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Microscopic insight into non-radiative decay in perovskite semiconductors from temperature-dependent luminescence blinking

Gerhard, Marina LU ; Louis, Boris LU ; Camacho, Rafael ; Merdasa, Aboma LU ; Li, Jun LU orcid ; Kiligaridis, Alexander LU ; Dobrovolsky, Alexander LU ; Hofkens, Johan and Scheblykin, Ivan G. LU orcid (2019) In Nature Communications 10(1).
Abstract

Organo-metal halide perovskites are promising solution-processed semiconductors, however, they possess diverse and largely not understood non-radiative mechanisms. Here, we resolve contributions of individual non-radiative recombination centers (quenchers) in nanocrystals of methylammonium lead iodide by studying their photoluminescence blinking caused by random switching of quenchers between active and passive states. We propose a model to describe the observed reduction of blinking upon cooling and determine energetic barriers of 0.2 to 0.8 eV for enabling the switching process, which points to ion migration as the underlying mechanism. Moreover, due to the strong influence of individual quenchers, the crystals show very... (More)

Organo-metal halide perovskites are promising solution-processed semiconductors, however, they possess diverse and largely not understood non-radiative mechanisms. Here, we resolve contributions of individual non-radiative recombination centers (quenchers) in nanocrystals of methylammonium lead iodide by studying their photoluminescence blinking caused by random switching of quenchers between active and passive states. We propose a model to describe the observed reduction of blinking upon cooling and determine energetic barriers of 0.2 to 0.8 eV for enabling the switching process, which points to ion migration as the underlying mechanism. Moreover, due to the strong influence of individual quenchers, the crystals show very individually-shaped photoluminescence enhancement upon cooling, suggesting that the high variety of activation energies of the PL enhancement reported in literature is not related to intrinsic properties but rather to the defect chemistry. Stabilizing the fluctuating quenchers in their passive states thus appears to be a promising strategy for improving the material quality.

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author
; ; ; ; ; ; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Nature Communications
volume
10
issue
1
article number
1698
publisher
Nature Publishing Group
external identifiers
  • pmid:30979903
  • scopus:85064345845
ISSN
2041-1723
DOI
10.1038/s41467-019-09640-w
language
English
LU publication?
yes
id
4fc96f5e-739d-4133-bff6-c6540d844f8d
date added to LUP
2019-05-02 14:09:22
date last changed
2023-11-18 19:36:33
@article{4fc96f5e-739d-4133-bff6-c6540d844f8d,
  abstract     = {{<p>Organo-metal halide perovskites are promising solution-processed semiconductors, however, they possess diverse and largely not understood non-radiative mechanisms. Here, we resolve contributions of individual non-radiative recombination centers (quenchers) in nanocrystals of methylammonium lead iodide by studying their photoluminescence blinking caused by random switching of quenchers between active and passive states. We propose a model to describe the observed reduction of blinking upon cooling and determine energetic barriers of 0.2 to 0.8 eV for enabling the switching process, which points to ion migration as the underlying mechanism. Moreover, due to the strong influence of individual quenchers, the crystals show very individually-shaped photoluminescence enhancement upon cooling, suggesting that the high variety of activation energies of the PL enhancement reported in literature is not related to intrinsic properties but rather to the defect chemistry. Stabilizing the fluctuating quenchers in their passive states thus appears to be a promising strategy for improving the material quality.</p>}},
  author       = {{Gerhard, Marina and Louis, Boris and Camacho, Rafael and Merdasa, Aboma and Li, Jun and Kiligaridis, Alexander and Dobrovolsky, Alexander and Hofkens, Johan and Scheblykin, Ivan G.}},
  issn         = {{2041-1723}},
  language     = {{eng}},
  month        = {{04}},
  number       = {{1}},
  publisher    = {{Nature Publishing Group}},
  series       = {{Nature Communications}},
  title        = {{Microscopic insight into non-radiative decay in perovskite semiconductors from temperature-dependent luminescence blinking}},
  url          = {{http://dx.doi.org/10.1038/s41467-019-09640-w}},
  doi          = {{10.1038/s41467-019-09640-w}},
  volume       = {{10}},
  year         = {{2019}},
}