Dual Redox‐Active Iron‐Based Metal–Organic Network for Digital‐Analog Memristors

ABSTRACT

Molecular memristors have shown great potential for digital memory and analog computing applications. However, developing molecular active layers with controllable structures and stable electrical properties remains challenging. Here, we employ a triphenylamine centered three armed terpyridine ligand (TPA‐(TPy) ₃ ) to construct a two‐dimensional (2D) iron based metal–organic network (Fe‐MON) film through interfacial coordination assembly. The three‐armed molecular topology promotes lateral network growth, enabling the formation of continuous and robust Fe‐MON films. In contrast, the structurally analogous two‐armed ligand (TPA‐(TPy) ₂ ) fails to generate continuous networks, resulting in inferior device stability. The resulting Al/Fe‐MON/ITO memristors exhibit reliable digital resistive switching characteristics with narrow ON/OFF voltage distributions, good retention, and endurance. Moreover, the synergistic redox activity of triphenylamine and Fe ²⁺ /Fe ³⁺ centers enables continuous conductance modulation under pulse stimulation, achieving 64 distinguishable multilevel conductance states. By integrating these conductance states into a convolutional neural network (CNN), the system achieves 96.57% accuracy in flower image recognition. This work demonstrates the capability of 2D metal–organic network films for digital‐analog dual‐mode memristors.