Oxygen Vacancy Ordering Modulation of Magnetic Anisotropy in Strained LaCoO3–x Thin Films

Oxygen vacancy configurations and concentration are coupled with the magnetic, electronic, and transport properties of perovskite oxides, and manipulating the physical properties by tuning the vacancy structures of thin films is crucial for applications in many functional devices. In this study, we report a direct atomic resolution observation of the preferred orientation of vacancy ordering structure in the epitaxial LaCoO3- x (LCO) thin films under various strains from large compressive to large tensile strain utilizing scanning transmission electron microscopy (STEM). Under compressive strains, the oxygen vacancy ordering prefers to be along the planes parallel to the heterointerface. Changing the strains from compressive to tensile, the oxygen vacancy planes turn to be perpendicular to the heterointerface. Aberration-corrected STEM images, electron diffractions, and X-ray diffraction combined with X-ray photoelectron spectroscopy demonstrate that the vacancy concentration increases with increasing misfit strains and vacancy distribution is more ordered and homogeneous. The temperature-dependent magnetization curves show the Curie temperature increases, displaying a positive correlation with the misfit strains. With change in the strain from compressive to tensile, anisotropy fields vary and show large values under tensile strains. It is proposed that oxygen vacancy concentration and preferred ordering planes are responsible for the enhanced magnetic properties of LCO films. Our results have realized a controllable preparation of oxygen vacancy ordering structures via strains and thus provide an effective method to regulate and optimize the physical properties such as magnetic properties by strain engineering.