Interface-Driven Assembly of Pentacene/MoS₂ Lateral Heterostructures

Mixed-dimensional van der Waals heterostructures formed by molecular assemblies and 2D materials provide a novel platform for fundamental nanoscience and future nanoelectronics applications. Here we investigate a prototypical hybrid heterostructure between pentacene molecules and 2D MoS₂ nanocrystals, deposited on Au(111) by combining pulsed laser deposition and organic molecular beam epitaxy. The obtained structures were investigated in situ by scanning tunneling microscopy and spectroscopy and analyzed theoretically by density functional theory calculations. Our results show the formation of atomically thin pentacene/MoS₂ lateral heterostructures on the Au substrate. The most stable pentacene adsorption site corresponds to MoS₂ terminations, where the molecules self-assemble parallel to the direction of MoS₂ edges. The density of states changes sharply across the pentacene/MoS₂ interface, indicating a weak interfacial coupling, which leaves the electronic signature of MoS₂ edge states unaltered. This work unveils the self-organization of abrupt mixed-dimensional lateral heterostructures, opening to hybrid devices based on organic/inorganic one-dimensional junctions.