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