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<p>Wide-bandgap (WBG) perovskite solar cells (PSCs) are employed for tandem solar cells. Understanding the crystallization mechanism of mixed-halide WBG perovskite will contribute to achieving the high-performance photovoltaics. Herein, we demonstrate that the asynchronous halide insertion is accompanied by random crystal facets and orientations, restricting the efficient carrier extraction. Guided by density functional theory calculations, we construct a π-conjugated molecular wall structure using o-phenylenediamine (OPD). The molecular wall at the grain boundary induces templated perovskite crystallization through the ortho-diamine group, enabling synchronous [PbBr<sub>6</sub>]<sup>4-</sup> and [PbI<sub>6</sub>]<sup>4-</sup> halide insertion. The OPD-treated perovskite film exhibits a preferred (100) facet and a highly vertical orientation. Benefited from the improved carrier extraction, the resulting WBG PSC (1.69 eV) achieves a power conversion efficiency of 24.13% (certified 23.43%), representing one of the highest values among WBG PSCs. Meanwhile, the improved perovskite crystal quality ensures the enhanced operational stability of the PSCs.</p>

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Halide insertion regulation for efficient and stable wide-bandgap perovskite photovoltaics

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年12月2日

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  • Zexin Song,
  • Ni Meng,
  • Yimeng Tian,
  • Jiwei Li,
  • Huiyang Ye,
  • Anming Mo,
  • Changjiu Sun,
  • Zhiqiang Li,
  • Shaopeng Yang,
  • Tingwei He

摘要

Wide-bandgap (WBG) perovskite solar cells (PSCs) are employed for tandem solar cells. Understanding the crystallization mechanism of mixed-halide WBG perovskite will contribute to achieving the high-performance photovoltaics. Herein, we demonstrate that the asynchronous halide insertion is accompanied by random crystal facets and orientations, restricting the efficient carrier extraction. Guided by density functional theory calculations, we construct a π-conjugated molecular wall structure using o-phenylenediamine (OPD). The molecular wall at the grain boundary induces templated perovskite crystallization through the ortho-diamine group, enabling synchronous [PbBr6]4- and [PbI6]4- halide insertion. The OPD-treated perovskite film exhibits a preferred (100) facet and a highly vertical orientation. Benefited from the improved carrier extraction, the resulting WBG PSC (1.69 eV) achieves a power conversion efficiency of 24.13% (certified 23.43%), representing one of the highest values among WBG PSCs. Meanwhile, the improved perovskite crystal quality ensures the enhanced operational stability of the PSCs.