Tailoring and Modifying an Organic Electron Acceptor toward the Cathode Interlayer for Highly Efficient Organic Solar Cells

Abstract With the rapid advance of organic photovoltaic materials, the energy level structure, active layer morphology, and fabrication procedure of organic solar cells (OSCs) are changed significantly. Thus, the photoelectronic properties of many traditional electrode interlayers have become unsuitable for modifying new active layers; this limits the further enhancement in OSC efficiencies. Herein, a new design strategy of tailoring the end‐capping unit, ITIC, to develop a cathode interlayer (CIL) material for achieving high power conversion efficiency (PCE) in OSCs is demonstrated. The excellent electron accepting capacity, suitable energy level, and good film‐forming ability endow the S‐3 molecule with an outstanding electron extraction property. A device with S‐3 shows a PCE of 16.6%, which is among the top values in the field of OSCs. More importantly, it is demonstrated that the electrostatic potential difference between the CIL molecule and the polymer donor plays a crucial role in promoting exciton dissociation at the CIL/active layer interface, contributing to additional charge generation; this is crucial for enhancement of the current density. The results of this work not only develop a new design strategy for high‐performance CIL, but also demonstrate a reliable approach of density functional theory (DFT) calculation to predict the effect of the CIL chemical structure on exciton dissociation in OSCs.