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<p>Self-assembled monolayers (SAMs) have become indispensable hole-selective contacts for high-efficiency inverted perovskite solar cells (PSCs). However, the intrinsically acidic head groups of conventional SAMs lead to interfacial inhomogeneity, limited charge transfer, and poor operational stability. Here, we introduce a family of alkali metal–based phosphonate salts (2PACz-M) through targeted head-group functionalization of the benchmark [2-(9H-carbazol-9-yl)ethyl]phosphonic acid (2PACz) SAM, achieving a chemically neutralized and electronically delocalized interface. The ionic phosphonate moiety enhances π-electron conjugation, improves energy-level alignment, and strengthens chemical coordination with metal oxide electrodes, resulting in homogeneous and stable surface coverage. Moreover, when combined with [4-(3,6-dimethyl-9H-carbazol-9-yl)butyl]phosphonic acid (Me-4PACz), the mixed-SAM interface exhibits a synergistic effect that facilitates efficient hole extraction, suppresses non-radiative recombination, and reinforces environmental robustness. This interfacial engineering enables 1.55 eV PSCs to achieve a champion power conversion efficiency (PCE) of 26.88% with a fill factor (FF) of 86.57%, alongside a 23.32% PCE for a 29.7 cm<sup>2</sup> module. The SAM synergy proves universal across perovskites of varied bandgaps, yielding two-terminal (2T) all-perovskite tandem solar cells with an enhanced PCE of 29.05%.</p>

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Ionic self-assembled monolayers enable neutral interfaces and synergistic charge extraction in high-efficiency perovskite solar cells

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年6月24日

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  • Yuxuan Yang,
  • Deimante Krisiune,
  • Yuliang Xu,
  • Xuehui Liu,
  • Qiangqiang Zhao,
  • Yongde Xu,
  • Hao Tian,
  • Ernestas Kasparavicius,
  • Zhiyu Gao,
  • Xu Fu,
  • Bao Zhang,
  • Jianxing Xia,
  • Chuanxiao Xiao,
  • Shuping Pang,
  • Vytautas Getautis,
  • Dewei Zhao,
  • Kasparas Rakstys,
  • Yi Zhang

摘要

Self-assembled monolayers (SAMs) have become indispensable hole-selective contacts for high-efficiency inverted perovskite solar cells (PSCs). However, the intrinsically acidic head groups of conventional SAMs lead to interfacial inhomogeneity, limited charge transfer, and poor operational stability. Here, we introduce a family of alkali metal–based phosphonate salts (2PACz-M) through targeted head-group functionalization of the benchmark [2-(9H-carbazol-9-yl)ethyl]phosphonic acid (2PACz) SAM, achieving a chemically neutralized and electronically delocalized interface. The ionic phosphonate moiety enhances π-electron conjugation, improves energy-level alignment, and strengthens chemical coordination with metal oxide electrodes, resulting in homogeneous and stable surface coverage. Moreover, when combined with [4-(3,6-dimethyl-9H-carbazol-9-yl)butyl]phosphonic acid (Me-4PACz), the mixed-SAM interface exhibits a synergistic effect that facilitates efficient hole extraction, suppresses non-radiative recombination, and reinforces environmental robustness. This interfacial engineering enables 1.55 eV PSCs to achieve a champion power conversion efficiency (PCE) of 26.88% with a fill factor (FF) of 86.57%, alongside a 23.32% PCE for a 29.7 cm2 module. The SAM synergy proves universal across perovskites of varied bandgaps, yielding two-terminal (2T) all-perovskite tandem solar cells with an enhanced PCE of 29.05%.