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Double perovskites Sr2FeOsO6 and Ca2FeOsO6 show puzzling magnetic properties,the former a low-temperature antiferromagnet while the later a high-temperatureinsulating ferrimagnet. Here, in order to understand the underlying mechanism,we have investigated the frustrated magnetism of A2FeOsO6 by employing densityfunctional theory and maximally-localized Wannier functions. We find thatlattice distortion enhances the antiferromagnetic nearest-neighboring Fe-O-Osinteraction but weakens the antiferromagnetic interactions through theOs-O-O-Os and Fe-O-Os-O-Fe paths, which is responsible for the magnetictransition from the low-temperature antiferromagnetism to the high-temperatureferrimagnetism with the decrease of the radius of the A2+ ions. We also discussthe 5d3-3d5 superexchange and propose such superexchange is intrinsicallyantiferromagnetic instead of the expected ferromagnetic. Our work illustratethat the magnetic frustration can be effectively relieved by latticedistortion, which provides another dimension to tune the complex magnetism inother 3d-5d (4d) double perovskites.

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