Vacuum Rabi splitting of a dark plasmonic cavity mode revealed by fast electrons

Abstract

Recent years have seen a growing interest in strong coupling between plasmons and excitons, as a way to generate new quantum optical testbeds and influence chemical dynamics and reactivity. Strong coupling to bright plasmonic modes has been achieved even with single quantum emitters. Dark plasmonic modes fare better in some applications due to longer lifetimes, but are difficult to probe as they are subradiant. Here, we apply electron energy loss (EEL) spectroscopy to demonstrate that a dark mode of an individual plasmonic bowtie can interact with a small number of quantum emitters, as evidenced by Rabi-split spectra. Coupling strengths of up to 85 meV place the bowtie-emitter devices at the onset of the strong coupling regime. Remarkably, the coupling occurs at the bowtie gap periphery, even while the electron beam probes their center. Our findings pave the way for using EEL spectroscopy to study exciton-plasmon interactions involving non-emissive photonic modes.

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• Using Electron Energy-Loss Spectroscopy to Measure Nanoscale Electronic and Vibrational Dynamics in a TEM
• Monitoring strong coupling in nonlocal plasmonics with electron spectroscopies
• Influence of experimental conditions on localized surface plasmon resonances measurement by electron energy loss spectroscopy
• Higher-Order Photon Statistics as a New Tool to Reveal Hidden Excited States in a Plasmonic Cavity
• Probing optical anapoles with fast electron beams
• Electroluminescence as a probe of strong exciton-plasmon coupling in few-layer WSe2
• Quantum Nanophotonics with Energetic Particles:X-rays and Free Electrons
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• Quantum Electrodynamics of graphene Landau levels in a deep-subwavelength hyperbolic phonon polariton cavity
• Spatio-spectral metrics in electron energy loss spectroscopy as a tool to resolve nearly degenerate plasmon modes in dimer plasmonic antennas
• Phonon-mediated dark to bright plasmon conversion