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Near-Unity Light Absorption in a Monolayer WS2 Van der Waals Heterostructure Cavity

  • Itai Epstein*
    Itai Epstein
    ICFO-Institut de Ciencies Fotoniques, The Barcelona Institute of Science and Technology, 08860 Castelldefels, Barcelona, Spain
    *Email: [email protected]
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    Orcidhttp://orcid.org/0000-0002-6174-4025
  • , 
  • Bernat Terrés
    Bernat Terrés
    ICFO-Institut de Ciencies Fotoniques, The Barcelona Institute of Science and Technology, 08860 Castelldefels, Barcelona, Spain
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  • , 
  • André J. Chaves
    André J. Chaves
    Grupo de Materiais Semicondutores e Nanotecnologia and Departamento de Física, Instituto Tecnológico de Aeronáutica, DCTA, 12228-900 São José dos Campos,Brazil
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  • , 
  • Varun-Varma Pusapati
    Varun-Varma Pusapati
    ICFO-Institut de Ciencies Fotoniques, The Barcelona Institute of Science and Technology, 08860 Castelldefels, Barcelona, Spain
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  • , 
  • Daniel A. Rhodes
    Daniel A. Rhodes
    Department of Mechanical Engineering, Columbia University, New York, New York 10027, United States
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  • , 
  • Bettina Frank
    Bettina Frank
    Fourth Physics Institute and Research Center SCoPE, University of Stuttgart, 70569 Stuttgart, Germany
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  • , 
  • Valentin Zimmermann
    Valentin Zimmermann
    Fourth Physics Institute and Research Center SCoPE, University of Stuttgart, 70569 Stuttgart, Germany
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  • , 
  • Ying Qin
    Ying Qin
    School for Engineering of Matter Transport and Energy, Arizona State University, Tempe, Arizona 85287, United States
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  • Kenji Watanabe
    Kenji Watanabe
    National Institute for Materials Science, 1-1 Namiki, Tsukuba 305-0044, Japan
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    Orcidhttp://orcid.org/0000-0003-3701-8119
  • , 
  • Takashi Taniguchi
    Takashi Taniguchi
    National Institute for Materials Science, 1-1 Namiki, Tsukuba 305-0044, Japan
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    Orcidhttp://orcid.org/0000-0002-1467-3105
  • , 
  • Harald Giessen
    Harald Giessen
    Fourth Physics Institute and Research Center SCoPE, University of Stuttgart, 70569 Stuttgart, Germany
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  • , 
  • Sefaattin Tongay
    Sefaattin Tongay
    School for Engineering of Matter Transport and Energy, Arizona State University, Tempe, Arizona 85287, United States
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    Orcidhttp://orcid.org/0000-0001-8294-984X
  • , 
  • James C. Hone
    James C. Hone
    Department of Mechanical Engineering, Columbia University, New York, New York 10027, United States
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  • , 
  • Nuno M. R. Peres
    Nuno M. R. Peres
    Centro de Física and Departamento de Física and QuantaLab, Universidade do Minho, P-4710-057 Braga, Portugal
    International Iberian Nanotechnology Laboratory (INL), Avenida Mestre José Veiga, 4715-330 Braga, Portugal
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  • , and 
  • Frank H. L. Koppens*
    Frank H. L. Koppens
    ICFO-Institut de Ciencies Fotoniques, The Barcelona Institute of Science and Technology, 08860 Castelldefels, Barcelona, Spain
    ICREA—Institució Catalana de Recerca i Estudis Avançats, 08010 Barcelona, Spain
    *Email: [email protected]
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    Orcidhttp://orcid.org/0000-0001-9764-6120
Cite this: Nano Lett. 2020, 20, 5, 3545–3552
Publication Date (Web):April 13, 2020
https://doi.org/10.1021/acs.nanolett.0c00492
Copyright © 2020 American Chemical Society
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    Abstract

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    Excitons in monolayer transition-metal-dichalcogenides (TMDs) dominate their optical response and exhibit strong light–matter interactions with lifetime-limited emission. While various approaches have been applied to enhance light-exciton interactions in TMDs, the achieved strength have been far below unity, and a complete picture of its underlying physical mechanisms and fundamental limits has not been provided. Here, we introduce a TMD-based van der Waals heterostructure cavity that provides near-unity excitonic absorption, and emission of excitonic complexes that are observed at ultralow excitation powers. Our results are in full agreement with a quantum theoretical framework introduced to describe the light–exciton–cavity interaction. We find that the subtle interplay between the radiative, nonradiative and dephasing decay rates plays a crucial role, and unveil a universal absorption law for excitons in 2D systems. This enhanced light–exciton interaction provides a platform for studying excitonic phase-transitions and quantum nonlinearities and enables new possibilities for 2D semiconductor-based optoelectronic devices.

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    • Theoretical modeling, fitting procedure, identification of excitonic complexes, structure optimization, and experimental and fabrication methods (PDF)

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