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Cyanamide Passivation Enables Robust Elemental Imaging of Metal Halide Perovskites at Atomic Resolution
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    Cyanamide Passivation Enables Robust Elemental Imaging of Metal Halide Perovskites at Atomic Resolution
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    • Jiakai Liu
      Jiakai Liu
      KAUST Catalysis Center (KCC), Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Kingdom of Saudi Arabia
      College of New Materials and New Energies, Shenzhen Technology University, Shenzhen 518118, China
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    • Kepeng Song
      Kepeng Song
      KAUST Advanced Membranes and Porous Materials Center, Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Kingdom of Saudi Arabia
      School of Chemistry and Chemical Engineering, Shandong University, Jinan 250100, China
      Suzhou Research Institute, Shandong University, Suzhou 215123, China
      More by Kepeng Song
    • Xiaopeng Zheng
      Xiaopeng Zheng
      KAUST Catalysis Center (KCC), Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Kingdom of Saudi Arabia
    • Jun Yin
      Jun Yin
      KAUST Advanced Membranes and Porous Materials Center, Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Kingdom of Saudi Arabia
      More by Jun Yin
    • Ke Xin Yao
      Ke Xin Yao
      College of Materials Science and Engineering, Chongqing University, Chongqing 400044, China
      More by Ke Xin Yao
    • Cailing Chen
      Cailing Chen
      KAUST Advanced Membranes and Porous Materials Center, Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Kingdom of Saudi Arabia
      More by Cailing Chen
    • Haoze Yang
      Haoze Yang
      KAUST Advanced Membranes and Porous Materials Center, Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Kingdom of Saudi Arabia
      More by Haoze Yang
    • Mohamed Nejib Hedhili
      Mohamed Nejib Hedhili
      Imaging and Characterization Core Lab, King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Kingdom of Saudi Arabia
    • Wang Zhang
      Wang Zhang
      College of New Materials and New Energies, Shenzhen Technology University, Shenzhen 518118, China
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    • Peigang Han
      Peigang Han
      College of New Materials and New Energies, Shenzhen Technology University, Shenzhen 518118, China
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    • Omar F. Mohammed
      Omar F. Mohammed
      KAUST Advanced Membranes and Porous Materials Center, Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Kingdom of Saudi Arabia
    • Yu Han*
      Yu Han
      KAUST Catalysis Center (KCC), Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Kingdom of Saudi Arabia
      KAUST Advanced Membranes and Porous Materials Center, Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Kingdom of Saudi Arabia
      *Email: [email protected]
      More by Yu Han
    • Osman M. Bakr*
      Osman M. Bakr
      KAUST Catalysis Center (KCC), Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Kingdom of Saudi Arabia
      *Email: [email protected]
    Other Access OptionsSupporting Information (1)

    The Journal of Physical Chemistry Letters

    Cite this: J. Phys. Chem. Lett. 2021, 12, 42, 10402–10409
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jpclett.1c02830
    Published October 21, 2021
    Copyright © 2021 American Chemical Society

    Abstract

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    Lead halide perovskites (LHPs) have attracted a tremendous amount of attention because of their applications in solar cells, lighting, and optoelectronics. However, the atomistic principles underlying their decomposition processes remain in large part obscure, likely due to the lack of precise information about their local structures and composition along regions with dimensions on the angstrom scale, such as crystal interfaces. Aberration-corrected scanning transmission electron microscopy combined with X-ray energy dispersive spectroscopy (EDS) is an ideal tool, in principle, for probing such information. However, atomic-resolution EDS has not been achieved for LHPs because of their instability under electron-beam irradiation. We report the fabrication of CsPbBr3 nanoplates with high beam stability through an interface-assisted regrowth strategy using cyanamide. The ultrahigh stability of the nanoplates primarily stems from two contributions: defect-healing self-assembly/regrowth processes and surface modulation by strong electron-withdrawing cyanamide molecules. The ultrahigh stability of as-prepared CsPbBr3 nanoplates enabled atomic-resolution EDS elemental mapping, which revealed atomically and elementally resolved details of the LHP nanostructures at an unprecedented level. While improving the stability of LHPs is critical for device applications, this work illustrates how improving the beam stability of LHPs is essential for addressing fundamental questions on structure–property relations in LHPs.

    Copyright © 2021 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jpclett.1c02830.

    • Experimental section, details about chemicals, CsPbBr3 NCs, and nanoplate synthesis, characterization, and computational details (PDF)

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    Cited By

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    This article is cited by 16 publications.

    1. Nuerbiya Aihemaiti, Zhenqin Li, Siying Peng. Perspective on High-Resolution Characterizations of Polarons in Halide Perovskites. Chemistry of Materials 2024, 36 (11) , 5297-5312. https://doi.org/10.1021/acs.chemmater.3c03012
    2. Kepeng Song, Yingcai Fan, Wei Qin. Structure and Charge Carrier Separation Promotion Effects of Antiphase Boundaries in Cesium Lead Bromide. The Journal of Physical Chemistry Letters 2024, 15 (8) , 2255-2261. https://doi.org/10.1021/acs.jpclett.4c00099
    3. Changjiu Sun, Yuanzhi Jiang, Li Zhang, Keyu Wei, Mingjian Yuan. Toward the Controlled Synthesis of Lead Halide Perovskite Nanocrystals. ACS Nano 2023, 17 (18) , 17600-17609. https://doi.org/10.1021/acsnano.3c05609
    4. Avijit Pramanik, Sudarson Sekhar Sinha, Kaelin Gates, Jing Nie, Fengxiang X Han, Paresh Chandra Ray. Light-Induced Wavelength Dependent Self Assembly Process for Targeted Synthesis of Phase Stable 1D Nanobelts and 2D Nanoplatelets of CsPbI3 Perovskites. ACS Omega 2023, 8 (14) , 13202-13212. https://doi.org/10.1021/acsomega.3c00477
    5. Sumit Kumar Dutta, Lucheng Peng, Biswajit Hudait, Renguo Xie, Narayan Pradhan. Halide Perovskite Cluster Precursors: A Paradigm for Obtaining Structure- and Color-Tunable Light-Emitting Nanocrystals. ACS Energy Letters 2022, 7 (9) , 3177-3186. https://doi.org/10.1021/acsenergylett.2c01638
    6. Kepeng Song, Yingcai Fan, Jiakai Liu, Dongqing Qi, Ning Lu, Wei Qin. Carrier Separation Enhanced by High Angle Twist Grain Boundaries in Cesium Lead Bromide Perovskites. The Journal of Physical Chemistry Letters 2022, 13 (31) , 7206-7212. https://doi.org/10.1021/acs.jpclett.2c01832
    7. Kepeng Song, Jiakai Liu, Dongqing Qi, Ning Lu, Wei Qin. Unravelling Structure and Formation Mechanisms of Ruddlesden–Popper-Phase-like Nanodomains in Inorganic Lead Halide Perovskites. The Journal of Physical Chemistry Letters 2022, 13 (9) , 2117-2123. https://doi.org/10.1021/acs.jpclett.2c00210
    8. Jiakai Liu, Xiaopeng Zheng, Omar F. Mohammed, Osman M. Bakr. Self-Assembly and Regrowth of Metal Halide Perovskite Nanocrystals for Optoelectronic Applications. Accounts of Chemical Research 2022, 55 (3) , 262-274. https://doi.org/10.1021/acs.accounts.1c00651
    9. Yeming 业铭 Xian 冼, Xiaoming 晓明 Wang 王, Yanfa 炎发 Yan 鄢. Revealing the microstructures of metal halide perovskite thin films via advanced transmission electron microscopy. Chinese Physics B 2024, 33 (9) , 096803. https://doi.org/10.1088/1674-1056/ad6259
    10. Ernest Ruby, Hugo Levy-Falk, Gaëlle Trippé-Allard, Frédéric Fossard, Maxime Vallet, Nicolas Guiblin, Jean-Sébastien Lauret, Emmanuelle Deleporte, Cédric R. Mayer. Influence of arylalkyl amines on the formation of hybrid CsPbBr 3 nanocrystals via a modified LARP method. Nanoscale Advances 2024, 6 (6) , 1704-1719. https://doi.org/10.1039/D3NA01105D
    11. Libing Yao, Liuwen Tian, Shaochen Zhang, Yuan Tian, Jingjing Xue, Siying Peng, Rui Wang. Low-dose transmission electron microscopy study on halide perovskites: Application and challenges. EnergyChem 2023, 5 (5) , 100105. https://doi.org/10.1016/j.enchem.2023.100105
    12. Noel Mireles Villegas, Josue C. Hernandez, Joshua C. John, Matthew Sheldon. Promoting solution-phase superlattices of CsPbBr 3 nanocrystals. Nanoscale 2023, 15 (22) , 9728-9737. https://doi.org/10.1039/D3NR00693J
    13. Zhihao Zhang, Lu Qiao, Ke Meng, Run Long, Gang Chen, Peng Gao. Rationalization of passivation strategies toward high-performance perovskite solar cells. Chemical Society Reviews 2023, 52 (1) , 163-195. https://doi.org/10.1039/D2CS00217E
    14. Xiaomei Wu, Xiaoxing Ke, Manling Sui. Recent progress on advanced transmission electron microscopy characterization for halide perovskite semiconductors. Journal of Semiconductors 2022, 43 (4) , 041106. https://doi.org/10.1088/1674-4926/43/4/041106
    15. Kepeng Song, Jiakai Liu, Ning Lu, Dongqing Qi, Wei Qin. Direct atomic-scale imaging of a screw dislocation core structure in inorganic halide perovskites. Physical Chemistry Chemical Physics 2022, 24 (11) , 6393-6397. https://doi.org/10.1039/D2CP00183G
    16. Biao Yuan, Yi Yu. High-resolution transmission electron microscopy of beam-sensitive halide perovskites. Chem 2022, 8 (2) , 327-339. https://doi.org/10.1016/j.chempr.2022.01.006

    The Journal of Physical Chemistry Letters

    Cite this: J. Phys. Chem. Lett. 2021, 12, 42, 10402–10409
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jpclett.1c02830
    Published October 21, 2021
    Copyright © 2021 American Chemical Society

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