Interfacial Modification and Defect Passivation by Crosslinking Interlayer for Efficient and Stable CuSCN-Based Perovskite Solar Cell

摘要： Study of the inorganic hole-transport layer (HTL) in perovskite solar cell (PSC) is gathering attention due to the drawback of conventional PSC design, where the organic HTL with salt dopants majorly participates in the degradation mechanisms. On the other hand, inorganic HTL secures better stability, while it offers difficulties in the deposition and interfacial control to realize high-performing devices. In this study, we demonstrate polydimethylsiloxane (PDMS) as an ideal polymeric interlayer which prevents the interfacial degradation, and improves both photovoltaic performance and stability of CuSCN-based PSC by its crosslinking behavior. Surprisingly, the PDMS polymers are identified to form chemical bonds with perovskite and CuSCN, as shown by Raman spectroscopy. This novel crosslinking interlayer of PDMS enhances the hole-transporting property at the interface and passivates the interfacial defects, realizing the PSC with high power-conversion efficiency over 19%. Furthermore, the utilization of PDMS interlayer greatly improves the stability of solar cells against both humidity and heat, by mitigating the interfacial defects and interdiffusion. The PDMS-interlayered PSCs retained over 90% of the initial efficiencies, both after 1000 h under ambient condition (unencapsulated) and after 500 h under 85°C/85% relative humidity (encapsulated).