Tailoring noncollinear magnetism and exchange interactions in epitaxial thin films
Phys. Rev. Materials 9, 064409 – Published 16 June, 2025
DOI: https://doi.org/10.1103/blnj-pfm4
Abstract
In orthorhombic perovskite oxides (), substituting rare-earth cations tailors the spin, orbital, and charge degrees of freedom of the central transition metal cations through lattice distortions. In turn, these modify also the surrounding environment of . When both and exhibit magnetic properties, phenomena such as spin reorientation and magnetization reversal can occur. In fact, the underlying exchange interactions between spins and magnetic moments enrich the multifunctional character of , particularly when combined with structural distortions. They play a crucial role in achieving appealing properties such as robust magnetoelectricity with noncollinear magnetic orders. Here, we explore the exchange coupling in epitaxial thin films, selectively probing the magnetism of cation sublattices, and uncovering simultaneous spin reorientation and magnetization reversal using spectroscopy techniques. By strain engineering, we manipulate the lattice distortions to rationalize their role in coupling spins and magnetic moments. Theorectical calculations show that octahedral rotations and Jahn-Teller distortions act as tuning mechanisms, promoting competition between orbital and spin orders. The observed coupling between magnetic cations and lattice distortions can be extended to other orthorhombic systems, advancing the understanding of controlling spins in engineered perovskite heterostructures and superlattices.