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Spatially resolved fluorescence of caesium lead halide perovskite supercrystals reveals quasi-atomic behavior of nanocrystals
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 mode...
Autores principales: | , , , , , , , , , , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group UK
2022
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8850480/ https://www.ncbi.nlm.nih.gov/pubmed/35173165 http://dx.doi.org/10.1038/s41467-022-28486-3 |
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author | Lapkin, Dmitry Kirsch, Christopher Hiller, Jonas Andrienko, Denis Assalauova, Dameli Braun, Kai Carnis, Jerome Kim, Young Yong Mandal, Mukunda Maier, Andre Meixner, Alfred J. Mukharamova, Nastasia Scheele, Marcus Schreiber, Frank Sprung, Michael Wahl, Jan Westendorf, Sophia Zaluzhnyy, Ivan A. Vartanyants, Ivan A. |
author_facet | Lapkin, Dmitry Kirsch, Christopher Hiller, Jonas Andrienko, Denis Assalauova, Dameli Braun, Kai Carnis, Jerome Kim, Young Yong Mandal, Mukunda Maier, Andre Meixner, Alfred J. Mukharamova, Nastasia Scheele, Marcus Schreiber, Frank Sprung, Michael Wahl, Jan Westendorf, Sophia Zaluzhnyy, Ivan A. Vartanyants, Ivan A. |
author_sort | Lapkin, Dmitry |
collection | PubMed |
description | 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. |
format | Online Article Text |
id | pubmed-8850480 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2022 |
publisher | Nature Publishing Group UK |
record_format | MEDLINE/PubMed |
spelling | pubmed-88504802022-03-04 Spatially resolved fluorescence of caesium lead halide perovskite supercrystals reveals quasi-atomic behavior of nanocrystals Lapkin, Dmitry Kirsch, Christopher Hiller, Jonas Andrienko, Denis Assalauova, Dameli Braun, Kai Carnis, Jerome Kim, Young Yong Mandal, Mukunda Maier, Andre Meixner, Alfred J. Mukharamova, Nastasia Scheele, Marcus Schreiber, Frank Sprung, Michael Wahl, Jan Westendorf, Sophia Zaluzhnyy, Ivan A. Vartanyants, Ivan A. Nat Commun Article 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. Nature Publishing Group UK 2022-02-16 /pmc/articles/PMC8850480/ /pubmed/35173165 http://dx.doi.org/10.1038/s41467-022-28486-3 Text en © The Author(s) 2022 https://creativecommons.org/licenses/by/4.0/Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) . |
spellingShingle | Article Lapkin, Dmitry Kirsch, Christopher Hiller, Jonas Andrienko, Denis Assalauova, Dameli Braun, Kai Carnis, Jerome Kim, Young Yong Mandal, Mukunda Maier, Andre Meixner, Alfred J. Mukharamova, Nastasia Scheele, Marcus Schreiber, Frank Sprung, Michael Wahl, Jan Westendorf, Sophia Zaluzhnyy, Ivan A. Vartanyants, Ivan A. Spatially resolved fluorescence of caesium lead halide perovskite supercrystals reveals quasi-atomic behavior of nanocrystals |
title | Spatially resolved fluorescence of caesium lead halide perovskite supercrystals reveals quasi-atomic behavior of nanocrystals |
title_full | Spatially resolved fluorescence of caesium lead halide perovskite supercrystals reveals quasi-atomic behavior of nanocrystals |
title_fullStr | Spatially resolved fluorescence of caesium lead halide perovskite supercrystals reveals quasi-atomic behavior of nanocrystals |
title_full_unstemmed | Spatially resolved fluorescence of caesium lead halide perovskite supercrystals reveals quasi-atomic behavior of nanocrystals |
title_short | Spatially resolved fluorescence of caesium lead halide perovskite supercrystals reveals quasi-atomic behavior of nanocrystals |
title_sort | spatially resolved fluorescence of caesium lead halide perovskite supercrystals reveals quasi-atomic behavior of nanocrystals |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8850480/ https://www.ncbi.nlm.nih.gov/pubmed/35173165 http://dx.doi.org/10.1038/s41467-022-28486-3 |
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