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<p>All-perovskite tandem solar cells are promising as next-generation high-efficiency photovoltaic devices. However, further progress in tin-lead (Sn–Pb) mixed perovskites, which are essential as the narrow-bandgap bottom sub-cell, is hampered by unbalanced crystallization processes, leading to inhomogeneous films and reduced power conversion efficiency (PCE). Here we provide a complete understanding of the formation of Sn–Pb films, from the precursor solution to the final film. We find that the total crystallization barrier for Sn-based perovskites is limited by the desorption of dimethyl sulfoxide (DMSO), while Pb-based perovskites experience a smaller DMSO desorption barrier. By engineering the reaction barrier in mixed films via tailoring the DMSO content, we obtain synchronous Sn–Pb perovskite crystallization and high-quality homogeneous films. On the basis of this understanding, we demonstrate single-junction Sn–Pb perovskite solar cells with a PCE of 22.88% and all-perovskite tandem devices with a certified PCE of 28.87%, fabricated by antisolvent-free methods. The unencapsulated tandem devices retain 87% of their initial PCE after about 450 h with maximum power point tracking under 1 sun illumination.</p>

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Understanding and manipulating the crystallization of Sn–Pb perovskites for efficient all-perovskite tandem solar cells

  • 期刊论文

  • 发表日期：

    2025年2月14日

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  • Xuke Yang,
  • Tianjun Ma,
  • Haojun Hu,
  • Wenjiang Ye,
  • Xin Li,
  • Mingyu Li,
  • Afei Zhang,
  • Ciyu Ge,
  • Xianglang Sun,
  • Yongxin Zhu,
  • Shuyu Yan,
  • Jun Yan,
  • Ying Zhou,
  • Zhong’an Li,
  • Chao Chen,
  • Haisheng Song,
  • Jiang Tang

摘要

All-perovskite tandem solar cells are promising as next-generation high-efficiency photovoltaic devices. However, further progress in tin-lead (Sn–Pb) mixed perovskites, which are essential as the narrow-bandgap bottom sub-cell, is hampered by unbalanced crystallization processes, leading to inhomogeneous films and reduced power conversion efficiency (PCE). Here we provide a complete understanding of the formation of Sn–Pb films, from the precursor solution to the final film. We find that the total crystallization barrier for Sn-based perovskites is limited by the desorption of dimethyl sulfoxide (DMSO), while Pb-based perovskites experience a smaller DMSO desorption barrier. By engineering the reaction barrier in mixed films via tailoring the DMSO content, we obtain synchronous Sn–Pb perovskite crystallization and high-quality homogeneous films. On the basis of this understanding, we demonstrate single-junction Sn–Pb perovskite solar cells with a PCE of 22.88% and all-perovskite tandem devices with a certified PCE of 28.87%, fabricated by antisolvent-free methods. The unencapsulated tandem devices retain 87% of their initial PCE after about 450 h with maximum power point tracking under 1 sun illumination.