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Deep strong light–matter coupling in plasmonic nanoparticle crystals

Author

Listed:
  • Niclas S. Mueller

    (Freie Universität Berlin)

  • Yu Okamura

    (Freie Universität Berlin)

  • Bruno G. M. Vieira

    (Freie Universität Berlin
    Universidade Federal do Ceará)

  • Sabrina Juergensen

    (Freie Universität Berlin)

  • Holger Lange

    (University of Hamburg)

  • Eduardo B. Barros

    (Universidade Federal do Ceará)

  • Florian Schulz

    (University of Hamburg)

  • Stephanie Reich

    (Freie Universität Berlin)

Abstract

In the regime of deep strong light–matter coupling, the coupling strength exceeds the transition energies of the material1–3, fundamentally changing its properties4,5; for example, the ground state of the system contains virtual photons and the internal electromagnetic field gets redistributed by photon self-interaction1,6. So far, no electronic excitation of a material has shown such strong coupling to free-space photons. Here we show that three-dimensional crystals of plasmonic nanoparticles can realize deep strong coupling under ambient conditions, if the particles are ten times larger than the interparticle gaps. The experimental Rabi frequencies (1.9 to 3.3 electronvolts) of face-centred cubic crystals of gold nanoparticles with diameters between 25 and 60 nanometres exceed their plasmon energy by up to 180 per cent. We show that the continuum of photons and plasmons hybridizes into polaritons that violate the rotating-wave approximation. The coupling leads to a breakdown of the Purcell effect—the increase of radiative damping through light–matter coupling—and increases the radiative polariton lifetime. The results indicate that metallic and semiconducting nanoparticles can be used as building blocks for an entire class of materials with extreme light–matter interaction, which will find application in nonlinear optics, the search for cooperative effects and ground states, polariton chemistry and quantum technology4,5.

Suggested Citation

  • Niclas S. Mueller & Yu Okamura & Bruno G. M. Vieira & Sabrina Juergensen & Holger Lange & Eduardo B. Barros & Florian Schulz & Stephanie Reich, 2020. "Deep strong light–matter coupling in plasmonic nanoparticle crystals," Nature, Nature, vol. 583(7818), pages 780-784, July.
  • Handle: RePEc:nat:nature:v:583:y:2020:i:7818:d:10.1038_s41586-020-2508-1
    DOI: 10.1038/s41586-020-2508-1
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    Cited by:

    1. Fenghao Sun & Qiwen Qu & Hui Li & Shicheng Jiang & Qingcao Liu & Shuai Ben & Yu Pei & Jiaying Liang & Jiawei Wang & Shanshan Song & Jian Gao & Weifeng Yang & Hongxing Xu & Jian Wu, 2024. "All-optical steering on the proton emission in laser-induced nanoplasmas," Nature Communications, Nature, vol. 15(1), pages 1-7, December.
    2. Tingting Wu & Chongwu Wang & Guangwei Hu & Zhixun Wang & Jiaxin Zhao & Zhe Wang & Ksenia Chaykun & Lin Liu & Mengxiao Chen & Dong Li & Song Zhu & Qihua Xiong & Zexiang Shen & Huajian Gao & Francisco J, 2024. "Ultrastrong exciton-plasmon couplings in WS2 multilayers synthesized with a random multi-singular metasurface at room temperature," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    3. María Barra-Burillo & Unai Muniain & Sara Catalano & Marta Autore & Fèlix Casanova & Luis E. Hueso & Javier Aizpurua & Ruben Esteban & Rainer Hillenbrand, 2021. "Microcavity phonon polaritons from the weak to the ultrastrong phonon–photon coupling regime," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    4. Joshua Mornhinweg & Laura Katharina Diebel & Maike Halbhuber & Michael Prager & Josef Riepl & Tobias Inzenhofer & Dominique Bougeard & Rupert Huber & Christoph Lange, 2024. "Mode-multiplexing deep-strong light-matter coupling," Nature Communications, Nature, vol. 15(1), pages 1-8, December.

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