Passivating A-Site and X-Site Vacancies Simultaneously via N-Heterocyclic Amines for Efficient Cs₂AgBiBr₆ Solar Cells

To address the toxicity and stability issues of traditional lead halide perovskite solar cells (PSCs), the development of lead-free PSCs, such as Cs2AgBiBr6 solar cells, is of great significance. However, due to the low defect formation energy of Cs2AgBiBr6, a large number of vacancies, including A-site vacancies and X-site vacancies, form during the fabrication process of the Cs2AgBiBr6 film, which seriously damage the performance of the devices. The traditional phenylethylammonium (PEA) cation, mainly focusing on passivating A-site vacancies, is incapable of reducing X-site vacancies and so results in a limited performance improvement in Cs2AgBiBr6 solar cells. Herein, inspired by the capability of the Lewis base to coordinate with metal cations, a series of N-heterocyclic amines are introduced to serve as a dual-site passivator, reducing A-site and X-site vacancies at the same time. The highest power conversion efficiency of modified Cs2AgBiBr6 solar cells has been increased 36% from 1.10 to 1.50%. Further investigation reveals that the higher electron density of additives would lead to a stronger interaction with metal cations like Ag+ and Bi3+, thus reducing more X-site defects and improving carrier dynamics. Our work provides a strategy for passivating perovskite with various kinds of defects and reveals the connection between the coordination capability of additives and device performance enhancement, which could be instructive in improving the performance of lead-free PSCs.