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<p>Self-assembled molecules (SAMs) are promising hole-selective layers for high-performance perovskite tandem solar cells. However, their inhomogeneous distribution and disordered packing on substrates lead to interfacial energy losses, limiting further improvements in efficiency and stability. Here, we design a SAM, Me-Ph2<i>m</i>PACz, through <i>meta</i>-disubstitution of dimethylcarbazole moieties on a phenyl linker. Compared to its monosubstituted carbazole counterpart, Me-Ph<i>p</i>PACz, Me-Ph2<i>m</i>PACz exhibits stronger adsorption energy and suppresses intermolecular hydrogen bond interaction via π-π stacking interactions. This inhibits the formation of large micelles, promoting a uniform, ordered and thermoresistant hole-selective layer. The resulting multilayer configuration retards crystallization and alleviates residual stress in the perovskite film, thereby reducing non-radiative recombination at the buried interface and enhancing hole extraction. The implementation of Me-Ph2<i>m</i>PACz as the hole-selective layer in 1.68 eV perovskite solar cells reduces interfacial non-radiative losses from 168 mV to 124 mV, accompanied by an increase in power conversion efficiency from 21.82% to 23.14%. The corresponding perovskite-silicon tandem solar cells achieve a champion PCE of 33.40% (certified 32.45% at National Renewable Energy Laboratory, NREL). Furthermore, encapsulated tandem devices based on Me-Ph2<i>m</i>PACz demonstrate exceptional stability, retaining 83% of their initial efficiency after 1000 h of maximum power point tracking under one-sun illumination at 85 °C in air. This work opens an avenue for designing high-performance and durable self-assembled molecules for perovskite tandem photovoltaics.</p>

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Uniform and ordered self-assembled hole-selective layers driven by π-π interactions for efficient perovskite-silicon tandem solar cells

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年4月24日

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  • Ming Luo,
  • Zhou Liu,
  • Qi Huang,
  • Yifan Chen,
  • Zhijie Wang,
  • Dongrui Jiang,
  • Rui Xia,
  • Danni Yu,
  • Rui He,
  • Dongsheng Yan,
  • Yi Mo,
  • Xueling Zhang,
  • Shengfan Wu,
  • Fengxian Xie,
  • Yingguo Yang,
  • Wallace C. H. Choy,
  • Yifeng Chen,
  • Yang Wang,
  • Jifan Gao,
  • Junhao Chu,
  • Hong Zhang

摘要

Self-assembled molecules (SAMs) are promising hole-selective layers for high-performance perovskite tandem solar cells. However, their inhomogeneous distribution and disordered packing on substrates lead to interfacial energy losses, limiting further improvements in efficiency and stability. Here, we design a SAM, Me-Ph2mPACz, through meta-disubstitution of dimethylcarbazole moieties on a phenyl linker. Compared to its monosubstituted carbazole counterpart, Me-PhpPACz, Me-Ph2mPACz exhibits stronger adsorption energy and suppresses intermolecular hydrogen bond interaction via π-π stacking interactions. This inhibits the formation of large micelles, promoting a uniform, ordered and thermoresistant hole-selective layer. The resulting multilayer configuration retards crystallization and alleviates residual stress in the perovskite film, thereby reducing non-radiative recombination at the buried interface and enhancing hole extraction. The implementation of Me-Ph2mPACz as the hole-selective layer in 1.68 eV perovskite solar cells reduces interfacial non-radiative losses from 168 mV to 124 mV, accompanied by an increase in power conversion efficiency from 21.82% to 23.14%. The corresponding perovskite-silicon tandem solar cells achieve a champion PCE of 33.40% (certified 32.45% at National Renewable Energy Laboratory, NREL). Furthermore, encapsulated tandem devices based on Me-Ph2mPACz demonstrate exceptional stability, retaining 83% of their initial efficiency after 1000 h of maximum power point tracking under one-sun illumination at 85 °C in air. This work opens an avenue for designing high-performance and durable self-assembled molecules for perovskite tandem photovoltaics.