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

Abstract

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.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. National Renewable Energy Laboratory Chemistry and Nanoscience Center 15013 Denver W Pkwy Golden CO 80401 USA
Publication Date:
Research Org.:
National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
OSTI Identifier:
1879895
Alternate Identifier(s):
OSTI ID: 1883378; OSTI ID: 1893772
Report Number(s):
NREL/JA-5900-82808
Journal ID: ISSN 2195-1071; 2200485
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Published Article
Journal Name:
Advanced Optical Materials
Additional Journal Information:
Journal Name: Advanced Optical Materials Journal Volume: 10 Journal Issue: 20; Journal ID: ISSN 2195-1071
Publisher:
Wiley Blackwell (John Wiley & Sons)
Country of Publication:
Germany
Language:
English
Subject:
36 MATERIALS SCIENCE; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; exciton-polaritons; MoS2; strong coupling; surface plasmon polaritons; transition-metal dichalcogenides; two-dimensional materials; ultrastrong coupling

Citation Formats

Rose, Aaron H., Aubry, Taylor J., Zhang, Hanyu, and van de Lagemaat, Jao. Ultrastrong Coupling of Band‐Nested Excitons in Few‐Layer Molybdenum Disulphide. Germany: N. p., 2022. Web. doi:10.1002/adom.202200485.
Rose, Aaron H., Aubry, Taylor J., Zhang, Hanyu, & van de Lagemaat, Jao. Ultrastrong Coupling of Band‐Nested Excitons in Few‐Layer Molybdenum Disulphide. Germany. https://doi.org/10.1002/adom.202200485
Rose, Aaron H., Aubry, Taylor J., Zhang, Hanyu, and van de Lagemaat, Jao. Thu . "Ultrastrong Coupling of Band‐Nested Excitons in Few‐Layer Molybdenum Disulphide". Germany. https://doi.org/10.1002/adom.202200485.
@article{osti_1879895,
title = {Ultrastrong Coupling of Band‐Nested Excitons in Few‐Layer Molybdenum Disulphide},
author = {Rose, Aaron H. and Aubry, Taylor J. and Zhang, Hanyu and van de Lagemaat, Jao},
abstractNote = {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.},
doi = {10.1002/adom.202200485},
journal = {Advanced Optical Materials},
number = 20,
volume = 10,
place = {Germany},
year = {Thu Aug 04 00:00:00 EDT 2022},
month = {Thu Aug 04 00:00:00 EDT 2022}
}

Journal Article:
Free Publicly Available Full Text
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https://doi.org/10.1002/adom.202200485

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