In‐Plane Magnetic Anisotropy and Large Topological Hall Effect in Self‐Intercalated Ferromagnet Cr1.61Te2

Self‐intercalated chromium tellurides Cr1+xTe2 have garnered growing attention due to their high‐temperature ferromagnetism, tunable spin structures and air stability, all of which are vital for versatile applications in next‐generation memory and information technology. Here, strong magnetic anisotropy and a large topological Hall effect (THE) in self‐intercalated Cr1.61Te2 single crystals are reported, which are both highly desirable properties for future spintronic applications. These results demonstrate that Cr1.61Te2 is a soft ferromagnet with strong in‐plane magnetic anisotropy. Remarkably, distinct THE behaviors are observed in different temperature regimes, reflecting the intricate spin structures and competing exchange interactions. More interestingly, a large topological Hall resistivity, induced by microscopic non‐coplanar spin structures, emerges in the temperature range 70–240 K, reaching a maximum value of 0.93 µΩ cm at 150 K. Moreover, a sign‐reversed and weak THE is observed at low temperatures below ≈ 70 K, indicating the emergence of an additional topological spin structure with opposite topological charges. This work not only offers valuable insights into the correlation between magnetocrystalline anisotropy and topological phenomena in Cr1+xTe2 systems, but also provides a robust platform for engineering the evolution of complex spin textures that can be leveraged in diverse spintronic device applications.