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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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    1. Ashish Arora & Matthias Drüppel & Robert Schmidt & Thorsten Deilmann & Robert Schneider & Maciej R. Molas & Philipp Marauhn & Steffen Michaelis de Vasconcellos & Marek Potemski & Michael Rohlfing & Ru, 2017. "Publisher Correction: Interlayer excitons in a bulk van der Waals semiconductor," Nature Communications, Nature, vol. 8(1), pages 1-1, December.
    2. Biswajit Datta & Mandeep Khatoniar & Prathmesh Deshmukh & Félix Thouin & Rezlind Bushati & Simone Liberato & Stephane Kena Cohen & Vinod M. Menon, 2022. "Highly nonlinear dipolar exciton-polaritons in bilayer MoS2," Nature Communications, Nature, vol. 13(1), pages 1-7, December.
    3. Zefang Wang & Daniel A. Rhodes & Kenji Watanabe & Takashi Taniguchi & James C. Hone & Jie Shan & Kin Fai Mak, 2019. "Evidence of high-temperature exciton condensation in two-dimensional atomic double layers," Nature, Nature, vol. 574(7776), pages 76-80, October.
    4. Ioannis Paradisanos & Shivangi Shree & Antony George & Nadine Leisgang & Cedric Robert & Kenji Watanabe & Takashi Taniguchi & Richard J. Warburton & Andrey Turchanin & Xavier Marie & Iann C. Gerber & , 2020. "Controlling interlayer excitons in MoS2 layers grown by chemical vapor deposition," Nature Communications, Nature, vol. 11(1), pages 1-7, December.
    5. Hangyong Shan & Ivan Iorsh & Bo Han & Christoph Rupprecht & Heiko Knopf & Falk Eilenberger & Martin Esmann & Kentaro Yumigeta & Kenji Watanabe & Takashi Taniguchi & Sebastian Klembt & Sven Höfling & S, 2022. "Brightening of a dark monolayer semiconductor via strong light-matter coupling in a cavity," Nature Communications, Nature, vol. 13(1), pages 1-7, December.
    6. Ashish Arora & Matthias Drüppel & Robert Schmidt & Thorsten Deilmann & Robert Schneider & Maciej R. Molas & Philipp Marauhn & Steffen Michaelis de Vasconcellos & Marek Potemski & Michael Rohlfing & Ru, 2017. "Interlayer excitons in a bulk van der Waals semiconductor," Nature Communications, Nature, vol. 8(1), pages 1-6, December.
    7. Kaihui Liu & Liming Zhang & Ting Cao & Chenhao Jin & Diana Qiu & Qin Zhou & Alex Zettl & Peidong Yang & Steve G. Louie & Feng Wang, 2014. "Evolution of interlayer coupling in twisted molybdenum disulfide bilayers," Nature Communications, Nature, vol. 5(1), pages 1-6, December.
    8. M. Goryca & J. Li & A. V. Stier & T. Taniguchi & K. Watanabe & E. Courtade & S. Shree & C. Robert & B. Urbaszek & X. Marie & S. A. Crooker, 2019. "Revealing exciton masses and dielectric properties of monolayer semiconductors with high magnetic fields," Nature Communications, Nature, vol. 10(1), pages 1-12, December.
    9. Archana Raja & Andrey Chaves & Jaeeun Yu & Ghidewon Arefe & Heather M. Hill & Albert F. Rigosi & Timothy C. Berkelbach & Philipp Nagler & Christian Schüller & Tobias Korn & Colin Nuckolls & James Hone, 2017. "Coulomb engineering of the bandgap and excitons in two-dimensional materials," Nature Communications, Nature, vol. 8(1), pages 1-7, August.
    10. Jie Gu & Valentin Walther & Lutz Waldecker & Daniel Rhodes & Archana Raja & James C. Hone & Tony F. Heinz & Stéphane Kéna-Cohen & Thomas Pohl & Vinod M. Menon, 2021. "Enhanced nonlinear interaction of polaritons via excitonic Rydberg states in monolayer WSe2," Nature Communications, Nature, vol. 12(1), pages 1-7, December.
    11. A. A. High & J. R. Leonard & A. T. Hammack & M. M. Fogler & L. V. Butov & A. V. Kavokin & K. L. Campman & A. C. Gossard, 2012. "Spontaneous coherence in a cold exciton gas," Nature, Nature, vol. 483(7391), pages 584-588, March.
    12. Valentin Walther & Robert Johne & Thomas Pohl, 2018. "Giant optical nonlinearities from Rydberg excitons in semiconductor microcavities," Nature Communications, Nature, vol. 9(1), pages 1-6, December.
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