Designing Optimal Distorted‐Octahedra Superlattices for Strong Topological Hall Effect

Abstract Topologically protected spin states hold great promise for applications in next generation of memory circuits and spintronic devices. These intriguing textures typically emerge in bulk materials or heterostructures with broken inversion symmetry, accompanied by an enhanced Dzyaloshinskii‐Moriya interaction (DMI). In this study, the topological Hall effect (THE) in atomically designed (DyScO 3 ) n /(SrRuO 3 ) n (D n S n ) superlattices over a significant range of temperatures (10–120 K) and thicknesses (16–40 nm) is successfully induced. Using magnetic force microscopy (MFM), the formation and stability of magnetic domains, such as topological skyrmions is observed. By precisely controlling the interlayer thickness ( n ) and biaxial strain, the mechanisms underlying the modulation and induction of magnetic topological states is elucidated. Supporting evidence is provided by scanning transmission electron microscopy (STEM) and X‐ray absorption spectroscopy (XAS), thereby lending further credence to this conclusions. These heterostructures offer a universal method for exploring topological phenomena driven by distorted octahedra, while enhancing the integrability and addressability of topologically protected functional devices.