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Nanoscale Manipulation of Exciton–Trion Interconversion in a MoSe2 Monolayer via Tip-Enhanced Cavity-Spectroscopy

  • Mingu Kang
    Mingu Kang
    Department of Physics, Pohang University of Science and Technology (POSTECH), Pohang 37673, Republic of Korea
    More by Mingu Kang
  • Su Jin Kim
    Su Jin Kim
    Department of Physics, Research Institute for Nanoscale Science and Technology, Chungbuk National University, Cheongju 28644, Republic of Korea
    More by Su Jin Kim
  • Huitae Joo
    Huitae Joo
    Department of Physics, Pohang University of Science and Technology (POSTECH), Pohang 37673, Republic of Korea
    More by Huitae Joo
  • Yeonjeong Koo
    Yeonjeong Koo
    Department of Physics, Pohang University of Science and Technology (POSTECH), Pohang 37673, Republic of Korea
  • Hyeongwoo Lee
    Hyeongwoo Lee
    Department of Physics, Pohang University of Science and Technology (POSTECH), Pohang 37673, Republic of Korea
  • Hyun Seok Lee*
    Hyun Seok Lee
    Department of Physics, Research Institute for Nanoscale Science and Technology, Chungbuk National University, Cheongju 28644, Republic of Korea
    *E-mail: [email protected]
  • Yung Doug Suh*
    Yung Doug Suh
    Department of Chemistry and School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan, 44919 Republic of Korea
    Center for Multidimensional Carbon Materials (CMCM), Institute for Basic Science (IBS), Ulsan 44919, Republic of Korea
    *E-mail: [email protected]
  • , and 
  • Kyoung-Duck Park*
    Kyoung-Duck Park
    Department of Physics, Pohang University of Science and Technology (POSTECH), Pohang 37673, Republic of Korea
    Center for Multidimensional Carbon Materials (CMCM), Institute for Basic Science (IBS), Ulsan 44919, Republic of Korea
    *E-mail: [email protected]
Cite this: Nano Lett. 2024, 24, 1, 279–286
Publication Date (Web):December 20, 2023
https://doi.org/10.1021/acs.nanolett.3c03920
Copyright © 2023 American Chemical Society

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    Abstract

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    Emerging light–matter interactions in metal–semiconductor hybrid platforms have attracted considerable attention due to their potential applications in optoelectronic devices. Here, we demonstrate plasmon-induced near-field manipulation of trionic responses in a MoSe2 monolayer using tip-enhanced cavity-spectroscopy (TECS). The surface plasmon–polariton mode on the Au nanowire can locally manipulate the exciton (X0) and trion (X-) populations of MoSe2. Furthermore, we reveal that surface charges significantly influence the emission and interconversion processes of X0 and X-. In the TECS configuration, the localized plasmon significantly affects the distributions of X0 and X- due to the modified radiative decay rate. Additionally, within the TECS cavity, the electric doping effect and hot electron generation enable dynamic interconversion between X0 and X- at the nanoscale. This work advances our understanding of plasmon–exciton–hot electron interactions in metal–semiconductor–metal hybrid structures, providing a foundation for an optimal trion-based nano-optoelectronic platform.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.nanolett.3c03920.

    • The methods for sample preparation, hyperspectral TECS setup, and FDTD simulation; Figure S1, illustration of fabricating MoSe2/AuNW structures on a SiO2 substrate; Figure S2, optical microscope images of the MoSe2/AuNW structures; Figure S3, angle-dependent scattering responses of an AuNW; Figure S4, AFM topography of the MoSe2/AuNW structure; Figure S5, tip–sample distance-dependent TEPL spectra of MoSe2 on the SiO2 substrate; Figure S6, hyperspectral TEPL images of X0 and X- from the MoSe2/AuNW structure; Figure S7, far-field and near-field line profiles of SPP and X- from the hyperspectral images (PDF)

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