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Title: Efficient and stable emission of warm-white light from lead-free halide double perovskites

Abstract

Lighting accounts for one-fifth of global electricity consumption. Single materials with efficient and stable white-light emission are ideal for lighting applications, but photon emission covering the entire visible spectrum is difficult to achieve using a single material. Metal halide perovskites have outstanding emission properties; however, the best-performing materials of this type contain lead and have unsatisfactory stability. Here we report a lead-free double perovskite that exhibits efficient and stable white-light emission via self-trapped excitons that originate from the Jahn–Teller distortion of the AgCl6 octahedron in the excited state. By alloying sodium cations into Cs2AgInCl6, we break the dark transition (the inversion-symmetry-induced parity-forbidden transition) by manipulating the parity of the wavefunction of the self-trapped exciton and reduce the electronic dimensionality of the semiconductor. This leads to an increase in photoluminescence efficiency by three orders of magnitude compared to pure Cs2AgInCl6. The optimally alloyed Cs2(Ag0.60Na0.40)InCl6 with 0.04 per cent bismuth doping emits warm-white light with 86 ± 5 per cent quantum efficiency and works for over 1,000 hours. We anticipate that these results will stimulate research on single-emitter-based white-light-emitting phosphors and diodes for next-generation lighting and display technologies.

Authors:
 [1];  [2];  [1];  [1];  [3];  [1];  [1];  [4];  [5];  [6];  [7];  [1];  [6];  [1];  [6];  [7];  [1];  [4];  [3];  [8] more »;  [2];  [9];  [1] « less
+ Show Author Affiliations
  1. Huazhong Univ. of Science and Technology (HUST), Wuhan (China)
  2. Univ. of Toledo, OH (United States)
  3. Monash Univ., Melbourne, VIC (Australia)
  4. Jilin Univ., Changchun (China). State Key Lab. of Superhard Materials
  5. Huazhong Univ. of Science and Technology (HUST), Wuhan (China); Univ. of Toronto, ON (Canada)
  6. Tsinghua Univ., Beijing (China)
  7. Chinese Academy of Sciences, Dalian (China)
  8. Wuhan Univ. (China)
  9. Univ. of Toronto, ON (Canada)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Hybrid Organic-Inorganic Semiconductors for Energy (CHOISE); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Univ. of California, Oakland, CA (United States); Duke Univ., Durham, NC (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1543773
Grant/Contract Number:  
AC02-05CH11231; EE0006712
Resource Type:
Accepted Manuscript
Journal Name:
Nature (London)
Additional Journal Information:
Journal Name: Nature (London); Journal Volume: 563; Journal Issue: 7732; Journal ID: ISSN 0028-0836
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Science & Technology - Other Topics

Citation Formats

Luo, Jiajun, Wang, Xiaoming, Li, Shunran, Liu, Jing, Guo, Yueming, Niu, Guangda, Yao, Li, Fu, Yuhao, Gao, Liang, Dong, Qingshun, Zhao, Chunyi, Leng, Meiying, Ma, Fusheng, Liang, Wenxi, Wang, Liduo, Jin, Shengye, Han, Junbo, Zhang, Lijun, Etheridge, Joanne, Wang, Jianbo, Yan, Yanfa, Sargent, Edward H., and Tang, Jiang. Efficient and stable emission of warm-white light from lead-free halide double perovskites. United States: N. p., 2018. Web. doi:10.1038/s41586-018-0691-0.
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Luo, Jiajun, Wang, Xiaoming, Li, Shunran, Liu, Jing, Guo, Yueming, Niu, Guangda, Yao, Li, Fu, Yuhao, Gao, Liang, Dong, Qingshun, Zhao, Chunyi, Leng, Meiying, Ma, Fusheng, Liang, Wenxi, Wang, Liduo, Jin, Shengye, Han, Junbo, Zhang, Lijun, Etheridge, Joanne, Wang, Jianbo, Yan, Yanfa, Sargent, Edward H., & Tang, Jiang. Efficient and stable emission of warm-white light from lead-free halide double perovskites. United States. https://doi.org/10.1038/s41586-018-0691-0
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Luo, Jiajun, Wang, Xiaoming, Li, Shunran, Liu, Jing, Guo, Yueming, Niu, Guangda, Yao, Li, Fu, Yuhao, Gao, Liang, Dong, Qingshun, Zhao, Chunyi, Leng, Meiying, Ma, Fusheng, Liang, Wenxi, Wang, Liduo, Jin, Shengye, Han, Junbo, Zhang, Lijun, Etheridge, Joanne, Wang, Jianbo, Yan, Yanfa, Sargent, Edward H., and Tang, Jiang. Wed . "Efficient and stable emission of warm-white light from lead-free halide double perovskites". United States. https://doi.org/10.1038/s41586-018-0691-0. https://www.osti.gov/servlets/purl/1543773.
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@article{osti_1543773,
title = {Efficient and stable emission of warm-white light from lead-free halide double perovskites},
author = {Luo, Jiajun and Wang, Xiaoming and Li, Shunran and Liu, Jing and Guo, Yueming and Niu, Guangda and Yao, Li and Fu, Yuhao and Gao, Liang and Dong, Qingshun and Zhao, Chunyi and Leng, Meiying and Ma, Fusheng and Liang, Wenxi and Wang, Liduo and Jin, Shengye and Han, Junbo and Zhang, Lijun and Etheridge, Joanne and Wang, Jianbo and Yan, Yanfa and Sargent, Edward H. and Tang, Jiang},
abstractNote = {Lighting accounts for one-fifth of global electricity consumption. Single materials with efficient and stable white-light emission are ideal for lighting applications, but photon emission covering the entire visible spectrum is difficult to achieve using a single material. Metal halide perovskites have outstanding emission properties; however, the best-performing materials of this type contain lead and have unsatisfactory stability. Here we report a lead-free double perovskite that exhibits efficient and stable white-light emission via self-trapped excitons that originate from the Jahn–Teller distortion of the AgCl6 octahedron in the excited state. By alloying sodium cations into Cs2AgInCl6, we break the dark transition (the inversion-symmetry-induced parity-forbidden transition) by manipulating the parity of the wavefunction of the self-trapped exciton and reduce the electronic dimensionality of the semiconductor. This leads to an increase in photoluminescence efficiency by three orders of magnitude compared to pure Cs2AgInCl6. The optimally alloyed Cs2(Ag0.60Na0.40)InCl6 with 0.04 per cent bismuth doping emits warm-white light with 86 ± 5 per cent quantum efficiency and works for over 1,000 hours. We anticipate that these results will stimulate research on single-emitter-based white-light-emitting phosphors and diodes for next-generation lighting and display technologies.},
doi = {10.1038/s41586-018-0691-0},
journal = {Nature (London)},
number = 7732,
volume = 563,
place = {United States},
year = {Wed Nov 07 00:00:00 EST 2018},
month = {Wed Nov 07 00:00:00 EST 2018}
}
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    Recent advances and perspectives on light emitting diodes fabricated from halide metal perovskite nanocrystals
    journal, January 2019

    • Cao, Muhan; Xu, Yong; Li, Pengli
    • Journal of Materials Chemistry C, Vol. 7, Issue 46
    • DOI: 10.1039/c9tc03978c

    Realizing an impressive red-emitting Ca 9 MnNa(PO 4 ) 7 phosphor through a dual function based on disturbing structural confinement and energy transfer
    journal, January 2020

    • Wang, Jindi; Shang, Mengmeng; Cui, Min
    • Journal of Materials Chemistry C, Vol. 8, Issue 1
    • DOI: 10.1039/c9tc05768d

    Thermal stability of CsPbBr 3 perovskite as revealed by in situ transmission electron microscopy
    journal, July 2019

    • Zhang, Chao; Fernando, Joseph F. S.; Firestein, Konstantin L.
    • APL Materials, Vol. 7, Issue 7
    • DOI: 10.1063/1.5108849

    Trion dynamics in lead halide perovskite nanocrystals
    journal, November 2019

    • Kanemitsu, Yoshihiko
    • The Journal of Chemical Physics, Vol. 151, Issue 17
    • DOI: 10.1063/1.5125628

    One-step solution synthesis of white-light-emitting films via dimensionality control of the Cs–Cu–I system
    journal, November 2019

    • Jun, Taehwan; Handa, Taketo; Sim, Kihyung
    • APL Materials, Vol. 7, Issue 11
    • DOI: 10.1063/1.5127300

    Synthesis and optical properties of colloidal Cs 2 AgSb 1−x Bi x Cl 6 double perovskite nanocrystals
    journal, October 2019

    • Kshirsagar, Anuraj S.; Nag, Angshuman
    • The Journal of Chemical Physics, Vol. 151, Issue 16
    • DOI: 10.1063/1.5127971

    Azetidinium as cation in lead mixed halide perovskite nanocrystals of optoelectronic quality
    journal, February 2020

    • Kesava, Sameer Vajjala; Hassan, Yasser; Privitera, Alberto
    • AIP Advances, Vol. 10, Issue 2
    • DOI: 10.1063/1.5133042

    Broadband emission of double perovskite Cs 2 Na 04 Ag 06 In 0995 Bi 0005 Cl 6 :Mn 2+ for single-phosphor white-light-emitting diodes
    journal, January 2019

    Lead-Free Perovskites for Lighting and Lasing Applications: A Minireview
    journal, November 2019

    • Ushakova, Elena V.; Cherevkov, Sergei A.; Kuznetsova, Vera A.
    • Materials, Vol. 12, Issue 23
    • DOI: 10.3390/ma12233845

    In Situ Regulating the Order–Disorder Phase Transition in Cs 2 AgBiBr 6 Single Crystal toward the Application in an X‐Ray Detector
    journal, March 2019

    • Yuan, Weinan; Niu, Guangda; Xian, Yeming
    • Advanced Functional Materials, Vol. 29, Issue 20
    • DOI: 10.1002/adfm.201900234

    Lead Halide Post‐Perovskite‐Type Chains for High‐Efficiency White‐Light Emission
    journal, February 2019

    • Gautier, Romain; Massuyeau, Florian; Galnon, Gabin
    • Advanced Materials, Vol. 31, Issue 14
    • DOI: 10.1002/adma.201807383

    Negative Thermal Quenching of Efficient White‐Light Emission in a 1D Ladder‐Like Organic/Inorganic Hybrid Material
    journal, July 2019

    • Barkaoui, Hamdi; Abid, Haitham; Zelewski, Szymon
    • Advanced Optical Materials, Vol. 7, Issue 20
    • DOI: 10.1002/adom.201900763

    Semiconductor Quantum Dots‐Embedded Inorganic Glasses: Fabrication, Luminescent Properties, and Potential Applications
    journal, August 2019

    • Xia, Mengling; Luo, Jiajun; Chen, Chao
    • Advanced Optical Materials, Vol. 7, Issue 21
    • DOI: 10.1002/adom.201900851

    A Highly Red-Emissive Lead-Free Indium-Based Perovskite Single Crystal for Sensitive Water Detection
    journal, March 2019

    • Zhou, Lei; Liao, Jin-Feng; Huang, Zeng-Guang
    • Angewandte Chemie International Edition, Vol. 58, Issue 16
    • DOI: 10.1002/anie.201814564

    Intrinsic Self‐Trapped Emission in 0D Lead‐Free (C 4 H 14 N 2 ) 2 In 2 Br 10 Single Crystal
    journal, October 2019

    • Zhou, Lei; Liao, Jin‐Feng; Huang, Zeng‐Guang
    • Angewandte Chemie International Edition, Vol. 58, Issue 43
    • DOI: 10.1002/anie.201907503

    Colloidal Synthesis and Optical Properties of All‐Inorganic Low‐Dimensional Cesium Copper Halide Nanocrystals
    journal, November 2019

    • Cheng, Pengfei; Sun, Lei; Feng, Lu
    • Angewandte Chemie International Edition, Vol. 58, Issue 45
    • DOI: 10.1002/anie.201909129

    Dimensional Reduction of Cs 2 AgBiBr 6 : A 2D Hybrid Double Perovskite with Strong Polarization Sensitivity
    journal, January 2020

    • Li, Yaobin; Yang, Tao; Xu, Zhiyun
    • Angewandte Chemie International Edition, Vol. 59, Issue 9
    • DOI: 10.1002/anie.201911551

    Recent Developments in Lead‐Free Double Perovskites: Structure, Doping, and Applications
    journal, December 2019

    • Dave, Kashyap; Fang, Mu Huai; Bao, Zhen
    • Chemistry – An Asian Journal, Vol. 15, Issue 2
    • DOI: 10.1002/asia.201901510

    Ag/In lead‐free double perovskites
    journal, February 2020

    • Liu, Fang; Marongiu, Daniela; Pau, Riccardo
    • EcoMat, Vol. 2, Issue 1
    • DOI: 10.1002/eom2.12017

    Synthesis and transformation of zero-dimensional Cs3BiX6 (X = Cl, Br) perovskite-analogue nanocrystals
    journal, December 2019

    Efficient sky-blue perovskite light-emitting diodes via photoluminescence enhancement
    journal, December 2019

    Prediction of room-temperature half-metallicity in layered halide double perovskites
    journal, November 2019

    Reversible 3D laser printing of perovskite quantum dots inside a transparent medium
    journal, November 2019

    Broadband white-light emission from supramolecular piperazinium-based lead halide perovskites linked by hydrogen bonds
    journal, January 2019

    • Jung, Mi-Hee; Ko, Kyoung Chul; Lee, Woo Ram
    • Dalton Transactions, Vol. 48, Issue 40
    • DOI: 10.1039/c9dt03469b

    (C 6 H 5 NH 3 )BiI 4 : a lead-free perovskite with >330 days humidity stability for optoelectronic applications
    journal, January 2019

    • Li, Xiao-Lei; Gao, Li-Li; Ding, Bin
    • Journal of Materials Chemistry A, Vol. 7, Issue 26
    • DOI: 10.1039/c9ta02421b

    Optically pumped white light-emitting diodes based on metal halide perovskites and perovskite-related materials
    journal, January 2020

    • Worku, Michael; Xu, Liang-Jin; Chaaban, Maya
    • APL Materials, Vol. 8, Issue 1
    • DOI: 10.1063/1.5140441

    Silica encapsulation of metal perovskite nanocrystals in a photoluminescence type display application
    journal, July 2019

    Tunable green lasing from circular grating distributed feedback based on CH 3 NH 3 PbBr 3 perovskite
    journal, January 2019

    • Jäckle, Matthäus; Linnenbank, Heiko; Hentschel, Mario
    • Optical Materials Express, Vol. 9, Issue 5
    • DOI: 10.1364/ome.9.002006

    Acetic Acid Assisted Crystallization Strategy for High Efficiency and Long‐Term Stable Perovskite Solar Cell
    journal, January 2020

    A Highly Red‐Emissive Lead‐Free Indium‐Based Perovskite Single Crystal for Sensitive Water Detection
    journal, February 2019

    • Zhou, Lei; Liao, Jin‐Feng; Huang, Zeng‐Guang
    • Angewandte Chemie, Vol. 131, Issue 16
    • DOI: 10.1002/ange.201814564

    Colloidal Synthesis and Optical Properties of All‐Inorganic Low‐Dimensional Cesium Copper Halide Nanocrystals
    journal, September 2019

    0D Cs 3 Cu 2 X 5 (X = I, Br, and Cl) Nanocrystals: Colloidal Syntheses and Optical Properties
    journal, December 2019

    Intrinsic White‐Light‐Emitting Metal–Organic Frameworks with Structurally Deformable Secondary Building Units
    journal, April 2019

    • Peng, Chengdong; Song, Xueling; Yin, Jinlin
    • Angewandte Chemie, Vol. 131, Issue 23
    • DOI: 10.1002/ange.201903665

    Water‐Assisted Synthesis of Blue Chip Excitable 2D Halide Perovskite with Green‐Red Dual Emissions for White LEDs
    journal, May 2019

    Lead‐Free Double Perovskites for Perovskite Solar Cells
    journal, August 2019

    Multi-quantum-well quantum dots with stable dual emission
    journal, January 2019

    • Xing, Weishuo; Zhang, Xinsu; Geng, Chong
    • Nanoscale, Vol. 11, Issue 17
    • DOI: 10.1039/c9nr00177h

    White light emission in low-dimensional perovskites
    journal, January 2019

    • Cortecchia, Daniele; Yin, Jun; Petrozza, Annamaria
    • Journal of Materials Chemistry C, Vol. 7, Issue 17
    • DOI: 10.1039/c9tc01036j

    Perovskite LEDs
    journal, January 2018

    • Friend, Richard H.; Di, Dawei; Lilliu, Samuele
    • Scientific Video Protocols, Vol. 1, Issue 1
    • DOI: 10.32386/scivpro.000008

    Dimensional Reduction of Cs 2 AgBiBr 6 : A 2D Hybrid Double Perovskite with Strong Polarization Sensitivity
    journal, January 2020

    WC 1−x ‐Coupled 3D Porous Defective g‐C 3 N 4 for Efficient Photocatalytic Overall Water Splitting
    journal, February 2019

    Efficient Red/Near‐Infrared‐Emissive Carbon Nanodots with Multiphoton Excited Upconversion Fluorescence
    journal, July 2019

    • Liu, Kai‐Kai; Song, Shi‐Yu; Sui, Lai‐Zhi
    • Advanced Science, Vol. 6, Issue 17
    • DOI: 10.1002/advs.201900766

    Ultrafast self-trapping of photoexcited carriers sets the upper limit on antimony trisulfide photovoltaic devices
    journal, October 2019

    Efficient sky-blue perovskite light-emitting diodes via photoluminescence enhancement
    journal, December 2019

    Lead-Free Perovskites for Lighting and Lasing Applications: A Minireview
    journal, November 2019

    • Ushakova, Elena V.; Cherevkov, Sergei A.; Kuznetsova, Vera A.
    • Materials, Vol. 12, Issue 23
    • DOI: 10.3390/ma12233845
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