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Manipulating crystallization dynamics through chelating molecules for bright perovskite emitters

Zou, Yatao ; Teng, Pengpeng ; Xu, Weidong ; Zheng, Guanhaojie ; Lin, Weihua LU ; Yin, Jun ; Kobera, Libor ; Abbrent, Sabina ; Li, Xiangchun and Steele, Julian A. , et al. (2021) In Nature Communications 12(1).
Abstract

Molecular additives are widely utilized to minimize non-radiative recombination in metal halide perovskite emitters due to their passivation effects from chemical bonds with ionic defects. However, a general and puzzling observation that can hardly be rationalized by passivation alone is that most of the molecular additives enabling high-efficiency perovskite light-emitting diodes (PeLEDs) are chelating (multidentate) molecules, while their respective monodentate counterparts receive limited attention. Here, we reveal the largely ignored yet critical role of the chelate effect on governing crystallization dynamics of perovskite emitters and mitigating trap-mediated non-radiative losses. Specifically, we discover that the chelate effect... (More)

Molecular additives are widely utilized to minimize non-radiative recombination in metal halide perovskite emitters due to their passivation effects from chemical bonds with ionic defects. However, a general and puzzling observation that can hardly be rationalized by passivation alone is that most of the molecular additives enabling high-efficiency perovskite light-emitting diodes (PeLEDs) are chelating (multidentate) molecules, while their respective monodentate counterparts receive limited attention. Here, we reveal the largely ignored yet critical role of the chelate effect on governing crystallization dynamics of perovskite emitters and mitigating trap-mediated non-radiative losses. Specifically, we discover that the chelate effect enhances lead-additive coordination affinity, enabling the formation of thermodynamically stable intermediate phases and inhibiting halide coordination-driven perovskite nucleation. The retarded perovskite nucleation and crystal growth are key to high crystal quality and thus efficient electroluminescence. Our work elucidates the full effects of molecular additives on PeLEDs by uncovering the chelate effect as an important feature within perovskite crystallization. As such, we open new prospects for the rationalized screening of highly effective molecular additives.

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publishing date
type
Contribution to journal
publication status
published
subject
in
Nature Communications
volume
12
issue
1
article number
4831
publisher
Nature Publishing Group
external identifiers
  • scopus:85112068240
  • pmid:34376647
ISSN
2041-1723
DOI
10.1038/s41467-021-25092-7
language
English
LU publication?
yes
id
8ea0d09d-d128-4527-a94c-99196c6ba3ed
date added to LUP
2021-09-03 14:15:32
date last changed
2024-06-16 18:13:58
@article{8ea0d09d-d128-4527-a94c-99196c6ba3ed,
  abstract     = {{<p>Molecular additives are widely utilized to minimize non-radiative recombination in metal halide perovskite emitters due to their passivation effects from chemical bonds with ionic defects. However, a general and puzzling observation that can hardly be rationalized by passivation alone is that most of the molecular additives enabling high-efficiency perovskite light-emitting diodes (PeLEDs) are chelating (multidentate) molecules, while their respective monodentate counterparts receive limited attention. Here, we reveal the largely ignored yet critical role of the chelate effect on governing crystallization dynamics of perovskite emitters and mitigating trap-mediated non-radiative losses. Specifically, we discover that the chelate effect enhances lead-additive coordination affinity, enabling the formation of thermodynamically stable intermediate phases and inhibiting halide coordination-driven perovskite nucleation. The retarded perovskite nucleation and crystal growth are key to high crystal quality and thus efficient electroluminescence. Our work elucidates the full effects of molecular additives on PeLEDs by uncovering the chelate effect as an important feature within perovskite crystallization. As such, we open new prospects for the rationalized screening of highly effective molecular additives.</p>}},
  author       = {{Zou, Yatao and Teng, Pengpeng and Xu, Weidong and Zheng, Guanhaojie and Lin, Weihua and Yin, Jun and Kobera, Libor and Abbrent, Sabina and Li, Xiangchun and Steele, Julian A. and Solano, Eduardo and Roeffaers, Maarten B.J. and Li, Jun and Cai, Lei and Kuang, Chaoyang and Scheblykin, Ivan G. and Brus, Jiri and Zheng, Kaibo and Yang, Ying and Mohammed, Omar F. and Bakr, Osman M. and Pullerits, Tönu and Bai, Sai and Sun, Baoquan and Gao, Feng}},
  issn         = {{2041-1723}},
  language     = {{eng}},
  number       = {{1}},
  publisher    = {{Nature Publishing Group}},
  series       = {{Nature Communications}},
  title        = {{Manipulating crystallization dynamics through chelating molecules for bright perovskite emitters}},
  url          = {{http://dx.doi.org/10.1038/s41467-021-25092-7}},
  doi          = {{10.1038/s41467-021-25092-7}},
  volume       = {{12}},
  year         = {{2021}},
}