Poly Schiff bases embedded polyrotaxane for flexible memristor and artificial synapses

Abstract Poly Schiff bases (PSBs) with tunable conductivity by reversible protonation and deprotonation, are promising memristive materials to mimic ion‐mediated signaling in biological synaptic transmission. However, most PSBs suffer from poor solubility and processability due to the rigid backbones, limiting the fabrication and performance of memristors. Herein, solution‐processable PSB was designed and synthesized by threading the conjugated chain through cyclodextrin macrocycles. The resulting PSB embedded polyrotaxanes based memristors exhibit excellent environmental stability (>8 months) and durability, high ON/OFF ratio (10 7 ), and high‐speed switching (25 ns) with fully addressed resistive switching mechanism. Moreover, the devices demonstrate remarkable mechanical flexibility, and the performance maintains even after 100 bending cycles at a curvature radius of 3 mm. Furthermore, synaptic behaviors such as short‐term, long‐term and spike‐timing‐dependent plasticity were emulated. The memristor was also implemented for image recognition, showing promising potential for neuromorphic computing. This work provides a new strategy to improve the solubility of PSB for flexible and wearable electronics.