Insulator–metal transition driven by pressure and B‐site disorder in double perovskite La2CoMnO6

The ground state of double perovskite oxide La₂CoMnO₆ (LCMO) and how it is influenced by external pressure and antisite disorder are investigated systematically by first‐principles calculations. We find, on the consideration of both the electron correlation and spin–orbital coupling effect, that the LCMO takes on insulating nature, yet is transformed to half metallicity once the external pressure is introduced. Such tuning is accompanied by a spin‐state transition of Co²⁺ from the high‐spin state (te) to low‐spin state (te) because of the enhancement of crystal‐field splitting under pressure. Using mean‐field approximation theory, Curie temperature of LCMO with Co²⁺ being in low‐spin state is predicted to be higher than that in high‐spin state, which is attributed to the enhanced ferromagnetic double exchange interaction arising from the shrinkage of Co? O and Mn? O bonds as well as to the increase in bond angle of Co? O? Mn under pressure. We also find that antisite disorder in LCMO enables such transition from insulating to half‐metallic state as well, which is associated with the spin‐state transition of antisite Co from high to low state. It is proposed that the substitution of La³⁺ for the rare‐earth (RE) ions with smaller ionic radii could open up an avenue to induce a spin‐state transition of Co, rendering thereby the RE₂CoMnO₆ a promising half‐metallic material. © 2012 Wiley Periodicals, Inc.