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Description:

Excitons in bilayer transition metal dichalcogenides (2L-TMDs) are Coulomb-bound electron/hole pairs that can be viewed as broadly tunable analogs of atomic or molecular systems. In particular, under an out-of-plane electric field, various inter- and intralayer excitons in 2L-TMDs are brought into energetic resonance, forming complex hybridized states with novel properties. However, previous studies were limited to only a few select states due to insufficient electric field strength. Here, to overcome this limit, we sandwich a 2L-TMD between layers of solid-state donor and organic acceptor molecules. Charge transfer across the donor/acceptor components allows applying an electric field reaching > 0.27 V nm-1, about twice higher than previously available. Additionally, the density of the top molecular layer can be tuned during the experiment, at cryogenic temperatures, with a new technique of in situ evaporation of acceptor molecules. Under a high electric field, we discover a range of new behaviors for excitons in 2L-TMDs. First, as the result of hybridization, intralayer excitons acquire an interlayer character. Second, the same hybridization allows us to detect new excitonic species, including the interlayer “B” exciton. Third, we observe an ultrastrong Stark splitting of > 380 meV with exciton energies tunable over a large range of the optical spectrum, with potential implications for optoelectronics. Our work creates new possibilities for using strong electric fields to unlock new physical regimes and control exciton hybridization in 2D heterostructures and other systems.

Rights:

• Creative Commons BY Attribution 4.0 International
  

Keyword: interlayer excitons
, 2D bilayers, molecular gating

Date published: 2025-11-10

Publisher: Springer Science and Business Media LLC

Journal:

• Nature Communications (ISSN: 20411723) vol. 16 issue. 1 9893

Funding:

• Deutsche Forschungsgemeinschaft TRR227
• Deutsche Forschungsgemeinschaft SfB1772
• Deutsche Forschungsgemeinschaft SfB951
• Deutsche Forschungsgemeinschaft GZ: BO 5142/4-1
• Bundesministerium für Bildung, Wissenschaft, Forschung und Technologie 05K2022 – ioARPES

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

MDR DOI:

First published URL: https://doi.org/10.1038/s41467-025-65431-6

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Updated at: 2026-05-25 08:56:29 +0900

Published on MDR: 2026-05-25 10:29:22 +0900