Tuning the Charge Transfer of Transition Metal Dichalcogenides via Misfit Layer Compounds

ABSTRACT Misfit layer compounds (MLCs) are a versatile platform for exploring the electronic phase diagram of two‐dimensional (2D) materials beyond the limits of conventional gating techniques. This work demonstrates the precise tunability of electron doping in monolayers through chemical alloying within the rocksalt layer of heterostructures. By combining first‐principles density functional theory (DFT) calculations with angle‐resolved photoemission spectroscopy (ARPES), we prove that the rocksalt unit acts as a universal electron donor. We show that varying the La/Pb ratio results in a rigid Fermi level shift, still preserving the electronic structure. Crucially, photon‐energy‐dependent ARPES confirms that the layers nearly maintain their intrinsic 2D character and orbital identity within the three‐dimensional misfit. This study establishes MLCs as a reliable platform for engineering emergent states in 2D transition metal dichalcogenides through precise stoichiometric control.