Publication date: 8th June 2021
Strong coupling between light and matter has been extensively studied due to its fundamental importance for the description of the solid-state excitations as well as its emerging applications e.g. in polaritonic lasers or manipulating the chemical reactions. It results into a formation of the hybrid light-matter excitations, known as polaritons, that is manifested by the Rabi splitting and Rabi oscillations. Strong light-matter coupling is observed in both natural systems (e.g. metal-dielectric surface supporting surface plasmon polaritons) and engineered devices (e.g. optical cavities coupled to a quantum emitter supporting exciton polaritons). Plasmonic nanostructures represent a particularly attractive class of open optical cavities due to their naturally low (deeply-subwavelength) mode volume. However, observations of the strong plasmon-exciton coupling using plasmonic nanostructures is extremely challenging due to unavoidable losses in the metallic material of the nanostructure.
In our contribution, we demonstrate the vacuum Rabi splitting between the dark plasmon mode in the bow-tie plasmonic antenna and the exciton state in quantum dots. We begin with a full modal characterization of localized plasmons in the bow-tie plasmonic antennas using electron energy loss spectroscopy (EELS) [1], including numerical simulations of the near field distribution [2]. Dark plasmon modes exhibit high Q-factor because of suppressed radiative losses; only intrinsic material losses are effective. With quantum dots deposited into the central part of the plasmonic antennas, a 160-meV Rabi splitting of the associated feature in the electron energy loss spectrum is demonstrated, corresponding to the onset of strong plasmon-exciton coupling [3]. The related coupling strength reads 83 meV. Similarly, with quantum dots resonant with the bright dipole mode of the plasmonic antennas, a 200-meV Rabi splitting and a 105-meV coupling strength is achieved. Our results demonstrate the ability of EELS to study the strong coupling of excitons to both bright and subradiant plasmon modes.
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