Enhanced Switching Performance in Single‐Crystalline PbTiO₃ Ferroelectric Memristors for Replicating Synaptic Plasticity

A large ON/OFF ratio in a memristor provides reliable state distinction, enabling precise weight updates to emulate synaptic plasticity. A well‐reproduced ferroelectric polarization in the perovskite oxide single layer obtained by growing high‐quality single crystals plays an important role in elevating the ON/OFF ratio. Herein, a single‐crystalline PbTiO 3 ‐based ferroelectric memristor is demonstrated, and structural investigations confirm its extremely sharp interface, well‐ordered lattice structure, and epitaxial growth. Pt/PbTiO 3 /Nb:SrTiO 3 metal–ferroelectric–semiconductor memristors exhibit promising resistive switching properties, including high repeatability, good endurance, long retention, and a larger ON/OFF ratio >10 5 (stable over 1200 for retention), which is larger than that of most single‐layer BaTiO 3 and BiFeO 3 memristors. PbTiO 3 ‐based memristors effectively mimic key synaptic plasticity, including spike‐amplitude‐dependent plasticity, paired‐pulse facilitation/depression, spike‐rate‐dependent plasticity, short‐term memory, transition from short‐term memory to long‐term memory, long‐term memory, and spike‐timing‐dependent plasticity. These have been systematically investigated based on stable pulse training on resistance modulations. Simulations of neuromorphic computing for different neuron network structures achieved pattern recognition rates of approximately 92%–96%, indicating high accuracy and versatility. This paper introduces an effective and straightforward strategy for enhancing the ON/OFF ratio of ferroelectric PbTiO 3 memristors, reinforcing their potential for use in hardware‐based neural networks.