Inducing Ferromagnetism by Structural Engineering in a Strongly Spin‐Orbit Coupled Oxide

ABSTRACT Magnetic materials with strong spin‐orbit coupling (SOC) are essential for the advancement of spin‐orbitronic devices, as they enable efficient spin‐charge conversion, complex magnetic structures, spin‐valley physics, topological phases and other exotic phenomena. 5d transition‐metal oxides such as SrIrO 3 feature large SOC, but usually show paramagnetic behavior due to broad bands and a low density of states at the Fermi level, accompanied by a relatively low Coulomb repulsion. Here, we unveil ferromagnetism in 5d SrIrO 3 thin films grown on SrTiO 3 (111). Through substrate‐induced structural engineering, a zigzag stacking of three‐unit‐cell thick layers along the [111] direction is achieved, stabilizing a ferromagnetic state at the interfaces. Magnetotransport measurements reveal an anomalous Hall effect below ∼30 K and hysteresis in the Hall conductivity below 7 K, indicating ferromagnetic ordering. X‐ray magnetic circular dichroism further supports these results. Theoretical analysis suggests that the structural engineering of the IrO 6 octahedral network enhances the density of states at the Fermi level and thus stabilizes Stoner ferromagnetism. This work highlights the potential of structurally engineered 5d oxides for spin‐orbitronic devices, where efficient control of SOC‐induced magnetic phases by electric currents can lead to lower energy consumption and improved performance in next‐generation device technologies.