In this study, bilayer TiO2/CoFe2O4 films were fabricated on Pt/Ti/SiO2/Si substrates via sol-gel spin-coating process. The bilayer films demonstrated resistance switching (RS) behavior, showing improved forming voltage distribution and consistent Set/Reset voltages. Additionally, the bilayer structure exhibited excellent cycling endurance and retention properties compared to pure CoFe2O4 and pure TiO2 films. Meanwhile, the TiO2/CoFe2O4 thin-film devices also displayed the capability to emulate various forms of synaptic plasticity as artificial synapses, demonstrating enhanced or inhibited behaviors through the modulation of pulse intervals and durations, which implied realization of both multi-level storage and synaptic functions in a single device. The underlying conduction mechanism is believed to involve ohmic conduction in the low-resistance state (LRS), while the high-resistance state (HRS) is governed by high-field Schottky emission combined with space-charge-limited current effects The resistance switching mechanism is believed to be driven by the creation and breakdown of conductive filaments composed of oxygen vacancies. Importantly, an increase in the film's saturation magnetization was observed after the forming process, regardless of whether it was in the HRS or LRS, compared to its initial fresh state. This phenomenon is caused by changes in the oxygen vacancy concentration due to resistance switching behavior, indicating simultaneous correlation between oxygen-vacancy modulation and magnetic variation. Overall, these findings suggest that bilayer TiO2/CoFe2O4 thin films hold significant promise for applications in resistive random access memory technology.
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