Substitutional effect of Mg2+ on structural and magnetic properties of La2MgxNi1‐xMnO6 double‐perovskite thin films

By doping different concentrations of Mg2+ at Ni site, the (00l)‐oriented La2MgxNi1‐xMnO6 (abbreviated as LMxNMO, x = 0, 0.1, 0.2, 0.3, 0.4) double‐perovskite thin films were epitaxially grown by pulsed laser deposition. The substitutional effect of Mg2+ on the structural and magnetic properties of the films is comprehensively investigated. It is found that with the increase of Mg‐doping concentration, the in‐plane and out‐of‐plane lattice constants as well as the cell volume of the LMxNMO thin films increase, which could be ascribed to the radius difference between Mg2+ and Ni2+/Ni3+ ions, resulting in the in‐plane compressive stress in LMxNMO films. When the Mg‐doping concentration is small (x ≤ 0.1), the doped Mg2+ tends to substitute Ni3+, which restrains the intensity of antiferromagnetic interaction between Ni3+‐O‐Mn3+, resulting in the reduced the exchange bias field as well as the increased the saturation magnetization. However, when the Mg‐doping concentration increases to x ≥ 0.2, Mg2+ becomes to mainly replace Ni2+ position, which could inhibit the super‐exchange ferromagnetic interaction between Ni2+‐O‐Mn4+ magnetic paths and thus reduce the saturation magnetization. The enhanced magnetic properties can be obtained in the LM0.1NMO double‐perovskite thin film, with a large saturation magnetization of 492.12 emu/cm3 and a high Curie temperature of 262.7 K. Reciprocal space maps of (a) symmetry (002) plane of LM0.1NMO film and (b‐f) asymmetry (103) plane of LMxNMO films (x = 0–0.4)