Facile Sol–Gel-Derived Craterlike Dual-Functioning TiO₂ Electron Transport Layer for High-Efficiency Perovskite Solar Cells

Organic–inorganic hybrid perovskite solar cells (PSCs) are considered promising materials for low-cost solar energy harvesting technology. An electron transport layer (ETL), which facilitates the extraction of photogenerated electrons and their transport to the electrodes, is a key component in planar PSCs. In this study, a new strategy to concurrently manipulate the electrical and optical properties of ETLs to improve the performance of PSCs is demonstrated. A careful control over the Ti alkoxide-based sol–gel chemistry leads to a craterlike porous/blocking bilayer TiO2 ETL with relatively uniform surface pores of 220 nm diameter. Additionally, the phase separation promoter added to the precursor solution enables nitrogen doping in the TiO2 lattice, thus generating oxygen vacancies. The craterlike surface morphology allows for better light transmission because of reduced reflection, and the electrically conductive craterlike bilayer ETL enhances charge extraction and transport. Through these synergetic improvements in both optical and electrical properties, the power conversion efficiency of craterlike bilayer TiO2 ETL-based PSCs could be increased from 13.7 to 16.0% as compared to conventional dense TiO2-based PSCs.