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

The chemical asymmetry at the hetero-structure interface offers an effective opportunity to design desirable electronic structures by controlling charge transfer and orbital hybridization across the interface. However, controlling the hetero-interface remains a daunting task. Here, we report the modulation of interfacial coupling of (La0.67Sr0.33MnO3)n/(SrTiO3)n superlattices by manipulating the periodic thickness with n unit cells of SrTiO3 and n unit cells of La0.67Sr0.33MnO3 with a fixed thickness of ~120 unit cells. The easy axis of magnetic anisotropy rotates ~45° towards the out-of-plane direction from n = 10 to n = 2 at reduced temperature TRe = T/TS = 0.87, where TS is the temperature at the onset of magnetization. Transmission electron microscopy reveals an enlarged tetragonal ratio >1 with breaking of volume conservation around the (La0.67Sr0.33MnO3)n/(SrTiO3)n interface and electronic charge transfer from Mn to Ti 3d orbitals across the interface. Orbital hybridization accompanying the charge transfer results in preferred occupancy of $${3d}_{3z^2-r^2}$$ 3 d 3 z 2 - r 2 orbitals at the interface and induces a stronger electronic hopping integral and interfacial magnetic anisotropy along the out-of-plane direction, which contributes to the rotation towards the out-of-plane direction of an effective magnetic easy axis for n = 2. We demonstrate that interfacial orbital hybridization with charge transfer in the superlattice of strongly correlated oxides may be a promising approach to tailor electronic and magnetic properties in device applications.