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<p>Growth-induced defects and strain in two-dimensional (2D) perovskites severely limit carrier transport and suppress radiative efficiency, thereby sacrificing the carrier lifetime and obscuring the advantages from quantum confinement. Here, we report a near-equilibrium isothermal (NEIT) growth paradigm of 2D perovskite single crystals that exhibits living growth characteristics analogous to living polymerization. This approach confines crystallization primarily to initial nuclei, resulting in ultra-low nucleation density and yielding centimeter-scale single crystals of PEA<sub>2</sub>PbI<sub>4</sub> (Pb-n1), PEA<sub>2</sub>MAPb<sub>2</sub>I<sub>7</sub> (Pb-n2), and PEA<sub>2</sub>MA<sub>2</sub>Pb<sub>3</sub>I<sub>10</sub> (Pb-n3) with enhanced crystallographic perfection. This process achieves ~89% utilization of Pb precursor for Pb-n1, significantly surpassing ~13% from conventional methods and aligning with green-chemistry and sustainable synthetic principles. Additionally, the trap density gets suppressed by one order of magnitude. This unlocks high photoluminescence quantum yields (PLQYs, 77 ± 2% for Pb-n1), first cavity-free lasing in 2D Pb-n1 perovskite flakes, and long carrier lifetimes with diffusion lengths up to ~1.92 μm rivaling 3D perovskites. Critically, the living NEIT growth successfully enables the epitaxy of 2D bulk perovskite heterostructures, driving 60-fold accelerated photocarrier separation in lateral photodetectors. This near-equilibrium living growth paradigm establishes defect-minimized 2D perovskites as a versatile and active platform for high-performance quantum-well optoelectronics.</p>

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Living growth of ultra-bright 2D perovskites with long-lived carriers

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年7月14日

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  • Yanxin Han,
  • Yahui Li,
  • Qingyang Wei,
  • Hongzhi Zhou,
  • Hongzhi Shen,
  • Wenbo Ma,
  • Zhongpu Wang,
  • Ming Xia,
  • Yanan Wang,
  • Lijun Chai,
  • Xin Sheng,
  • Yiling Zhang,
  • Xiaohe Miao,
  • Yunfan Guo,
  • Zexin Jin,
  • Yang Michael Yang,
  • Juan Du,
  • Long Yuan,
  • Enzheng Shi

摘要

Growth-induced defects and strain in two-dimensional (2D) perovskites severely limit carrier transport and suppress radiative efficiency, thereby sacrificing the carrier lifetime and obscuring the advantages from quantum confinement. Here, we report a near-equilibrium isothermal (NEIT) growth paradigm of 2D perovskite single crystals that exhibits living growth characteristics analogous to living polymerization. This approach confines crystallization primarily to initial nuclei, resulting in ultra-low nucleation density and yielding centimeter-scale single crystals of PEA2PbI4 (Pb-n1), PEA2MAPb2I7 (Pb-n2), and PEA2MA2Pb3I10 (Pb-n3) with enhanced crystallographic perfection. This process achieves ~89% utilization of Pb precursor for Pb-n1, significantly surpassing ~13% from conventional methods and aligning with green-chemistry and sustainable synthetic principles. Additionally, the trap density gets suppressed by one order of magnitude. This unlocks high photoluminescence quantum yields (PLQYs, 77 ± 2% for Pb-n1), first cavity-free lasing in 2D Pb-n1 perovskite flakes, and long carrier lifetimes with diffusion lengths up to ~1.92 μm rivaling 3D perovskites. Critically, the living NEIT growth successfully enables the epitaxy of 2D bulk perovskite heterostructures, driving 60-fold accelerated photocarrier separation in lateral photodetectors. This near-equilibrium living growth paradigm establishes defect-minimized 2D perovskites as a versatile and active platform for high-performance quantum-well optoelectronics.