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.
Original language | English |
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Article number | 4377 |
Journal | Nature Communications |
Volume | 15 |
DOIs | |
Publication status | Published - 23 May 2024 |
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Dataset supporting Highly Tunable Ground and Excited State Excitonic Dipoles in Multilayer 2H-MoSe2
Shun, F. (Creator), Campbell, A. (Contributor), Brotons i Gisbert, M. (Contributor), Andres-Penares, D. (Contributor), Baek, H. (Contributor), Taniguchi, T. (Contributor), Watanabe, K. (Contributor), Urbaszek, B. (Contributor), Gerber, I. C. (Contributor) & Gerardot, B. D. (Contributor), Heriot-Watt University, 1 Feb 2023
DOI: 10.17861/5a2ae35f-9787-47bc-bb0e-a0395f064509
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