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Gate-Tunable Bound Exciton Manifolds in Monolayer MoSe2
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    Gate-Tunable Bound Exciton Manifolds in Monolayer MoSe2
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    • Yuan Chen
      Yuan Chen
      Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore 117543, Singapore
      More by Yuan Chen
    • Haidong Liang
      Haidong Liang
      Centre for Ion Beam Applications (CIBA), Department of Physics, National University of Singapore, Singapore 117542, Singapore
      Department of Physics, National University of Singapore, 2 Science Drive 3, Singapore 117551, Singapore
    • Leyi Loh
      Leyi Loh
      Department of Physics, National University of Singapore, 2 Science Drive 3, Singapore 117551, Singapore
      Department of Materials Science and Engineering, National University of Singapore, 9 Engineering Drive 1, Singapore 117575, Singapore
      More by Leyi Loh
    • Yiwei Ho
      Yiwei Ho
      Department of Physics, National University of Singapore, 2 Science Drive 3, Singapore 117551, Singapore
      More by Yiwei Ho
    • Ivan Verzhbitskiy
      Ivan Verzhbitskiy
      Department of Physics, National University of Singapore, 2 Science Drive 3, Singapore 117551, Singapore
    • Kenji Watanabe
      Kenji Watanabe
      Research Centre for Functional Materials, National Institute for Materials Science, Tsukuba 305-0044, Japan
    • Takashi Taniguchi
      Takashi Taniguchi
      International Centre for Materials Nanoarchitectonics, National Institute for Materials Science, Tsukuba 305-0044, Japan
    • Michel Bosman
      Michel Bosman
      Department of Materials Science and Engineering, National University of Singapore, 9 Engineering Drive 1, Singapore 117575, Singapore
      Institute of Materials Research and Engineering, Agency for Science, Technology and Research (A*STAR), 2 Fusionopolis Way, Singapore 138634, Singapore
    • Andrew A. Bettiol
      Andrew A. Bettiol
      Centre for Ion Beam Applications (CIBA), Department of Physics, National University of Singapore, Singapore 117542, Singapore
      Department of Physics, National University of Singapore, 2 Science Drive 3, Singapore 117551, Singapore
    • Goki Eda*
      Goki Eda
      Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore 117543, Singapore
      Department of Physics, National University of Singapore, 2 Science Drive 3, Singapore 117551, Singapore
      Centre for Advanced 2D Materials, National University of Singapore, 117542, Singapore, Singapore
      *Email for G.E.: [email protected]).
      More by Goki Eda
    Other Access OptionsSupporting Information (1)

    Nano Letters

    Cite this: Nano Lett. 2023, 23, 10, 4456–4463
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    https://doi.org/10.1021/acs.nanolett.3c00814
    Published May 3, 2023
    Copyright © 2023 American Chemical Society

    Abstract

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    Two-dimensional (2D) semiconductors with point defects are predicted to host a variety of bound exciton complexes analogous to trions and biexcitons due to strong many-body effects. However, despite the common observation of defect-mediated subgap emission, the existence of such complexes remains elusive. Here, we report the observation of bound exciton (BX) complex manifolds in monolayer MoSe2 with intentionally created monoselenium vacancies (VSe) using proton beam irradiation. The emission intensity of different BX peaks is found to exhibit contrasting dependence on electrostatic doping near the onset of free electron injection. The observed trend is consistent with the model in which free excitons exist in equilibrium with excitons bound to neutral and charged VSe defects, which act as deep acceptors. These complexes are more strongly bound than trions and biexcitons, surviving up to around 180 K, and exhibit moderate valley polarization memory, indicating partial free exciton character.

    Copyright © 2023 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.nanolett.3c00814.

    • Lorentz fitting of BX emissions, effect of proton beam fluence on BX emissions, spatial PL mapping, STEM statistics, hBN encapsulation effect, transfer curve, gate-dependent PL, time-resolved PL, and a comparison of the two-particle model and bound-exciton-model with our experimental data (PDF)

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    Nano Letters

    Cite this: Nano Lett. 2023, 23, 10, 4456–4463
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.nanolett.3c00814
    Published May 3, 2023
    Copyright © 2023 American Chemical Society

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