A new family of polythienothiophene-co-benzodithiophene copolymers with different amounts of fluorine decoration (PBF x ) had been successfully synthesized. Detailed structure–property investigations covering physical properties, morphology, and solar cell performance with respect to the fluorine content in the polymers were performed by a series of structural characterization techniques. A PCE of 8.75% was obtained with the highest fluorinated polymer; the morphological trends, as well as the crystalline structure, were also investigated, shedding light on this important material modification.

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A new processing protocol based on non‐halogenated solvent and additive is developed to produce polymer solar cells with power conversion efficiencies better than those processed from commonly used halogenated solvent‐additive pair. Morphology studies show that good performance correlates with a finely distributed nanomorphology with a well‐defined polymer fibril network structure, which leads to balanced charge transport in device operation.