Electron beam interrogation and control of ultrafast plexcitonic dynamics

Alexandra Crai, Angela Demetriadou, Ortwin Hess

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n the strong coupling regime, photons and excitons exchange energy very rapidly such that they blend together, forming hybrid plexcitonic states. Recently, strong coupling of plasmons with a single fluorescent molecule was realized for the first time at room temperature using plasmonic nanocavities. Here, we show that the electron beam excitation of a plasmonic nanocavity allows us to dynamically control the light-matter interaction forming the plexciton without changing the plasmonic nanocavity. Unlike dark-field microscopy, an electron beam has the ability to excite dark plasmons which, due to their non-radiative nature, allow for more energy cycles between the plasmon and the emitter to survive in a very lossy system. Directly comparing effective 2D (nanowire) and 3D (nanosphere) plasmonic nanocavities we demonstrate that the dark modes inherently present at lower frequencies in the nanowire-nanocavity can be used as a means to extend the quantum coherence between the plasmon and emitter, opening the way towards dynamic tuning of the strong-coupling dynamics via the electron beam velocity. This opens new routes for dynamically addressing and controlling quantum emitters in the strong coupling regime via (the velocity of) the electron beam.
Original languageEnglish
JournalACS Photonics
Early online date27 Dec 2019
Publication statusE-pub ahead of print - 27 Dec 2019


  • strong coupling
  • electron beam
  • quantum emitters
  • quantum dynamics
  • plasmonic nanocavities


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