Graphdiyne Derivative as Multifunctional Solid Additive in Binary Organic Solar Cells with 17.3% Efficiency and High Reproductivity

Morphology tuning of the blend film in organic solar cells (OSCs) is a key approach to improve device efficiencies. Among various strategies, solid additive is proposed as a simple and new way to enable morphology tuning. However, there exist few solid additives reported to meet such expectations. Herein, chlorine‐functionalized graphdiyne (GCl) is successfully applied as a multifunctional solid additive to fine‐tune the morphology and improve device efficiency as well as reproductivity for the first time. Compared with 15.6% efficiency for control devices, a record high efficiency of 17.3% with the certified one of 17.1% is obtained along with the simultaneous increase of short‐circuit current (Jsc) and fill factor (FF), displaying the state‐of‐the‐art binary organic solar cells at present. The redshift of the film absorption, enhanced crystallinity, prominent phase separation, improved mobility, and decreased charge recombination synergistically account for the increase of Jsc and FF after introducing GCl into the blend film. Moreover, the addition of GCl dramatically reduces batch‐to‐batch variations benefiting mass production owing to the nonvolatile property of GCl. All these results confirm the efficacy of GCl to enhance device performance, demonstrating a promising application of GCl as a multifunctional solid additive in the field of OSCs. A highly efficient organic solar cell is demonstrated by applying a chlorine‐functionalized graphdiyne (GCl) multifunctional solid additive. A record‐high efficiency of 17.3%, with certified efficiency of 17.1%, is obtained along with the simultaneous increase of short‐circuit current (Jsc) and fill factor (FF), displaying state‐of‐the‐art binary organic solar cells at present.