Aryl Diammonium Iodide Passivation for Efficient and Stable Hybrid Organ‐Inorganic Perovskite Solar Cells

Abstract Surface passivation is increasingly one of the most prominent strategies to promote the efficiency and stability of perovskite solar cells (PSCs). However, most passivation molecules hinder carrier extraction due to poorly conductive aggregation between perovskite surface and carrier transportation layer. Herein, a novel molecule: p ‐phenyl dimethylammonium iodide (PDMAI) with ammonium group on both terminals is introduced, and its passivation effect is systematically investigated. It is found that PDMAI can mitigate defects at the surface and promote carrier extraction from perovskite to the hole transporting layer, leading to a lift of open‐circuit voltage of 40 mV. Profiting from superior PDMAI passivation, the average efficiency of PSCs has been elevated from 19.69% to 20.99%. As demonstrated with density functional theory calculations, PDMAI probably tends to anchor onto the perovskite surface with both NH 3 I tails, and enhances the adhesion and contact to perovskite layer. The exposed hydrophobic aryl core protects perovskite against detrimental environmental factors. In addition, the alkyl component between aryl and ammonium groups is demonstrated to be essentially vital in triggering passivation function, which offers the guidance for the design of passivation molecules.