Hybridized Exciton-Photon-Phonon States in a Transition Metal Dichalcogenide van der Waals Heterostructure Microcavity

Journal Article · 23 February 2022 · Physical Review Letters

DOI: https://doi.org/10.1103/physrevlett.128.087401 · OSTI ID:1980265

Li, Donghai  ^[1]; Shan, Hangyong ^[2]; Rupprecht, Christoph  ^[3]; Knopf, Heiko ^[4]; Watanabe, Kenji  ^[5]; Taniguchi, Takashi ^[5]; Qin, Ying ^[6]; Tongay, Sefaattin  ^[6]; Nuß, Matthias ^[3]; Schröder, Sven ^[7]; Eilenberger, Falk ^[4]; Höfling, Sven  ^[3]; Schneider, Christian ^[8]; Brixner, Tobias  ^[3]

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1. Univ. of Wurzburg (Germany); Univ. of Science and Technology of China, Hefei (China); OSTI
2. University of Oldenburg (Germany)
3. Univ. of Wurzburg (Germany)
4. Friedrich Schiller Univ., Jena (Germany); Fraunhofer Institute for Applied Optics and Precision Engineering, Jena (Germany); Max Planck School of Photonics, Jena (Germany)
5. National Institute for Materials Science (NIMS), Tsukuba (Japan)
6. Arizona State Univ., Tempe, AZ (United States)
7. Fraunhofer Institute for Applied Optics and Precision Engineering, Jena (Germany)
8. University of Oldenburg (Germany); Univ. of Wurzburg (Germany)

Excitons in atomically thin transition-metal dichalcogenides (TMDs) have been established as an attractive platform to explore polaritonic physics, owing to their enormous binding energies and giant oscillator strength. Basic spectral features of exciton polaritons in TMD microcavities, thus far, were conventionally explained via two-coupled-oscillator models. This ignores, however, the impact of phonons on the polariton energy structure. Here we establish and quantify the threefold coupling between excitons, cavity photons, and phonons. For this purpose, we employ energy-momentum-resolved photoluminescence and spatially resolved coherent two-dimensional spectroscopy to investigate the spectral properties of a high-quality-factor microcavity with an embedded WSe₂ van der Waals heterostructure at room temperature. Our approach reveals a rich multibranch structure which thus far has not been captured in previous experiments. Simulation of the data reveals hybridized exciton-photon-phonon states, providing new physical insight into the exciton polariton system based on layered TMDs.

• Research Organization: Arizona State Univ., Tempe, AZ (United States)
• Sponsoring Organization: European Research Council (ERC); Federal Ministry of Education and Research of Germany (BMBF); Japan Society for the Promotion of Science (JSPS); National Science Foundation (NSF); USDOE Office of Science (SC)
• Grant/Contract Number: SC0020653
• OSTI ID: 1980265
• Journal Information: Physical Review Letters, Journal Name: Physical Review Letters Journal Issue: 8 Vol. 128; ISSN 0031-9007
• Publisher: American Physical Society (APS)Copyright Statement
• Country of Publication: United States
• Language: English