Charge Density Wave and Ferromagnetism in Intercalated CrSBr

Abstract In materials with 1D electronic bands, electron–electron interactions can produce intriguing quantum phenomena, including spin‐charge separation and charge density waves (CDW). Most of these systems, however, are non‐magnetic, motivating a search for anisotropic materials where the coupling of charge and spin may affect emergent quantum states. Here, chemical intercalation of the van der Waals magnetic semiconductor CrSBr yields Li 0.17(2) (tetrahydrofuran) 0.26(3) CrSBr, which possesses an electronically driven quasi‐1D CDW with an onset temperature above room temperature. Concurrently, electron doping increases the magnetic ordering temperature from 132 to 200 K and switches its interlayer magnetic coupling from antiferromagnetic to ferromagnetic. The spin‐polarized nature of the anisotropic bands that give rise to this CDW enforces an intrinsic coupling of charge and spin. The coexistence and interplay of ferromagnetism and charge modulation in this exfoliatable material provide a promising platform for studying tunable quantum phenomena across a range of temperatures and thicknesses.