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

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 Mukharamova, Marcus Scheele (), Frank Schreiber, Michael Sprung, Jan Wahl, Sophia Westendorf, Ivan A. Zaluzhnyy and Ivan A. Vartanyants ()
Additional contact information
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
Alfred J. Meixner: Institut für Physikalische und Theoretische Chemie, Universität Tübingen
Nastasia Mukharamova: Deutsches Elektronen-Synchrotron DESY
Marcus Scheele: Institut für Physikalische und Theoretische Chemie, Universität Tübingen
Frank Schreiber: Center for Light-Matter Interaction, Sensors & Analytics LISA+, 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

Nature Communications, 2022, vol. 13, issue 1, 1-10

Abstract: 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.

Date: 2022
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DOI: 10.1038/s41467-022-28486-3

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