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Performance Enhanced Light-Emitting Diodes Fabricated from Nanocrystalline CsPbBr3 with In Situ Zn2+ Addition

  • Parth Vashishtha*
    Parth Vashishtha
    School of Materials Science and Engineering, Nanyang Technological University (NTU), 50 Nanyang Avenue, Singapore 639798, Singapore
    *Email: [email protected]
  • Benjamin E. Griffith
    Benjamin E. Griffith
    School of Materials Science and Engineering, Nanyang Technological University (NTU), 50 Nanyang Avenue, Singapore 639798, Singapore
    Department of Physics, University of Warwick, Gibbet Hill Rd., Coventry CV4 7AL, United Kingdom
  • Alasdair A.M. Brown
    Alasdair A.M. Brown
    Energy Research Institute @NTU (ERI@N), Research Techno Plaza, X-Frontier Block, Level 5, 50 Nanyang Drive, Singapore 637553, Singapore
    School of Engineering, Faculty of Engineering and Physical Sciences, University of Southampton, Southampton SO17 1BJ, United Kingdom
    University of Southampton, Malaysia, Iskandar Puteri, 79200 Johor, Malaysia
  • Thomas J.N. Hooper
    Thomas J.N. Hooper
    School of Materials Science and Engineering, Nanyang Technological University (NTU), 50 Nanyang Avenue, Singapore 639798, Singapore
    Energy Research Institute @NTU (ERI@N), Research Techno Plaza, X-Frontier Block, Level 5, 50 Nanyang Drive, Singapore 637553, Singapore
    High-Field NMR Facility, School of Physics and Mathematical Sciences, Nanyang Technological University, 637371, Singapore
  • Yanan Fang
    Yanan Fang
    School of Materials Science and Engineering, Nanyang Technological University (NTU), 50 Nanyang Avenue, Singapore 639798, Singapore
    More by Yanan Fang
  • Mohammed S. Ansari
    Mohammed S. Ansari
    School of Materials Science and Engineering, Nanyang Technological University (NTU), 50 Nanyang Avenue, Singapore 639798, Singapore
  • Annalisa Bruno
    Annalisa Bruno
    Energy Research Institute @NTU (ERI@N), Research Techno Plaza, X-Frontier Block, Level 5, 50 Nanyang Drive, Singapore 637553, Singapore
  • Suan Hui Pu
    Suan Hui Pu
    School of Engineering, Faculty of Engineering and Physical Sciences, University of Southampton, Southampton SO17 1BJ, United Kingdom
    University of Southampton, Malaysia, Iskandar Puteri, 79200 Johor, Malaysia
    More by Suan Hui Pu
  • Subodh G. Mhaisalkar
    Subodh G. Mhaisalkar
    School of Materials Science and Engineering, Nanyang Technological University (NTU), 50 Nanyang Avenue, Singapore 639798, Singapore
    Energy Research Institute @NTU (ERI@N), Research Techno Plaza, X-Frontier Block, Level 5, 50 Nanyang Drive, Singapore 637553, Singapore
  • Tim White*
    Tim White
    School of Materials Science and Engineering, Nanyang Technological University (NTU), 50 Nanyang Avenue, Singapore 639798, Singapore
    *Email: [email protected]
    More by Tim White
  • , and 
  • John V. Hanna*
    John V. Hanna
    School of Materials Science and Engineering, Nanyang Technological University (NTU), 50 Nanyang Avenue, Singapore 639798, Singapore
    Department of Physics, University of Warwick, Gibbet Hill Rd., Coventry CV4 7AL, United Kingdom
    *Email: [email protected]
Cite this: ACS Appl. Electron. Mater. 2020, 2, 12, 4002–4011
Publication Date (Web):December 4, 2020
https://doi.org/10.1021/acsaelm.0c00827
Copyright © 2020 American Chemical Society

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    Abstract

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    Inorganic cesium lead halide perovskite nanocrystals are promising materials for optoelectronic applications as they exhibit high thermal stability alongside precise color tunability and high color purity; however, their optical properties are degraded by surface defects. This work demonstrates a room temperature synthesis of CsPbBr3 nanocrystals facilitating in situ surface passivation via the incorporation of Zn2+ cations. The facile incorporation ZnBr2 into the precursor solution facilitates Zn2+ and Br substitution into the nanocrystal surface/subsurface layers to induce passivation of existing Pb2+ and Br vacancies and increase the photoluminescence quantum yield from ∼48 to 86%. The XPS and solid-state 1H MAS NMR techniques show that the key modification is a reduction of the octylamine:oleic acid ratio leading to a near-neutral surface charge; this is accompanied by the appearance of larger nanosheets and nanowires observed by quantitative powder XRD and HR-TEM. The suitability of these perovskite nanocrystals for electrically driven applications was confirmed by the fabrication of light-emitting diodes, which demonstrate that the in situ Zn2+ passivation strategy enhanced the external quantum efficiency by ∼60%.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsaelm.0c00827.

    • Experimental section for characterization techniques; remaining XRD analysis, TEM micrographs, and histograms; 133Cs T1 NMR data; remaining optical properties and device efficiency data; XPS data; XRD of Cs4PbBr6; EDXS spectra; a table for fitting parameters of Rietveld refinements; a table for 1H MAS NMR data; a table showing carrier lifetime components extracted from TRPL spectra (PDF)

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