<p>The integration of crystallographic control into solution-processed perovskite films remains a challenge for efficient light emission, as disordered optical dipoles fundamentally limit photon extraction, a bottleneck constraining both classical and quantum planar optoelectronic devices. Here, we address this by developing an in situ formation strategy for oriented quasi-2D perovskite nanosheets within films via ligand-engineered crystallization. By designing and orchestrating steric hindrance and π–π interactions of ligands, we direct the crystallization kinetics to yield regular face-on nanosheets exhibiting enhanced horizontal transition dipole moment orientation compared to conventional isotropic films. The in situ architectural control also elevates both the photoluminescence quantum yield beyond 90% and carrier mobility comparable to 3D perovskite levels. These synergies enable perovskite light-emitting diodes (PeLEDs) with an external quantum efficiency (EQE) of 31.2% for pure-red emission at 635 nm, comparing favorably to other pure-red PeLEDs. Concurrently, the peak luminance and operational stability of the in situ nanosheet PeLEDs exhibit significant improvements.</p>

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In-situ formation of oriented perovskite nanosheets with tailored optical dipoles enabling >30% EQE in pure-red LEDs

  • Shaowei Liu,
  • Dezhong Zhang,
  • Lei Wang,
  • Binhe Li,
  • Wei Yuan,
  • Ziheng Xiong,
  • Kai Chen,
  • Helong Zhu,
  • Wenping Wu,
  • Shuang Li,
  • Liu Yang,
  • Yunzhuo Liu,
  • Hongmei Zhan,
  • Chuanli Qin,
  • Jiaqi Zhang,
  • Jun Liu,
  • Lixiang Wang,
  • Chuanjiang Qin

摘要

The integration of crystallographic control into solution-processed perovskite films remains a challenge for efficient light emission, as disordered optical dipoles fundamentally limit photon extraction, a bottleneck constraining both classical and quantum planar optoelectronic devices. Here, we address this by developing an in situ formation strategy for oriented quasi-2D perovskite nanosheets within films via ligand-engineered crystallization. By designing and orchestrating steric hindrance and π–π interactions of ligands, we direct the crystallization kinetics to yield regular face-on nanosheets exhibiting enhanced horizontal transition dipole moment orientation compared to conventional isotropic films. The in situ architectural control also elevates both the photoluminescence quantum yield beyond 90% and carrier mobility comparable to 3D perovskite levels. These synergies enable perovskite light-emitting diodes (PeLEDs) with an external quantum efficiency (EQE) of 31.2% for pure-red emission at 635 nm, comparing favorably to other pure-red PeLEDs. Concurrently, the peak luminance and operational stability of the in situ nanosheet PeLEDs exhibit significant improvements.