High Performing Ambipolar Organic Electrochemical Transistors and Solid‐State Inverters Enabled by Hydrophilic/Hydrophobic Side Chains Integration

Progress in solid-state organic electrochemical transistors (SS-OECTs) and complementary circuits is limited by the lack of high-performance single component ambipolar mixed ionic-electronic conductors (AMIECs). Herein, two DPP-V-based terpolymers, p(gDPP-V-B05) and p(gDPP-V-B20) are designed, featuring an ambipolar backbone and tunable integrated hydrophilic/hydrophobic side-chain engineering to optimize mixed conduction. Both polymers exhibited state-of-the-art ambipolar performance in aqueous OECTs, with p(gDPP-V-B05) demonstrating the record µC* values of 384.8 F cm^-1 V^-1 s^-1 (n-type) and 691.7 F cm^-1 V^-1 s^-1 (p-type), along with a state-of-the-art normalized transconductance of 72.6 S cm^-1for n-type. These exceptional performances are attributed to the synergistic enhancement of electronic mobility and optimized ion capacity. Aqueous inverters based on single-component p(gDPP-V-B05) delivered a high voltage gain of 393 V V^-1, benefiting from well-balanced n/p-type characteristics. Notably, this material also enabled high-performing SS-OECTs, which retained strong transconductance and current output, and exhibited typical antiambipolar behavior. Furthermore, single-component solid-state inverters (SS-inverters) achieved a record-high voltage gain of 163 V V^-1, representing the first SS-inverters based on AMIECs and the highest value reported for SS-inverter systems to date. These results underscore the effectiveness of the molecular design strategy and highlight the promise of ambipolar polymeric mixed ionic-electronic conductors (PMIECs) for scalable, solid-state, bio-integrated electronic circuits.