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How Antisolvent-Induced Ligand Stripping Shapes CsPbX3 Nanocrystals and Their Assemblies

Hiller, Jonas L. ; Thalwitzer, Robert ; Bozkurt, Ata ; Carter, Ross Ewan ; Hettiger, Theresa ; Fröhlich, Markus ; Hodak, Richard ; Gomes Ferreira, Matheus LU orcid ; Eberle, Martin and Kneschaurek, Ekaterina , et al. (2026) In Nano Letters 26(8). p.2955-2963
Abstract

Supercrystals of lead-halide perovskite nanocrystals combine the semiconducting properties of bulk perovskites with quantum confinement effects and extend them to the macroscopic scale. Supercrystals assembled via a two-layer phase diffusion process using an acetonitrile antisolvent were recently shown to be unusually robust. We investigate how the acetonitrile-assisted self-assembly process influences surface chemistry, the atomic lattice of nanocrystals, and the structure of the supercrystal. Using quantitative NMR spectroscopy, nanofocused X-ray diffraction, and optical spectroscopy, we show that a reduced density of the ligand shell caused by the exposure to acetonitrile in the assembly underlies the mechanical robustness of these... (More)

Supercrystals of lead-halide perovskite nanocrystals combine the semiconducting properties of bulk perovskites with quantum confinement effects and extend them to the macroscopic scale. Supercrystals assembled via a two-layer phase diffusion process using an acetonitrile antisolvent were recently shown to be unusually robust. We investigate how the acetonitrile-assisted self-assembly process influences surface chemistry, the atomic lattice of nanocrystals, and the structure of the supercrystal. Using quantitative NMR spectroscopy, nanofocused X-ray diffraction, and optical spectroscopy, we show that a reduced density of the ligand shell caused by the exposure to acetonitrile in the assembly underlies the mechanical robustness of these supercrystals. Ligand stripping further drives a highly size-selecting lateral growth of the supercrystal and induces anisotropic relaxation of the nanocrystal atomic lattice while preserving the electronic coupling and robust light-emitting properties of the assembly. That enables the mechanical manipulation of supercrystals such as stacking, thereby opening new avenues for integration into optoelectronic devices.

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Please use this url to cite or link to this publication:
@article{f4b97b6c-ee17-47d7-942e-1c0bce012a09,
  abstract     = {{<p>Supercrystals of lead-halide perovskite nanocrystals combine the semiconducting properties of bulk perovskites with quantum confinement effects and extend them to the macroscopic scale. Supercrystals assembled via a two-layer phase diffusion process using an acetonitrile antisolvent were recently shown to be unusually robust. We investigate how the acetonitrile-assisted self-assembly process influences surface chemistry, the atomic lattice of nanocrystals, and the structure of the supercrystal. Using quantitative NMR spectroscopy, nanofocused X-ray diffraction, and optical spectroscopy, we show that a reduced density of the ligand shell caused by the exposure to acetonitrile in the assembly underlies the mechanical robustness of these supercrystals. Ligand stripping further drives a highly size-selecting lateral growth of the supercrystal and induces anisotropic relaxation of the nanocrystal atomic lattice while preserving the electronic coupling and robust light-emitting properties of the assembly. That enables the mechanical manipulation of supercrystals such as stacking, thereby opening new avenues for integration into optoelectronic devices.</p>}},
  author       = {{Hiller, Jonas L. and Thalwitzer, Robert and Bozkurt, Ata and Carter, Ross Ewan and Hettiger, Theresa and Fröhlich, Markus and Hodak, Richard and Gomes Ferreira, Matheus and Eberle, Martin and Kneschaurek, Ekaterina and Hinsley, Gerard N. and Wang, Bihan and Ngoi, Kuan Hoon and Nadler, Elke and Roseker, Wojciech and Westermeier, Fabian and Sprung, Michael and Baranov, Dmitry and Lauth, Jannika and Schreiber, Frank and Vartanyants, Ivan A. and Scheele, Marcus and Zaluzhnyy, Ivan A.}},
  issn         = {{1530-6992}},
  language     = {{eng}},
  month        = {{03}},
  number       = {{8}},
  pages        = {{2955--2963}},
  publisher    = {{The American Chemical Society (ACS)}},
  series       = {{Nano Letters}},
  title        = {{How Antisolvent-Induced Ligand Stripping Shapes CsPbX<sub>3</sub> Nanocrystals and Their Assemblies}},
  url          = {{http://dx.doi.org/10.1021/acs.nanolett.5c06380}},
  doi          = {{10.1021/acs.nanolett.5c06380}},
  volume       = {{26}},
  year         = {{2026}},
}