Memristive Baffle Systems: Design, Simulation, and Applications

ABSTRACT Valence change memory (VCM)‐based memristors have emerged as promising artificial synapses for neuromorphic computing, yet their nonlinear conductance modulation and limited endurance remain major bottlenecks. Here, we introduce the baffle system concept into HfO 2 ‐based VCM memristors to regulate oxygen vacancy (V O ) transport and improve both synaptic linearity and cycling reliability. Guided by a multiscale simulation framework that integrates density functional theory calculations and finite element method‐based multiphysics modeling, dual Al 2 O 3 interlayers were strategically incorporated as nanoscale barriers within the HfO 2 matrix to modulate V O migration. The appropriately engineered baffle barriers promote lateral filament growth, enhancing synaptic linearity by up to 43%, while simultaneously confining V O s to achieve over a 60× improvement in endurance. The proposed memristive baffle system provides a practical materials design strategy for precise control of ion transport and filament dynamics, contributing to the development of advanced memristive materials and enhancing their feasibility for neuromorphic applications.