Oxygen-Mediated Electronic Reconstruction and Element-Selective Magnetism in Sr-Based High-Entropy Perovskite Oxide Thin Films

Abstract

High-entropy perovskite oxides offer a promising platform for tailoring magnetic functionality through compositional complexity; however, it remains unclear how targeted substitution of 4d transition metals modifies oxygen-mediated electronic structure and element-specific magnetic interactions. To address this question, we investigate the effect of Mo and Ru substitution on the electronic structure and magnetism of high-entropy perovskite oxide thin films using O K-edge and transition-metal L-edge X-ray absorption spectroscopy, X-ray magnetic circular dichroism (XMCD), and X-ray linear dichroism. O K-edge spectra reveal that Ru enhances O 2p–metal d hybridization, whereas Mo modifies charge distribution and local exchange pathways within the transition-metal sublattice. Multiplet analysis shows that Mn and Ni retain stable Mn4+ and Ni2+ states, while Co acts as the primary charge-compensation reservoir through changes in the Co2+/Co3+ ratio. Temperature-dependent XMCD demonstrates that these substitutions selectively reshape the magnetic exchange network, redistributing spin polarization among the constituent elements. Quantitative XMCD sum-rule analysis reveals that Mo substitution produces the highest reconstructed total magnetic moment across the measured temperature range, reaching values at low temperature that are nearly an order of magnitude larger than those observed in the Ru-containing compositions. These results establish a composition-driven strategy for tuning covalency, charge redistribution, and the balance between localized and itinerant magnetism in high-entropy oxide thin films, providing a pathway toward the design of tunable spintronic and multifunctional oxide materials.