IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v10y2019i1d10.1038_s41467-019-08611-5.html
   My bibliography  Save this article

Quantum electrodynamics at room temperature coupling a single vibrating molecule with a plasmonic nanocavity

Author

Listed:
  • Oluwafemi S. Ojambati

    (University of Cambridge)

  • Rohit Chikkaraddy

    (University of Cambridge)

  • William D. Deacon

    (University of Cambridge)

  • Matthew Horton

    (University of Cambridge)

  • Dean Kos

    (University of Cambridge)

  • Vladimir A. Turek

    (University of Cambridge)

  • Ulrich F. Keyser

    (University of Cambridge)

  • Jeremy J. Baumberg

    (University of Cambridge)

Abstract

Interactions between a single emitter and cavity provide the archetypical system for fundamental quantum electrodynamics. Here we show that a single molecule of Atto647 aligned using DNA origami interacts coherently with a sub-wavelength plasmonic nanocavity, approaching the cooperative regime even at room temperature. Power-dependent pulsed excitation reveals Rabi oscillations, arising from the coupling of the oscillating electric field between the ground and excited states. The observed single-molecule fluorescent emission is split into two modes resulting from anti-crossing with the plasmonic mode, indicating the molecule is strongly coupled to the cavity. The second-order correlation function of the photon emission statistics is found to be pump wavelength dependent, varying from g(2)(0) = 0.4 to 1.45, highlighting the influence of vibrational relaxation on the Jaynes-Cummings ladder. Our results show that cavity quantum electrodynamic effects can be observed in molecular systems at ambient conditions, opening significant potential for device applications.

Suggested Citation

  • Oluwafemi S. Ojambati & Rohit Chikkaraddy & William D. Deacon & Matthew Horton & Dean Kos & Vladimir A. Turek & Ulrich F. Keyser & Jeremy J. Baumberg, 2019. "Quantum electrodynamics at room temperature coupling a single vibrating molecule with a plasmonic nanocavity," Nature Communications, Nature, vol. 10(1), pages 1-7, December.
    • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-08611-5
    DOI: 10.1038/s41467-019-08611-5
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-019-08611-5
    File Function: Abstract
    Download Restriction: no
    File URL: https://libkey.io/10.1038/s41467-019-08611-5?utm_source=ideas
    LibKey link: if access is restricted and if your library uses this service, LibKey will redirect you to where you can use your library subscription to access this item
    ---><---

    Citations

    Citations are extracted by the CitEc Project, subscribe to its RSS feed for this item.
    as


    Cited by:

    1. Raj Pandya & Richard Y. S. Chen & Qifei Gu & Jooyoung Sung & Christoph Schnedermann & Oluwafemi S. Ojambati & Rohit Chikkaraddy & Jeffrey Gorman & Gianni Jacucci & Olimpia D. Onelli & Tom Willhammar &, 2021. "Microcavity-like exciton-polaritons can be the primary photoexcitation in bare organic semiconductors," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
    2. Christian Schäfer & Johannes Flick & Enrico Ronca & Prineha Narang & Angel Rubio, 2022. "Shining light on the microscopic resonant mechanism responsible for cavity-mediated chemical reactivity," Nature Communications, Nature, vol. 13(1), pages 1-9, December.

    More about this item

    Statistics

    Access and download statistics

    Corrections

    All material on this site has been provided by the respective publishers and authors. You can help correct errors and omissions. When requesting a correction, please mention this item's handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-08611-5. See general information about how to correct material in RePEc.

    If you have authored this item and are not yet registered with RePEc, we encourage you to do it here. This allows to link your profile to this item. It also allows you to accept potential citations to this item that we are uncertain about.

    We have no bibliographic references for this item. You can help adding them by using this form .

    If you know of missing items citing this one, you can help us creating those links by adding the relevant references in the same way as above, for each refering item. If you are a registered author of this item, you may also want to check the "citations" tab in your RePEc Author Service profile, as there may be some citations waiting for confirmation.

    For technical questions regarding this item, or to correct its authors, title, abstract, bibliographic or download information, contact: Sonal Shukla or Springer Nature Abstracting and Indexing (email available below). General contact details of provider: http://www.nature.com .

    Please note that corrections may take a couple of weeks to filter through the various RePEc services.

    IDEAS is a RePEc service. RePEc uses bibliographic data supplied by the respective publishers.