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Superlattices are greener on the other side : How light transforms self-assembled mixed halide perovskite nanocrystals

Brennan, Michael C. ; Toso, Stefano ; Pavlovetc, Ilia M. ; Zhukovskyi, Maksym ; Marras, Sergio ; Kuno, Masaru ; Manna, Liberato and Baranov, Dmitry LU orcid (2020) In ACS Energy Letters 5(5). p.1465-1473
Abstract

Perovskite nanocrystal superlattices (NC SLs) are the nearest real-world approximations to monodisperse NC ensembles. NC SLs thus represent ideal model systems for evaluating the optical and structural stability of CsPb(I1xBrx)3 NCs at a macroscopic level. Here, photoinduced changes to CsPb(I1xBrx)3 NC SLs (0 < x < 1.0) are probed via in situ photoluminescence, X-ray diffraction, and electron microscopy. We find that prolonged (∼10−20 h) ultraviolet−visible irradiation causes irreversible PL blueshifts, photobrightening, and crystal structure contractions. These changes stem from gradual photoinduced I2 sublimation, which... (More)

Perovskite nanocrystal superlattices (NC SLs) are the nearest real-world approximations to monodisperse NC ensembles. NC SLs thus represent ideal model systems for evaluating the optical and structural stability of CsPb(I1xBrx)3 NCs at a macroscopic level. Here, photoinduced changes to CsPb(I1xBrx)3 NC SLs (0 < x < 1.0) are probed via in situ photoluminescence, X-ray diffraction, and electron microscopy. We find that prolonged (∼10−20 h) ultraviolet−visible irradiation causes irreversible PL blueshifts, photobrightening, and crystal structure contractions. These changes stem from gradual photoinduced I2 sublimation, which transforms CsPb(I1xBrx)3 into CsPbBr3. Despite eliminating half of the initial halides from individual CsPb(I0.53Br0.47)3 particles, NCs within SLs remarkably preserve their initial crystallinity, cuboidal shapes, edge lengths, and size distributions. This work illustrates compositional control toward generating precisely engineered perovskite NC SLs. It also highlights iodide photo-oxidation as a hurdle that must be overcome if mixed halide perovskite nanomaterials are to be applied beyond fundamental studies.

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author
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publishing date
type
Contribution to journal
publication status
published
in
ACS Energy Letters
volume
5
issue
5
pages
9 pages
publisher
The American Chemical Society (ACS)
external identifiers
  • scopus:85087200931
ISSN
2380-8195
DOI
10.1021/acsenergylett.0c00630
language
English
LU publication?
no
additional info
Publisher Copyright: © 2020 American Chemical Society. All rights reserved.
id
73720770-31e6-4634-8435-0945a061e93d
date added to LUP
2023-01-17 11:56:52
date last changed
2023-01-26 15:06:53
@article{73720770-31e6-4634-8435-0945a061e93d,
  abstract     = {{<p>Perovskite nanocrystal superlattices (NC SLs) are the nearest real-world approximations to monodisperse NC ensembles. NC SLs thus represent ideal model systems for evaluating the optical and structural stability of CsPb(I<sub>1</sub>−<sub>x</sub>Br<sub>x</sub>)<sub>3</sub> NCs at a macroscopic level. Here, photoinduced changes to CsPb(I<sub>1</sub>−<sub>x</sub>Br<sub>x</sub>)<sub>3</sub> NC SLs (0 &lt; x &lt; 1.0) are probed via in situ photoluminescence, X-ray diffraction, and electron microscopy. We find that prolonged (∼10−20 h) ultraviolet−visible irradiation causes irreversible PL blueshifts, photobrightening, and crystal structure contractions. These changes stem from gradual photoinduced I<sub>2</sub> sublimation, which transforms CsPb(I<sub>1</sub>−<sub>x</sub>Br<sub>x</sub>)<sub>3</sub> into CsPbBr<sub>3</sub>. Despite eliminating half of the initial halides from individual CsPb(I<sub>0.53</sub>Br<sub>0.47</sub>)<sub>3</sub> particles, NCs within SLs remarkably preserve their initial crystallinity, cuboidal shapes, edge lengths, and size distributions. This work illustrates compositional control toward generating precisely engineered perovskite NC SLs. It also highlights iodide photo-oxidation as a hurdle that must be overcome if mixed halide perovskite nanomaterials are to be applied beyond fundamental studies.</p>}},
  author       = {{Brennan, Michael C. and Toso, Stefano and Pavlovetc, Ilia M. and Zhukovskyi, Maksym and Marras, Sergio and Kuno, Masaru and Manna, Liberato and Baranov, Dmitry}},
  issn         = {{2380-8195}},
  language     = {{eng}},
  number       = {{5}},
  pages        = {{1465--1473}},
  publisher    = {{The American Chemical Society (ACS)}},
  series       = {{ACS Energy Letters}},
  title        = {{Superlattices are greener on the other side : How light transforms self-assembled mixed halide perovskite nanocrystals}},
  url          = {{http://dx.doi.org/10.1021/acsenergylett.0c00630}},
  doi          = {{10.1021/acsenergylett.0c00630}},
  volume       = {{5}},
  year         = {{2020}},
}