Chlorine Vacancy Passivation in Mixed-Halide Perovskite Quantum Dots by Organic Pseudohalides Enables Efficient Rec. 2020 Blue Light-Emitting Diodes

Xiaopeng Zheng; Shuai Yuan; Jiakai Liu; Jun Yin; Fanglong Yuan; Wan-Shan Shen; Kexin Yao; Mingyang Wei; Chun Zhou; Kepeng Song; Bin-Bin Zhang; Yuanbao Lin; Mohamed N. Hedhili; Nimer Wehbe; Yu Han; Hong-Tao Sun; Zheng-Hong Lu; Thomas D. Anthopoulos; Omar F. Mohammed; Edward H. Sargent; Liang-Sheng Liao; Osman Bakr

doi:10.1021/acsenergylett.0c00057

Chlorine Vacancy Passivation in Mixed-Halide Perovskite Quantum Dots by Organic Pseudohalides Enables Efficient Rec. 2020 Blue Light-Emitting Diodes

Xiaopeng Zheng, Shuai Yuan, Jiakai Liu, Jun Yin, Fanglong Yuan, Wan-Shan Shen, Kexin Yao, Mingyang Wei, Chun Zhou, Kepeng Song, Bin-Bin Zhang, Yuanbao Lin, Mohamed N. Hedhili, Nimer Wehbe, Yu Han, Hong-Tao Sun, Zheng-Hong Lu, Thomas D. Anthopoulos, Omar F. Mohammed, Edward H. SargentLiang-Sheng Liao, Osman Bakr

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239 Scopus citations

Abstract

Blue-emitting perovskites can be easily attained by precisely tuning the halide ratio of mixed halide (Br/Cl) perovskites (MHPs). However, the adjustable halide ratio hinders the passivation of Cl vacancies, the main source of trap states leading to inferior performance of blue MHP lightemitting diodes (LEDs). Here, we report a strategy for passivating Cl vacancies in MHP quantum dots (QDs) using nonpolar solvent-soluble organic pseudohalide [n-dodecylammonium thiocyanate (DAT)], enabling blue MHP LEDs with greatly enhanced efficiency. Density functional theory calculations reveal that the thiocyanate (SCN−) groups fill in the Cl vacancies and remove electron traps within the bandgap. DAT-treated CsPb(BrxCl1−x)3 QDs exhibit near unity (∼100%) photoluminescence quantum yields, and their blue (∼470 nm) LEDs are spectrally stable with an external quantum efficiency of 6.3%, a record for perovskite LEDs emitting in the range of 460−480 nm relevant to Rec. 2020 display standards, and a halflifetime of ∼99 s.

Original language	English (US)
Pages (from-to)	793-798
Number of pages	6
Journal	ACS Energy Letters
DOIs	https://doi.org/10.1021/acsenergylett.0c00057
State	Published - Feb 11 2020

Bibliographical note

KAUST Repository Item: Exported on 2020-10-01
Acknowledgements: The authors acknowledge the funding support from KAUST, the National Natural Science Foundation of China (Grants 61575136 and 51773141), and the Collaborative Innovation Centre of Suzhou Nano Science and Technology (Nano-CIC) by the Priority Academic Program. E.H.S. and all co-authors from the Department of Electrical and Computer Engineering at the University of Toronto acknowledge the financial support from the Ontario Research Fund−Research Excellence Program and from the Natural Sciences and Engineering Research Council of Canada (NSERC).

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Zheng, X., Yuan, S., Liu, J., Yin, J., Yuan, F., Shen, W.-S., Yao, K., Wei, M., Zhou, C., Song, K., Zhang, B.-B., Lin, Y., Hedhili, M. N., Wehbe, N., Han, Y., Sun, H.-T., Lu, Z.-H., Anthopoulos, T. D., Mohammed, O. F., ... Bakr, O. (2020). Chlorine Vacancy Passivation in Mixed-Halide Perovskite Quantum Dots by Organic Pseudohalides Enables Efficient Rec. 2020 Blue Light-Emitting Diodes. ACS Energy Letters, 793-798. https://doi.org/10.1021/acsenergylett.0c00057

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title = "Chlorine Vacancy Passivation in Mixed-Halide Perovskite Quantum Dots by Organic Pseudohalides Enables Efficient Rec. 2020 Blue Light-Emitting Diodes",

abstract = "Blue-emitting perovskites can be easily attained by precisely tuning the halide ratio of mixed halide (Br/Cl) perovskites (MHPs). However, the adjustable halide ratio hinders the passivation of Cl vacancies, the main source of trap states leading to inferior performance of blue MHP lightemitting diodes (LEDs). Here, we report a strategy for passivating Cl vacancies in MHP quantum dots (QDs) using nonpolar solvent-soluble organic pseudohalide [n-dodecylammonium thiocyanate (DAT)], enabling blue MHP LEDs with greatly enhanced efficiency. Density functional theory calculations reveal that the thiocyanate (SCN−) groups fill in the Cl vacancies and remove electron traps within the bandgap. DAT-treated CsPb(BrxCl1−x)3 QDs exhibit near unity (∼100%) photoluminescence quantum yields, and their blue (∼470 nm) LEDs are spectrally stable with an external quantum efficiency of 6.3%, a record for perovskite LEDs emitting in the range of 460−480 nm relevant to Rec. 2020 display standards, and a halflifetime of ∼99 s.",

author = "Xiaopeng Zheng and Shuai Yuan and Jiakai Liu and Jun Yin and Fanglong Yuan and Wan-Shan Shen and Kexin Yao and Mingyang Wei and Chun Zhou and Kepeng Song and Bin-Bin Zhang and Yuanbao Lin and Hedhili, {Mohamed N.} and Nimer Wehbe and Yu Han and Hong-Tao Sun and Zheng-Hong Lu and Anthopoulos, {Thomas D.} and Mohammed, {Omar F.} and Sargent, {Edward H.} and Liang-Sheng Liao and Osman Bakr",

note = "KAUST Repository Item: Exported on 2020-10-01 Acknowledgements: The authors acknowledge the funding support from KAUST, the National Natural Science Foundation of China (Grants 61575136 and 51773141), and the Collaborative Innovation Centre of Suzhou Nano Science and Technology (Nano-CIC) by the Priority Academic Program. E.H.S. and all co-authors from the Department of Electrical and Computer Engineering at the University of Toronto acknowledge the financial support from the Ontario Research Fund−Research Excellence Program and from the Natural Sciences and Engineering Research Council of Canada (NSERC).",

year = "2020",

month = feb,

day = "11",

doi = "10.1021/acsenergylett.0c00057",

language = "English (US)",

pages = "793--798",

journal = "ACS Energy Letters",

issn = "2380-8195",

publisher = "American Chemical Society",

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Zheng, X, Yuan, S, Liu, J, Yin, J, Yuan, F, Shen, W-S, Yao, K, Wei, M, Zhou, C, Song, K, Zhang, B-B, Lin, Y, Hedhili, MN , Wehbe, N, Han, Y, Sun, H-T, Lu, Z-H, Anthopoulos, TD, Mohammed, OF, Sargent, EH, Liao, L-S & Bakr, O 2020, 'Chlorine Vacancy Passivation in Mixed-Halide Perovskite Quantum Dots by Organic Pseudohalides Enables Efficient Rec. 2020 Blue Light-Emitting Diodes', ACS Energy Letters, pp. 793-798. https://doi.org/10.1021/acsenergylett.0c00057

TY - JOUR

T1 - Chlorine Vacancy Passivation in Mixed-Halide Perovskite Quantum Dots by Organic Pseudohalides Enables Efficient Rec. 2020 Blue Light-Emitting Diodes

AU - Zheng, Xiaopeng

AU - Yuan, Shuai

AU - Liu, Jiakai

AU - Yin, Jun

AU - Yuan, Fanglong

AU - Shen, Wan-Shan

AU - Yao, Kexin

AU - Wei, Mingyang

AU - Zhou, Chun

AU - Song, Kepeng

AU - Zhang, Bin-Bin

AU - Lin, Yuanbao

AU - Hedhili, Mohamed N.

AU - Wehbe, Nimer

AU - Han, Yu

AU - Sun, Hong-Tao

AU - Lu, Zheng-Hong

AU - Anthopoulos, Thomas D.

AU - Mohammed, Omar F.

AU - Sargent, Edward H.

AU - Liao, Liang-Sheng

AU - Bakr, Osman

N1 - KAUST Repository Item: Exported on 2020-10-01 Acknowledgements: The authors acknowledge the funding support from KAUST, the National Natural Science Foundation of China (Grants 61575136 and 51773141), and the Collaborative Innovation Centre of Suzhou Nano Science and Technology (Nano-CIC) by the Priority Academic Program. E.H.S. and all co-authors from the Department of Electrical and Computer Engineering at the University of Toronto acknowledge the financial support from the Ontario Research Fund−Research Excellence Program and from the Natural Sciences and Engineering Research Council of Canada (NSERC).

PY - 2020/2/11

Y1 - 2020/2/11

N2 - Blue-emitting perovskites can be easily attained by precisely tuning the halide ratio of mixed halide (Br/Cl) perovskites (MHPs). However, the adjustable halide ratio hinders the passivation of Cl vacancies, the main source of trap states leading to inferior performance of blue MHP lightemitting diodes (LEDs). Here, we report a strategy for passivating Cl vacancies in MHP quantum dots (QDs) using nonpolar solvent-soluble organic pseudohalide [n-dodecylammonium thiocyanate (DAT)], enabling blue MHP LEDs with greatly enhanced efficiency. Density functional theory calculations reveal that the thiocyanate (SCN−) groups fill in the Cl vacancies and remove electron traps within the bandgap. DAT-treated CsPb(BrxCl1−x)3 QDs exhibit near unity (∼100%) photoluminescence quantum yields, and their blue (∼470 nm) LEDs are spectrally stable with an external quantum efficiency of 6.3%, a record for perovskite LEDs emitting in the range of 460−480 nm relevant to Rec. 2020 display standards, and a halflifetime of ∼99 s.

AB - Blue-emitting perovskites can be easily attained by precisely tuning the halide ratio of mixed halide (Br/Cl) perovskites (MHPs). However, the adjustable halide ratio hinders the passivation of Cl vacancies, the main source of trap states leading to inferior performance of blue MHP lightemitting diodes (LEDs). Here, we report a strategy for passivating Cl vacancies in MHP quantum dots (QDs) using nonpolar solvent-soluble organic pseudohalide [n-dodecylammonium thiocyanate (DAT)], enabling blue MHP LEDs with greatly enhanced efficiency. Density functional theory calculations reveal that the thiocyanate (SCN−) groups fill in the Cl vacancies and remove electron traps within the bandgap. DAT-treated CsPb(BrxCl1−x)3 QDs exhibit near unity (∼100%) photoluminescence quantum yields, and their blue (∼470 nm) LEDs are spectrally stable with an external quantum efficiency of 6.3%, a record for perovskite LEDs emitting in the range of 460−480 nm relevant to Rec. 2020 display standards, and a halflifetime of ∼99 s.

UR - http://hdl.handle.net/10754/661562

UR - https://pubs.acs.org/doi/10.1021/acsenergylett.0c00057

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U2 - 10.1021/acsenergylett.0c00057

DO - 10.1021/acsenergylett.0c00057

M3 - Article

SN - 2380-8195

SP - 793

EP - 798

JO - ACS Energy Letters

JF - ACS Energy Letters

ER -

Chlorine Vacancy Passivation in Mixed-Halide Perovskite Quantum Dots by Organic Pseudohalides Enables Efficient Rec. 2020 Blue Light-Emitting Diodes

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