Modulating Aggregation Behavior by Ternary Strategies for Efficient and Stable Thick‐Film Organic Solar Cells

Functional third components targeted to improve a specific property of organic solar cells is an effective strategy. However, introducing a third component to simultaneously improve efficiency and stability and achieve good performance in thick-film devices has rarely been reported. Herein, low diffusion third components IDCN and ID2CN are reported to achieve a power conversion efficiency (PCE) of 18.08% and a high short-circuit current (J _SC) of 27.82 mA cm^-2, one of the highest values based on PM6:Y6. They increase light harvesting in the range of 400-500 nm while enhancing energy transfer via Förster resonance energy transfer (FRET). A tightly ordered molecular arrangement is achieved by modulating the preaggregation and film formation kinetics of Y6, which enhance exciton dissociation and charge transport. Moreover, the low-diffusion third component can effectively restrict the diffusion of Y6 to improve the morphology stability, and the T₉₀ lifetime is increased from 689 to 1545 h. In 300 nm thick-film devices, PM6:ID2CN:Y6 achieves a PCE of 15.01%, much higher than PM6:Y6's 12.83%, demonstrating the great potential of ID2CN in thick-film devices.