Semiconducting pi-conjugated polymers are the most promising candidates for flexible electronics owing to their facile processability and mechanical robustness; however, achieving steep and stable switching operations in polymer thin-film transistors (TFTs) remains a serious challenge. Herein, it is shown that whole optimizations for eliminating interfacial carrier traps throughout the conductive path are necessary in achieving TFTs showing both exceptionally sharp switching and bias-stress-free characteristics. Inverted-coplanar-type TFTs composed of a highly lyophobic amorphous perfluoropolymer gate-dielectric interfaced with a push-coated semiconducting polymer layer are manufactured. The use of the dielectric allows the establishment of bias-stress-free characteristics with minimized contact resistance. Additionally, fairly sharp on/off switching TFTs with the smallest normalized subthreshold swing can be obtained by utilizing a particular donor-acceptor copolymer that involves a self-passivation mechanism working to achieve a trap-minimized interface. These findings have opened a way for low-power and robust device operations in polymer-based flexible electronics.
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