Zwitterionic Fluoropolymer‐Engineered Synaptic Clefts Enhance Ion Dynamics in Neuromorphic OECTs

Abstract Organic electrochemical transistors (OECTs) offer a compelling platform for hardware synapses, yet ion transport through the common semi‐crystalline PVDF‐HFP electrolyte suppresses switching speed and energy efficiency. Here, DPVDF‐SZ, a soft zwitterionic fluoropolymer ion gel engineered by grafting sulfobetaine side chains onto a flexible PVDF‐CTFE backbone, is introduced. Crystallinity drops to ≈3%, and fracture strain rises to 84%. Paired with PEDOT:PSS, DPVDF‐SZ achieves a µC * of 127 F V ⁻¹ s ⁻¹ cm ⁻¹ —where µC * is the product of charge carrier mobility and volumetric capacitance—while tripling transconductance and reducing the threshold voltage by 0.3 V under sub −1.5 V operation. Soft zwitterionic interfaces deliver >90% current retention after 70 pulses, linear bidirectional weight updates across 60 write/erase cycles, and tunable paired‐pulse plasticity. In a 4 × 4 OECT reservoir array, DPVDF‐SZ classifies temporal pulse patterns and reconstructs 16 × 16 images with minimal energy. DPVDF‐SZ‐based OECTs address signal retention and ion migration challenges, enabling efficient neuromorphic systems and potentially bridging AI with biological neural processing.