Multifunctional Imidazolidinyl Urea Additive Initiated Complex with PbI2 Toward Efficient and Stable Perovskite Solar Cells

Abstract High‐quality perovskite absorption layer is the fundamental basis for efficient and stable perovskite solar cells (PSCs). Due to the ionic nature of perovskite components, plentiful charged defects and suspension bonds remain on the surface of perovskite grains after continuous high‐temperature annealing. Here, the complex initiated by the introduction of a multifunctional imidazolidinyl urea (IU) additive into the PbI 2 precursor solution could serve as nucleation sites and crystallization templates for perovskite crystals to optimize the growth of high‐quality perovskite films. By anchoring at the grain boundaries of perovskite films, IU molecules could passivate various types of defects, improve the hydrophobic properties, and inhibit lead leakage. Attributed to reduced defect density, improved charge transport, and inhibited α ‐FAPbI 3 transition, the PSCs prepared based on IU additives achieved a champion power conversion efficiency of 23.18% (21.51% for the control PSCs) with negligible hysteresis and satisfactory stability.