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Non-thermal emission in gap-mode plasmon photoluminescence

Author

Listed:
  • Robert Lemasters

    (Emory University)

  • Manoj Manjare

    (Emory University)

  • Ryan Freeman

    (Emory University)

  • Feng Wang

    (Emory University)

  • Luka Guy Pierce

    (Emory University)

  • Gordon Hua

    (Emory University)

  • Sergei Urazhdin

    (Emory University)

  • Hayk Harutyunyan

    (Emory University)

Abstract

Photoluminescence from spatially inhomogeneous plasmonic nanostructures exhibits fascinating wavelength-dependent nonlinear behaviors due to the intraband recombination of hot electrons excited into the conduction band of the metal. The properties of the excited carrier distribution and the role of localized plasmonic modes are subjects of debate. In this work, we use plasmonic gap-mode resonators with precise nanometer-scale confinement to show that the nonlinear photoluminescence behavior can become dominated by non-thermal contributions produced by the excited carrier population that strongly deviates from the Fermi-Dirac distribution due to the confinement-induced large-momentum free carrier absorption beyond the dipole approximation. These findings open new pathways for controllable light conversion using nonequilibrium electron states at the nanoscale.

Suggested Citation

  • Robert Lemasters & Manoj Manjare & Ryan Freeman & Feng Wang & Luka Guy Pierce & Gordon Hua & Sergei Urazhdin & Hayk Harutyunyan, 2024. "Non-thermal emission in gap-mode plasmon photoluminescence," Nature Communications, Nature, vol. 15(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-48928-4
    DOI: 10.1038/s41467-024-48928-4
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    References listed on IDEAS

    as
    1. Tal Heilpern & Manoj Manjare & Alexander O. Govorov & Gary P. Wiederrecht & Stephen K. Gray & Hayk Harutyunyan, 2018. "Determination of hot carrier energy distributions from inversion of ultrafast pump-probe reflectivity measurements," Nature Communications, Nature, vol. 9(1), pages 1-6, December.
    2. Judit Budai & Zsuzsanna Pápa & Péter Petrik & Péter Dombi, 2022. "Ultrasensitive probing of plasmonic hot electron occupancies," Nature Communications, Nature, vol. 13(1), pages 1-6, December.
    3. Wen Chen & Philippe Roelli & Aqeel Ahmed & Sachin Verlekar & Huatian Hu & Karla Banjac & Magalí Lingenfelder & Tobias J. Kippenberg & Giulia Tagliabue & Christophe Galland, 2021. "Intrinsic luminescence blinking from plasmonic nanojunctions," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
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