Synthesis of epitaxial monolayer Janus SPtSe

Janus single-layer transition metal dichalcogenides, in which the two chalcogen layers have a different chemical nature, push chemical composition control beyond what is usually achievable with van der Waals heterostructures. Here, we report such a Janus compound, SPtSe, which is predicted to exhibit strong Rashba spin-orbit coupling. We synthetized it by conversion of a single-layer of PtSe2 on Pt(111) via sulfurization under H2S atmosphere. Our in situ and operando structural analysis with grazing incidence synchrotron X-ray diffraction reveals the process by which the Janus alloy forms. The crystalline long-range order of the as-grown PtSe2 monolayer is first lost due to thermal annealing. A subsequent recrystallization in presence of a source of sulfur yields a highly ordered SPtSe alloy, which is isostructural to the pristine PtSe2. The chemical composition is resolved, layer-by-layer, using angle-resolved X-ray photoelectron spectroscopy, demonstrating that Se-by-S substitution occurs selectively in the topmost chalcogen layer.