Abstract

As traditional memory technologies approach their physical and scaling limits, new materials and mechanisms are urgently needed to enable next-generation memory and neuromorphic computing. Ferroelectric materials, especially in two-dimensional (2D) van der Waals form, offer unique advantages due to their non-volatility, low power consumption, and compatibility with ultrathin integration. This work focuses on the development and application of van der Waals antiferroelectric CuCrP₂S₆ for memristive devices. Three main advances are presented: 1) We demonstrate that CuCrP₂S₆, previously regarded as antiferroelectric, can be electrically switched into a ferroelectric phase with robust polarization even down to atomic thickness, stable up to 200 °C. Based on this, we build the first van der Waals antiferroelectric-based memristor and reveal its synaptic-like behavior through nanoscale domain evolution. 2) To enable scalable integration, we design and fabricate a fully 2D ferroelectric one-transistor–one-memristor (1T1M) heterostructure by stacking CuCrP₂S₆, MoS₂, and h-BN. This architecture achieves low leakage current, high tunability, and effectively suppresses sneak path currents, which addresses major challenges in memristor arrays. 3) We further enhance memristive performance through nanodomain engineering, achieved by composition tuning in CuInP₂(S_1−xSe_x)₆. Smaller domain sizes lower the switching energy and enable smoother stepwise conductance modulation, which is desirable for neuromorphic computing. These studies significantly expand the available material options beyond existing candidates and provide pathways for designing and integrating low-dimensional materials into memory and neuromorphic systems.