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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. 

Sneak path current is a fundamental issue and a major roadblock to the wide application of memristor crossbar arrays. Traditional selectors such as transistors compromise the 2D scalability and 3D stack‐ability of the array, while emerging selectors with highly nonlinear current–voltage relations contradict the requirement of a linear current–voltage relation for efficient multiplication by directly using Ohm's law. Herein, the concept of a timing selector is proposed and demonstrated, which addresses the sneak path issue with a voltage‐dependent delay time of its transient switching behavior, while preserving a linear current–voltage relationship for computation. Crossbar arrays with silver‐based diffusive memristors as the timing selectors are built and the operation principle and operational windows are experimentally demonstrated. The timing selector enables large memristor crossbar arrays that can be used to solve large‐dimension real‐world problems in machine intelligence and neuromorphic computing.