Electronic properties of single-layer tungsten disulfide on epitaxial graphene on silicon carbide

This work reports an electronic and micro-structural study of an appealing system for optoelectronics: tungsten disulfide (WS₂) on epitaxial graphene (EG) on SiC(0001). The WS₂ is grown via chemical vapor deposition (CVD) onto the EG. Low-energy electron diffraction (LEED) measurements assign the zero-degree orientation as the preferential azimuthal alignment for WS₂/EG. The valence-band (VB) structure emerging from this alignment is investigated by means of photoelectron spectroscopy measurements, with both high space and energy resolution. We find that the spin-orbit splitting of monolayer WS₂ on graphene is of 462 meV, larger than what is reported to date for other substrates. We determine the value of the work function for the WS₂/EG to be 4.5 ± 0.1 eV. A large shift of the WS₂ VB maximum is observed as well, due to the lowering of the WS₂ work function caused by the donor-like interfacial states of EG. Density functional theory (DFT) calculations carried out on a coincidence supercell confirm the experimental band structure to an excellent degree. X-ray photoemission electron microscopy (XPEEM) measurements performed on single WS₂ crystals confirm the van der Waals nature of the interface coupling between the two layers. In virtue of its band alignment and large spin-orbit splitting, this system gains strong appeal for optical spin-injection experiments and opto-spintronic applications in general.