Bottom-up multi-interface modification boosts the performance of carbon-based HTL-free all-inorganic CsPbI₂Br perovskite solar cells

The inferior interface quality between CsPbI₂Br perovskite and the electron transport layer (ETL) as well as carbon electrode limits the stability and power conversion efficiency (PCE) of hole transport layer (HTL) free carbon-based all-inorganic CsPbI₂Br perovskite solar cells (C-IPSCs). Herein, perfluoropropionic acid (PFPA) is designed as a bottom-up multiple surface defect passivator that can simultaneously passivate perovskite/TiO₂ interface and perovskite/carbon electrode interface. The comprehensive experiments demonstrate that PFPA can not only optimize the electron mobility, conductivity, and band structure of the TiO₂ ETL through passivating oxygen vacancies (V_O), but also diffuse to the upper surface of perovskite film through grain boundaries to passivate the surface lead defects, thereby facilitating the gradient alignment of the perovskite surface energy levels with the carbon electrode. At the same time, PFPA can effectively release the tensile stress at the interface of perovskite and reduce the delocalization state of the band tail caused by lattice distortion, so as to prepare high-quality perovskite films. As a result of the above interaction, the PCE of HTL-free CsPbI₂Br C-IPSCs after PFPA modification is increased from 12.24% (control device) to 14.15%. In addition, the modified unencapsulated devices show superior long-term stability and thermal stability.