Ultrastrong Coupling of Band‐Nested Excitons in Few‐Layer Molybdenum Disulphide

Rose, Aaron H.; Aubry, Taylor J.; Zhang, Hanyu; van de Lagemaat, Jao

doi:10.1002/adom.202200485

Title: Ultrastrong Coupling of Band‐Nested Excitons in Few‐Layer Molybdenum Disulphide

Journal Article · 03 August 2022 · Advanced Optical Materials

DOI: https://doi.org/10.1002/adom.202200485 · OSTI ID:1879895

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National Renewable Energy Laboratory Chemistry and Nanoscience Center 15013 Denver W Pkwy Golden CO 80401 USA

Abstract The 2D transition‐metal dichalcogenides (2D TMDCs) are an intriguing platform for studying strong light–matter interactions because they combine the electronic properties of conventional semiconductors with the optical resonances found in organic systems. However, the coupling strengths demonstrated in strong exciton–polariton coupling in the 2D TMDCs remain much lower than those found in organic systems. In this paper, a new approach is taken by utilizing the large oscillator strength of the above‐band gap C exciton in few‐layer molybdenum disulphide (FL‐MoS ₂ ). A k ‐space Rabi splitting of 293 meV is shown when coupling FL‐MoS ₂ C excitons to surface plasmon polaritons at room temperature. This value is 11% of the uncoupled exciton energy (2.67 eV or 464 nm), ≈2× what is typically seen in the TMDCs, placing the system in the ultrastrong coupling regime. The results take a step toward finally achieving the efficient quantum coherent processes of ultrastrong coupling in a CMOS‐compatible system—the 2D TMDCs—in the visible spectrum.

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Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 1879895

Report Number(s):: NREL/JA-5900-82808; 2200485

Journal Information:: Advanced Optical Materials, Journal Name: Advanced Optical Materials Journal Issue: 20 Vol. 10; ISSN 2195-1071

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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Title: Ultrastrong Coupling of Band‐Nested Excitons in Few‐Layer Molybdenum Disulphide

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