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Universal scaling laws for charge-carrier interactions with quantum confinement in lead-halide perovskites

Author

Listed:
  • Philippe Tamarat

    (Université de Bordeaux, LP2N
    Institut d’Optique and CNRS, LP2N)

  • Elise Prin

    (Université de Bordeaux, LP2N
    Institut d’Optique and CNRS, LP2N)

  • Yuliia Berezovska

    (Empa-Swiss Federal Laboratories for Materials Science and Technology
    ETH Zürich)

  • Anastasiia Moskalenko

    (Empa-Swiss Federal Laboratories for Materials Science and Technology
    ETH Zürich)

  • Thi Phuc Tan Nguyen

    (Univ Rennes, ENSCR, CNRS, ISCR-UMR 6226)

  • Chenghui Xia

    (Université de Bordeaux, LP2N
    Institut d’Optique and CNRS, LP2N)

  • Lei Hou

    (Université de Bordeaux, LP2N
    Institut d’Optique and CNRS, LP2N)

  • Jean-Baptiste Trebbia

    (Université de Bordeaux, LP2N
    Institut d’Optique and CNRS, LP2N)

  • Marios Zacharias

    (Univ Rennes, INSA Rennes, CNRS, Institut FOTON—UMR 6082)

  • Laurent Pedesseau

    (Univ Rennes, INSA Rennes, CNRS, Institut FOTON—UMR 6082)

  • Claudine Katan

    (Univ Rennes, ENSCR, CNRS, ISCR-UMR 6226)

  • Maryna I. Bodnarchuk

    (Empa-Swiss Federal Laboratories for Materials Science and Technology)

  • Maksym V. Kovalenko

    (Empa-Swiss Federal Laboratories for Materials Science and Technology
    ETH Zürich)

  • Jacky Even

    (Univ Rennes, INSA Rennes, CNRS, Institut FOTON—UMR 6082)

  • Brahim Lounis

    (Université de Bordeaux, LP2N
    Institut d’Optique and CNRS, LP2N)

Abstract

Lead halide perovskites open great prospects for optoelectronics and a wealth of potential applications in quantum optical and spin-based technologies. Precise knowledge of the fundamental optical and spin properties of charge-carrier complexes at the origin of their luminescence is crucial in view of the development of these applications. On nearly bulk Cesium-Lead-Bromide single perovskite nanocrystals, which are the test bench materials for next-generation devices as well as theoretical modeling, we perform low temperature magneto-optical spectroscopy to reveal their entire band-edge exciton fine structure and charge-complex binding energies. We demonstrate that the ground exciton state is dark and lays several millielectronvolts below the lowest bright exciton sublevels, which settles the debate on the bright-dark exciton level ordering in these materials. More importantly, combining these results with spectroscopic measurements on various perovskite nanocrystal compounds, we show evidence for universal scaling laws relating the exciton fine structure splitting, the trion and biexciton binding energies to the band-edge exciton energy in lead-halide perovskite nanostructures, regardless of their chemical composition. These scaling laws solely based on quantum confinement effects and dimensionless energies offer a general predictive picture for the interaction energies within charge-carrier complexes photo-generated in these emerging semiconductor nanostructures.

Suggested Citation

  • Philippe Tamarat & Elise Prin & Yuliia Berezovska & Anastasiia Moskalenko & Thi Phuc Tan Nguyen & Chenghui Xia & Lei Hou & Jean-Baptiste Trebbia & Marios Zacharias & Laurent Pedesseau & Claudine Katan, 2023. "Universal scaling laws for charge-carrier interactions with quantum confinement in lead-halide perovskites," Nature Communications, Nature, vol. 14(1), pages 1-8, December.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-35842-4
    DOI: 10.1038/s41467-023-35842-4
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    References listed on IDEAS

    as
    1. Ming Fu & Philippe Tamarat & Jean-Baptiste Trebbia & Maryna I. Bodnarchuk & Maksym V. Kovalenko & Jacky Even & Brahim Lounis, 2018. "Unraveling exciton–phonon coupling in individual FAPbI3 nanocrystals emitting near-infrared single photons," Nature Communications, Nature, vol. 9(1), pages 1-10, December.
    2. Michael A. Becker & Roman Vaxenburg & Georgian Nedelcu & Peter C. Sercel & Andrew Shabaev & Michael J. Mehl & John G. Michopoulos & Samuel G. Lambrakos & Noam Bernstein & John L. Lyons & Thilo Stöferl, 2018. "Bright triplet excitons in caesium lead halide perovskites," Nature, Nature, vol. 553(7687), pages 189-193, January.
    3. Victor I. Klimov & Sergei A. Ivanov & Jagjit Nanda & Marc Achermann & Ilya Bezel & John A. McGuire & Andrei Piryatinski, 2007. "Single-exciton optical gain in semiconductor nanocrystals," Nature, Nature, vol. 447(7143), pages 441-446, May.
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