Published February 26, 2021 | Version v1
Journal article Open

Complex plasmon-exciton dynamics revealed through quantum dot light emission in a nanocavity

  • 1. Department of Chemical and Biological Physics, Weizmann Institute of Science, Rehovot, Israel
  • 2. 2Department of Chemical Research Support, Weizmann Institute of Science, Rehovot, Israel
  • 3. Materials Physics Center CSIC-UPV/EHU, Paseo Manuel de Lardizabal 5, Donostia-San Sebastian, Spain
  • 4. Schulich Faculty of Chemistry, Technion-Israel Institute of Technology, Haifa, Israel

Description

Plasmonic cavities can confine electromagnetic radiation to deep sub-wavelength regimes. This facilitates strong coupling phenomena to be observed at the limit of individual quantum emitters. Here, we report an extensive set of measurements of plasmonic cavities hosting one to a few semiconductor quantum dots. Scattering spectra show Rabi splitting, demonstrating that these devices are close to the strong coupling regime. Using Hanbury Brown and Twiss interferometry, we observe non-classical emission, allowing us to directly determine the number of emitters in each device. Surprising features in photoluminescence spectra point to the contribution of multiple excited states. Using model simulations based on an extended Jaynes-Cummings Hamiltonian, we find that the involvement of a dark state of the quantum dots explains the experimental findings. The coupling of quantum emitters to plasmonic cavities thus exposes complex relaxation pathways and emerges as an unconventional means to control dynamics of quantum states.

Notes

S.N.G. thanks the Government of Israel for a Planning and Budgeting Committee Fellowship. G.H. is the incumbent of the Hilda Pomeraniec Memorial Professorial Chair. R.E., T.N. and J.A. acknowledge funding from projects FIS2016-80174-P and PID2019-107432GB-I00 of the Spanish Ministry of Science, Innovation and Universities MICINN, as well as funding from grant IT1164-19 for consolidated groups of the Basque University, through the Department of Universities of the Basque Government. This project received partial support from the European Union's Horizon 2020 research and innovation programme under grant agreement no. 861950, project POSEIDON, and grant agreement no. 810626, project SINNCE. We thank Garnett W. Bryant and Peter Nordlander for stimulating discussions.

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