Van der Waals interfacial reconstruction in monolayer transition-metal dichalcogenides and gold heterojunctions

The structures and properties of van der Waals (vdW) heterojunctions between semiconducting two-dimensional transition-metal dichalcogenides (2D TMDs) and conductive metals, such as gold, significantly influence the performances of 2D-TMD based electronic devices. Chemical vapor deposition is one of the most promising approaches for large-scale synthesis and fabrication of 2D TMD electronics with naturally formed TMD/metal vdW interfaces. However, the structure and chemistry of the vdW interfaces are less known. Here we report the interfacial reconstruction between TMD monolayers and gold substrates. The participation of sulfur leads to the reconstruction of Au {001} surface with the formation of a metastable Au₄S₄ interfacial phase which is stabilized by the top MoS₂ and WS₂ monolayers. Moreover, the enhanced vdW interaction between the reconstructed Au₄S₄ interfacial phase and TMD monolayers results in the transition from n-type TMD-Au Schottky contact to p-type one with reduced energy barrier height.