Understanding the Different Exciton–Plasmon Coupling Regimes in Two-Dimensional Semiconductors Coupled with Plasmonic Lattices: A Combined Experimental and Unified Equation of Motion Approach

Abstract

We study exciton–plasmon coupling in two-dimensional semiconductors coupled with Ag plasmonic lattices via angle-resolved reflectance spectroscopy and by solving the equations of motion (EOM) in a coupled oscillator model accounting for all the resonances of the system. Five resonances are considered in the EOM model: semiconductor A and B excitons, localized surface plasmon resonances (LSPRs) of plasmonic nanostructures, and the lattice diffraction modes of the plasmonic array. We investigated the exciton–plasmon coupling in different 2D semiconductors and plasmonic lattice geometries, including monolayer MoS2 and WS2 coupled with Ag nanodisk and bowtie arrays and examined the dispersion and line shape evolution in the coupled systems via the EOM model with different exciton–plasmon coupling parameters. The EOM approach provides a unified description of the exciton–plasmon interaction in the weak, intermediate, and strong coupling cases with correctly explaining the dispersion and lineshapes of the complex system. This study provides a much deeper understanding of light–matter interactions in multilevel systems in general and will be useful to instruct the design of novel two-dimensional exciton–plasmonic devices for a variety of optoelectronic applications with precisely tailored responses.