Bioinspired High‐Performance Neuromorphic Devices Enabled by Thienoviologen‐Based Electrochemical Ion Gating

Abstract Neuromorphic computing is a bioinspired paradigm that emulates the structure and functionality of biological neural networks, demanding cutting‐edge materials and device architectures. In this work, we present a bioinspired electrochemical neuromorphic device (BEND) utilizing a thienoviologen‐based electrolyte. The incorporation of thiophene groups into the viologen structure (ThV 2+ ) leads to a reduced energy gap, improved radical stability, and enhanced electrochemical activity. The device exhibits excellent ambient stability and continuously tunable conductivity in response to voltage pulse stimulation. When integrated into a convolutional neural network (CNN) for image recognition, BEND achieves an accuracy of nearly 80% on the Fashion‐MNIST dataset. Moreover, the device successfully mimics essential synaptic functions such as spike‐timing‐dependent plasticity (STDP), Pavlovian learning, and supports dual‐terminal logic gate operations. These results significantly expand the functional versatility of viologen‐based materials in neuromorphic electronics and offer new insights into the design of next‐generation electrochemical artificial synapses.