Emergent 3D Fermiology and Magnetism in an Intercalated Van der Waals System

Intercalation of magnetic atoms into van der Waals materials provides a versatile platform for tailoring unconventional magnetic properties. However, its impact on electronic dimensionality and exchange mechanisms remains poorly understood. Using Fe‐intercalated as a model system, we combine x‐ray absorption and resonant inelastic scattering with angle‐resolved photoemission and first‐principles calculations to reveal that intercalation reshapes the host electronic structure. We identify a spin‐polarized intercalant‐host hybridized band with pronounced out‐of‐plane dispersion crossing the Fermi level, providing an itinerant channel for interlayer magnetic exchange. This mechanism explains the breakdown of a purely atomic picture and establishes a direct link between lattice geometry, electronic dispersion, and magnetic order. Our findings demonstrate that intercalant‐induced itinerancy enables tunable interlayer coupling in otherwise layered magnets, offering a general microscopic framework for engineering magnetic dimensionality in a broad class of intercalated vdW materials.