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 Bakr; Tönu Pullerits; Sai Bai; Baoquan Sun; Feng Gao

doi:10.1038/s41467-021-25092-7

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. MohammedOsman Bakr, Tönu Pullerits, Sai Bai, Baoquan Sun, Feng Gao

Research output: Contribution to journal › Article › peer-review

74 Scopus citations

Abstract

AbstractMolecular 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.

Original language	English (US)
Journal	Nature Communications
Volume	12
Issue number	1
DOIs	https://doi.org/10.1038/s41467-021-25092-7
State	Published - Aug 10 2021

Bibliographical note

KAUST Repository Item: Exported on 2021-08-12
Acknowledgements: The authors thank Prof. Annamaria Petrozza, Dr. Tiankai Zhang for valuable discussions, and Kaichuan Wen and Prof. Jianpu Wang for help with the PLQE measurements. We acknowledge the support from the ERC Starting Grant (No. 717026), the Swedish Energy Agency Energimyndigheten (Nos. 48758-1 and 44651-1), Swedish Research Council VR, NanoLund, and the Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linköping University (Faculty Grant SFO-Mat-LiU No. 2009-00971). The authors would like to thank the NCD-SWEET beamline at ALBA Synchrotron from Spain for providing the beamtime. J.Y, O.F.M., and O.M.B. acknowledge the Supercomputing Laboratory at KAUST for their computational and storage resources. Y.Z., L.C., and B.S. thanks the National Natural Science Foundation of China (91833303, 61974098, 62005126), the National Key Research and Development Program (2016YFA0201900), Jiangsu High Educational Natural Science Foundation (18KJA430012), the 111 Program and Collaborative Innovation Center of Suzhou Nano Science and Technology, and Collaborative Innovation Center of Suzhou Nano Science & Technology. J.A.S. acknowledges financial support from the Research Foundation - Flanders (FWO: grant No.’s 12Y7218N and 12Y7221N). M.B.J.R. acknowledges financial support from the Research Foundation - Flanders (FWO, G098319N) and the KU Leuven Research Fund (C14/19/079). Y.Z. (No. 201806920071), P.T. (No. 201906830040, J.L. (No. 201608530162), W.L. (No. 201806460021) also thank the financial support from China Scholarship Council. F.G. is a Wallenberg Academy Fellow

ASJC Scopus subject areas

General Biochemistry, Genetics and Molecular Biology
General Chemistry
General Physics and Astronomy

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10.1038/s41467-021-25092-7

https://repository.kaust.edu.sa/bitstream/10754/670557/1/s41467-021-25092-7.pdf

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Zou, Y., Teng, P., Xu, W., Zheng, G., Lin, W., Yin, J., Kobera, L., Abbrent, S., Li, X., Steele, J. A., Solano, E., Roeffaers, M. B. J., Li, J., Cai, L., Kuang, C., Scheblykin, I. G., Brus, J., Zheng, K., Yang, Y., ... Gao, F. (2021). Manipulating crystallization dynamics through chelating molecules for bright perovskite emitters. Nature Communications, 12(1). https://doi.org/10.1038/s41467-021-25092-7

@article{cf6c6c6c6013472982b4f1c84f960bd0,

title = "Manipulating crystallization dynamics through chelating molecules for bright perovskite emitters",

abstract = "AbstractMolecular 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.",

author = "Yatao Zou and Pengpeng Teng and Weidong Xu and Guanhaojie Zheng and Weihua Lin and Jun Yin and Libor Kobera and Sabina Abbrent and Xiangchun Li and Steele, {Julian A.} and Eduardo Solano and Roeffaers, {Maarten B. J.} and Jun Li and Lei Cai and Chaoyang Kuang and Scheblykin, {Ivan G.} and Jiri Brus and Kaibo Zheng and Ying Yang and Mohammed, {Omar F.} and Osman Bakr and T{\"o}nu Pullerits and Sai Bai and Baoquan Sun and Feng Gao",

note = "KAUST Repository Item: Exported on 2021-08-12 Acknowledgements: The authors thank Prof. Annamaria Petrozza, Dr. Tiankai Zhang for valuable discussions, and Kaichuan Wen and Prof. Jianpu Wang for help with the PLQE measurements. We acknowledge the support from the ERC Starting Grant (No. 717026), the Swedish Energy Agency Energimyndigheten (Nos. 48758-1 and 44651-1), Swedish Research Council VR, NanoLund, and the Swedish Government Strategic Research Area in Materials Science on Functional Materials at Link{\"o}ping University (Faculty Grant SFO-Mat-LiU No. 2009-00971). The authors would like to thank the NCD-SWEET beamline at ALBA Synchrotron from Spain for providing the beamtime. J.Y, O.F.M., and O.M.B. acknowledge the Supercomputing Laboratory at KAUST for their computational and storage resources. Y.Z., L.C., and B.S. thanks the National Natural Science Foundation of China (91833303, 61974098, 62005126), the National Key Research and Development Program (2016YFA0201900), Jiangsu High Educational Natural Science Foundation (18KJA430012), the 111 Program and Collaborative Innovation Center of Suzhou Nano Science and Technology, and Collaborative Innovation Center of Suzhou Nano Science & Technology. J.A.S. acknowledges financial support from the Research Foundation - Flanders (FWO: grant No.{\textquoteright}s 12Y7218N and 12Y7221N). M.B.J.R. acknowledges financial support from the Research Foundation - Flanders (FWO, G098319N) and the KU Leuven Research Fund (C14/19/079). Y.Z. (No. 201806920071), P.T. (No. 201906830040, J.L. (No. 201608530162), W.L. (No. 201806460021) also thank the financial support from China Scholarship Council. F.G. is a Wallenberg Academy Fellow",

year = "2021",

month = aug,

day = "10",

doi = "10.1038/s41467-021-25092-7",

language = "English (US)",

volume = "12",

journal = "Nature Communications",

issn = "2041-1723",

publisher = "Nature Research",

number = "1",

}

Zou, Y, Teng, P, Xu, W, Zheng, G, Lin, W, Yin, J, Kobera, L, Abbrent, S, Li, X, Steele, JA, Solano, E, Roeffaers, MBJ, Li, J, Cai, L, Kuang, C, Scheblykin, IG, Brus, J, Zheng, K, Yang, Y, Mohammed, OF , Bakr, O, Pullerits, T, Bai, S, Sun, B & Gao, F 2021, 'Manipulating crystallization dynamics through chelating molecules for bright perovskite emitters', Nature Communications, vol. 12, no. 1. https://doi.org/10.1038/s41467-021-25092-7

TY - JOUR

T1 - Manipulating crystallization dynamics through chelating molecules for bright perovskite emitters

AU - Zou, Yatao

AU - Teng, Pengpeng

AU - Xu, Weidong

AU - Zheng, Guanhaojie

AU - Lin, Weihua

AU - Yin, Jun

AU - Kobera, Libor

AU - Abbrent, Sabina

AU - Li, Xiangchun

AU - Steele, Julian A.

AU - Solano, Eduardo

AU - Roeffaers, Maarten B. J.

AU - Li, Jun

AU - Cai, Lei

AU - Kuang, Chaoyang

AU - Scheblykin, Ivan G.

AU - Brus, Jiri

AU - Zheng, Kaibo

AU - Yang, Ying

AU - Mohammed, Omar F.

AU - Bakr, Osman

AU - Pullerits, Tönu

AU - Bai, Sai

AU - Sun, Baoquan

AU - Gao, Feng

N1 - KAUST Repository Item: Exported on 2021-08-12 Acknowledgements: The authors thank Prof. Annamaria Petrozza, Dr. Tiankai Zhang for valuable discussions, and Kaichuan Wen and Prof. Jianpu Wang for help with the PLQE measurements. We acknowledge the support from the ERC Starting Grant (No. 717026), the Swedish Energy Agency Energimyndigheten (Nos. 48758-1 and 44651-1), Swedish Research Council VR, NanoLund, and the Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linköping University (Faculty Grant SFO-Mat-LiU No. 2009-00971). The authors would like to thank the NCD-SWEET beamline at ALBA Synchrotron from Spain for providing the beamtime. J.Y, O.F.M., and O.M.B. acknowledge the Supercomputing Laboratory at KAUST for their computational and storage resources. Y.Z., L.C., and B.S. thanks the National Natural Science Foundation of China (91833303, 61974098, 62005126), the National Key Research and Development Program (2016YFA0201900), Jiangsu High Educational Natural Science Foundation (18KJA430012), the 111 Program and Collaborative Innovation Center of Suzhou Nano Science and Technology, and Collaborative Innovation Center of Suzhou Nano Science & Technology. J.A.S. acknowledges financial support from the Research Foundation - Flanders (FWO: grant No.’s 12Y7218N and 12Y7221N). M.B.J.R. acknowledges financial support from the Research Foundation - Flanders (FWO, G098319N) and the KU Leuven Research Fund (C14/19/079). Y.Z. (No. 201806920071), P.T. (No. 201906830040, J.L. (No. 201608530162), W.L. (No. 201806460021) also thank the financial support from China Scholarship Council. F.G. is a Wallenberg Academy Fellow

PY - 2021/8/10

Y1 - 2021/8/10

N2 - AbstractMolecular 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.

AB - AbstractMolecular 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.

UR - http://hdl.handle.net/10754/670557

UR - https://www.nature.com/articles/s41467-021-25092-7

U2 - 10.1038/s41467-021-25092-7

DO - 10.1038/s41467-021-25092-7

M3 - Article

C2 - 34376647

SN - 2041-1723

VL - 12

JO - Nature Communications

JF - Nature Communications

IS - 1

ER -

Manipulating crystallization dynamics through chelating molecules for bright perovskite emitters

Abstract

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