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

Author

Listed:
  • Satyendra Nath Gupta

    (Department of Chemical and Biological Physics, Weizmann Institute of Science)

  • Ora Bitton

    (Department of Chemical Research Support, Weizmann Institute of Science)

  • Tomas Neuman

    (Materials Physics Center CSIC-UPV/EHU, Paseo Manuel de Lardizabal 5
    Donostia International Physics Center DIPC, Paseo Manuel de Lardizabal 4)

  • Ruben Esteban

    (Materials Physics Center CSIC-UPV/EHU, Paseo Manuel de Lardizabal 5
    Donostia International Physics Center DIPC, Paseo Manuel de Lardizabal 4)

  • Lev Chuntonov

    (Schulich Faculty of Chemistry, Technion-Israel Institute of Technology)

  • Javier Aizpurua

    (Materials Physics Center CSIC-UPV/EHU, Paseo Manuel de Lardizabal 5
    Donostia International Physics Center DIPC, Paseo Manuel de Lardizabal 4)

  • Gilad Haran

    (Department of Chemical and Biological Physics, Weizmann Institute of Science)

Abstract

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.

Suggested Citation

  • Satyendra Nath Gupta & Ora Bitton & Tomas Neuman & Ruben Esteban & Lev Chuntonov & Javier Aizpurua & Gilad Haran, 2021. "Complex plasmon-exciton dynamics revealed through quantum dot light emission in a nanocavity," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-21539-z
    DOI: 10.1038/s41467-021-21539-z
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    Cited by:

    1. Joel Kuttruff & Marco Romanelli & Esteban Pedrueza-Villalmanzo & Jonas Allerbeck & Jacopo Fregoni & Valeria Saavedra-Becerril & Joakim Andréasson & Daniele Brida & Alexandre Dmitriev & Stefano Corni &, 2023. "Sub-picosecond collapse of molecular polaritons to pure molecular transition in plasmonic photoswitch-nanoantennas," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    2. Shu Hu & Junyang Huang & Rakesh Arul & Ana Sánchez-Iglesias & Yuling Xiong & Luis M. Liz-Marzán & Jeremy J. Baumberg, 2024. "Robust consistent single quantum dot strong coupling in plasmonic nanocavities," Nature Communications, Nature, vol. 15(1), pages 1-8, December.
    3. Renming Liu & Ming Geng & Jindong Ai & Xinyi Fan & Zhixiang Liu & Yu-Wei Lu & Yanmin Kuang & Jing-Feng Liu & Lijun Guo & Lin Wu, 2024. "Deterministic positioning and alignment of a single-molecule exciton in plasmonic nanodimer for strong coupling," Nature Communications, Nature, vol. 15(1), pages 1-11, December.

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