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<p>Wide bandgap (WBG) perovskites hold tremendous potential for enabling efficient perovskite/silicon tandem solar cells. However, interfacial energy losses at the perovskite/electron selective contact interface remain a substantial obstacle in approaching its theoretical efficiency limit. Herein, for the first time, a multifunctional cage-like diammonium chloride molecule, featuring Lewis acid/base groups and strong molecular polarity, is designed to reduce film defects and modulate the interfacial dipole, thereby suppressing non-radiative recombination and optimizing surface band alignment. More importantly, the unique cage-like cation can induce the formation of a phase-pure quasi-2D perovskite with spontaneous in-plane orientation and exhibits a pronounced ferroelectric effect, facilitating carrier further apart and extraction by upshifting the surface work function. Consequently, we achieve 1.68 eV perovskite solar cells with power conversion efficiencies (PCEs) of 22.6% (0.1 cm<sup>2</sup>) and 21.0% (1.21 cm<sup>2</sup>). Furthermore, two-terminal monolithic perovskite/silicon tandem solar cells based on tunnel oxide passivating contact yield an impressive PCE of 31.1% (1.0 cm<sup>2</sup>) and demonstrate a decent operational stability (ISOS-L-1, T<sub>85</sub> &gt; 1020 h in ambient conditions without encapsulation). The ferroelectric interface physics opens new possibilities for efficient and stable perovskite-based tandem photovoltaics.</p>

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Minimizing interfacial energy losses via multifunctional cage-like diammonium molecules for efficient perovskite/silicon tandem solar cells

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年9月30日

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  • Xin Li,
  • Zhiqin Ying,
  • Linhui Liu,
  • Jun Wu,
  • Haofan Ma,
  • Ziyu He,
  • Yunyun Yu,
  • Yihan Sun,
  • Meili Zhang,
  • Xuchao Guo,
  • Yuheng Zeng,
  • Xi Yang,
  • Jichun Ye

摘要

Wide bandgap (WBG) perovskites hold tremendous potential for enabling efficient perovskite/silicon tandem solar cells. However, interfacial energy losses at the perovskite/electron selective contact interface remain a substantial obstacle in approaching its theoretical efficiency limit. Herein, for the first time, a multifunctional cage-like diammonium chloride molecule, featuring Lewis acid/base groups and strong molecular polarity, is designed to reduce film defects and modulate the interfacial dipole, thereby suppressing non-radiative recombination and optimizing surface band alignment. More importantly, the unique cage-like cation can induce the formation of a phase-pure quasi-2D perovskite with spontaneous in-plane orientation and exhibits a pronounced ferroelectric effect, facilitating carrier further apart and extraction by upshifting the surface work function. Consequently, we achieve 1.68 eV perovskite solar cells with power conversion efficiencies (PCEs) of 22.6% (0.1 cm2) and 21.0% (1.21 cm2). Furthermore, two-terminal monolithic perovskite/silicon tandem solar cells based on tunnel oxide passivating contact yield an impressive PCE of 31.1% (1.0 cm2) and demonstrate a decent operational stability (ISOS-L-1, T85 > 1020 h in ambient conditions without encapsulation). The ferroelectric interface physics opens new possibilities for efficient and stable perovskite-based tandem photovoltaics.