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<p>Buried defects at the interface between the wide-bandgap perovskite and the self-assembled monolayer (SAM) limit the performance of p–i–n solar cells, particularly in textured monolithic perovskite–silicon tandem solar cells. Here we reveal that uncontrolled perovskite crystallization dynamics on conventional SAMs drives the co-evolution of electronic defects and morphological degradation at the buried interface. This stems from structural and energetic incompatibility between the perovskite precursor solution and the SAM. To precisely control the perovskite crystallization, we develop a tailored SAM that mitigates defect formation and enhances interfacial electronic coupling. Integrated into a perovskite–silicon tandem solar cell, this approach enables a power conversion efficiency of 33.86% (certified as 33.59%) for a device with a 1-cm<sup>2</sup> area and a power conversion efficiency of 29.25% (certified as 28.53%) for an area of 16 cm<sup>2</sup>. The tandem device demonstrates remarkable operational stability, retaining more than 90% of the initial power conversion efficiency after 2,000 h of operational under 1-sun illumination.</p>

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Perovskite crystallization control via an engineered self-assembled monolayer in perovskite–silicon tandem solar cells

  • 期刊论文

  • 发表日期：

    2025年10月20日

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  • Daoyong Zhang,
  • Boning Yan,
  • Rui Xia,
  • Biao Li,
  • Ruilin Li,
  • Pengjie Hang,
  • Haimeng Xin,
  • Jiyao Wei,
  • Ming Lei,
  • Yifeng Chen,
  • Jifan Gao,
  • Hengyu Zhang,
  • Zhenyi Ni,
  • Deren Yang,
  • Xuegong Yu

摘要

Buried defects at the interface between the wide-bandgap perovskite and the self-assembled monolayer (SAM) limit the performance of p–i–n solar cells, particularly in textured monolithic perovskite–silicon tandem solar cells. Here we reveal that uncontrolled perovskite crystallization dynamics on conventional SAMs drives the co-evolution of electronic defects and morphological degradation at the buried interface. This stems from structural and energetic incompatibility between the perovskite precursor solution and the SAM. To precisely control the perovskite crystallization, we develop a tailored SAM that mitigates defect formation and enhances interfacial electronic coupling. Integrated into a perovskite–silicon tandem solar cell, this approach enables a power conversion efficiency of 33.86% (certified as 33.59%) for a device with a 1-cm2 area and a power conversion efficiency of 29.25% (certified as 28.53%) for an area of 16 cm2. The tandem device demonstrates remarkable operational stability, retaining more than 90% of the initial power conversion efficiency after 2,000 h of operational under 1-sun illumination.