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<p>The popular and effective top-surface mixed-dimensional heterojunction in n–i–p perovskite photovoltaics is frequently ineffective in p–i–n architectures due to the intrinsic p-type character of most reported two-dimensional (2D) or low-dimensional perovskites. Here we deploy electronic engineering to realize the p<i>-</i> to n<i>-</i>type transition in 2D Ruddlesden–Popper perovskites through molecular dipole tuning and chemically designable n-type defects. Parahalogenated piperidine derivatives induce a favourable p<i>-</i> to n<i>-</i>type transition in 2D perovskites, thereby improving energy-level alignment at the perovskite–electron transport layer interface. This tailored band alignment effectively reduces interfacial energy barriers, suppresses non-radiative recombination losses for wide-bandgap perovskites and enhances stability. Notably, p–i–n wide-bandgap (~1.68 eV) perovskite solar cells with an n-type 2D capping layer exhibit more than 100 mV enhancement in open-circuit voltage, resulting in a certified power conversion efficiency of 33.64% when integrated with industrial 110-μm-thick Czochralski heterojunction silicon. Furthermore, such monolithic perovskite/silicon tandem cells retain 92% of their initial efficiency after 1,100 h of continuous operation under maximum-power-point tracking. Our chemical design of p<i>-</i> to n<i>-</i>type transition for 2D perovskite establishes a molecular-level strategy for optimizing interfacial energetics towards high-performance perovskite/silicon tandem photovoltaics.</p>

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Modulating p–n transition of two-dimensional perovskites for efficient and stable perovskite/Si tandem photovoltaics

  • 期刊论文

  • 发表日期：

    2026年7月30日

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  • Jiahao Guo,
  • Zeyu Zhang,
  • Zhen Jia,
  • Fang Liu,
  • Menglei Feng,
  • Wenji Zhan,
  • Haifei Wang,
  • Xiaoyu Wang,
  • Yide Chang,
  • Yao Wang,
  • Kanrui Jiang,
  • Yuetian Chen,
  • Yanfeng Miao,
  • Bowei Li,
  • Yanming Wang,
  • Zijia Li,
  • Yixin Zhao

摘要

The popular and effective top-surface mixed-dimensional heterojunction in n–i–p perovskite photovoltaics is frequently ineffective in p–i–n architectures due to the intrinsic p-type character of most reported two-dimensional (2D) or low-dimensional perovskites. Here we deploy electronic engineering to realize the p- to n-type transition in 2D Ruddlesden–Popper perovskites through molecular dipole tuning and chemically designable n-type defects. Parahalogenated piperidine derivatives induce a favourable p- to n-type transition in 2D perovskites, thereby improving energy-level alignment at the perovskite–electron transport layer interface. This tailored band alignment effectively reduces interfacial energy barriers, suppresses non-radiative recombination losses for wide-bandgap perovskites and enhances stability. Notably, p–i–n wide-bandgap (~1.68 eV) perovskite solar cells with an n-type 2D capping layer exhibit more than 100 mV enhancement in open-circuit voltage, resulting in a certified power conversion efficiency of 33.64% when integrated with industrial 110-μm-thick Czochralski heterojunction silicon. Furthermore, such monolithic perovskite/silicon tandem cells retain 92% of their initial efficiency after 1,100 h of continuous operation under maximum-power-point tracking. Our chemical design of p- to n-type transition for 2D perovskite establishes a molecular-level strategy for optimizing interfacial energetics towards high-performance perovskite/silicon tandem photovoltaics.