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    Tailoring noncollinear magnetism and 3d−4f exchange interactions in RVO3 epitaxial thin films

    Olivier Copie1,*, Julien Varignon2, Ingrid Cañero Infante3, Mariam Martirosyan1, Fadi Choueikani4, Philippe Ohresser4, Pierre-Eymeric Janolin5, Alain Pautrat2, Adrian David2 et al.

    Philippe Ghosez6 and Wilfrid Prellier2

    • *Contact author: olivier.copie@univ-lorraine.fr

    Phys. Rev. Materials 9, 064409 – Published 16 June, 2025

    DOI: https://doi.org/10.1103/blnj-pfm4

    Abstract

    In orthorhombic perovskite oxides (RMO3), substituting R3+ rare-earth cations tailors the spin, orbital, and charge degrees of freedom of the central M3+ transition metal cations through lattice distortions. In turn, these modify also the surrounding environment of R3+. When both R3+ and M3+ exhibit magnetic properties, phenomena such as spin reorientation and magnetization reversal can occur. In fact, the underlying exchange interactions between M−3d spins and R−4f magnetic moments enrich the multifunctional character of RMO3, 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 PrVO3 thin films, selectively probing the magnetism of cation sublattices, and uncovering simultaneous V3+3d spin reorientation and Pr3+4f magnetization reversal using spectroscopy techniques. By strain engineering, we manipulate the lattice distortions to rationalize their role in coupling 3d spins and 4f 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 RMO3 systems, advancing the understanding of controlling spins in engineered perovskite heterostructures and superlattices.

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