Interfacial Engineering of Ferromagnetism in Epitaxial Manganite/Ruthenate Superlattices via Interlayer Chemical Doping

Interfacial charge transfer and structural proximity effects are the two essential routes to trigger and tune numerous functionalities of perovskite oxide heterostructures. However, the cooperation and competition of these two interfacial effects in one epitaxial system have not been fully understood. Herein, we fabricate a series of La0.67Ca0.33MnO3/CaRuO3 superlattices and introduce various chemical doping in the nonmagnetic CaRuO3 interlayers. We found that Ti, Sr, and La doping in the CaRuO3 layer can effectively tune the interfacial charge transfer and octahedral rotation, thus modulating the ferromagnetism of the superlattices. Specifically, the B-site Ti doping depletes the Ru 4d band and suppresses the interfacial charge transfer, leading to a decay of ferromagnetic Curie temperature (TC). In contrast, the A-site Sr doping maintains a sizable charge transfer and meanwhile suppresses the octahedral rotation, which facilitates ferromagnetism and significantly enhances the TC up to 291 K. The La doping turns out to localize the itinerant electrons in the CaRuO3 layer, which suppresses both the interfacial charge transfer and ferromagnetism. The observed intriguing interfacial engineering of magnetism would pave a new way to understand the collective effects of interfacial charge transfer and structural proximity on the physical properties of oxide heterostructures.