lattice instability extending over LiH series ( = Fe, Co, Ni, and Cu), we showed that the balance is in fact reflected in their thermodynamic stability.