Exciton-dielectric mode coupling in MoS2 nanoflakes visualized by cathodoluminescence

Abstract

Abstract Two-dimensional (2D) transition metal dichalcogenides (TMDCs), possessing unique exciton luminescence properties, have attracted significant attention for use in optical and electrical devices. TMDCs are also high refractive index materials that can strongly confine the electromagnetic field in nanoscale dimensions when patterned into nanostructures, thus resulting in complex light emission that includes exciton and dielectric resonances. Here, we use cathodoluminescence (CL) to experimentally visualize the emission modes of single molybdenum disulfide (MoS2) nanoflakes and to investigate luminescence enhancement due to dielectric resonances in nanoscale dimensions, by using a scanning transmission electron microscope. Specifically, we identify dielectric modes whose resonant wavelength is sensitive to the shape and size of the nanoflake, and exciton emission peaks whose energies are insensitive to the geometry of the flakes. Using a four-dimensional CL method and boundary element method simulations, we further theoretically and experimentally visualize the emission polarization and angular emission patterns, revealing the coupling of the exciton and dielectric resonant modes. Such nanoscopic observation provides a detailed understanding of the optical responses of MoS2 including modal couplings of excitons and dielectric resonances which play a crucial role in the development of energy conversion devices, single-photon emitters, and nanophotonic circuits with enhanced light-matter interactions.