Toward Efficient Charge Transport of Polymer-Based Organic Field-Effect Transistors: Molecular Design, Processing, and Functional Utilization

ConspectusPolymer-based organic field-effect transistors (OFETs) have attracted great attention owing to their significantly improved performance and the recently emerged prospects for broad applications. The charge carrier mobility of polymer-based OFETs has been improved from 10–5 to more than 10 cm2 V–1 s–1 over the past three decades. With the carrier mobility close to or higher than that of amorphous silicon, the application fields of polymer-based OFETs have been extended from sensing to logic or drive circuits. During OFET operation, the charge carriers are successively injected in and then transferred across the semiconducting channel under an external electric field. The behavior of the charge carriers is determined by both charge injection and charge transport. Well-matched frontier molecular orbital (FMO) energy levels and optimized hierarchical structures of semiconducting polymers are essential for the realization of high-performance polymer-based OFETs.In this Account, we mainly demonstrate our recent progress in molecular design strategies and fabrication processing methods for high-performance semiconducting polymers. Moreover, we provide some examples of integrated applications of polymer-based OFETs. The convenient FMO energy level modulation and excellent molecular designability of donor–acceptor (D–A) conjugated polymers facilitate studies on their performance enhancement in OFETs. Proper molecular design of the D–A polymer backbone and side chain can significantly contribute to charge injection enhancement, transport pathway establishment, and trap reduction, thereby resulting in efficient charge transport. Moreover, special fabrication processes of OFET devices can further enhance the charge transport by optimizing the hierarchical structures of semiconducting polymers, thereby enhancing their carrier mobility and stability. By employing high-performance semiconducting polymers as the semiconducting channel of OFETs, various applications can be implemented. These applications range from small-scale logic signal processing and periodic signal generation to complex visual perception systems, indicating broad application prospects in human life. The works on performance improvement and functional utilization of the semiconducting polymers in OFETs might provide insights for molecular design strategies and applications for future plastic electronics.