Rational selection of the polymeric structure for interface engineering of perovskite solar cells

Tedious trial-and-error procedures are commonly practiced for surface modification of the perovskite solar cell (PSC) active layers. A guideline to rationally choose the passivating functional groups of the polymeric structure that is eminently effective in passivating the charged defects and elongating the device lifetime is hence in urgent demand. Herein, three prototypical polymers, poly(vinyl acetate) (PVA), polyethylene glycol (PEG), and poly(9-vinylcarbazole) (PVK), are selected to investigate the structural effect of the polymeric modification agents on the PSCs. We found that PVA possesses the Lewis base functional group with the minimized steric hindrance and the strongest electron-donating ability, enabling the most effective defect passivation on the perovskite film surface and the most enhanced carrier diffusion capacity. It demonstrates a power conversion efficiency (PCE) of 23.20% and noticeably enhanced operational stability. Our work provides important insights toward the selection of polymeric modification agents for high-performance and long-term stable PSCs.