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Abstract Mixtures of Ce‐doped rare‐earth aluminum perovskites are drawing a significant amount of attention as potential scintillating devices. However, the synthesis of complex perovskite systems leads to many challenges. Designing the A‐site cations with an equiatomic ratio allows for the stabilization of a single‐crystal phase driven by an entropic regime. This work describes the synthesis of a highly epitaxial thin film of configurationally disordered rare‐earth aluminum perovskite oxide (La_0.2Lu_0.2Y_0.2Gd_0.2Ce_0.2)AlO₃and characterizes the structural and optical properties. The thin films exhibit three equivalent epitaxial domains having an orthorhombic structure resulting from monoclinic distortion of the perovskite cubic cell. An excitation of 286.5 nm from Gd³⁺and energy transfer to Ce³⁺with 405 nm emission are observed, which represents the potential for high‐energy conversion. These experimental results also offer the pathway to tunable optical properties of high‐entropy rare‐earth epitaxial perovskite films for a range of 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.