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Entropic stabilization has evolved into a strategy to create new oxide materials and realize novel functional properties engineered through the alloy composition. Achieving an atomistic understanding of these properties to enable their design, however, has been challenging due to the local compositional and structural disorder that underlies their fundamental structure-property relationships. Here, we combine high-throughput atomistic calculations and linear regression algorithms to investigate the role of local configurational and structural disorder on the thermodynamics of vacancy formation in (MgCoNiCuZn)O-based entropy-stabilized oxides (ESOs) and their influence on the electrical properties. We find that the cation-vacancy formation energies decrease with increasing local tensile strain caused by the deviation of the bond lengths in ESOs from the equilibrium bond length in the binary oxides. The oxygen-vacancy formation strongly depends on structural distortions associated with the local configuration of chemical species. Vacancies in ESOs exhibit deep thermodynamic transition levels that inhibit electrical conduction. By applying the charge-neutrality condition, we determine that the equilibrium concentrations of both oxygen and cation vacancies increase with increasing Cu mole fraction. Our results demonstrate that tuning the local chemistry and associated structural distortions by varying alloy composition acts an engineering principle that enables controlled defect formation in multi-component alloys.

Rapid advances in the semiconductor industry, driven largely by device scaling, are now approaching fundamental physical limits and face severe power, performance, and cost constraints. Multifunctional materials and devices may lead to a paradigm shift toward new, intelligent, and efficient computing systems, and are being extensively studied. Herein examines how, by controlling the internal ion distribution in a solid‐state film, a material's chemical composition and physical properties can be reversibly reconfigured using an applied electric field, at room temperature and after device fabrication. Reconfigurability is observed in a wide range of materials, including commonly used dielectric films, and has led to the development of new device concepts such as resistive random‐access memory. Physical reconfigurability further allows memory and logic operations to be merged in the same device for efficient in‐memory computing and neuromorphic computing systems. By directly changing the chemical composition of the material, coupled electrical, optical, and magnetic effects can also be obtained. A survey of recent fundamental material and device studies that reveal the dynamic ionic processes is included, along with discussions on systematic modeling efforts, device and material challenges, and future research directions.

Memristors have emerged as transformative devices to enable neuromorphic and in‐memory computing, where success requires the identification and development of materials that can overcome challenges in retention and device variability. Here, high‐entropy oxide composed of Zr, Hf, Nb, Ta, Mo, and W oxides is first demonstrated as a switching material for valence change memory. This multielement oxide material provides uniform distribution and higher concentration of oxygen vacancies, limiting the stochastic behavior in resistive switching. (Zr, Hf, Nb, Ta, Mo, W) high‐entropy‐oxide‐based memristors manifest the “cocktail effect,” exhibiting comparable retention with HfO₂‐ or Ta₂O₅‐based memristors while also demonstrating the gradual conductance modulation observed in WO₃‐based memristors. The electrical characterization of these high‐entropy‐oxide‐based memristors demonstrates forming‐free operation, low device and cycle variability, gradual conductance modulation, 6‐bit operation, and long retention which are promising for neuromorphic applications.