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Cooling-Induced Order-Disorder Phase Transition in CsPbBr3 Nanocrystal Superlattices

Filippi, Umberto LU ; Toso, Stefano LU ; Zaffalon, Matteo L. ; Pianetti, Andrea ; Li, Zhanzhao ; Marras, Sergio ; Goldoni, Luca ; Meinardi, Francesco ; Brovelli, Sergio and Baranov, Dmitry LU orcid , et al. (2025) In Advanced Materials 37(3).
Abstract
Perovskite nanocrystal superlattices are being actively studied after reports have emerged on collective excitonic properties at cryogenic temperatures, where energetic disorder is minimized due to the frozen lattice vibrations. However, an important issue related to structural disorder of superlattices at low temperatures has received little attention to date. In this work, it is shown that CsPbBr3 nanocrystal superlattices undergo a reversible order–disorder transition upon cooling to 90 K. The transition consists of the loss of structural coherence, that is, increased nanocrystal misalignment, and contraction of the superlattices, as revealed by temperature-dependent X-ray diffraction, and is ascribed to the solidification of... (More)
Perovskite nanocrystal superlattices are being actively studied after reports have emerged on collective excitonic properties at cryogenic temperatures, where energetic disorder is minimized due to the frozen lattice vibrations. However, an important issue related to structural disorder of superlattices at low temperatures has received little attention to date. In this work, it is shown that CsPbBr3 nanocrystal superlattices undergo a reversible order–disorder transition upon cooling to 90 K. The transition consists of the loss of structural coherence, that is, increased nanocrystal misalignment, and contraction of the superlattices, as revealed by temperature-dependent X-ray diffraction, and is ascribed to the solidification of ligands (on the basis of Raman spectroscopy). Introducing shorter amines on the nanocrystal surface allows to mitigate these changes, improve order, and shorten interparticle distance. It is demonstrated that the low temperature phase of the short ligand-capped nanocrystal superlattices is characterized by a strong exciton migration observable in the photoluminescence decay, which is due to the shrinkage of the inter-nanocrystal distance. (Less)
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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Advanced Materials
volume
37
issue
3
article number
e2410949
publisher
John Wiley & Sons Inc.
external identifiers
  • pmid:39568247
  • scopus:85209719008
ISSN
1521-4095
DOI
10.1002/adma.202410949
project
Engineering of Superfluorescent Nanocrystal Solids
language
English
LU publication?
yes
additional info
© 2024 The Author(s). Advanced Materials published by Wiley‐VCH GmbH.
id
40b17651-c8bd-4298-8b16-d2010fe53f71
date added to LUP
2024-11-27 16:02:55
date last changed
2025-06-12 19:37:07
@article{40b17651-c8bd-4298-8b16-d2010fe53f71,
  abstract     = {{Perovskite nanocrystal superlattices are being actively studied after reports have emerged on collective excitonic properties at cryogenic temperatures, where energetic disorder is minimized due to the frozen lattice vibrations. However, an important issue related to structural disorder of superlattices at low temperatures has received little attention to date. In this work, it is shown that CsPbBr<sub>3</sub> nanocrystal superlattices undergo a reversible order–disorder transition upon cooling to 90 K. The transition consists of the loss of structural coherence, that is, increased nanocrystal misalignment, and contraction of the superlattices, as revealed by temperature-dependent X-ray diffraction, and is ascribed to the solidification of ligands (on the basis of Raman spectroscopy). Introducing shorter amines on the nanocrystal surface allows to mitigate these changes, improve order, and shorten interparticle distance. It is demonstrated that the low temperature phase of the short ligand-capped nanocrystal superlattices is characterized by a strong exciton migration observable in the photoluminescence decay, which is due to the shrinkage of the inter-nanocrystal distance.}},
  author       = {{Filippi, Umberto and Toso, Stefano and Zaffalon, Matteo L. and Pianetti, Andrea and Li, Zhanzhao and Marras, Sergio and Goldoni, Luca and Meinardi, Francesco and Brovelli, Sergio and Baranov, Dmitry and Manna, Liberato}},
  issn         = {{1521-4095}},
  language     = {{eng}},
  number       = {{3}},
  publisher    = {{John Wiley & Sons Inc.}},
  series       = {{Advanced Materials}},
  title        = {{Cooling-Induced Order-Disorder Phase Transition in CsPbBr<sub>3</sub> Nanocrystal Superlattices}},
  url          = {{http://dx.doi.org/10.1002/adma.202410949}},
  doi          = {{10.1002/adma.202410949}},
  volume       = {{37}},
  year         = {{2025}},
}