Cooperatively tuning magnetic anisotropy and colossal magnetoresistance via atomic-scale buffer layers in highly strained La_0.7Sr_0.3MnO₃ films

Achieving simultaneous control over multiple functional properties, such as magnetic anisotropy, magnetoresistance, and metal-insulator transition, with atomic precision remains a major challenge for realizing advanced spintronic functionalities. Here, we demonstrate a unique approach to cooperatively tune these multiple functional properties in highly strained La0.7Sr0.3MnO3 (LSMO) thin films. By inserting varying perovskite buffer layers, compressively strained LSMO films transition from a ferromagnetic insulator with out-of-plane magnetic anisotropy to a metallic state with in-plane anisotropy. Remarkably, atomic-scale control of the buffer layer thickness enables precise tuning of this magnetic and electronic phase transformation. We achieve a colossal magnetoresistance tuning of 10,000% and an exceptionally sharp transition from out-of-plane to in-plane magnetic anisotropy within just a few atomic layers. These results demonstrate an unprecedented level of control over multiple functional properties, paving the way for the rational design of multifunctional oxide spintronic devices.