Download file (1.59 MB)
Download as zip (1.12 MB)

Collection

Citation

Description:

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 dipolar physics with strong light-matter interactions.

Rights:

• Creative Commons BY Attribution 4.0 International
  

Keyword: Exciton properties, interlayer excitons, electric-field-driven

Date published: 2024-05-23

Publisher: Springer Science and Business Media LLC

Journal:

• Nature Communications (ISSN: 20411723) vol. 15 issue. 1 4377

Funding:

Manuscript type: Publisher's version (Version of record)

MDR DOI:

First published URL: https://doi.org/10.1038/s41467-024-48476-x

Related item:

Other identifier(s):

Contact agent:

Updated at: 2025-02-07 16:30:36 +0900

Published on MDR: 2025-02-07 16:30:36 +0900