Comparative Electronic Structures of the Chiral Helimagnets Cr(1/3)NbS(2) and Cr(1/3)TaS(2)

[Image: see text] Magnetic materials with noncollinear spin textures are promising for spintronic applications. To realize practical devices, control over the length and energy scales of such spin textures is imperative. The chiral helimagnets Cr(1/3)NbS(2) and Cr(1/3)TaS(2) exhibit analogous magnetic-phase diagrams with different real-space periodicities and field dependence, positioning them as model systems for studying the relative strengths of the microscopic mechanisms giving rise to exotic spin textures. Although the electronic structure of the Nb analogue has been experimentally investigated, the Ta analogue has received far less attention. Here, we present a comprehensive suite of electronic structure studies on both Cr(1/3)NbS(2) and Cr(1/3)TaS(2) using angle-resolved photoemission spectroscopy and density functional theory. We show that bands in Cr(1/3)TaS(2) are more dispersive than their counterparts in Cr(1/3)NbS(2), resulting in markedly different Fermi wavevectors. The fact that their qualitative magnetic phase diagrams are nevertheless identical shows that hybridization between the intercalant and host lattice mediates the magnetic exchange interactions in both of these materials. We ultimately find that ferromagnetic coupling is stronger in Cr(1/3)TaS(2), but larger spin–orbit coupling (and a stronger Dzyaloshinskii–Moriya interaction) from the heavier host lattice ultimately gives rise to shorter spin textures.