Synergistic Optimization of Buried Interface by Multifunctional Organic–Inorganic Complexes for Highly Efficient Planar Perovskite Solar Cells

For the further improvement of the power conversion efficiency (PCE) and stability of perovskite solar cells (PSCs), the buried interface between the perovskite and the electron transport layer is crucial. However, it is challenging to effectively optimize this interface as it is buried beneath the perovskite film. Herein, we have designed and synthesized a series of multifunctional organic–inorganic (OI) complexes as buried interfacial material to promote electron extraction, as well as the crystal growth of the perovskite. The OI complex with BF(4)(−) group not only eliminates oxygen vacancies on the SnO(2) surface but also balances energy level alignment between SnO(2) and perovskite, providing a favorable environment for charge carrier extraction. Moreover, OI complex with amine (− NH(2)) functional group can regulate the crystallization of the perovskite film via interaction with PbI(2), resulting in highly crystallized perovskite film with large grains and low defect density. Consequently, with rational molecular design, the PSCs with optimal OI complex buried interface layer which contains both BF(4)(−) and −NH(2) functional groups yield a champion device efficiency of 23.69%. More importantly, the resulting unencapsulated device performs excellent ambient stability, maintaining over 90% of its initial efficiency after 2000 h storage, and excellent light stability of 91.5% remaining PCE in the maximum power point tracking measurement (under continuous 100 mW cm(−2) light illumination in N(2) atmosphere) after 500 h. [Image: see text] SUPPLEMENTARY INFORMATION: The online version contains supplementary material available at 10.1007/s40820-023-01130-5.