Photoelectric Multilevel Memory Device based on Covalent Organic Polymer Film with Keto–Enol Tautomerism for Harsh Environments Applications

Abstract Covalent organic polymers (COPs) memristors with multilevel memory behavior in harsh environments and photoelectric regulation are crucial for high‐density storage and high‐efficiency neuromorphic computing. Here, a donor–acceptor (D–A)‐type COP film (Py‐COP‐3), which is initiated by keto–enol tautomerism, is proposed for high‐performance memristors. Satisfactorily, the indium tin oxide (ITO)/Py‐COP‐3/Ag device demonstrates multilevel memory performance, even in high temperatures, acid‐base corrosion, and various organic solvents. Moreover, the performance can be modulated by the photoelectric effect to maintain a great switching behavior. By contrast, Py‐COP‐0, with similar structure and chemical composition to Py‐COP‐3 but without keto–enol tautomerism, exhibits binary storage performance. Further studies unravel that both the formation of conductive filaments and charge transfer within D‐A Py‐COP‐3 film contribute to the resistive switching behavior of memory devices.