A 3-Fluoro-4-hexylthiophene-Based Wide Bandgap Donor Polymer for 10.9% Efficiency Eco-Friendly Nonfullerene Organic Solar Cells.

Nonfullerene organic solar cells (NFOSCs) are attracting increasing academic and industrial interest due to their potential uses for flexible and lightweight products using low-cost roll-to-roll technology. In this work, two wide bandgap (WBG) polymers, namely P(fTh-BDT)-C6 and P(fTh-2DBDT)-C6, are designed and synthesized using benzodithiophene (BDT) derivatives. Good oxidation stability and high solubility are achieved by simultaneously introducing fluorine and alkyl chains to a single thiophene (Th) unit. Solid P(fTh-2DBDT)-C6 films present WBG optical absorption, suitable frontier orbital levels, and strong π-π stacking effects. In addition, P(fTh-2DBDT)-C6 exhibits good solubility in both halogenated and nonhalogenated solvents, suggesting its suitability as donor polymer for NFOSCs. The P(fTh-2DBDT)-C6:3,9-bis(2-methylene-(3-(1,1-dicyanomethylene)-indanone))-5,5,11,11-tetrakis(5-hexylthienyl)-dithieno[2,3-d:2',3'-d']-s-indaceno[1,2-b:5,6-b']dithiophene (ITIC-Th) based device processed using chlorobenzene/1,8-diiodooctane (CB/DIO) exhibits a remarkably high power conversion efficiency (PCE) of 11.1%. Moreover, P(fTh-2DBDT)-C6:ITIC-Th reaches a high PCE of 10.9% when processed using eco-friendly solvents, such as o-xylene/diphenyl ether (DPE). The cell processed using CB/DIO maintains 100% efficiency after 1272 h, while that processed using o-xylene/DPE presents a 101% increase in efficiency after 768 h and excellent long-term stability. The results of this study demonstrate that simultaneous fluorination and alkylation are effective methods for designing donor polymers appropriate for high-performance NFOSCs.