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 (HfO2) dielectrics that promote tunable synaptic behavior in transistor-based electronics. By incorporating sodium fluoride (NaF) into electrochemically exfoliated hafnium disulfide (HfS2) nanosheets, followed by thermal oxidation, a uniform, ultrathin (≈8 nm) HfO2 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 HfO2-based devices exhibiting short-term switching behavior and NaF-incorporated HfO2 (NaF-HfO2)-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.
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