Dramatically enhanced performances and ideally controlled nano-morphology via co-solvent processing in low bandgap polymer solar cells

Abstract The device performance of photovoltaics with a polymer:fullerene bulk heterojunction (BHJ) structure, consisting of DT-PDPP2T-TT donor polymer and poly(3-hexylthiophene):[6,6]phenyl-C61-butyric acid methyl ester (PC61BM) acceptor compound, was investigated as a function of co-solvent composition. An enhancement of the photocurrent density and fill factor is observed in diodes made by spin-coating with chloroform mixed with ortho-dichlorobenzene, which allows a significantly higher device efficiency of 5.55% compared to diodes made from neat chloroform (efficiency = 3.61%). To clarify the role of the co-solvent, we investigated the nanoscale morphology with AFM, TEM and 2D-GIWAXS techniques and also the free-charge carrier mobility via space-charge limited current theory. We obtained the result that, under such supersaturated conditions, co-solvents induce increased polymer crystalline aggregation into a 3D phase structure and boost charge-carrier transport characteristics. This provides a rational basis for the development of ideally-controlled BHJ films that yield efficient DT-PDPP2T-TT:PCBM solar cells. Therefore, carefully selecting solvent mixtures provides an approach toward efficient low bandgap polymer solar cells.