Polaron Delocalization in Donor–Acceptor Polymers and its Impact on Organic Electrochemical Transistor Performance

Donor–acceptor (D-A) polymers are promising materials for organic electrochemical transistors (OECTs), as they minimize detrimental faradaic side-reactions during OECT operation, yet their steady-state performance still lags far behind all-donor counterparts. We report three D-A based on the diketopyrrolopyrrole unit that afford performances similar to those of polymers, hence representing a significant improvement previously developed copolymers. In addition improved performance, DFT simulations and respective hole polarons also reveal positive correlation between polaron delocalization providing new insights into design materials. Importantly, we demonstrate how can be tuned directly at molecular level by selection building blocks comprising polymers’ conjugated backbone, thus paving way development even higher performing polymers.