Polar Magnetism Above 600 K with High Adaptability in Perovskite Oxides

High magnetic order temperature, sustainable polar insulating state, and tolerance to device integrations are substantial advantages for applications in next-generation spintronics. However, engineering such functionality in a single-phase system remains a challenge owing to the contradicted chemical and electronic requirements for polar nature and magnetism, especially with an ordering state highly above room temperature. Perovskite-related oxides with unique flexibility allow electron-unpaired subsystems to merge into the polar lattice to induce magnetic interactions, combined with their inherent asymmetry, thereby promising polar magnet design. Herein, by atomic-level composition assembly, a family of Ti/Fe co-occupied perovskite oxide films Pb(Ti1–x,Fex)O3 (PFT(x)) with a Ruddlesden–Popper superstructure are successfully synthesized on several different substrates, demonstrating exceptional adaptability to different integration conditions. Furthermore, second-harmonic generation measurements convince the symmetry-breaking polar character. Notably, a ferromagnetic ground state up to 600 K and a steady insulating state far beyond room temperature were achieved simultaneously in these films. This strategy of constructing layered modular superlattices in perovskite oxides could be extended to other strongly correlated systems for triggering nontrivial quantum physical phenomena.