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Mechanically Robust Supercrystals from Antisolvent-Induced Assembly of Perovskite Nanocrystals

Hiller, Jonas L. ; Thalwitzer, Robert ; Bozkurt, Ata ; Ferreira, Matheus Gomes LU orcid ; Hodak, Richard ; Strauß, Fabian ; Nadler, Elke ; Hinsley, Gerard N. ; Wang, Bihan and Ngoi, Kuan Hoon , et al. (2025) In ACS Nano 19(28).
Abstract

Ordered arrays of nanocrystals, called supercrystals, have attracted significant attention owing to the collective quantum effects arising from the coupling between neighboring nanocrystals. In particular, lead halide perovskite nanocrystals are widely used because of the combination of the optical properties and faceted cubic shape, which enables the formation of highly ordered supercrystals. The most frequently used method for the fabrication of perovskite supercrystals is based on the self-assembly of nanocrystals from solution via slow evaporation of the solvent. However, the supercrystals produced with this technique grow in random positions on the substrate. Moreover, they are mechanically soft due to the presence of organic... (More)

Ordered arrays of nanocrystals, called supercrystals, have attracted significant attention owing to the collective quantum effects arising from the coupling between neighboring nanocrystals. In particular, lead halide perovskite nanocrystals are widely used because of the combination of the optical properties and faceted cubic shape, which enables the formation of highly ordered supercrystals. The most frequently used method for the fabrication of perovskite supercrystals is based on the self-assembly of nanocrystals from solution via slow evaporation of the solvent. However, the supercrystals produced with this technique grow in random positions on the substrate. Moreover, they are mechanically soft due to the presence of organic ligands around the individual nanocrystals. Therefore, such supercrystals cannot be easily manipulated with microgrippers, which hinders their use in applications. In this work, we synthesize mechanically robust supercrystals built from cubic lead halide perovskite nanocrystals by a two-layer phase diffusion self-assembly with acetonitrile as the antisolvent. This method yields highly faceted thick supercrystals, which are robust enough to be picked up and relocated by microgrippers. We employed X-ray nanodiffraction together with high-resolution scanning electron microscopy and atomic force microscopy to reveal the structure of CsPbBr3, CsPbBr2Cl, and CsPbCl3 supercrystals assembled using the two-layer phase diffusion technique and explain their unusual mechanical robustness. Our findings are crucial for further experiments and applications in which supercrystals need to be placed in a precise location, for example, between the electrodes in an electro-optical modulator.

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organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
atomic force microscopy AFM, lead halide perovskite, nanocrystals, scanning electron microscopy SEM, self-assembly, supercrystals, X-ray diffraction
in
ACS Nano
volume
19
issue
28
publisher
The American Chemical Society (ACS)
external identifiers
  • pmid:40634268
  • scopus:105010191954
ISSN
1936-0851
DOI
10.1021/acsnano.5c07289
project
Engineering of Superfluorescent Nanocrystal Solids
language
English
LU publication?
yes
additional info
Publisher Copyright: © 2025 The Authors. Published by American Chemical Society.
id
1e51beb5-8b5e-4905-a803-bbc6ef6ab5a4
date added to LUP
2025-07-29 08:56:58
date last changed
2025-10-21 17:14:41
@article{1e51beb5-8b5e-4905-a803-bbc6ef6ab5a4,
  abstract     = {{<p>Ordered arrays of nanocrystals, called supercrystals, have attracted significant attention owing to the collective quantum effects arising from the coupling between neighboring nanocrystals. In particular, lead halide perovskite nanocrystals are widely used because of the combination of the optical properties and faceted cubic shape, which enables the formation of highly ordered supercrystals. The most frequently used method for the fabrication of perovskite supercrystals is based on the self-assembly of nanocrystals from solution via slow evaporation of the solvent. However, the supercrystals produced with this technique grow in random positions on the substrate. Moreover, they are mechanically soft due to the presence of organic ligands around the individual nanocrystals. Therefore, such supercrystals cannot be easily manipulated with microgrippers, which hinders their use in applications. In this work, we synthesize mechanically robust supercrystals built from cubic lead halide perovskite nanocrystals by a two-layer phase diffusion self-assembly with acetonitrile as the antisolvent. This method yields highly faceted thick supercrystals, which are robust enough to be picked up and relocated by microgrippers. We employed X-ray nanodiffraction together with high-resolution scanning electron microscopy and atomic force microscopy to reveal the structure of CsPbBr<sub>3</sub>, CsPbBr<sub>2</sub>Cl, and CsPbCl<sub>3</sub> supercrystals assembled using the two-layer phase diffusion technique and explain their unusual mechanical robustness. Our findings are crucial for further experiments and applications in which supercrystals need to be placed in a precise location, for example, between the electrodes in an electro-optical modulator.</p>}},
  author       = {{Hiller, Jonas L. and Thalwitzer, Robert and Bozkurt, Ata and Ferreira, Matheus Gomes and Hodak, Richard and Strauß, Fabian and Nadler, Elke and Hinsley, Gerard N. and Wang, Bihan and Ngoi, Kuan Hoon and Rudzinski, Witold and Kneschaurek, Ekaterina and Roseker, Wojciech and Sprung, Michael and Lapkin, Dmitry and Baranov, Dmitry and Schreiber, Frank and Vartanyants, Ivan A. and Scheele, Marcus and Zaluzhnyy, Ivan A.}},
  issn         = {{1936-0851}},
  keywords     = {{atomic force microscopy AFM; lead halide perovskite; nanocrystals; scanning electron microscopy SEM; self-assembly; supercrystals; X-ray diffraction}},
  language     = {{eng}},
  month        = {{07}},
  number       = {{28}},
  publisher    = {{The American Chemical Society (ACS)}},
  series       = {{ACS Nano}},
  title        = {{Mechanically Robust Supercrystals from Antisolvent-Induced Assembly of Perovskite Nanocrystals}},
  url          = {{http://dx.doi.org/10.1021/acsnano.5c07289}},
  doi          = {{10.1021/acsnano.5c07289}},
  volume       = {{19}},
  year         = {{2025}},
}