<p>Maximizing quasi-Fermi level splitting is essential for achieving high photovoltage in perovskite solar cells. Conventional strategies that prioritize rapid charge extraction at the perovskite/fullerene interface, can deplete interfacial carrier populations, limiting quasi-Fermi level splitting and photovoltage. Here we demonstrate that rational interface design benefits for slowed extraction rate, preserving interfacial carriers while minimizing non-radiative recombination. We introduce 3PDPA, a molecularly engineered electron-selective self-assembled monolayer at the perovskite/C<sub>60</sub> interface. 3PDPA slows electron extraction, anchors undercoordinated Pb<sup>2+</sup> ions and forms stable six-membered hydrogen-bonded rings with FA<sup>+</sup> cations, delivering robust passivation and excellent chemical stability. 3PDPA further enables π–π interactions with C<sub>60</sub>, improving interfacial contact and reducing potential fluctuations. Inverted cells incorporating 3PDPA achieve efficiencies of 26.82% for 1.53 eV bandgap cells and 21.2% for 1.77 eV bandgap cells, alongside a T<sub>90</sub> lifetime of ~1,000 h under International Summit on Organic Photovoltaic Stability (ISOS-L-3) stress conditions.</p>

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A molecularly engineered electron-selective self-assembled monolayer enhances quasi-Fermi level splitting in inverted perovskite solar cells

  • Mubai Li,
  • Yuanhang Yang,
  • Sheng Li,
  • Xiaotian Yang,
  • Yixuan Zheng,
  • Siyang Cheng,
  • Junjie Feng,
  • Hao Li,
  • Qiuhan Yu,
  • Zhongchen Xu,
  • Houguo Fei,
  • Yong Liu,
  • Cunlan Guo,
  • Shengjun Yuan,
  • Qianqian Lin,
  • Zhiping Wang

摘要

Maximizing quasi-Fermi level splitting is essential for achieving high photovoltage in perovskite solar cells. Conventional strategies that prioritize rapid charge extraction at the perovskite/fullerene interface, can deplete interfacial carrier populations, limiting quasi-Fermi level splitting and photovoltage. Here we demonstrate that rational interface design benefits for slowed extraction rate, preserving interfacial carriers while minimizing non-radiative recombination. We introduce 3PDPA, a molecularly engineered electron-selective self-assembled monolayer at the perovskite/C60 interface. 3PDPA slows electron extraction, anchors undercoordinated Pb2+ ions and forms stable six-membered hydrogen-bonded rings with FA+ cations, delivering robust passivation and excellent chemical stability. 3PDPA further enables π–π interactions with C60, improving interfacial contact and reducing potential fluctuations. Inverted cells incorporating 3PDPA achieve efficiencies of 26.82% for 1.53 eV bandgap cells and 21.2% for 1.77 eV bandgap cells, alongside a T90 lifetime of ~1,000 h under International Summit on Organic Photovoltaic Stability (ISOS-L-3) stress conditions.