Interfacial
passivation of defective perovskite films with a dipole
molecule shows a great potential for high-efficiency perovskite solar
cells (PSCs). Herein, by regulating the side group of an aniline-based
molecule with an electron-withdrawing nitryl (−NO2) or electron-donating methoxyl (−OCH3), the binding
energy between −NH2 and under-coordinated Pb2+ in the CsPbBr3 lattice is reinforced, and the
dipole-moment-induced surface energy level reconstruction allows for
efficient hole extraction for the −OCH3-tailored
molecule because of the changed intramolecular electron distribution,
whereas −NO2 displays the opposite effect. Finally,
the all-inorganic CsPbBr3 PSC achieves a power conversion
efficiency (PCE) of 9.81% with an open-circuit voltage (V
oc) of 1.632 V and an excellent stability in both high
humidity and light irradiation. Upon doping Sm3+ into CsPbBr3, the PCE and V
oc are further
increased to 10.75% and 1.675 V. This work confirms the importance
of a side group on an interface dipole molecule to maximize the charge
scavenging, especially for V
oc improvement.