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Photoluminescence upconversion in monolayer WSe2 activated by plasmonic cavities through resonant excitation of dark excitons

Author

Listed:
  • Niclas S. Mueller

    (University of Cambridge
    Fritz Haber Institute of the Max Planck Society)

  • Rakesh Arul

    (University of Cambridge)

  • Gyeongwon Kang

    (University of Cambridge
    Kangwon National University)

  • Ashley P. Saunders

    (Stanford University)

  • Amalya C. Johnson

    (Stanford University)

  • Ana Sánchez-Iglesias

    (CIC biomaGUNE, Basque Research and Technology Alliance (BRTA)
    CSIC-UPV/EHU)

  • Shu Hu

    (University of Cambridge)

  • Lukas A. Jakob

    (University of Cambridge)

  • Jonathan Bar-David

    (University of Cambridge)

  • Bart Nijs

    (University of Cambridge)

  • Luis M. Liz-Marzán

    (CIC biomaGUNE, Basque Research and Technology Alliance (BRTA)
    Ikerbasque, Basque Foundation for Science
    Centro de Investigación Biomédica en Red, Bioingeniería, Biomateriales y Nanomedicina (CIBER-BBN))

  • Fang Liu

    (Stanford University)

  • Jeremy J. Baumberg

    (University of Cambridge)

Abstract

Anti-Stokes photoluminescence (PL) is light emission at a higher photon energy than the excitation, with applications in optical cooling, bioimaging, lasing, and quantum optics. Here, we show how plasmonic nano-cavities activate anti-Stokes PL in WSe2 monolayers through resonant excitation of a dark exciton at room temperature. The optical near-fields of the plasmonic cavities excite the out-of-plane transition dipole of the dark exciton, leading to light emission from the bright exciton at higher energy. Through statistical measurements on hundreds of plasmonic cavities, we show that coupling to the dark exciton leads to a near hundred-fold enhancement of the upconverted PL intensity. This is further corroborated by experiments in which the laser excitation wavelength is tuned across the dark exciton. We show that a precise nanoparticle geometry is key for a consistent enhancement, with decahedral nanoparticle shapes providing an efficient PL upconversion. Finally, we demonstrate a selective and reversible switching of the upconverted PL via electrochemical gating. Our work introduces the dark exciton as an excitation channel for anti-Stokes PL in WSe2 and paves the way for large-area substrates providing nanoscale optical cooling, anti-Stokes lasing, and radiative engineering of excitons.

Suggested Citation

  • Niclas S. Mueller & Rakesh Arul & Gyeongwon Kang & Ashley P. Saunders & Amalya C. Johnson & Ana Sánchez-Iglesias & Shu Hu & Lukas A. Jakob & Jonathan Bar-David & Bart Nijs & Luis M. Liz-Marzán & Fang , 2023. "Photoluminescence upconversion in monolayer WSe2 activated by plasmonic cavities through resonant excitation of dark excitons," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-41401-8
    DOI: 10.1038/s41467-023-41401-8
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    References listed on IDEAS

    as
    1. Minhao He & Pasqual Rivera & Dinh Tuan & Nathan P. Wilson & Min Yang & Takashi Taniguchi & Kenji Watanabe & Jiaqiang Yan & David G. Mandrus & Hongyi Yu & Hanan Dery & Wang Yao & Xiaodong Xu, 2020. "Valley phonons and exciton complexes in a monolayer semiconductor," Nature Communications, Nature, vol. 11(1), pages 1-7, December.
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