Semiconducting Properties and Geometry-Directed Self-Assembly of Heptacyclic Anthradithiophene Diimide-Based Polymers

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Backbone geometry and side-chain self-assembly are key factors that govern the aggregation of conjugated semiconducting polymers and affect charge transport. Tuning of charge transport properties hinges on being able to strike a balance between electronic structures, self-assembly, and robustness to disorder. This work describes a top-down design strategy focusing on the geometry of polymer aggregates. A heptacyclic acceptor anthradithiophene diimide was designed to build self-assembled polymers. The corresponding polymers possess a pseudolinear rodlike backbone geometry with interdigitated alkyl chains. Using a fluorinated comonomer suppresses the rotational disorder and preserves the backbone symmetry at a relatively long length scale, leading to improved planarity and facilitating intrachain charge transport. These polymers exhibit ambipolar transistor performance with the maximum hole mobility of 4.21 cm 2 V –1 s –1 . The experimental microstructures are in good agreement with the simulated unit cells, indicating an extended dimensionality of charge transport pathways. These promising results may help to complement the design rationales of semiconducting polymers.