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Magnetic materials with noncollinear spin textures are promising forspintronic applications. To realize practical devices, control over the lengthand energy scales of such spin textures is imperative. The chiral helimagnetsCr1/3NbS2 and Cr1/3TaS2 exhibit analogous magnetic phase diagrams withdifferent real-space periodicities and field dependence, positioning them asmodel systems for studying the relative strengths of the microscopic mechanismsgiving rise to exotic spin textures. Here, we carry out a comparative study ofthe electronic structures of Cr1/3NbS2 and Cr1/3TaS2 using angle-resolvedphotoemission spectroscopy and density functional theory. We show that bands inCr1/3TaS2 are more dispersive than their counterparts in Cr1/3NbS2 and connectthis result to bonding and orbital overlap in these materials. We alsounambiguously distinguish exchange splitting from surface termination effectsby studying the dependence of their photoemission spectra on polarization,temperature, and beam size. We find strong evidence that hybridization betweenintercalant and host lattice electronic states mediates the magnetic exchangeinteractions in these materials, suggesting that band engineering is a routetoward tuning their spin textures. Overall, these results underscore how themodular nature of intercalated transition metal dichalcogenides translatesvariation in composition and electronic structure to complex magnetism.

Comparative Electronic Structures of the Chiral Helimagnets Cr1/3NbS2 and Cr1/3TaS2