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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. 

Abstract A variety of mechanisms are reported to play critical roles in contributing to the high carrier/electron mobility in oxide/SrTiO₃(STO) heterostructures. By using La_0.95Sr_0.05TiO₃(LSTO) epitaxially grown on different single crystal substrates (such as STO, GdScO₃, LaAlO₃, (LaAlO₃)_0.3(Sr₂AlTaO₆)_0.7, and CeO₂buffered STO) as the model systems, the formation of a conducting substrate surface layer (CSSL) on STO substrate is shown at relatively low growth temperature and high oxygen pressure (725 °C, 5 × 10^–4 Torr), which contributes to the enhanced conductivity of the LSTO/STO heterostructures. Different from the conventional oxygen vacancy model, this work reveals that the formation of the CSSL occurs when growing an oxide layer (LSTO in this case) on STO, while neither annealing nor the growth of an Au layer alone at the exact same growth condition generates the CSSL in STO. It demonstrates that the oxide layer actively pulls oxygen from STO substrate at given growth conditions, leading to the formation of the CSSL. The observations emphasize the oxygen transfer across film/substrate interface during the synthesis of oxide heterostructures playing a critical role in functional properties.