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Spatially resolved fluorescence of caesium lead halide perovskite supercrystals reveals quasi-atomic behavior of nanocrystals

Author

Listed:
  • Dmitry Lapkin

    (Deutsches Elektronen-Synchrotron DESY)

  • Christopher Kirsch

    (Institut für Physikalische und Theoretische Chemie, Universität Tübingen)

  • Jonas Hiller

    (Institut für Physikalische und Theoretische Chemie, Universität Tübingen)

  • Denis Andrienko

    (Max Planck Institute for Polymer Research)

  • Dameli Assalauova

    (Deutsches Elektronen-Synchrotron DESY)

  • Kai Braun

    (Institut für Physikalische und Theoretische Chemie, Universität Tübingen)

  • Jerome Carnis

    (Deutsches Elektronen-Synchrotron DESY)

  • Young Yong Kim

    (Deutsches Elektronen-Synchrotron DESY)

  • Mukunda Mandal

    (Max Planck Institute for Polymer Research)

  • Andre Maier

    (Institut für Physikalische und Theoretische Chemie, Universität Tübingen
    Center for Light-Matter Interaction, Sensors & Analytics LISA+, Universität Tübingen)

  • Alfred J. Meixner

    (Institut für Physikalische und Theoretische Chemie, Universität Tübingen
    Center for Light-Matter Interaction, Sensors & Analytics LISA+, Universität Tübingen)

  • Nastasia Mukharamova

    (Deutsches Elektronen-Synchrotron DESY)

  • Marcus Scheele

    (Institut für Physikalische und Theoretische Chemie, Universität Tübingen
    Center for Light-Matter Interaction, Sensors & Analytics LISA+, Universität Tübingen)

  • Frank Schreiber

    (Center for Light-Matter Interaction, Sensors & Analytics LISA+, Universität Tübingen
    Institut für Angewandte Physik, Universität Tübingen)

  • Michael Sprung

    (Deutsches Elektronen-Synchrotron DESY)

  • Jan Wahl

    (Institut für Physikalische und Theoretische Chemie, Universität Tübingen)

  • Sophia Westendorf

    (Institut für Physikalische und Theoretische Chemie, Universität Tübingen)

  • Ivan A. Zaluzhnyy

    (Institut für Angewandte Physik, Universität Tübingen)

  • Ivan A. Vartanyants

    (Deutsches Elektronen-Synchrotron DESY
    National Research Nuclear University MEPhI (Moscow Engineering Physics Institute))

Abstract

We correlate spatially resolved fluorescence (-lifetime) measurements with X-ray nanodiffraction to reveal surface defects in supercrystals of self-assembled cesium lead halide perovskite nanocrystals and study their effect on the fluorescence properties. Upon comparison with density functional modeling, we show that a loss in structural coherence, an increasing atomic misalignment between adjacent nanocrystals, and growing compressive strain near the surface of the supercrystal are responsible for the observed fluorescence blueshift and decreased fluorescence lifetimes. Such surface defect-related optical properties extend the frequently assumed analogy between atoms and nanocrystals as so-called quasi-atoms. Our results emphasize the importance of minimizing strain during the self-assembly of perovskite nanocrystals into supercrystals for lighting application such as superfluorescent emitters.

Suggested Citation

  • Dmitry Lapkin & Christopher Kirsch & Jonas Hiller & Denis Andrienko & Dameli Assalauova & Kai Braun & Jerome Carnis & Young Yong Kim & Mukunda Mandal & Andre Maier & Alfred J. Meixner & Nastasia Mukha, 2022. "Spatially resolved fluorescence of caesium lead halide perovskite supercrystals reveals quasi-atomic behavior of nanocrystals," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-28486-3
    DOI: 10.1038/s41467-022-28486-3
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    References listed on IDEAS

    as
    1. Ihor Cherniukh & Gabriele Rainò & Thilo Stöferle & Max Burian & Alex Travesset & Denys Naumenko & Heinz Amenitsch & Rolf Erni & Rainer F. Mahrt & Maryna I. Bodnarchuk & Maksym V. Kovalenko, 2021. "Perovskite-type superlattices from lead halide perovskite nanocubes," Nature, Nature, vol. 593(7860), pages 535-542, May.
    2. Florian Fetzer & Andre Maier & Martin Hodas & Olympia Geladari & Kai Braun & Alfred J. Meixner & Frank Schreiber & Andreas Schnepf & Marcus Scheele, 2020. "Structural order enhances charge carrier transport in self-assembled Au-nanoclusters," Nature Communications, Nature, vol. 11(1), pages 1-8, December.
    3. Justin G. Bohnet & Zilong Chen & Joshua M. Weiner & Dominic Meiser & Murray J. Holland & James K. Thompson, 2012. "A steady-state superradiant laser with less than one intracavity photon," Nature, Nature, vol. 484(7392), pages 78-81, April.
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