Neutralizing Charge Centers Radius via Dipole‐Charge Interaction in Perovskites

ABSTRACT Organic–inorganic perovskite materials face challenges related to the presence of non‐neutralized charge centers, such as positively charged local defects arising from lattice imperfections like point‐vacancies and under‐coordinated lead ions at lattice edges, hindering their photoelectric intrinsic properties. We introduce 3,3‐difluoropyrrolidine hydrochloride (GOSO‐005), a novel dipolar molecule, as an effective solution for neutralizing positive charge centers within perovskites. GOSO‐005, with its high dipole moment and fluorinated groups, interacts with charged defects to neutralize them, thus reducing defect density and minimizing the effective electron‐capturing radius. This neutralizing strategy enhances charge transport, reduces Shockley‐Read‐Hall recombination, and boosts an impressive efficiency of 26.09% (certified 26.12%) for perovskite solar cells. In parallel, the fluorinated dipolar molecule introduces additional hydrophobicity to the resultant perovskite, thereby significantly enhancing the long‐term environmental, continuous illumination operational, and thermal stabilities of the perovskite solar cells.