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Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides

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  • Malte Selig

    (Institut für Theoretische Physik, Nichtlineare Optik und Quantenelektronik, Technische Universität Berlin)

  • Gunnar Berghäuser

    (Institut für Theoretische Physik, Nichtlineare Optik und Quantenelektronik, Technische Universität Berlin)

  • Archana Raja

    (Columbia University
    Stanford University)

  • Philipp Nagler

    (Institut für Experimentelle und Angewandte Physik, Universität Regensburg)

  • Christian Schüller

    (Institut für Experimentelle und Angewandte Physik, Universität Regensburg)

  • Tony F. Heinz

    (Stanford University
    SLAC National Accelerator Laboratory
    Columbia University)

  • Tobias Korn

    (Institut für Experimentelle und Angewandte Physik, Universität Regensburg)

  • Alexey Chernikov

    (Institut für Experimentelle und Angewandte Physik, Universität Regensburg
    Columbia University)

  • Ermin Malic

    (Chalmers University of Technology)

  • Andreas Knorr

    (Institut für Theoretische Physik, Nichtlineare Optik und Quantenelektronik, Technische Universität Berlin)

Abstract

Atomically thin transition metal dichalcogenides are direct-gap semiconductors with strong light–matter and Coulomb interactions. The latter accounts for tightly bound excitons, which dominate their optical properties. Besides the optically accessible bright excitons, these systems exhibit a variety of dark excitonic states. They are not visible in the optical spectra, but can strongly influence the coherence lifetime and the linewidth of the emission from bright exciton states. Here, we investigate the microscopic origin of the excitonic coherence lifetime in two representative materials (WS2 and MoSe2) through a study combining microscopic theory with spectroscopic measurements. We show that the excitonic coherence lifetime is determined by phonon-induced intravalley scattering and intervalley scattering into dark excitonic states. In particular, in WS2, we identify exciton relaxation processes involving phonon emission into lower-lying dark states that are operative at all temperatures.

Suggested Citation

  • Malte Selig & Gunnar Berghäuser & Archana Raja & Philipp Nagler & Christian Schüller & Tony F. Heinz & Tobias Korn & Alexey Chernikov & Ermin Malic & Andreas Knorr, 2016. "Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides," Nature Communications, Nature, vol. 7(1), pages 1-6, December.
    • Handle: RePEc:nat:natcom:v:7:y:2016:i:1:d:10.1038_ncomms13279
    DOI: 10.1038/ncomms13279
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    Cited by:

    1. Rui Cai & Indrajit Wadgaonkar & Jia Wei Melvin Lim & Stefano Dal Forno & David Giovanni & Minjun Feng & Senyun Ye & Marco Battiato & Tze Chien Sum, 2023. "Zero-field quantum beats and spin decoherence mechanisms in CsPbBr3 perovskite nanocrystals," Nature Communications, Nature, vol. 14(1), pages 1-7, December.
    2. M. Wurdack & T. Yun & M. Katzer & A. G. Truscott & A. Knorr & M. Selig & E. A. Ostrovskaya & E. Estrecho, 2023. "Negative-mass exciton polaritons induced by dissipative light-matter coupling in an atomically thin semiconductor," Nature Communications, Nature, vol. 14(1), pages 1-7, December.
    3. Ke Wei & Qirui Liu & Yuxiang Tang & Yingqian Ye & Zhongjie Xu & Tian Jiang, 2023. "Charged biexciton polaritons sustaining strong nonlinearity in 2D semiconductor-based nanocavities," Nature Communications, Nature, vol. 14(1), pages 1-8, December.
    4. Abhijeet M. Kumar & Denis Yagodkin & Roberto Rosati & Douglas J. Bock & Christoph Schattauer & Sarah Tobisch & Joakim Hagel & Bianca Höfer & Jan N. Kirchhof & Pablo Hernández López & Kenneth Burfeindt, 2024. "Strain fingerprinting of exciton valley character in 2D semiconductors," Nature Communications, Nature, vol. 15(1), pages 1-8, December.
    5. Roberto Rosati & Robert Schmidt & Samuel Brem & Raül Perea-Causín & Iris Niehues & Johannes Kern & Johann A. Preuß & Robert Schneider & Steffen Michaelis de Vasconcellos & Rudolf Bratschitsch & Ermin , 2021. "Dark exciton anti-funneling in atomically thin semiconductors," Nature Communications, Nature, vol. 12(1), pages 1-7, December.
    6. Roberto Rosati & Ioannis Paradisanos & Libai Huang & Ziyang Gan & Antony George & Kenji Watanabe & Takashi Taniguchi & Laurent Lombez & Pierre Renucci & Andrey Turchanin & Bernhard Urbaszek & Ermin Ma, 2023. "Interface engineering of charge-transfer excitons in 2D lateral heterostructures," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    7. Shuo Dong & Samuel Beaulieu & Malte Selig & Philipp Rosenzweig & Dominik Christiansen & Tommaso Pincelli & Maciej Dendzik & Jonas D. Ziegler & Julian Maklar & R. Patrick Xian & Alexander Neef & Avaise, 2023. "Observation of ultrafast interfacial Meitner-Auger energy transfer in a Van der Waals heterostructure," Nature Communications, Nature, vol. 14(1), pages 1-8, December.
    8. Yihong Wang & Bin Zhou & Rong Zhao & Bubin Wang & Qi Liu & Minglu Dai, 2022. "Super-Accuracy Calculation for the Half Width of a Voigt Profile," Mathematics, MDPI, vol. 10(2), pages 1-14, January.
    9. Haonan Wang & Heejun Kim & Duanfei Dong & Keisuke Shinokita & Kenji Watanabe & Takashi Taniguchi & Kazunari Matsuda, 2024. "Quantum coherence and interference of a single moiré exciton in nano-fabricated twisted monolayer semiconductor heterobilayers," Nature Communications, Nature, vol. 15(1), pages 1-9, December.

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