Kinetic modelling of intraband carrier relaxation in bulk and nanocrystalline lead-halide perovskites
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Author(s)
Type
Journal Article
Abstract
The relaxation of high-energy “hot” carriers in semiconductors is known to involve the redistribution of energy between hot and cold carriers, as well as the transfer of energy from hot carriers to phonons. Over the past few years, these two processes have been identified in lead-halide perovskites (LHPs) using ultrafast pump-probe experiments, but their interplay is not fully understood. Here we present a practical and intuitive kinetic model that accounts for the effects of both hot and cold carriers on carrier relaxation in LHPs. We apply this model to describe the dynamics of hot carriers in bulk and nanocrystal CsPbBr3 as observed by multi-pulse “pump-push-probe” spectroscopy. The model captures the slowing of relaxation dynamics in the materials as the number of hot carriers increases, which has previously been explained by a “hot-phonon bottleneck” mechanism. The model also correctly predicts an acceleration of the relaxation kinetics as the number of cold carriers in the samples is increased. Using a series of natural approximations, we reduce our model to a simple form containing terms for the carrier-carrier and carrier-phonon interactions. The model can be instrumental for evaluating the details of carrier relaxation and carrier-phonon couplings in LHPs and other soft optoelectronic materials.
Date Issued
2020-07-22
Date Acceptance
2020-07-21
Citation
Physical Chemistry Chemical Physics, 2020, 22 (31), pp.17605-17611
ISSN
1463-9076
Publisher
Royal Society of Chemistry (RSC)
Start Page
17605
End Page
17611
Journal / Book Title
Physical Chemistry Chemical Physics
Volume
22
Issue
31
Copyright Statement
© 2020 The Author(s). This article is licensed under a Creative Commons Attribution-NonCommercial 3.0 Unported Licence (http://creativecommons.org/licenses/by-nc/3.0/).
License URL
Sponsor
The Royal Society
Commission of the European Communities
Identifier
https://pubs.rsc.org/en/Content/ArticleLanding/2020/CP/D0CP01599G#!divAbstract
Grant Number
UF130178
639750
Subjects
02 Physical Sciences
03 Chemical Sciences
09 Engineering
Chemical Physics
Publication Status
Published
Date Publish Online
2020-07-22