Over 60 h of Stable Water-Operation for N-Type Organic Electrochemical Transistors with Fast Response and Ambipolarity

Organic electrochemical transistors (OECTs) are of great interest in low-power bioelectronics and neuromorphic computing, as they utilize organic mixed ionic-electronic conductors (OMIECs) to transduce ionic signals into electrical signals. However, the poor environmental stability of OMIEC materials significantly restricts the practical application of OECTs. Therefore, the non-fused planar naphthalenediimide (NDI)-dialkoxybithiazole (2Tz) copolymers are fine-tuned through varying ethylene glycol (EG) side chain lengths from tri(ethylene glycol) to hexa(ethylene glycol) (namely P-XO, X = 3-6) to achieve OECTs with high-stability and low threshold voltage. As a result, the NDI-2Tz copolymers exhibit ambipolarity, rapid response (<10 ms), and ultra-high n-type stability. Notably, the P-6O copolymers display a threshold voltage as low as 0.27 V. They can operate in n-type mode in an aqueous solution for over 60 h, maintaining an on-off ratio of over 10. This work sheds light on the design of exceptional n-type/ambipolar materials for OECTs. It demonstrates the potential of incorporating these ambipolar polymers into water-operational integrated circuits for long-term biosensing systems and energy-efficient brain-inspired computing.