Coherent Excitation and Control of Plasmons on Gold Using Two-Dimensional Transition Metal Dichalcogenides

[Image: see text] The hybrid combination of two-dimensional (2D) transition metal dichalcogenides (TMDs) and plasmonic materials open up novel means of (ultrafast) optoelectronic applications and manipulation of nanoscale light–matter interaction. However, control of the plasmonic excitations by TMDs themselves has not been investigated. Here, we show that the ultrathin 2D WSe(2) crystallites permit nanoscale spatially controlled coherent excitation of surface plasmon polaritons (SPPs) on smooth Au films. The resulting complex plasmonic interference patterns are recorded with nanoscale resolution in a photoemission electron microscope. Modeling shows good agreement with experiments and further indicates how SPPs can be tailored with high spatiotemporal precision using the shape of the 2D TMDs with thicknesses down to single molecular layers. We demonstrate the use of WSe(2) nanocrystals as 2D optical elements for exploring the ultrafast dynamics of SPPs. Using few-femtosecond laser pulse pairs we excite an SPP at the boundary of a WSe(2) crystal and then have a WSe(2) monolayer wedge act as a delay line inducing a spatially varying phase difference down to the attosecond time range. The observed effects are a natural yet unexplored consequence of high dielectric functional values of TMDs in the visible range that should be considered when designing metal–TMD hybrid devices. As the 2D TMD crystals are stable in air, can be defect free, can be synthesized in many shapes, and are reliably positioned on metal surfaces, using them to excite and steer SPPs adds an interesting alternative in designing hybrid structures for plasmonic control.