Understanding Magnetism in Double Double Perovskites: A Complex Multiple Magnetic Sublattice System

Abstract: Understanding magnetism in multiple magnetic sublattice system, driven by the interplay of varied nature of magnetic exchanges, is on one hand challenging and on other hand intriguing. Motivated by the recent synthesis of AA'BB'O_6 double double perovskites with multiple magnetic ions both at A- and B-sites, we investigate the mechanism of magnetic behavior in these interesting class of compounds. We find that the magnetism in such multiple sublattice compounds is governed by the interplay and delicate balance between two distinct mechanisms, a) kinetic energy-driven multiple sublattice double exchange mechanism and b) the conventional super-exchange mechanism. The derived spin Hamiltonian based on first-principles calculations is solved by the classical Monte Carlo technique which reproduces the observed magnetic properties. Finally, the influence of off-stoichiometry, as in experimental samples, is discussed. Some of these double double perovskite compounds are found to possess large total magnetic moment and also are found to be half-metallic, which raises the hope of future applications of these large magnetic moment half-metallic oxides in spintronics and memory devices.