Confinement and Exciton Binding Energy Effects on Hot Carrier Cooling in Lead Halide Perovskite Nanomaterials
Research output: Contribution to journal › Research article › Contributed › peer-review
Contributors
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.
Details
Original language | English |
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Pages (from-to) | 6638-6648 |
Number of pages | 11 |
Journal | ACS nano |
Volume | 17 |
Issue number | 7 |
Publication status | Published - 11 Apr 2023 |
Peer-reviewed | Yes |
External IDs
PubMed | 36939330 |
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WOS | 000962222000001 |
Keywords
Subject groups, research areas, subject areas according to Destatis
Sustainable Development Goals
ASJC Scopus subject areas
Keywords
- hot carriers, nanocrystals, nanoplatelets, two-dimensional perovskites, ultrafast spectroscopy, Nanoplatelets, Nanocrystals, Two-dimensional perovskites, Hot carriers, Ultrafast spectroscopy