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Abstract Emerging non-volatile memristor-based devices with resistive switching (RS) materials are being widely researched as promising contenders for the next generation of data storage and neuromorphic technologies. Titanium nitride (TiN_x) is a common industry-friendly electrode system for RS; however, the precise TiN_xproperties required for optimum RS performance is still lacking. Herein, using ion-assisted DC magnetron sputtering, we demonstrate the key importance not only of engineering the TiN_xbottom electrodes to be dense, smooth, and conductive, but also understoichiometric in N. With these properties, RS in HfO₂-based memristive devices is shown to be optimised for TiN_0.96. These devices have switching voltages ≤ ±1 V with promising device-to-device uniformity, endurance, memory window of ~40, and multiple non-volatile intermediate conductance levels. This study highlights the importance of precise tuning of TiN_xbottom electrodes to achieve robust performance of oxide resistive switching materials. 

Resistive switching devices are promising candidates for the next generation of nonvolatile memory and neuromorphic computing applications. Despite the advantages in retention and on/off ratio, filamentary-based memristors still suffer from challenges, particularly endurance (flash being a benchmark system showing 10⁴to 10⁶ cycles) and uniformity. Here, we use WO₃as a complementary metal-oxide semiconductor–compatible switching oxide and demonstrate a proof-of-concept materials design approach to enhance endurance and device-to-device uniformity in WO₃-based memristive devices while preserving other performance metrics. These devices show stable resistive switching behavior with >10⁶ cycles, >10⁵-second retention, >10 on/off ratio, and good device-to-device uniformity, without using current compliance. All these metrics are achieved using a one-step pulsed laser deposition process to create self-assembled nanocomposite thin films that have regular guided filaments of ≈100-nanometer pitch, preformed between WO₃grains and interspersed smaller Ce₂O₃grains. 

Highly promising performance for future computing applications is achieved based on a new materials design. 

Here, in ionically conducting Na 0.5 Bi 0.5 TiO 3 (NBT), we explore the link between growth parameters, stoichiometry and resistive switching behavior and show NBT to be a highly tunable system. We show that the combination of oxygen ionic vacancies and low-level electronic conduction is important for controlling Schottky barrier interfacial switching. We achieve a large ON/OFF ratio for high resistance/low resistance ( R HRS / R LRS ), enabled by an almost constant R HRS of ∼10 9 Ω, and composition-tunable R LRS value modulated by growth temperature. R HRS / R LRS ratios of up to 10 4 and pronounced resistive switching at low voltages (SET voltage of <1.2 V without high-voltage electroforming), strong endurance (no change in resistance states after several 10 3 cycles), uniformity, stable switching and fast switching speed are achieved. Of particular interest is that the best performance is achieved at the lowest growth temperature studied (600 °C), which is opposite to the case of most other perovskite oxides for memristors, where higher growth temperatures are required for optimum performance. This is understood based on the oxygen vacancy control of interfacial switching in NBT, whereas a range of other mechanisms (including filamentary switching) occur in other perovskites. The study of NBT has enabled us to determine key parameters for achieving high performance memristors. 

Abstract Defect engineering in valence change memories aimed at tuning the concentration and transport of oxygen vacancies are studied extensively, however mostly focusing on contribution from individual extended defects such as single dislocations and grain boundaries. In this work, the impact of engineering large numbers of grain boundaries on resistive switching mechanisms and performances is investigated. Three different grain morphologies, that is, “random network,” “columnar scaffold,” and “island‐like,” are realized in CeO₂thin films. The devices with the three grain morphologies demonstrate vastly different resistive switching behaviors. The best overall resistive switching performance is shown in the devices with “columnar scaffold” morphology, where the vertical grain boundaries extending through the film facilitate the generation of oxygen vacancies as well as their migration under external bias. The observation of both interfacial and filamentary switching modes only in the devices with a “columnar scaffold” morphology further confirms the contribution from grain boundaries. In contrast, the “random network” or “island‐like” structures result in excessive or insufficient oxygen vacancy concentration migration paths. The research provides design guidelines for grain boundary engineering of oxide‐based resistive switching materials to tune the resistive switching performances for memory and neuromorphic computing applications. 

Abstract Interface‐type (IT) resistive switching (RS) memories are promising for next generation memory and computing technologies owing to the filament‐free switching, high on/off ratio, low power consumption, and low spatial variability. Although the switching mechanisms of memristors have been widely studied in filament‐type devices, they are largely unknown in IT memristors. In this work, using the simple Au/Nb:SrTiO₃(Nb:STO) as a model Schottky system, it is identified that protons from moisture are key element in determining the RS characteristics in IT memristors. The Au/Nb:STO devices show typical Schottky interface controlled current–voltage (I–V) curves with a large on/off ratio under ambient conditions. Surprisingly, in a controlled environment without protons/moisture, the largeI–Vhysteresis collapses with the disappearance of a high resistance state (HRS) and the Schottky barrier. Once the devices are re‐exposed to a humid environment, the typical largeI–Vhysteresis can be recovered within hours as the HRS and Schottky interface are restored. The RS mechanism in Au/Nb:STO is attributed to the Schottky barrier modulation by a proton assisted electron trapping and detrapping process. This work highlights the important role of protons/moisture in the RS properties of IT memristors and provides fundamental insight for switching mechanisms in metal oxides‐based memory devices.