Optical Propagation of Exciton Polaritons in Ultrathin van der Waals Microcrystals down to Few Monolayers

The exciton polariton is a kind of quasiparticles and provides a promising opportunity to explore fundamental quantum phenomena for photonic applications. Transition-metal dichalcogenide (TMD) materials provide the platform of nanophotonics that supports the propagative exciton polaritons even at room-temperature. Previously, real space studies on thin flakes of TMDs by scattering-type scanning nearfield optical microscopy (s-SNOM) were limited to waveguide thickness down to 30 nm. In this work, we present the nano-optical imaging of ordinary transverse electric modes of exciton polaritons in MoS₂ and WSe₂ down to a few atomic layers, measured by atomic force microscope-based s-SNOM. Surprisingly, the interference fringe patterns can be observed clearly at the prepared ultrathin TMD flakes with thickness down to ~3 nm (4 ML) and ~8 nm (12 ML) for MoS₂ and WSe₂, respectively, which breaks greatly the previous measurement limitation. The wavevectors stay around 1.6k₀–1.7k₀ constantly when the thickness approaching to a few MLs, instead of 1k₀ according to the theory. These modes are supported by the nearly-freestanding TMD microflakes in the form of three-layer symmetric waveguide to confine the exciton polaritons. Our results provide in-depth understanding and open new avenues to explore the polaritonic devices operating at the near infrared region based on ultrathin TMD materials.