Unveiling Capacitive Coupling and Dynamic Modulation of Memristive Switching in Zn–Al Layered Double Hydroxide Films

To address the demand for rapid, high-density information storage, memristors have garnered significant research interest owing to their structural simplicity, rapid switching speed, and low power consumption. Layered double hydroxides (LDHs), a class of two-dimensional materials, show promise for emerging neuromorphic applications. In this work, we fabricated Zn–Al LDH thin-film memristive devices using a low-cost synthesis route. This layered structure exhibits a unique coupling between capacitive and resistive switching behaviors. Notably, the devices demonstrate sustained current retention even after external bias removal, enabling simultaneous memristive and memcapacitive functionalities. The Zn–Al LDH thin-film memristor (1 μm) exhibits a switching ratio exceeding 10 at a low operating voltage of 0.7 V. Crucially, the device demonstrates robust endurance, maintaining stable switching over 300 write/erase cycles with highly uniform and reproducible hysteresis characteristics. Furthermore, external stimuli (e.g., voltage) induce reversible transitions between capacitively coupled memristive states and pure memristive operation. This capability enhances the feasibility of implementing second-order associative memory circuits, as these neuromorphic devices inherently mimic neural network structures. Consequently, it expands the application potential for “self-generated” memory within neural network architectures.