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

Shun Feng, Aidan J. Campbell, Mauro Brotons-Gisbert (), Daniel Andres-Penares, Hyeonjun Baek, Takashi Taniguchi, Kenji Watanabe, Bernhard Urbaszek, Iann C. Gerber and Brian D. Gerardot ()
Additional contact information
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

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: 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.

Date: 2024
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DOI: 10.1038/s41467-024-48476-x

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