In this study, a high-performance bio-organic memristor with a crossbar array structure using milk as a resistive switching layer (RSL) is proposed. To ensure compatibility with the complementary metal oxide semiconductor process of milk RSL, a high-k Ta2O5 layer was deposited as a capping layer; this layer enables high-density, integration-capable, photolithography processes. The fabricated crossbar array memristors contain milk–Ta2O5 hybrid membranes, and they exhibit bipolar resistance switching behavior and uniform resistance distribution across hundreds of repeated test cycles. In terms of the artificial synaptic behavior and synaptic weight changes, milk–Ta2O5 hybrid crossbar array memristors have a stable analog RESET process, and the memristors are highly responsive to presynaptic stimulation via paired-pulse facilitation excitatory post-synaptic current. Moreover, spike-timing-dependent plasticity and potentiation and depression behaviors, which closely emulate long-term plasticity and modulate synaptic weights, were evaluated. Finally, an artificial neural network was designed and trained to recognize the pattern of the Modified National Institute of Standards and Technology (MNIST) digits to evaluate the capability of the neuromorphic computing system. Consequently, a high recognition rate of over 88% was achieved. Thus, the milk–Ta2O5 hybrid crossbar array memristor is a promising electronic platform for in-memory computing systems.
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