Complementary circuits based on organic electrochemical transistors (OECTs) are attractive for the development of inexpensive and disposable point-ofcare bioelectronic devices. Ambipolar OECTs, which employ a single channel material, could decrease the fabrication complexity and manufacturing costs of such circuits. An ideal channel material for ambipolar OECTs should be electrochemically stable in aqueous environments, afford facile ion insertion for both cations and anions, and also facilitate high and balanced electron and hole transport. In this study, triethylene glycol functionalized diketopyrrolopyrrole (DPP)-based polymer is proposed for the development of ambipolar OECTs. It is shown that DPP-based OECTs have a high and comparable figure of merit for both n-and p-type operations. Logic NOT, NAND, and NOR operations with corresponding complementary circuits constructed from identical DPP-based OECT devices are demonstrated. This study is an important step toward the development of sophisticated complementary metal-oxidesemiconductor-like logic circuits using single-component OECTs.
Electrochemical doping is central to a host of important applications such as bio-sensing, neuromorphic computing and charge storage. However, the mechanisms that enable electrochemical dopability and the various parameters that control doping efficiencies are poorly understood. Here, employing complementary electrochemical and spectroelectrochemical measurements, we report a charge-polarity dependent ion insertion asymmetry in a diketopyrrolopyrrole-based ambipolar π-conjugated polymer. We argue that electrostatic interactions are insufficient to fully account for the observed charge-specific ion insertion into the polymer matrix. Using polymer side-chain dependent electrochemical doping studies, we show that electron density donating and accepting tendencies of polymer side-chains sufficiently describe the observed charge-polarity dependent electrochemical doping. Our observations are akin to the solvation of dopant ions by polymer side-chains. We propose that Gutmann donor/acceptor number framework qualifies the ‘solvent-like’ properties of polymer side-chains and provides a rational basis for designing π-conjugated polymers with favorable mixed ionic electronic transport properties.
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