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Dark exciton-exciton annihilation in monolayer WSe2

Daniel Erkensten1, Samuel Brem2, Koloman Wagner3,7, Roland Gillen4, Raül Perea-Causín1, Jonas D. Ziegler3,7, Takashi Taniguchi5, Kenji Watanabe6, Janina Maultzsch4 et al.

Alexey Chernikov3,7 and Ermin Malic2,1

  • 1Department of Physics, Chalmers University of Technology, 41296 Gothenburg, Sweden
  • 2Department of Physics, Philipps-Universität Marburg, 35037 Marburg, Germany
  • 3Department of Physics, University of Regensburg, D-93040 Regensburg, Germany
  • 4Department of Physics, Friedrich-Alexander-Universität Erlangen-Nürnberg, 91058 Erlangen-Nürnberg, Germany
  • 5International Center for Materials Nanoarchitectonics, National Institute for Materials Science, 1-1 Namiki, Tsukuba 305-004, Japan
  • 6Research Center for Functional Materials, National Institute for Materials Science, Tsukuba, 1-1 Namiki, Tsukuba 305-004, Japan
  • 7Dresden Integrated Center for Applied Physics and Photonic Materials (IAPP) and Würzburg-Dresden Cluster of Excellence ct.qmat, Technische Universität Dresden, 01062 Dresden, Germany

Phys. Rev. B 104, L241406 – Published 17 December, 2021

DOI: https://doi.org/10.1103/PhysRevB.104.L241406

Abstract

The exceptionally strong Coulomb interaction in semiconducting transition-metal dichalcogenides (TMDs) gives rise to a rich exciton landscape consisting of bright and dark exciton states. At elevated densities, excitons can interact through exciton-exciton annihilation (EEA), an Auger-like recombination process limiting the efficiency of optoelectronic applications. Although EEA is a well-known and particularly important process in atomically thin semiconductors determining exciton lifetimes and affecting transport at elevated densities, its microscopic origin has remained elusive. In this joint theory-experiment study combining microscopic and material-specific theory with time- and temperature-resolved photoluminescence measurements, we demonstrate the key role of dark intervalley states that are found to dominate the EEA rate in monolayer WSe2. We reveal an intriguing, characteristic temperature dependence of Auger scattering in this class of materials with an excellent agreement between theory and experiment. Our study provides microscopic insights into the efficiency of technologically relevant Auger scattering channels within the remarkable exciton landscape of atomically thin semiconductors.

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