Abstract
A π‐conjugated Lewis base is introduced into perovskite solar cells, namely, indacenodithiophene end‐capped with 1.1‐dicyanomethylene‐3‐indanone (IDIC), as a multifunctional interlayer, which combines efficient trap‐passivation and electron‐extraction. Perovskite solar cells with IDIC layers yield higher photovoltages and photocurrents, and 45% enhanced efficiency compared with control devices without IDIC.