Crystal Growth, Noncoplanar Magnetism, and Topological Hall Response in Dual-Intercalated (Fe,Cr)1/3NbS2

Dual intercalation provides an effective crystal-chemical route to tune magnetic interactions and functional transport properties in layered dichalcogenides. Here, we grow dual-intercalated (Fe,Cr)1/3NbS2 single crystals by chemical vapor transport and establish the structure–property relationships through single-crystal X-ray diffraction, magnetic and transport measurements, first-principles calculations, and magnetic force microscopy. Structural refinement confirms that the as-grown (Fe,Cr)1/3NbS2 crystal has a hexagonal P6322 structure with mixed Fe/Cr occupation of the intercalated sublattice. The crystals exhibit pronounced magnetic anisotropy with the c axis as the easy magnetization axis and obvious hysteresis loops in the out-of-plane direction below 30 K. In the same temperature range, butterfly-like magnetoresistance and anomalous Hall loops are observed near the coercive fields. A finite topological Hall appears in (Fe,Cr)1/3NbS2 after subtraction of the ordinary and anomalous Hall components from the raw Hall data. Combined first-principles calculations and magnetic force microscopy further suggest that the topological Hall effect is associated with noncoplanar spin textures. This study highlights dual intercalation as an effective route to engineer competing magnetic states and topology-related magneto-transport in layered materials.