Confinement and Exciton Binding Energy Effects on Hot Carrier Cooling in Lead Halide Perovskite Nanomaterials
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Date
2023-04-11
Publication Type
Journal Article
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Abstract
The relaxation of the above-gap ("hot") carriers in lead halide perovskites (LHPs) is important for applications in photovoltaics and offers insights into carrier-carrier and carrier-phonon interactions. However, the role of quantum confinement in the hot carrier dynamics of nanosystems is still disputed. Here, we devise a single approach, ultrafast pump- push-probe spectroscopy, to study carrier cooling in six different size-controlled LHP nanomaterials. In cuboidal nanocrystals, we observe only a weak size effect on the cooling dynamics. In contrast, two-dimensional systems show suppression of the hot phonon bottleneck effect common in bulk perovskites. The proposed kinetic model describes the intrinsic and density-dependent cooling times accurately in all studied perovskite systems using only carrier-carrier, carrier-phonon, and excitonic coupling constants. This highlights the impact of exciton formation on carrier cooling and promotes dimensional confinement as a tool for engineering carrier-phonon and carrier-carrier interactions in LHP optoelectronic materials.
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published
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Volume
17 (7)
Pages / Article No.
6638 - 6648
Publisher
American Chemical Society
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Subject
hot carriers; two-dimensional perovskites; nanoplatelets; nanocrystals; ultrafast spectroscopy
Organisational unit
03934 - Kovalenko, Maksym / Kovalenko, Maksym
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Funding
899141 - Polariton logic (EC)