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Tailoring Auger Recombination Dynamics in CsPbI3 Perovskite Nanocrystals via Transition Metal Doping

Meng, Jie LU ; Lan, Zhenyun ; Lin, Weihua LU ; Castelli, Ivano E. ; Pullerits, Tönu LU and Zheng, Kaibo LU (2024) In Nano Letters 24(27). p.8386-8393
Abstract

Auger recombination is a pivotal process for semiconductor nanocrystals (NCs), significantly affecting charge carrier generation and collection in optoelectronic devices. This process depends mainly on the NCs’ electronic structures. In our study, we investigated Auger recombination dynamics in manganese (Mn2+)-doped CsPbI3 NCs using transient absorption (TA) spectroscopy combined with theoretical and experimental structural characterization. Our results show that Mn2+ doping accelerates Auger recombination, reducing the biexciton lifetime from 146 to 74 ps with increasing Mn doping concentration up to 10%. This accelerated Auger recombination in Mn-doped NCs is attributed to increased band edge wave... (More)

Auger recombination is a pivotal process for semiconductor nanocrystals (NCs), significantly affecting charge carrier generation and collection in optoelectronic devices. This process depends mainly on the NCs’ electronic structures. In our study, we investigated Auger recombination dynamics in manganese (Mn2+)-doped CsPbI3 NCs using transient absorption (TA) spectroscopy combined with theoretical and experimental structural characterization. Our results show that Mn2+ doping accelerates Auger recombination, reducing the biexciton lifetime from 146 to 74 ps with increasing Mn doping concentration up to 10%. This accelerated Auger recombination in Mn-doped NCs is attributed to increased band edge wave function overlap of excitons and a larger density of final states of Auger recombination due to Mn orbital involvement. Moreover, Mn doping reduces the dielectric screening of the excitons, which also contributes to the accelerated Auger recombination. Our study demonstrates the potential of element doping to regulate Auger recombination rates by modifying the materials’ electronic structure.

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author
; ; ; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
Auger recombination, dielectric screening, electronic structures, halide perovskite, Mn doping
in
Nano Letters
volume
24
issue
27
pages
8 pages
publisher
The American Chemical Society (ACS)
external identifiers
  • scopus:85197578161
  • pmid:38934731
ISSN
1530-6984
DOI
10.1021/acs.nanolett.4c02032
language
English
LU publication?
yes
id
120987b7-71f6-4b9f-9ab7-0c4fee09fad4
date added to LUP
2024-09-24 15:46:31
date last changed
2024-09-24 15:47:04
@article{120987b7-71f6-4b9f-9ab7-0c4fee09fad4,
  abstract     = {{<p>Auger recombination is a pivotal process for semiconductor nanocrystals (NCs), significantly affecting charge carrier generation and collection in optoelectronic devices. This process depends mainly on the NCs’ electronic structures. In our study, we investigated Auger recombination dynamics in manganese (Mn<sup>2+</sup>)-doped CsPbI<sub>3</sub> NCs using transient absorption (TA) spectroscopy combined with theoretical and experimental structural characterization. Our results show that Mn<sup>2+</sup> doping accelerates Auger recombination, reducing the biexciton lifetime from 146 to 74 ps with increasing Mn doping concentration up to 10%. This accelerated Auger recombination in Mn-doped NCs is attributed to increased band edge wave function overlap of excitons and a larger density of final states of Auger recombination due to Mn orbital involvement. Moreover, Mn doping reduces the dielectric screening of the excitons, which also contributes to the accelerated Auger recombination. Our study demonstrates the potential of element doping to regulate Auger recombination rates by modifying the materials’ electronic structure.</p>}},
  author       = {{Meng, Jie and Lan, Zhenyun and Lin, Weihua and Castelli, Ivano E. and Pullerits, Tönu and Zheng, Kaibo}},
  issn         = {{1530-6984}},
  keywords     = {{Auger recombination; dielectric screening; electronic structures; halide perovskite; Mn doping}},
  language     = {{eng}},
  number       = {{27}},
  pages        = {{8386--8393}},
  publisher    = {{The American Chemical Society (ACS)}},
  series       = {{Nano Letters}},
  title        = {{Tailoring Auger Recombination Dynamics in CsPbI<sub>3</sub> Perovskite Nanocrystals via Transition Metal Doping}},
  url          = {{http://dx.doi.org/10.1021/acs.nanolett.4c02032}},
  doi          = {{10.1021/acs.nanolett.4c02032}},
  volume       = {{24}},
  year         = {{2024}},
}