Structural and electronic properties of MoS2 and MoSe2 monolayers grown by chemical vapor deposition on Au(111)†

The exceptional electronic and photonic properties of the monolayers of transition metal dichalcogenides including the spin–orbit splitting of the valence and conduction bands at the K points of the Brillouin zone make them promising for novel applications in electronics, photonics and optoelectronics. Scalable growth of these materials and understanding of their interaction with the substrate is crucial for these applications. Here we report the growth of MoS2 and MoSe2 monolayers on Au(111) by chemical vapor deposition at ambient pressure as well as the analysis of their structural and electronic properties down to the atomic scale. To this aim, we apply ultrahigh vacuum surface sensitive techniques including scanning tunneling microscopy and spectroscopy, low-energy electron diffraction, X-ray and angle-resolved ultraviolet photoelectron spectroscopy in combination with Raman spectroscopy at ambient conditions. We demonstrate the growth of high-quality epitaxial single crystalline MoS2 and MoSe2 monolayers on Au(111) and show the impact of annealing on the monolayer/substrate interaction. Thus, as-grown and moderately annealed (<100 °C) MoSe2 monolayers are decoupled from the substrate by excess Se atoms, whereas annealing at higher temperatures (>250 °C) results in their strong coupling with the
substrate caused by desorption of the excess Se. The MoS2 monolayers are strongly coupled to the substrate and the interaction remains almost unchanged even after annealing up to 450 °C.