Surface‐Energy‐Regulated Growth of α‐Phase Cs _0.03 FA _0.97 PbI ₃ for Highly Efficient and Stable Inverted Perovskite Solar Cells

Methylammonium (MA)-free formamidinium (FA)-dominated CsxFA1−xPbI3 is rising as the most promising candidate for highly efficient and stable perovskite solar cells. However, the growth of high-quality CsxFA1−xPbI3 black-phase perovskite structure without ion doping in the lattice remains a challenge. Herein, propeller-shaped halogenated tertiary ammonium is synthesized, showing high binding energy on the perovskite surface and large steric hindrance. This molecule can significantly reduce the barrier of high surface energy that suppresses the growth of the α-phase CsxFA1−xPbI3 structure. As a result, the α-phase structure can be formed at room temperature, which can further act as a seed for the growth of high-quality film. Solar cells based on the film show a record efficiency up to 23.6% for MA free CsxFA1−xPbI3 solar cells with inverted structure and excellent stability at 85 °C over 200 h.