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Highly tunable ground and excited state excitonic dipoles in multilayer 2H-MoSe2

Author

Listed:
  • Shun Feng

    (Heriot-Watt University)

  • Aidan J. Campbell

    (Heriot-Watt University)

  • Mauro Brotons-Gisbert

    (Heriot-Watt University)

  • Daniel Andres-Penares

    (Heriot-Watt University)

  • Hyeonjun Baek

    (Heriot-Watt University)

  • Takashi Taniguchi

    (National Institute for Materials Science)

  • Kenji Watanabe

    (National Institute for Materials Science)

  • Bernhard Urbaszek

    (Technische Universität Darmstadt)

  • Iann C. Gerber

    (Université de Toulouse)

  • Brian D. Gerardot

    (Heriot-Watt University)

Abstract

The fundamental properties of an exciton are determined by the spin, valley, energy, and spatial wavefunctions of the Coulomb-bound electron and hole. In van der Waals materials, these attributes can be widely engineered through layer stacking configuration to create highly tunable interlayer excitons with static out-of-plane electric dipoles, at the expense of the strength of the oscillating in-plane dipole responsible for light-matter coupling. Here we show that interlayer excitons in bi- and tri-layer 2H-MoSe2 crystals exhibit electric-field-driven coupling with the ground (1s) and excited states (2s) of the intralayer A excitons. We demonstrate that the hybrid states of these distinct exciton species provide strong oscillator strength, large permanent dipoles (up to 0.73 ± 0.01 enm), high energy tunability (up to ~200 meV), and full control of the spin and valley characteristics such that the exciton g-factor can be manipulated over a large range (from −4 to +14). Further, we observe the bi- and tri-layer excited state (2s) interlayer excitons and their coupling with the intralayer excitons states (1s and 2s). Our results, in good agreement with a coupled oscillator model with spin (layer)-selectivity and beyond standard density functional theory calculations, promote multilayer 2H-MoSe2 as a highly tunable platform to explore exciton-exciton interactions with strong light-matter interactions.

Suggested Citation

  • Shun Feng & Aidan J. Campbell & Mauro Brotons-Gisbert & Daniel Andres-Penares & Hyeonjun Baek & Takashi Taniguchi & Kenji Watanabe & Bernhard Urbaszek & Iann C. Gerber & Brian D. Gerardot, 2024. "Highly tunable ground and excited state excitonic dipoles in multilayer 2H-MoSe2," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-48476-x
    DOI: 10.1038/s41467-024-48476-x
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