<p>Two-step fabrication method of formamidinium–caesium metal halide perovskites (FA<sub>1-<i>x</i></sub>Cs<sub><i>x</i></sub>PbI<sub>3</sub>) offers superior control over crystallization regulation and therefore is more suitable for solar cell manufacturing. However, forming the ideal α phase required for stable devices remains challenging due to limited Cs<sup>+</sup> incorporation and unclear phase transition mechanism. Here we design caesium 4-(diphenylphosphino)benzoate to enable efficient Cs<sup>+</sup> doping and to homogenize cation distribution, obtaining high-quality perovskite films with improved phase stability. As a result, the solar cells fabricated via the two-step process achieve an efficiency of 26.91% (certified 26.61%). The devices incorporating a thermally stable charge-transport layer retain 95% of their initial efficiency (23.76%) after continuous operation under 1-sun illumination at the maximum power point tracking and 85 °C (ISOS-L-2 protocol) for 1,500 hours. This study provides insights into the phase transition pathway and the corresponding transition-state structure of FA<sub>0.9</sub>Cs<sub>0.1</sub>PbI<sub>3</sub> as well as the mechanism of Cs<sup>+</sup>-driven lattice stabilization in perovskites.</p>

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Controlled Cs⁺ incorporation through organocaesium salts in α-FA–Cs perovskite solar cells with a certified efficiency of 26.61%

  • Jiacheng He,
  • Zhao Guo,
  • Kaikai Liu,
  • Wangping Sheng,
  • Xiao Luo,
  • Licheng Tan,
  • Yiwang Chen

摘要

Two-step fabrication method of formamidinium–caesium metal halide perovskites (FA1-xCsxPbI3) offers superior control over crystallization regulation and therefore is more suitable for solar cell manufacturing. However, forming the ideal α phase required for stable devices remains challenging due to limited Cs+ incorporation and unclear phase transition mechanism. Here we design caesium 4-(diphenylphosphino)benzoate to enable efficient Cs+ doping and to homogenize cation distribution, obtaining high-quality perovskite films with improved phase stability. As a result, the solar cells fabricated via the two-step process achieve an efficiency of 26.91% (certified 26.61%). The devices incorporating a thermally stable charge-transport layer retain 95% of their initial efficiency (23.76%) after continuous operation under 1-sun illumination at the maximum power point tracking and 85 °C (ISOS-L-2 protocol) for 1,500 hours. This study provides insights into the phase transition pathway and the corresponding transition-state structure of FA0.9Cs0.1PbI3 as well as the mechanism of Cs+-driven lattice stabilization in perovskites.