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The asymmetry of chemical nature at the hetero-structural interface offers anunique opportunity to design desirable electronic structure by controllingcharge transfer and orbital hybridization across the interface. However, thecontrol of hetero-interface remains a daunting task. Here, we report themodulation of interfacial coupling of (La0.67Sr0.33MnO3)n/(SrTiO3)nsuperlattices by manipulating the periodic thickness with n unit cells ofSrTiO3 and n unit cells La0.67Sr0.33MnO3. The easy axis of magnetic anisotropyrotates from in-plane (n = 10) to out-of-plane (n = 2) orientation at 150 K.Transmission electron microscopy reveals enlarged tetragonal ratio > 1 withbreaking of volume conservation around the (La0.67Sr0.33MnO3)n/(SrTiO3)ninterface, and electronic charge transfer from Mn to Ti 3d orbitals across theinterface. Orbital hybridization accompanying the charge transfer results inpreferred occupancy of 3d3z2-r2 orbital at the interface, which induces astronger electronic hopping integral along the out-of-plane direction andcorresponding out-of-plane magnetic easy axis for n = 2. We demonstrate thatinterfacial orbital hybridization in superlattices of strongly correlatedoxides may be a promising approach to tailor electronic and magnetic propertiesin device applications.

Control of magnetic anisotropy by orbital hybridization in (La0.67Sr0.33MnO3)n/(SrTiO3)n superlattice