Here we present recent work on the synthesis and characterization of two-dimensional transition metal dichalcogenides (TMDs) grown by molecular beam epitaxy (MBE). Bulk TMD crystals consist of two-dimensional layers bonded together by van der Waal interactions; the lack of primary bonds at the TMD interface allow for the growth of TMD heterostructures on a variety of substrates without the need to consider lattice constant mismatch or crystal structure of the substrate which we aim to demonstrate. TMDs are grown and characterized in an all in-vacuo ultra-high vacuum system which enables the simultaneous co-deposition of multiple transition metals and chalcogens allowing for the study of TMD ternary alloys and layered heterostructures followed by their compositional and intrinsic electronic characterization prior to atmospheric exposure. Presented will be a review of our work studying the interface chemistry between TMD and conventional semiconducting substrates, as well as our investigations of 2D-2D heterostructure grown by MBE.

Figure 1 shows an example of in-vacuo x-ray photoelectron spectroscopy (XPS) carried out on GaAs(001) before an after the growth of monolayer MoSe₂. The sample was initial passivated by a sulfur based treatment, and the presence of sulfur bonded to the surface can be observed in the As 2p and Ga 2p spectra. The asymmetry observed in the As 2p and Ga 2p core-levels suggest that some reactions with Se take place during the growth. The thermal stability of this interface will be investigated using in-situ UHV heating and XPS.

In separate work we evaluated the valence band offsets using in-vacuo XPS and UPS (ultraviolet photoelectron spectroscopy). This is achieved by measuring core-level to valence band maximum separation for control samples as well as the core-level shifts in heterostructure. In-vacuo XPS analysis can also be used to reveal any interface reactors that may occur between the TMDs. It is found that for chalcogen deficient growths, metallic signatures can be detected.

Of particular interest is the process structure relationships. Presented will be parametric studies showing impact of growth temperature and relative metal-chalcogen flux ratios on the electronic structure and interface chemistry in both the 2D-2D and 2D-3D systems. The all in-vacuo synthesis and analysis cluster tool allows these investigations to be carried out without air exposure which can induce substantial changes in the chemistry of these materials.