Pyrrole‐Based Fully Non‐fused Acceptor for Efficient and Stable Organic Solar Cells

Abstract Organic solar cells (OSCs) are still suffering from the low light utilization and unstable under ultraviolet irradiation. To tackle these challenges, we design and synthesize a non‐fused acceptor based on 1‐(2‐butyloctyl)‐1H‐pyrrole as π‐bridge unit, denoted as GS70, which serves as active layer in the front‐cell for constructing tandem OSCs with a parallel configuration. Benefiting from the well‐complementary absorption spectra with the rear‐cell, GS70‐based parallel tandem OSCs exhibit an improved photoelectron response over the range between 600–700 nm, yielding a high short‐circuit current density of 28.4 mA cm −2 . The improvement in light utilization translates to a power conversion efficiency of 19.4 %, the highest value among all parallel tandem OSCs. Notably, owing to the intrinsic stability of GS70, the manufactured parallel tandem OSCs retain 84.9 % of their initial PCE after continuous illumination for 1000 hours. Overall, this work offers novel insight into the molecular design of low‐cost and stability non‐fused acceptors, emphasizing the importance of adopting a parallel tandem configuration for achieving efficient light harvesting and improved photostability in OSCs.