Tailoring Interfacial Dipole Molecules to Mitigate Carrier and Energy Losses in Perovskite Solar Cells

Abstract Interface engineering has become the mainstream for improving the performance of perovskite solar cells (PSCs). Interfacial dipole (ID) molecules have emerged as a feasible and effective strategy to alleviate the charge carrier loss and energy loss in PSCs. Here, the three symmetrical donor–acceptor interfacial dipole molecules (named PzT, PzTE, and PzTN) are designed and synthesized with identical hole transport backbone and different anchoring groups. The ID molecule is introduced into the interface between the perovskite layer and the hole transport layer. The dipole moments of ID molecules regulate the surface work function and energy‐level alignment of perovskites, improve charge extraction, and reduce energy loss at the interface. Meanwhile, the anchoring groups of ID molecules coordinate with the defects on the surface of PVK and HTL, reduce interfacial trap state density and charge accumulation, and mitigate the carrier non‐radiative recombination losses. As a result, PzTN‐modified PSC achieved a champion power conversion efficiency of 25.34% with a photovoltage of 1.176 V and a fill factor (FF) of 83.27%, accompanied by almost undetectable hysteresis and excellent operating stability. This research demonstrates a feasible strategy for efficient and stable PSCs by interfacial dipole molecules.