<p>Despite substantial advances in green and red metal halide perovskite light-emitting diodes (PeLEDs), blue PeLEDs, particularly deep-blue ones (defined as Commission International de l’Eclairage <i>y</i> coordinate (CIE<sub><i>y</i></sub>) less than 0.06) that meet the latest Rec. 2020 colour gamut standard, lag dramatically behind owing to a severe phase segregation-induced electroluminescent spectral shift and low exciton utilization in broadened bandgap perovskite emitters. Here we propose a multivalent immobilization strategy to realize high-efficiency and spectrally stable deep-blue PeLEDs by introducing a polyfluorinated oxygen-containing molecule. Systematic experiments and extensive 5,000 fs ab initio molecular dynamics simulations reveal that a crucial role of the multivalent effect stemming from three kinds of interaction of hydrogen bond (F···H–N), ionic bond (F–Pb) and coordination bond (C=O:Pb) with perovskite is to synergistically stabilize the perovskite phase and enhance exciton radiative recombination. The resultant exciton concentration and exciton recombination rate of the deep-blue perovskite emitter are increased by factors of 1.66 and 1.64, respectively. In this context, our target PeLEDs demonstrate a peak external quantum efficiency of up to 15.36% at a deep-blue emission wavelength of 459 nm and a half-lifetime of 144 min at a constant current density of 0.45 mA cm<sup>−</sup><sup>2</sup>. Moreover, the deep-blue PeLEDs maintain a constant spectrum peak with CIE chromaticity coordinates of (0.136, 0.051) under a steady driving current for 60 min.</p>

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Multivalent-effect immobilization of reduced-dimensional perovskites for efficient and spectrally stable deep-blue light-emitting diodes

  • Jianchao Dong,
  • Bin Zhao,
  • Huiyu Ji,
  • Ziang Zang,
  • Lingmei Kong,
  • Chunshuang Chu,
  • Dongyuan Han,
  • Jie Wang,
  • Yuhao Fu,
  • Zi-Hui Zhang,
  • Yingguo Yang,
  • Lijun Zhang,
  • Xuyong Yang,
  • Ning Wang

摘要

Despite substantial advances in green and red metal halide perovskite light-emitting diodes (PeLEDs), blue PeLEDs, particularly deep-blue ones (defined as Commission International de l’Eclairage y coordinate (CIEy) less than 0.06) that meet the latest Rec. 2020 colour gamut standard, lag dramatically behind owing to a severe phase segregation-induced electroluminescent spectral shift and low exciton utilization in broadened bandgap perovskite emitters. Here we propose a multivalent immobilization strategy to realize high-efficiency and spectrally stable deep-blue PeLEDs by introducing a polyfluorinated oxygen-containing molecule. Systematic experiments and extensive 5,000 fs ab initio molecular dynamics simulations reveal that a crucial role of the multivalent effect stemming from three kinds of interaction of hydrogen bond (F···H–N), ionic bond (F–Pb) and coordination bond (C=O:Pb) with perovskite is to synergistically stabilize the perovskite phase and enhance exciton radiative recombination. The resultant exciton concentration and exciton recombination rate of the deep-blue perovskite emitter are increased by factors of 1.66 and 1.64, respectively. In this context, our target PeLEDs demonstrate a peak external quantum efficiency of up to 15.36% at a deep-blue emission wavelength of 459 nm and a half-lifetime of 144 min at a constant current density of 0.45 mA cm2. Moreover, the deep-blue PeLEDs maintain a constant spectrum peak with CIE chromaticity coordinates of (0.136, 0.051) under a steady driving current for 60 min.