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Aging of Self-Assembled Lead Halide Perovskite Nanocrystal Superlattices : Effects on Photoluminescence and Energy Transfer

Baranov, Dmitry LU orcid ; Fieramosca, Antonio ; Yang, Ruo Xi ; Polimeno, Laura ; Lerario, Giovanni ; Toso, Stefano ; Giansante, Carlo ; Giorgi, Milena De ; Tan, Liang Z. and Sanvitto, Daniele , et al. (2021) In ACS Nano 15(1). p.650-664
Abstract
Excitonic coupling, electronic coupling, and cooperative interactions in
self-assembled lead halide perovskite nanocrystals were reported to
give rise to a red-shifted collective emission peak with accelerated
dynamics. Here we report that similar spectroscopic features could
appear as a result of the nanocrystal reactivity within the
self-assembled superlattices. This is demonstrated by studying CsPbBr3
nanocrystal superlattices over time with room-temperature and cryogenic
micro-photoluminescence spectroscopy, X-ray diffraction, and electron
microscopy. It is shown that a gradual contraction of the superlattices
and subsequent coalescence of the nanocrystals occurs over several days... (More)
Excitonic coupling, electronic coupling, and cooperative interactions in
self-assembled lead halide perovskite nanocrystals were reported to
give rise to a red-shifted collective emission peak with accelerated
dynamics. Here we report that similar spectroscopic features could
appear as a result of the nanocrystal reactivity within the
self-assembled superlattices. This is demonstrated by studying CsPbBr3
nanocrystal superlattices over time with room-temperature and cryogenic
micro-photoluminescence spectroscopy, X-ray diffraction, and electron
microscopy. It is shown that a gradual contraction of the superlattices
and subsequent coalescence of the nanocrystals occurs over several days
of keeping such structures under vacuum. As a result, a narrow,
low-energy emission peak is observed at 4 K with a concomitant
shortening of the photoluminescence lifetime due to the energy transfer
between nanocrystals. When exposed to air, self-assembled CsPbBr3 nanocrystals develop bulk-like CsPbBr3
particles on top of the superlattices. At 4 K, these particles produce a
distribution of narrow, low-energy emission peaks with short lifetimes
and excitation fluence-dependent, oscillatory decays. Overall, the aging
of CsPbBr3 nanocrystal assemblies dramatically alters their
emission properties and that should not be overlooked when studying
collective optoelectronic phenomena nor confused with superfluorescence
effects. (Less)
Please use this url to cite or link to this publication:
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publishing date
type
Contribution to journal
publication status
published
keywords
energy transfer, environmental stability, low-temperature photoluminescence, nanocrystal superlattices, perovskite nanocrystals, reactivity, self-assembly
in
ACS Nano
volume
15
issue
1
pages
15 pages
publisher
The American Chemical Society (ACS)
external identifiers
  • scopus:85099041613
  • pmid:33350811
ISSN
1936-0851
DOI
10.1021/acsnano.0c06595
language
English
LU publication?
no
additional info
Publisher Copyright: © 2021 American Chemical Society. All rights reserved.
id
c881edca-12a4-48bf-8bd4-56b14ea38141
date added to LUP
2023-01-17 11:56:07
date last changed
2024-09-19 22:44:22
@article{c881edca-12a4-48bf-8bd4-56b14ea38141,
  abstract     = {{Excitonic coupling, electronic coupling, and cooperative interactions in<br>
 self-assembled lead halide perovskite nanocrystals were reported to <br>
give rise to a red-shifted collective emission peak with accelerated <br>
dynamics. Here we report that similar spectroscopic features could <br>
appear as a result of the nanocrystal reactivity within the <br>
self-assembled superlattices. This is demonstrated by studying CsPbBr<sub>3</sub><br>
 nanocrystal superlattices over time with room-temperature and cryogenic<br>
 micro-photoluminescence spectroscopy, X-ray diffraction, and electron <br>
microscopy. It is shown that a gradual contraction of the superlattices <br>
and subsequent coalescence of the nanocrystals occurs over several days <br>
of keeping such structures under vacuum. As a result, a narrow, <br>
low-energy emission peak is observed at 4 K with a concomitant <br>
shortening of the photoluminescence lifetime due to the energy transfer <br>
between nanocrystals. When exposed to air, self-assembled CsPbBr<sub>3</sub> nanocrystals develop bulk-like CsPbBr<sub>3</sub><br>
 particles on top of the superlattices. At 4 K, these particles produce a<br>
 distribution of narrow, low-energy emission peaks with short lifetimes <br>
and excitation fluence-dependent, oscillatory decays. Overall, the aging<br>
 of CsPbBr<sub>3</sub> nanocrystal assemblies dramatically alters their <br>
emission properties and that should not be overlooked when studying <br>
collective optoelectronic phenomena nor confused with superfluorescence <br>
effects.}},
  author       = {{Baranov, Dmitry and Fieramosca, Antonio and Yang, Ruo Xi and Polimeno, Laura and Lerario, Giovanni and Toso, Stefano and Giansante, Carlo and Giorgi, Milena De and Tan, Liang Z. and Sanvitto, Daniele and Manna, Liberato}},
  issn         = {{1936-0851}},
  keywords     = {{energy transfer; environmental stability; low-temperature photoluminescence; nanocrystal superlattices; perovskite nanocrystals; reactivity; self-assembly}},
  language     = {{eng}},
  month        = {{01}},
  number       = {{1}},
  pages        = {{650--664}},
  publisher    = {{The American Chemical Society (ACS)}},
  series       = {{ACS Nano}},
  title        = {{Aging of Self-Assembled Lead Halide Perovskite Nanocrystal Superlattices : Effects on Photoluminescence and Energy Transfer}},
  url          = {{http://dx.doi.org/10.1021/acsnano.0c06595}},
  doi          = {{10.1021/acsnano.0c06595}},
  volume       = {{15}},
  year         = {{2021}},
}