Interfacial Electronic and Magnetic Reconstructions in Manganite/Titanate Superlattices

Abstract Complex oxide heterointerfaces provide a spacious arena for creating emergent phenomena that are unattainable in the constituent bulk counterparts. Herein, The BaTiO₃/La_1‐xSr_xMnO₃ [BTO/LSMO (x)] superlattice (SL) as a model system to investigate the intimately coupled interfacial effects and their resultant phenomena is focused on. The experimental and Density Functional Theory (DFT) calculations reveal that the induced magnetism on Ti originates from both the charge transfer process between Mn and Ti at the titanate/manganite heterointerfaces and the cation intermixing, both contributing comparably to the overall magnetic effect. Upon changing x, the orbital reconstruction of the Mn 3d electrons, tailored by the strain state of the LSMO (x) layers, efficiently modifies the magnetic exchange coupling between Mn–Ti and Mn–Mn at the interfaces, which are proved to account for the modulations of the macroscopic magnetism of the SLs. This work demonstrates the significance of interfacial reconstructions for magnetism, paving a new pathway to manipulate the magnetic properties of artificial oxide heterostructures.