Abstract

We present a tunable plasmonic platform that allows room temperature hybridization of dissimilar excitons, namely of Wannier-Mott excitons in monolayer (1L) WS₂ and Frenkel excitons in molecular J-aggregates via simultaneous strong coupling to surface plasmon polaritons. It is based on a simple layered design consisting of a thin planar silver film and a dielectric spacer on which monolayer and the aggregates are assembled. Strong coupling is revealed by angle-dependent spectroscopic ellipsometry measurements in total internal reflection geometry by the observation of double Rabi splitting at the two excitonic resonances. We analyze the exciton-exciton-plasmon system with the coupled oscillator model and demonstrate modulation of polariton character and dynamics by the number of molecules participating in the coupling. Furthermore, we propose a route to remotely control the mode splitting at the Frenkel excitonic resonance via electrostatic gating of the 1L-WS₂ and to switch the molecule-plasmon interaction between the weak and strong coupling regime.

Abstract

We present a tunable plasmonic platform that allows room temperature hybridization of dissimilar excitons, namely of Wannier-Mott excitons in monolayer (1L) WS₂ and Frenkel excitons in molecular J-aggregates via simultaneous strong coupling to surface plasmon polaritons. It is based on a simple layered design consisting of a thin planar silver film and a dielectric spacer on which monolayer and the aggregates are assembled. Strong coupling is revealed by angle-dependent spectroscopic ellipsometry measurements in total internal reflection geometry by the observation of double Rabi splitting at the two excitonic resonances. We analyze the exciton-exciton-plasmon system with the coupled oscillator model and demonstrate modulation of polariton character and dynamics by the number of molecules participating in the coupling. Furthermore, we propose a route to remotely control the mode splitting at the Frenkel excitonic resonance via electrostatic gating of the 1L-WS₂ and to switch the molecule-plasmon interaction between the weak and strong coupling regime.

Abstract

We present a tunable plasmonic platform that allows room temperature hybridization of dissimilar excitons, namely of Wannier-Mott excitons in monolayer (1L) WS₂ and Frenkel excitons in molecular J-aggregates via simultaneous strong coupling to surface plasmon polaritons. It is based on a simple layered design consisting of a thin planar silver film and a dielectric spacer on which monolayer and the aggregates are assembled. Strong coupling is revealed by angle-dependent spectroscopic ellipsometry measurements in total internal reflection geometry by the observation of double Rabi splitting at the two excitonic resonances. We analyze the exciton-exciton-plasmon system with the coupled oscillator model and demonstrate modulation of polariton character and dynamics by the number of molecules participating in the coupling. Furthermore, we propose a route to remotely control the mode splitting at the Frenkel excitonic resonance via electrostatic gating of the 1L-WS₂ and to switch the molecule-plasmon interaction between the weak and strong coupling regime.

Abstract

We present a tunable plasmonic platform that allows room temperature hybridization of dissimilar excitons, namely of Wannier-Mott excitons in monolayer (1L) WS₂ and Frenkel excitons in molecular J-aggregates via simultaneous strong coupling to surface plasmon polaritons. It is based on a simple layered design consisting of a thin planar silver film and a dielectric spacer on which monolayer and the aggregates are assembled. Strong coupling is revealed by angle-dependent spectroscopic ellipsometry measurements in total internal reflection geometry by the observation of double Rabi splitting at the two excitonic resonances. We analyze the exciton-exciton-plasmon system with the coupled oscillator model and demonstrate modulation of polariton character and dynamics by the number of molecules participating in the coupling. Furthermore, we propose a route to remotely control the mode splitting at the Frenkel excitonic resonance via electrostatic gating of the 1L-WS₂ and to switch the molecule-plasmon interaction between the weak and strong coupling regime.