Understanding the Magnetic Puzzles of Double Perovskites A2FeOsO6 (A=Ca, Sr)

Abstract: Double perovskites Sr2FeOsO6 and Ca2FeOsO6 show puzzling magnetic properties, the former a low-temperature antiferromagnet while the later a high-temperature insulating ferrimagnet. Here, in order to understand the underlying mechanism, we have investigated the frustrated magnetism of A2FeOsO6 by employing density functional theory and maximally-localized Wannier functions. We find that lattice distortion enhances the antiferromagnetic nearest-neighboring Fe-O-Os interaction but weakens the antiferromagnetic interactions through the Os-O-O-Os and Fe-O-Os-O-Fe paths, which is responsible for the magnetic transition from the low-temperature antiferromagnetism to the high-temperature ferrimagnetism with the decrease of the radius of the A2+ ions. We also discuss the 5d3-3d5 superexchange and propose such superexchange is intrinsically antiferromagnetic instead of the expected ferromagnetic. Our work illustrate that the magnetic frustration can be effectively relieved by lattice distortion, which provides another dimension to tune the complex magnetism in other 3d-5d (4d) double perovskites.