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<p>Two-dimensional (2D) perovskites have garnered significant interest in photoelectric devices due to their tunable optoelectronic properties. However, they still suffer from inefficient charge carrier extraction and significant ion migration, which largely hinder the practical application of perovskite photodetectors. Herein, we report a symmetry-broken 2D Dion–Jacobson (DJ) phase mixed halide perovskite (DMPD)Pb(I<sub>0.96</sub>Br<sub>0.04</sub>)<sub>4</sub> (DMPD = 3-(dimethylamino)-1-propylammonium), achieved through the doping of Br<sup>−</sup> ions. The preferred distribution of Br<sup>−</sup> ions at axial halide sites triggers local structural symmetry breaking, which drives energy band splitting, increases activation energy for ion migration, and effectively relaxes microstrain, as evidenced by both theoretical and experimental investigations. The lattice structure and energy band modifications synergistically contribute to reduced charge carrier recombination, enhanced charge carrier transport and extraction, and suppressed ion migration. As a result, our 2D (DMPD)Pb(I<sub>0.96</sub>Br<sub>0.04</sub>)<sub>4</sub> single crystal photodetector achieves an impressive detectivity of 7.12 × 10<sup>12</sup> Jones, ranking among the highest reported for 2D DJ phase perovskite devices. With these findings, we aim to offer a conducive guidance for the design of effective 2D perovskites toward advanced optoelectronics.</p>

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Locally symmetry-broken 2D Dion–Jacobson mixed halide perovskites for efficient photodetectors

  • 期刊论文

  • 发表日期：

    2025年5月9日

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  • Jie Yang,
  • Kuan Kuang,
  • Mingkai Li,
  • Zixian Yu,
  • Fangfang Xia,
  • Lei Zhang,
  • Tianyou Zhai,
  • Yunbin He,
  • Junnian Chen

摘要

Two-dimensional (2D) perovskites have garnered significant interest in photoelectric devices due to their tunable optoelectronic properties. However, they still suffer from inefficient charge carrier extraction and significant ion migration, which largely hinder the practical application of perovskite photodetectors. Herein, we report a symmetry-broken 2D Dion–Jacobson (DJ) phase mixed halide perovskite (DMPD)Pb(I0.96Br0.04)4 (DMPD = 3-(dimethylamino)-1-propylammonium), achieved through the doping of Br− ions. The preferred distribution of Br− ions at axial halide sites triggers local structural symmetry breaking, which drives energy band splitting, increases activation energy for ion migration, and effectively relaxes microstrain, as evidenced by both theoretical and experimental investigations. The lattice structure and energy band modifications synergistically contribute to reduced charge carrier recombination, enhanced charge carrier transport and extraction, and suppressed ion migration. As a result, our 2D (DMPD)Pb(I0.96Br0.04)4 single crystal photodetector achieves an impressive detectivity of 7.12 × 1012 Jones, ranking among the highest reported for 2D DJ phase perovskite devices. With these findings, we aim to offer a conducive guidance for the design of effective 2D perovskites toward advanced optoelectronics.