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    Doping-Enhanced Short-Range Order of Perovskite Nanocrystals for Near-Unity Violet Luminescence Quantum Yield

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    Type
    Article
    Authors
    Yong, Zi-Jun
    Guo, Shao-Qiang
    Ma, Ju-Ping
    Zhang, Jun-Ying
    Li, Zhi-Yong
    Chen, Ya-Meng
    Zhang, Bin-Bin
    Zhou, Yang
    Shu, Jie
    Gu, Jia-Li
    Zheng, Li-Rong
    Bakr, Osman cc
    Sun, Hong-Tao
    KAUST Department
    Functional Nanomaterials Lab (FuNL)
    KAUST Catalysis Center (KCC)
    Material Science and Engineering Program
    Physical Science and Engineering (PSE) Division
    Date
    2018-07-16
    Online Publication Date
    2018-07-16
    Print Publication Date
    2018-08-08
    Permanent link to this record
    http://hdl.handle.net/10754/630766
    
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    Abstract
    All-inorganic perovskite nanocrystals (NCs) have emerged as a new generation of low-cost semiconducting luminescent system for optoelectronic applications. The room-temperature photoluminescence quantum yields (PLQYs) of these NCs in the green and red spectral range approach unity. However, their PLQYs in the violet are much lower, and an insightful understanding of such poor performance remains missing. We report a general strategy for the synthesis of all-inorganic violet-emitting perovskite NCs with near-unity PLQYs through engineering local order of the lattice by nickel ion doping. A broad range of experimental characterizations, including steady-state and time-resolved luminescence spectroscopy, X-ray absorption spectra, and magic angle spinning nuclear magnetic resonance spectra, reveal that the low PLQY in undoped NCs is associated with short-range disorder of the lattice induced by intrinsic defects such as halide vacancies and that Ni doping can substantially eliminate these defects and result in increased short-range order of the lattice. Density functional theory calculations reveal that Ni doping of perovskites causes an increase of defect formation energy and does not introduce deep trap states in the band gap, which is suggested to be the main reason for the improved local structural order and near-unity PLQY. Our ability to obtain violet-emitting perovskite NCs with near-perfect properties opens the door for a range of applications in violet-emitting perovskite-based devices such as light-emitting diodes, single-photon sources, lasers, and beyond.
    Citation
    Yong Z-J, Guo S-Q, Ma J-P, Zhang J-Y, Li Z-Y, et al. (2018) Doping-Enhanced Short-Range Order of Perovskite Nanocrystals for Near-Unity Violet Luminescence Quantum Yield. Journal of the American Chemical Society 140: 9942–9951. Available: http://dx.doi.org/10.1021/jacs.8b04763.
    Sponsors
    This work was supported by the National Natural Science Foundation of China (Grant Nos. 11574225 and 51672106), a project funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD), and a project supported by State Key Laboratory of Luminescence and Applications. We thank the staff at the 1W2B beamline at the Beijing Synchrotron Radiation Facility for XAFS measurements.
    Publisher
    American Chemical Society (ACS)
    Journal
    Journal of the American Chemical Society
    DOI
    10.1021/jacs.8b04763
    Additional Links
    https://pubs.acs.org/doi/pdf/10.1021/jacs.8b04763
    ae974a485f413a2113503eed53cd6c53
    10.1021/jacs.8b04763
    Scopus Count
    Collections
    Articles; Physical Science and Engineering (PSE) Division; Material Science and Engineering Program; KAUST Catalysis Center (KCC)

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