Donor Engineering Tuning the Analog Switching Range and Operational Stability of Organic Synaptic Transistors for Neuromorphic Systems

Organic artificial synapses are becoming the most desirable format for neuromorphic computing due to their highly tunable resistive states. However, repressively low analog switching range, inferior memory retention, and operational instability greatly hinder the further development of organic synapses. Herein, two donor‐acceptor copolymers consisting of electron‐deficient isoindigo coupled with variable donating moieties for three‐terminal organic synaptic transistors (TOSTs) are reported. It is found that the synaptic function and device stability of TOSTs are significantly improved by enhancing the electron‐donating strength of donor units. Polymer alkylated isoindigo‐bis‐ethylenedioxythiophene exhibits high analog switching range of 170 ×, two orders of magnitude higher than that of normal organic neuromorphic devices. They also demonstrate excellent memory retention of over 5 × 103 s, low switching energy of 13 fJ, and ultrahigh operational stability with 99% of its original current after 100 000 write‐read events in air. Furthermore, the high viability of strong donor strategy is showcased by demonstrating flexible TOSTs with stable synaptic function after repeated mechanical bending as well as organic synapses capable of simulating image information processing. Overall, this work highlights the advantages of the strong donor functionalization strategy to boost the synaptic performance and device stability of TOSTs. Two isoindigo based copolymers coupled with variable electron‐donating companion moieties are used for three‐terminal organic synaptic transistors. Enhancing the electron‐donating strength of donor units leads to improved analog switching range, memory retention, and operational stability of the device. Through strong donor strategy, organic synaptic devices can access desirable performance metrics in neuromorphic applications.