Effect of Alkyl Side Chain Length on Electrical Performance of Ion-Gel-Gated OFETs Based on Difluorobenzothiadiazole-Based D-A Copolymers

The performance of organic field-effect transistors (OFETs) is highly dependent on the dielectric-semiconductor interface, especially in ion-gel-gated OFETs, where a significantly high carrier density is induced at the interface at a low gate voltage. This study investigates how altering the alkyl side chain length of donor-acceptor (D-A) copolymers impacts the electrical performance of ion-gel-gated OFETs. Two difluorobenzothiadiazole-based D-A copolymers, PffBT4T-2OD and PffBT4T-2DT, are compared, where the latter features longer alkyl side chains. Although PffBT4T-2DT shows a 2.4-fold enhancement of charge mobility in the SiO₂-gated OFETs compared to its counterpart due to higher crystallinity in the film, PffBT4T-2OD outperforms PffBT4T-2DT in the ion-gel-gated OFETs, manifested by an extraordinarily high mobility of 17.7 cm²/V s. The smoother surface morphology, as well as stronger interfacial interaction between the ion-gel dielectric and PffBT4T-2OD, enhances interfacial charge accumulation, which leads to higher mobility. Furthermore, PffBT4T-2OD is blended with a polymeric elastomer SEBS to achieve ion-gel-gated flexible OFETs. The blend devices exhibit high mobility of 8.6 cm²/V s and high stretchability, retaining 45% of initial mobility under 100% tensile strain. This study demonstrates the importance of optimizing the chain structure of polymer semiconductors and the semiconductor-dielectric interface to develop low-voltage and high-performance flexible OFETs for wearable electronics applications.