Redox-based memristive devices have shown great potential for application in neuromorphic computing systems. However, the demands on the device characteristics depend on the implemented computational scheme and unifying the desired properties in one stable device is still challenging. Understanding how and to what extend the device characteristics can be tuned and stabilized is crucial for developing application specific designs. Here, we present memristive devices with a functional trilayer of HfOx/Al2O3/TiO2 tailored by the stoichiometry of HfOx (x = 1.8, 2) and the operating conditions. The device properties are experimentally analyzed, and a physics-based device model is developed to provide a microscopic interpretation and explain the role of the Al2O3 layer for a stable performance. Our results demonstrate that the resistive switching mechanism can be tuned from area type to filament type in the same device, which is well explained by the model: the Al2O3 layer stabilizes the area-type switching mechanism by controlling the formation of oxygen vacancies at the Al2O3/HfOx interface with an estimated formation energy of ≈ 1.65 ± 0.05 eV. Such stabilized area-type devices combine multi-level analog switching, linear resistance change, and long retention times (≈ 107–108 s) without external current compliance and initial electroforming cycles. This combination is a significant improvement compared to previous bilayer devices and makes the devices potentially interesting for future integration into memristive circuits for neuromorphic applications.

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