Systematics Of Spin Crossovers Across The Rare-earth Cobaltites (RECoO3)

English Abstract:

Using first-principles plane-wave calculations, we investigate the structural and electronic properties of rare-earth cobaltites (RECoO₃). Structurally consistent Hubbard U treatment was shown to essential for proper description of strongly correlated cobalt-d electrons. We successfully capture the experimentally observed structural trends and give first-principles insights on interesting phenomena related with the cobalt spin state change. It was demonstrated that increase of crystal-field splitting energy between e_g-t_2g orbitals and shrinking of unoccupied σ*-bonding e_g bands are responsible for the increase of onset spin-state transition temperature along the series. We believe that Hubbard U values presented in this study will allow further predictive studies of cobaltites.