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Are Shockley-Read-Hall and ABC models valid for lead halide perovskites?

Kiligaridis, Alexander LU ; Frantsuzov, Pavel A. LU ; Yangui, Aymen LU ; Seth, Sudipta LU ; Li, Jun LU orcid ; An, Qingzhi ; Vaynzof, Yana and Scheblykin, Ivan G. LU orcid (2021) In Nature Communications 12.
Abstract

Metal halide perovskites are an important class of emerging semiconductors. Their charge carrier dynamics is poorly understood due to limited knowledge of defect physics and charge carrier recombination mechanisms. Nevertheless, classical ABC and Shockley-Read-Hall (SRH) models are ubiquitously applied to perovskites without considering their validity. Herein, an advanced technique mapping photoluminescence quantum yield (PLQY) as a function of both the excitation pulse energy and repetition frequency is developed and employed to examine the validity of these models. While ABC and SRH fail to explain the charge dynamics in a broad range of conditions, the addition of Auger recombination and trapping to the SRH model enables a... (More)

Metal halide perovskites are an important class of emerging semiconductors. Their charge carrier dynamics is poorly understood due to limited knowledge of defect physics and charge carrier recombination mechanisms. Nevertheless, classical ABC and Shockley-Read-Hall (SRH) models are ubiquitously applied to perovskites without considering their validity. Herein, an advanced technique mapping photoluminescence quantum yield (PLQY) as a function of both the excitation pulse energy and repetition frequency is developed and employed to examine the validity of these models. While ABC and SRH fail to explain the charge dynamics in a broad range of conditions, the addition of Auger recombination and trapping to the SRH model enables a quantitative fitting of PLQY maps and low-power PL decay kinetics, and extracting trap concentrations and efficacies. However, PL kinetics at high power are too fast and cannot be explained. The proposed PLQY mapping technique is ideal for a comprehensive testing of theories and applicable to any semiconductor.

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author
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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Nature Communications
volume
12
article number
3329
publisher
Nature Publishing Group
external identifiers
  • scopus:85107577151
  • pmid:34099662
ISSN
2041-1723
DOI
10.1038/s41467-021-23275-w
language
English
LU publication?
yes
id
bd50c3da-c9f7-4732-a75e-acebd477251b
date added to LUP
2021-07-01 13:49:28
date last changed
2024-06-29 14:13:29
@article{bd50c3da-c9f7-4732-a75e-acebd477251b,
  abstract     = {{<p>Metal halide perovskites are an important class of emerging semiconductors. Their charge carrier dynamics is poorly understood due to limited knowledge of defect physics and charge carrier recombination mechanisms. Nevertheless, classical ABC and Shockley-Read-Hall (SRH) models are ubiquitously applied to perovskites without considering their validity. Herein, an advanced technique mapping photoluminescence quantum yield (PLQY) as a function of both the excitation pulse energy and repetition frequency is developed and employed to examine the validity of these models. While ABC and SRH fail to explain the charge dynamics in a broad range of conditions, the addition of Auger recombination and trapping to the SRH model enables a quantitative fitting of PLQY maps and low-power PL decay kinetics, and extracting trap concentrations and efficacies. However, PL kinetics at high power are too fast and cannot be explained. The proposed PLQY mapping technique is ideal for a comprehensive testing of theories and applicable to any semiconductor.</p>}},
  author       = {{Kiligaridis, Alexander and Frantsuzov, Pavel A. and Yangui, Aymen and Seth, Sudipta and Li, Jun and An, Qingzhi and Vaynzof, Yana and Scheblykin, Ivan G.}},
  issn         = {{2041-1723}},
  language     = {{eng}},
  publisher    = {{Nature Publishing Group}},
  series       = {{Nature Communications}},
  title        = {{Are Shockley-Read-Hall and ABC models valid for lead halide perovskites?}},
  url          = {{http://dx.doi.org/10.1038/s41467-021-23275-w}},
  doi          = {{10.1038/s41467-021-23275-w}},
  volume       = {{12}},
  year         = {{2021}},
}