Route to achieving perfect B-site ordering in double perovskite thin films

Double perovskites (DP, A2BB’O6) exhibit a breadth of multifunctional properties with a huge potential range of applications, including magneto-optic and spintronic devices. However, spontaneous cation ordering is limited by the similar size and charge of B and B’ cations. We introduce a route to stimulate B-site rock-salt ordering. By growing thin films on (111)-oriented substrates, ‘in-plane’ strain acts on the intrinsically tilted oxygen octahedra of the DP and produces two different B-site cages (in size and shape), stimulating spontaneous cation ordering. For the ferromagnetic insulator La2CoMnO6, clear Co/Mn ordering was achieved by growing on (111)-oriented substrates. The difference in B-site cages was further enhanced when grown under minor (111) in-plane compressive strain, resulting in long-range ordering with a saturation magnetization of 5.8 μB/formula unit (f.u.), close to the theoretical 6 μB/f.u., without antiferromagnetic behavior. Our approach enables the study of many new ordered DPs which have never been made before.