Unraveling Polymer–Ion Interactions in Electrochromic Polymers for their Implementation in Organic Electrochemical Synaptic Devices

Abstract

Owing to low‐power, fast and highly adaptive operability, as well as scalability, electrochemical random‐access memory (ECRAM) technology is one of the most promising approaches for neuromorphic computing based on artificial neural networks. Despite recent advances, practical implementation of ECRAMs remains challenging due to several limitations including high write noise, asymmetric weight updates, and insufficient dynamic ranges. Here, inspired by similarities in structural and functional requirements between electrochromic devices and ECRAMs, high‐performance, single‐transistor and neuromorphic devices based on electrochromic polymers (ECPs) are demonstrated. To effectively translate electrochromism into electrochemical ion memory in polymers, this study systematically investigates polymer–ion interactions, redox activity, mixed ionic–electronic conduction, and stability of ECPs both experimentally and computationally using select electrolytes. The best‐performing ECP‐electrolyte combination is then implemented into an ECRAM device to further explore synaptic plasticity behaviors. The resulting ECRAM exhibits high linearity and symmetric conductance modulation, high dynamic range (≈1 mS or ≈6x), and high training accuracy (>84% within five training cycles on a standard image recognition dataset), comparable to existing state‐of‐the‐art ECRAMs. This study offers a promising approach to discover and design novel polymer materials for organic ECRAMs and demonstrates potential applications, taking advantage of mature knowledge basis on electrochromic materials and devices.

Robust Chemiresistive Behavior in Conductive Polymer/MOF Composites

“…We select the ProDOT‐BTD c P for its reversible redox‐activity, low onset oxidation voltage, charge capacity, electrical conductivity to enhance the device response in presence of the analyte. [ 32,33 ] Particularly, the c P is designed to serve as a secondary NO 2 ‐affine component endowed by its polar sidechains, [ 34–37 ] as well as a binding matrix to physically unify c MOF crystallites and improve electrical communication throughout the bulk (Figure 1c,d). We then select two classes of c MOFs based on HHTP and HITP ligands (Figure 1a), which typically exhibit irreversible gas sensing behaviors in their pristine form.…”

Ultrasoft and High-Adhesion Block Copolymers for Neuromorphic Computing

“…Traditional computing faces the “von Neumann bottleneck”, , resulting from the storage-processing division. Scientists draw inspiration from the brain’s operations to build a new computing system . This innovative system incorporates artificial synapses, paving the way for the next generation of energy-efficient, brain-like computers capable of efficient data processing. − Currently, various synaptic devices, including two- and three-terminal configurations, have been engineered to mimic synaptic functionality. , Among these, three-terminal transistors stand out due to their ability to reduce crosstalk and seamlessly integrate with diverse circuits, making them ideal for neural morphology applications .…”

Preparation of PANI/CuPc/PDMS Composite Elastomer with High Dielectric Constant and Low Modulus Assisted by Electric Fields

“…Electroactive polymers (EAPs) can be divided into ionic EAPs and electronic EAPs according to their driving mechanisms [ 1 , 2 , 3 ]. Ionic EAPs respond to the electric field by the diffusion of ions in the material, which requires an electrolyte environment to work, and hence, limits their applications in dry or extreme environments [ 4 , 5 ]. Compared with ionic EAPs, electronic EAPs have the advantages of a wide linear response range, high flexibility, long life, good reliability, and high efficiency [ 6 , 7 ].…”