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Tuning perovskite nanocrystal superlattices for superradiance in the presence of disorder

Nguyen, T. P.Tan ; Tan, Liang Z. and Baranov, Dmitry LU orcid (2023) In Journal of Chemical Physics 159(20).
Abstract

The cooperative emission of interacting nanocrystals is an exciting topic fueled by recent reports of superfluorescence and superradiance in assemblies of perovskite nanocubes. Several studies estimated that coherent coupling is localized to a small fraction of nanocrystals (10−7-10−3) within the assembly, raising questions about the origins of localization and ways to overcome it. In this work, we examine single-excitation superradiance by calculating radiative decays and the distribution of superradiant wave function in two-dimensional CsPbBr3 nanocube superlattices. The calculations reveal that the energy disorder caused by size distribution and large interparticle separations reduces radiative... (More)

The cooperative emission of interacting nanocrystals is an exciting topic fueled by recent reports of superfluorescence and superradiance in assemblies of perovskite nanocubes. Several studies estimated that coherent coupling is localized to a small fraction of nanocrystals (10−7-10−3) within the assembly, raising questions about the origins of localization and ways to overcome it. In this work, we examine single-excitation superradiance by calculating radiative decays and the distribution of superradiant wave function in two-dimensional CsPbBr3 nanocube superlattices. The calculations reveal that the energy disorder caused by size distribution and large interparticle separations reduces radiative coupling and leads to the excitation localization, with the energy disorder being the dominant factor. The single-excitation model clearly predicts that, in the pursuit of cooperative effects, having identical nanocubes in the superlattice is more important than achieving a perfect spatial order. The monolayers of large CsPbBr3 nanocubes (LNC = 10-20 nm) are proposed as model systems for experimental tests of superradiance under conditions of non-negligible size dispersion, while small nanocubes (LNC = 5-10 nm) are preferred for realizing the Dicke state under ideal conditions.

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author
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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Journal of Chemical Physics
volume
159
issue
20
article number
204703
publisher
American Institute of Physics (AIP)
external identifiers
  • pmid:37991161
  • scopus:85178386219
ISSN
0021-9606
DOI
10.1063/5.0167542
language
English
LU publication?
yes
additional info
Funding Information: D.B. was funded by the European Union (ERC Starting Grant PROMETHEUS, project No. 101039683). Views and opinions expressed are however those of the authors only and do not necessarily reflect those of the European Union or the European Research Council Executive Agency. Neither the European Union nor the granting authority can be held responsible for them. Funding Information: L.Z.T. was supported by the Molecular Foundry, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. This research used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. Publisher Copyright: © 2023 Author(s).
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cd940c1c-ea37-4488-8141-b0b0056eead9
date added to LUP
2024-01-03 14:44:51
date last changed
2024-09-07 00:37:13
@article{cd940c1c-ea37-4488-8141-b0b0056eead9,
  abstract     = {{<p>The cooperative emission of interacting nanocrystals is an exciting topic fueled by recent reports of superfluorescence and superradiance in assemblies of perovskite nanocubes. Several studies estimated that coherent coupling is localized to a small fraction of nanocrystals (10<sup>−7</sup>-10<sup>−3</sup>) within the assembly, raising questions about the origins of localization and ways to overcome it. In this work, we examine single-excitation superradiance by calculating radiative decays and the distribution of superradiant wave function in two-dimensional CsPbBr<sub>3</sub> nanocube superlattices. The calculations reveal that the energy disorder caused by size distribution and large interparticle separations reduces radiative coupling and leads to the excitation localization, with the energy disorder being the dominant factor. The single-excitation model clearly predicts that, in the pursuit of cooperative effects, having identical nanocubes in the superlattice is more important than achieving a perfect spatial order. The monolayers of large CsPbBr<sub>3</sub> nanocubes (L<sub>NC</sub> = 10-20 nm) are proposed as model systems for experimental tests of superradiance under conditions of non-negligible size dispersion, while small nanocubes (L<sub>NC</sub> = 5-10 nm) are preferred for realizing the Dicke state under ideal conditions.</p>}},
  author       = {{Nguyen, T. P.Tan and Tan, Liang Z. and Baranov, Dmitry}},
  issn         = {{0021-9606}},
  language     = {{eng}},
  month        = {{11}},
  number       = {{20}},
  publisher    = {{American Institute of Physics (AIP)}},
  series       = {{Journal of Chemical Physics}},
  title        = {{Tuning perovskite nanocrystal superlattices for superradiance in the presence of disorder}},
  url          = {{http://dx.doi.org/10.1063/5.0167542}},
  doi          = {{10.1063/5.0167542}},
  volume       = {{159}},
  year         = {{2023}},
}