VS2 is a challenging material to prepare stoichiometrically in the bulk, and the single layer has not been successfully isolated before now. Here we report the first realization of single-layer VS2, which we have prepared epitaxially with high quality on Au(1 1 1) in the octahedral (1T) structure. We find that we can deplete the VS2 lattice of S by annealing in vacuum so as to create an entirely new 2D compound that has no bulk analogue. The transition is reversible upon annealing in an H2S gas atmosphere. We report the structural properties of both the stoichiometric and S-depleted compounds on the basis of low-energy electron diffraction, x-ray photoelectron spectroscopy and diffraction, and scanning tunneling microscopy experiments.
