The charge transport properties of conjugated polymers are commonly limited by the energetic disorder. Recently several classes of rigid-rod conjugated polymers with planar backbone conformations and low energetic disorder despite being only weakly crystalline have been investigated for applications in field-effect transistors and thermoelectrics. However, there is no clear strategy to finely tune the interchain π-π contacts of these polymers which severely restricts the energetic disorder of interchain charge transport. Herein, we demonstrate that it is feasible to achieve excellent conductivity and thermoelectric performance in a class of these polymers based on thiophenefused benzodifurandione oligo(p-phenylenevinylene) (TBDOPV) through reducing the crystallization rate of the alkyl side chains and in this way carefully controlling the degree of interchain π-π interactions. A temperature-independent, barrier-free charge transport behavior in doped films was observed and n-type (p-type) conductivities over 100 S cm−1 (400 S cm−1) and power factors over 200 μW m−1 K−2 (100 μW m−1 K−2) were achieved within a single polymer by using different dopants. It was further demonstrated the state-of-the-art power output of the first flexible single-polymer thermoelectric generator.

High n-type and p-type conductivities and power factors achieved in a single conjugated polymer

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