Confinement and exciton binding energy effects on hot carrier cooling in lead halide perovskite nanomaterials
Author(s)
Type
Journal Article
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.
Date Issued
2023-04-11
Date Acceptance
2023-03-13
Citation
ACS Nano, 2023, 17 (7), pp.6638-6648
ISSN
1936-0851
Publisher
American Chemical Society
Start Page
6638
End Page
6648
Journal / Book Title
ACS Nano
Volume
17
Issue
7
Copyright Statement
Copyright © 2022 The Authors. Published by American Chemical Society. This publication is licensed under
CC-BY 4.0.
CC-BY 4.0.
License URL
Identifier
https://www.webofscience.com/api/gateway?GWVersion=2&SrcApp=PARTNER_APP&SrcAuth=LinksAMR&KeyUT=WOS:000962222000001&DestLinkType=FullRecord&DestApp=ALL_WOS&UsrCustomerID=a2bf6146997ec60c407a63945d4e92bb
Subjects
ABSORPTION
Chemistry
Chemistry, Multidisciplinary
Chemistry, Physical
CSPBBR3 NANOCRYSTALS
DYNAMICS
ELECTRON
hot carriers
IODIDE PEROVSKITE
Materials Science
Materials Science, Multidisciplinary
nanocrystals
nanoplatelets
Nanoscience & Nanotechnology
PHONON BOTTLENECK
PHOTOLUMINESCENCE
Physical Sciences
QUANTUM DOTS
RELAXATION
Science & Technology
Science & Technology - Other Topics
Technology
THERMALIZATION
two-dimensional perovskites
ultrafast spectroscopy
Publication Status
Published
Date Publish Online
2023-03-20