Alkali Ion‐Incorporated HfO ₂ Dielectrics for Reconfigurable Neuromorphic Computing

Abstract Neuromorphic computing system requires precise control over synaptic retention characteristics to emulate both short‐term and long‐term memory functions of biological neural networks. Here, a solution‐processed approach is presented for the fabrication of alkali metal cation‐embedded hafnium dioxide (HfO 2 ) dielectrics that promote tunable synaptic behavior in transistor‐based electronics. By incorporating sodium fluoride (NaF) into electrochemically exfoliated hafnium disulfide (HfS 2 ) nanosheets, followed by thermal oxidation, a uniform, ultrathin (≈8 nm) HfO 2 film is produced with embedded mobile alkali ions on a wafer‐scale substrate. With a semiconducting indium gallium zinc oxide layer, the resulting transistors demonstrate distinct retention characteristics, with pristine HfO 2 ‐based devices exhibiting short‐term switching behavior and NaF‐incorporated HfO 2 (NaF‐HfO 2 )‐based devices demonstrating long‐term retention exceeding 30 s with tunable synaptic plasticity. It successfully demonstrates the practical application of these ion‐engineered dielectrics in 1‐transistor‐1‐synapse memory arrays, synaptic comparators, and reconfigurable AND/OR logic gates that mimic brain‐like information processing. The solution‐processable approach expands the range of dielectric modification, providing a scalable pathway for next‐generation neuromorphic computing technologies with controllable synaptic functionalities.