IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v14y2023i1d10.1038_s41467-023-41401-8.html
   My bibliography  Save this article

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
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-023-41401-8
    File Function: Abstract
    Download Restriction: no

    File URL: https://libkey.io/10.1038/s41467-023-41401-8?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
    ---><---

    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.
    2. K. Mergenthaler & N. Anttu & N. Vainorius & M. Aghaeipour & S. Lehmann & M. T. Borgström & L. Samuelson & M.-E. Pistol, 2017. "Anti-Stokes photoluminescence probing k-conservation and thermalization of minority carriers in degenerately doped semiconductors," Nature Communications, Nature, vol. 8(1), pages 1-6, December.
    3. Zhipeng Li & Tianmeng Wang & Chenhao Jin & Zhengguang Lu & Zhen Lian & Yuze Meng & Mark Blei & Shiyuan Gao & Takashi Taniguchi & Kenji Watanabe & Tianhui Ren & Sefaattin Tongay & Li Yang & Dmitry Smir, 2019. "Emerging photoluminescence from the dark-exciton phonon replica in monolayer WSe2," Nature Communications, Nature, vol. 10(1), pages 1-7, December.
    4. M. Manca & M. M. Glazov & C. Robert & F. Cadiz & T. Taniguchi & K. Watanabe & E. Courtade & T. Amand & P. Renucci & X. Marie & G. Wang & B. Urbaszek, 2017. "Enabling valley selective exciton scattering in monolayer WSe2 through upconversion," Nature Communications, Nature, vol. 8(1), pages 1-7, April.
    5. Marie-Elena Kleemann & Rohit Chikkaraddy & Evgeny M. Alexeev & Dean Kos & Cloudy Carnegie & Will Deacon & Alex Casalis Pury & Christoph Große & Bart Nijs & Jan Mertens & Alexander I. Tartakovskii & Je, 2017. "Strong-coupling of WSe2 in ultra-compact plasmonic nanocavities at room temperature," Nature Communications, Nature, vol. 8(1), pages 1-7, December.
    6. J. Jadczak & L. Bryja & J. Kutrowska-Girzycka & P. Kapuściński & M. Bieniek & Y.-S. Huang & P. Hawrylak, 2019. "Room temperature multi-phonon upconversion photoluminescence in monolayer semiconductor WS2," Nature Communications, Nature, vol. 10(1), pages 1-10, December.
    Full references (including those not matched with items on IDEAS)

    Most related items

    These are the items that most often cite the same works as this one and are cited by the same works as this one.
    1. Zhiheng Huang & Yunfei Bai & Yanchong Zhao & Le Liu & Xuan Zhao & Jiangbin Wu & Kenji Watanabe & Takashi Taniguchi & Wei Yang & Dongxia Shi & Yang Xu & Tiantian Zhang & Qingming Zhang & Ping-Heng Tan , 2024. "Observation of phonon Stark effect," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    2. Xin Cong & Parisa Ali Mohammadi & Mingyang Zheng & Kenji Watanabe & Takashi Taniguchi & Daniel Rhodes & Xiao-Xiao Zhang, 2023. "Interplay of valley polarized dark trion and dark exciton-polaron in monolayer WSe2," Nature Communications, Nature, vol. 14(1), pages 1-7, December.
    3. Kai-Qiang Lin & Jonas D. Ziegler & Marina A. Semina & Javid V. Mamedov & Kenji Watanabe & Takashi Taniguchi & Sebastian Bange & Alexey Chernikov & Mikhail M. Glazov & John M. Lupton, 2022. "High-lying valley-polarized trions in 2D semiconductors," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    4. Juan Francisco Gonzalez Marin & Dmitrii Unuchek & Zhe Sun & Cheol Yeon Cheon & Fedele Tagarelli & Kenji Watanabe & Takashi Taniguchi & Andras Kis, 2022. "Room-temperature electrical control of polarization and emission angle in a cavity-integrated 2D pulsed LED," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    5. Pablo Hernández López & Sebastian Heeg & Christoph Schattauer & Sviatoslav Kovalchuk & Abhijeet Kumar & Douglas J. Bock & Jan N. Kirchhof & Bianca Höfer & Kyrylo Greben & Denis Yagodkin & Lukas Linhar, 2022. "Strain control of hybridization between dark and localized excitons in a 2D semiconductor," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    6. Erfu Liu & Jeremiah Baren & Zhengguang Lu & Takashi Taniguchi & Kenji Watanabe & Dmitry Smirnov & Yia-Chung Chang & Chun Hung Lui, 2021. "Exciton-polaron Rydberg states in monolayer MoSe2 and WSe2," Nature Communications, Nature, vol. 12(1), pages 1-8, December.
    7. 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.
    8. Saroj B. Chand & John M. Woods & Jiamin Quan & Enrique Mejia & Takashi Taniguchi & Kenji Watanabe & Andrea Alù & Gabriele Grosso, 2023. "Interaction-driven transport of dark excitons in 2D semiconductors with phonon-mediated optical readout," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    9. Soungmin Bae & Kana Matsumoto & Hannes Raebiger & Ken-ichi Shudo & Yong-Hoon Kim & Ørjan Sele Handegård & Tadaaki Nagao & Masahiro Kitajima & Yuji Sakai & Xiang Zhang & Robert Vajtai & Pulickel Ajayan, 2022. "K-point longitudinal acoustic phonons are responsible for ultrafast intervalley scattering in monolayer MoSe2," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    10. Xiaotong Chen & Zhen Lian & Yuze Meng & Lei Ma & Su-Fei Shi, 2023. "Excitonic Complexes in Two-Dimensional Transition Metal Dichalcogenides," Nature Communications, Nature, vol. 14(1), pages 1-5, December.
    11. 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.

    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:14:y:2023:i:1:d:10.1038_s41467-023-41401-8. 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.

    If CitEc recognized a bibliographic reference but did not link an item in RePEc to it, you can help with 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.