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<p>Achieving uniform crystallization across both top and buried interfaces in perovskite films is crucial for unlocking their full photovoltaic potential, yet remains an unresolved challenge. The buried interface, in particular, suffers from poor crystallization relative to the top surface, resulting in suboptimal crystal quality and increased defect densities. Here we propose a one-step strategy to induce the spontaneous formation of near-phase-pure two-dimensional perovskites at the buried interface via the introduction of organic cation halide salts in the perovskite precursor solution. Single-crystal structure analysis highlights the pivotal role of molecular engineering in facilitating the spontaneous formation of buried two-dimensional perovskite phases. The low dipole moments and planar rigidity structures of organic spacers promote their aggregation at perovskite grain boundaries, followed by their migration to the film’s bottom interface. The two-dimensional perovskite layer simultaneously promotes uniform crystallization and efficient defect passivation at the buried interface, leading to a power conversion efficiency of 26.31% (certified 26.02%). Unencapsulated devices retain 95% of their initial power conversion efficiency after 1,000 hours of continuous illumination.</p>

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Spontaneous 2D perovskite formation at the buried interface of perovskite solar cells enhances crystallization uniformity and defect passivation

  • 期刊论文

  • 发表日期：

    2025年11月24日

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  • Yuping Gao,
  • Hang Liu,
  • Zonglong Song,
  • Yu Chen,
  • Liu Yang,
  • Ziyang Hu,
  • Yu Zou,
  • Yongsheng Chen,
  • Yongsheng Liu

摘要

Achieving uniform crystallization across both top and buried interfaces in perovskite films is crucial for unlocking their full photovoltaic potential, yet remains an unresolved challenge. The buried interface, in particular, suffers from poor crystallization relative to the top surface, resulting in suboptimal crystal quality and increased defect densities. Here we propose a one-step strategy to induce the spontaneous formation of near-phase-pure two-dimensional perovskites at the buried interface via the introduction of organic cation halide salts in the perovskite precursor solution. Single-crystal structure analysis highlights the pivotal role of molecular engineering in facilitating the spontaneous formation of buried two-dimensional perovskite phases. The low dipole moments and planar rigidity structures of organic spacers promote their aggregation at perovskite grain boundaries, followed by their migration to the film’s bottom interface. The two-dimensional perovskite layer simultaneously promotes uniform crystallization and efficient defect passivation at the buried interface, leading to a power conversion efficiency of 26.31% (certified 26.02%). Unencapsulated devices retain 95% of their initial power conversion efficiency after 1,000 hours of continuous illumination.