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Narrow-band high-lying excitons with negative-mass electrons in monolayer WSe2

Author

Listed:
  • Kai-Qiang Lin

    (University of Regensburg)

  • Chin Shen Ong

    (University of California at Berkeley
    Lawrence Berkeley National Laboratory)

  • Sebastian Bange

    (University of Regensburg)

  • Paulo E. Faria Junior

    (University of Regensburg)

  • Bo Peng

    (University of Cambridge)

  • Jonas D. Ziegler

    (University of Regensburg)

  • Jonas Zipfel

    (University of Regensburg)

  • Christian Bäuml

    (University of Regensburg)

  • Nicola Paradiso

    (University of Regensburg)

  • Kenji Watanabe

    (National Institute for Materials Science)

  • Takashi Taniguchi

    (National Institute for Materials Science)

  • Christoph Strunk

    (University of Regensburg)

  • Bartomeu Monserrat

    (University of Cambridge
    University of Cambridge)

  • Jaroslav Fabian

    (University of Regensburg)

  • Alexey Chernikov

    (University of Regensburg
    Technische Universität Dresden)

  • Diana Y. Qiu

    (University of California at Berkeley
    Lawrence Berkeley National Laboratory
    Yale University)

  • Steven G. Louie

    (University of California at Berkeley
    Lawrence Berkeley National Laboratory)

  • John M. Lupton

    (University of Regensburg)

Abstract

Monolayer transition-metal dichalcogenides (TMDCs) show a wealth of exciton physics. Here, we report the existence of a new excitonic species, the high-lying exciton (HX), in single-layer WSe2 with an energy of ~3.4 eV, almost twice the band-edge A-exciton energy, with a linewidth as narrow as 5.8 meV. The HX is populated through momentum-selective optical excitation in the K-valleys and is identified in upconverted photoluminescence (UPL) in the UV spectral region. Strong electron-phonon coupling results in a cascaded phonon progression with equidistant peaks in the luminescence spectrum, resolvable to ninth order. Ab initio GW-BSE calculations with full electron-hole correlations explain HX formation and unmask the admixture of upper conduction-band states to this complex many-body excitation. These calculations suggest that the HX is comprised of electrons of negative mass. The coincidence of such high-lying excitonic species at around twice the energy of band-edge excitons rationalizes the excitonic quantum-interference phenomenon recently discovered in optical second-harmonic generation (SHG) and explains the efficient Auger-like annihilation of band-edge excitons.

Suggested Citation

  • Kai-Qiang Lin & Chin Shen Ong & Sebastian Bange & Paulo E. Faria Junior & Bo Peng & Jonas D. Ziegler & Jonas Zipfel & Christian Bäuml & Nicola Paradiso & Kenji Watanabe & Takashi Taniguchi & Christoph, 2021. "Narrow-band high-lying excitons with negative-mass electrons in monolayer WSe2," Nature Communications, Nature, vol. 12(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-25499-2
    DOI: 10.1038/s41467-021-25499-2
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    Cited by:

    1. 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.

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