We report on the atomic ordering of B-site transition metals and magnetic properties of epitaxial La2CrFeO6 double-perovskite films grown by pulsed-laser deposition under various conditions. The highest-ordered sample exhibited a fraction of antisite disorder of only 0.05 and a saturation magnetization of ∼2 μB per formula unit at 5 K. The result is consistent with the antiferromagnetic ordering of local spin moment (3d3↓3d5↑; S = −3/2 + 5/2 = 1). Therefore, the magnetic ground state of La2CrFeO6 double perovskite that has been long debated is unambiguously revealed to be ferrimagnetic. Our results present a wide opportunity to explore novel magnetic properties of binary transition-metal perovskites upon epitaxial stabilization of the ordered phase.
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