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<p>The development of molecular engineering has substantially increased the power conversion efficiency of inverted p-i-n perovskite solar cells (PSCs) over the past five years, surpassing that of regular n-i-p PSCs. The strategic design of symmetric molecules to alleviate steric hindrance, thereby facilitating long-range-ordered <i>π</i>–<i>π</i> stacking on substrates, offers an effective approach for enhancing the structural organization in molecular self-assembly. Here we synthesize an axially symmetric molecule with homogeneous electron delocalization, (2-(pyren-2-yl)ethyl)phosphonic acid (<i>p</i>Py), which can form a long-range-ordered <i>π</i>–<i>π</i> stacking assembly on indium tin oxide substrates. Additionally, the <i>p</i>Py thin film demonstrates an intense and integrated Debye–Scherrer ring at <i>q</i> = 0.27 Å<sup>−1</sup> with a highly ordered face-on orientation and displays more spatial uniform distribution, which effectively facilitates charge transport. The as-fabricated <i>p</i>Py-based PSCs achieve a power conversion efficiency of 26.6% and maintain 94% of the initial efficiency after 3,000 h of continuous simulated solar illumination following the ISOS-L-1I protocol.</p><p></p>

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Symmetry-driven engineering of long-range-ordered π–π stacking molecules for high-efficiency perovskite photovoltaics

  • 期刊论文

  • 发表日期：

    2025年9月30日

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  • Peide Zhu,
  • Zhixin Liu,
  • Xia Lei,
  • Siru He,
  • Deng Wang,
  • Jie Zeng,
  • Lida Wang,
  • Fei Su,
  • Wenbo Peng,
  • Zheng Liang,
  • Yuxin Sun,
  • Zhiwei Lei,
  • Zhitong Li,
  • Hsien-Yi Hsu,
  • Xu Pan,
  • Xingzhu Wang,
  • Jingbai Li,
  • Yong Zhang,
  • Baomin Xu

摘要

The development of molecular engineering has substantially increased the power conversion efficiency of inverted p-i-n perovskite solar cells (PSCs) over the past five years, surpassing that of regular n-i-p PSCs. The strategic design of symmetric molecules to alleviate steric hindrance, thereby facilitating long-range-ordered π–π stacking on substrates, offers an effective approach for enhancing the structural organization in molecular self-assembly. Here we synthesize an axially symmetric molecule with homogeneous electron delocalization, (2-(pyren-2-yl)ethyl)phosphonic acid (pPy), which can form a long-range-ordered π–π stacking assembly on indium tin oxide substrates. Additionally, the pPy thin film demonstrates an intense and integrated Debye–Scherrer ring at q = 0.27 Å−1 with a highly ordered face-on orientation and displays more spatial uniform distribution, which effectively facilitates charge transport. The as-fabricated pPy-based PSCs achieve a power conversion efficiency of 26.6% and maintain 94% of the initial efficiency after 3,000 h of continuous simulated solar illumination following the ISOS-L-1I protocol.