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Structural and spectral dynamics of single-crystalline Ruddlesden-Popper phase halide perovskite blue light-emitting diodes.

  • Author(s): Chen, Hong
  • Lin, Jia
  • Kang, Joohoon
  • Kong, Qiao
  • Lu, Dylan
  • Kang, Jun
  • Lai, Minliang
  • Quan, Li Na
  • Lin, Zhenni
  • Jin, Jianbo
  • Wang, Lin-Wang
  • Toney, Michael F
  • Yang, Peidong
  • et al.
Abstract

Achieving perovskite-based high-color purity blue-emitting light-emitting diodes (LEDs) is still challenging. Here, we report successful synthesis of a series of blue-emissive two-dimensional Ruddlesden-Popper phase single crystals and their high-color purity blue-emitting LED demonstrations. Although this approach successfully achieves a series of bandgap emissions based on the different layer thicknesses, it still suffers from a conventional temperature-induced device degradation mechanism during high-voltage operations. To understand the underlying mechanism, we further elucidate temperature-induced device degradation by investigating the crystal structural and spectral evolution dynamics via in situ temperature-dependent single-crystal x-ray diffraction, photoluminescence (PL) characterization, and density functional theory calculation. The PL peak becomes asymmetrically broadened with a marked intensity decay, as temperature increases owing to [PbBr6]4- octahedra tilting and the organic chain disordering, which results in bandgap decrease. This study indicates that careful heat management under LED operation is a key factor to maintain the sharp and intense emission.

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