Layered thio- and seleno-phosphate ferroelectrics, such as CuInP₂S₆, are promising building blocks for next-generation nonvolatile memory devices. However, because of the low Curie point, the CuInP₂S₆-based memory devices suffer from poor thermal stability (<42 °C). Here, exploiting the electric field-driven phase transition in the rarely studied antiferroelectric CuCrP₂S₆ crystals, we develop a nonvolatile memristor showing a sizable resistive-switching ratio of ~ 1000, high switching endurance up to 20,000 cycles, low cycle-to-cycle variation, and robust thermal stability up to 120 °C. The resistive switching is attributed to the ferroelectric polarization-modulated thermal emission accompanied by the Fowler–Nordheim tunneling across the interfaces. First-principles calculations reveal that the good device performances are associated with the exceptionally strong ferroelectric polarization in CuCrP₂S₆ crystal. Furthermore, the typical biological synaptic learning rules, such as long-term potentiation/depression and spike amplitude/spike time-dependent plasticity, are also demonstrated. The results highlight the great application potential of van der Waals antiferroelectrics in high-performance synaptic devices for neuromorphic computing.

层状硫代磷酸盐和硒代磷酸盐铁电体，例如 CuInP ₂ S ₆ ，是有前途的下一代非易失性存储器件的构建模块。然而，由于居里点较低，CuInP ₂ S ₆基存储器件的热稳定性较差（<42 id=27>2 S ₆晶体，我们开发了一种非易失性忆阻器，其电阻切换比约为 1000 、高达 20,000 次循环的高开关耐久性、低循环变化以及高达 120°C 的强大热稳定性电阻开关归因于铁电极化调制热发射以及界面上的福勒-诺德海姆隧道效应。第一原理计算表明，良好的器件性能与 CuCrP ₂ S ₆晶体中异常强的铁电极化有关，此外，典型的生物突触学习规则，例如长期增强/抑制和尖峰幅度/尖峰时间。研究结果还证明了范德华反铁电体在神经形态计算的高性能突触设备中的巨大应用潜力。