Manipulating crystallization dynamics through chelating molecules for bright perovskite emitters

Yatao Zou, Pengpeng Teng, Weidong Xu (), Guanhaojie Zheng, Weihua Lin, Jun Yin, Libor Kobera, Sabina Abbrent, Xiangchun Li, Julian A. Steele, Eduardo Solano, Maarten B. J. Roeffaers, Jun Li, Lei Cai, Chaoyang Kuang, Ivan G. Scheblykin, Jiri Brus, Kaibo Zheng, Ying Yang, Omar F. Mohammed, Osman M. Bakr, Tönu Pullerits, Sai Bai, Baoquan Sun () and Feng Gao ()
Additional contact information
Yatao Zou: Linköping University
Pengpeng Teng: Linköping University
Weidong Xu: Linköping University
Guanhaojie Zheng: Linköping University
Weihua Lin: Lund University
Jun Yin: King Abdullah University of Science and Technology
Libor Kobera: Institute of Macromolecular Chemistry of the Czech Academy of Sciences
Sabina Abbrent: Institute of Macromolecular Chemistry of the Czech Academy of Sciences
Xiangchun Li: Nanjing University of Posts & Telecommunications
Julian A. Steele: cMACS, Department of Microbial and Molecular Systems, KU Leuven
Eduardo Solano: NCD-SWEET beamline, ALBA Synchrotron Light Source
Maarten B. J. Roeffaers: cMACS, Department of Microbial and Molecular Systems, KU Leuven
Jun Li: Lund University
Lei Cai: Soochow University
Chaoyang Kuang: Linköping University
Ivan G. Scheblykin: Lund University
Jiri Brus: Institute of Macromolecular Chemistry of the Czech Academy of Sciences
Kaibo Zheng: Lund University
Ying Yang: Nanjing University of Aeronautics and Astronautics
Omar F. Mohammed: King Abdullah University of Science and Technology
Osman M. Bakr: King Abdullah University of Science and Technology
Tönu Pullerits: Lund University
Sai Bai: Linköping University
Baoquan Sun: Soochow University
Feng Gao: Linköping University

Nature Communications, 2021, vol. 12, issue 1, 1-10

Abstract: 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 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.

Date: 2021
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DOI: 10.1038/s41467-021-25092-7

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