Origins of multi-sublattice magnetism and superexchange interactions in double-double perovskite CaMnCrSbO6 (2205.02452v2)

Abstract: We have deployed density functional theory, Wannier function analysis and mean-field calculations to investigate the double-double perovskite compound CaMnCrSbO_{6}. The crystallographically non-equivalent Mn atoms in the unit cell have tetrahedral and planar oxygen coordinations (labelled as Mn(1) and Mn(2)), while the Cr atom is in the centre of distorted oxygen octahedron. While the bulk magnetization and neutron diffraction suggest a simpler ferrimagnetic order (T_C=49 K) between Mn2+ and Cr3+ spins, the exchange interactions are more complex than that expected from a two sublattice magnetic system. The electronic structure calculations yield a ferrimagnetic insulating ground state even in absence of Hubbard U which persists for a wide range of U. The Mn(1)-O-Mn(2) (out of plane and in-plane), Mn(1)-O-Cr and Mn(2)-O-Cr superexchange interactions are found to be anti-ferromagnetic, while the Cr-O-O-Cr super-superexchange is found to be ferromagnetic. The Mn(2)-O-Cr superexchange is weaker than the Mn(1)-O-Cr superexchange, thus effectively resulting in ferrimagnetism. From a simple 3-site Hubbard model, we derived expressions for the antiferromagnetic superexchange strength J_AFM and the weaker ferromagnetic J_FM. The relative strengths of JAFM for the various superexchange interactions are in agreement with those obtained from DFT. The expression for Cr-O-O-Cr super-superexchange strength (J_SS), which is derived considering a 4-site Hubbard model, predicts a ferromagnetic exchange in agreement with DFT. Finally, our mean field calculations reveal that assuming a set of four magnetic sub-lattice for Mn2+ spins and a single magnetic sublattice for Cr3+ spins yields a much improved T_C, while a simple two magnetic sublattice model yields a much higher T_C.