Monolithically‐Integrated van der Waals Synaptic Memory via Bulk Nano‐Crystallization

Monolithically‐integrated van der Waals synaptic memory is presented via bulk nano‐crystallization, which overcomes the conventional limitations of 3D device integration technologies. Furthermore, bipolar resistive switching (LRS/HRS) dynamics is spatially resolved with conductive atomic force microscopy, scanning‐transmission electron microscopy, and X‐ray photoelectron spectroscopy. The monolithic‐integrated 1S1R device exhibits the low leakage currents, robust switching ratios, and reliable bipolar memory states with synaptic response. The monolithically‐integrated resistive memory will offer the generalizable platform for next‐generation 3D integrated neuromorphic device and edge‐computing AI hardware. Abstract Owing to the evolution of data‐driven technologies, including the large language models, generative artificial intelligence, autonomous driving, and the internet of things requires advanced memory technology. However, conventional memory device structures and fabrication process have significant limitations for high‐density integration. Herein, this study reports the monolithically‐integrated 1‐selector and 1‐resistive (1S1R) synaptic memory in van der Waals (vdW) heterostructure, which overcomes the conventional limitations of device integration technologies. Single‐step direct synthesis of vdW heterostructure and its corresponding 1S1R cell is fabricated via plasma‐enhanced lattice‐distortion. Scanning‐transmission electron microscopy, and X‐ray photoelectron spectroscopy are correlatively applied to observe the effects of plasma‐enhanced nano‐crystallization of bulk vdW VSe2. Furthermore, bipolar resistive switching dynamics have been spatially resolved with conductive atomic force microscopy. Furthermore, the artificial vdW heterostructure exhibits the synaptic functionality with interfacial charge accumulation at the 2D/3D interface, enabling linear weight updates across multiple resistance states with minimal nonlinearity. In conclusion, it envision that the monolithically‐integrated 1S1R cell can offers a systematic device platform for next‐generation vdW electronics and its corresponding monolithic 3D integration. Monolithically-integrated van der Waals synaptic memory is presented via bulk nano-crystallization, which overcomes the conventional limitations of 3D device integration technologies. Furthermore, bipolar resistive switching (LRS/HRS) dynamics is spatially resolved with conductive atomic force microscopy, scanning-transmission electron microscopy, and X-ray photoelectron spectroscopy. The monolithic-integrated 1S1R device exhibits the low leakage currents, robust switching ratios, and reliable bipolar memory states with synaptic response. The monolithically-integrated resistive memory will offer the generalizable platform for next-generation 3D integrated neuromorphic device and edge-computing AI hardware. Abstract Owing to the evolution of data-driven technologies, including the large language models, generative artificial intelligence, autonomous driving, and the internet of things requires advanced memory technology. However, conventional memory device structures and fabrication process have significant limitations for high-density integration. Herein, this study reports the monolithically-integrated 1-selector and 1-resistive (1S1R) synaptic memory in van der Waals (vdW) heterostructure, which overcomes the conventional limitations of device integration technologies. Single-step direct synthesis of vdW heterostructure and its corresponding 1S1R cell is fabricated via plasma-enhanced lattice-distortion. Scanning-transmission electron microscopy, and X-ray photoelectron spectroscopy are correlatively applied to observe the effects of plasma-enhanced nano-crystallization of bulk vdW VSe 2. Furthermore, bipolar resistive switching dynamics have been spatially resolved with conductive atomic force microscopy. Furthermore, the artificial vdW heterostructure exhibits the synaptic functionality with interfacial charge accumulation at the 2D/3D interface, enabling linear weight updates across multiple resistance states with minimal nonlinearity. In conclusion, it envision that the monolithically-integrated 1S1R cell can offers a systematic device platform for next-generation vdW electronics and its corresponding monolithic 3D integration. Advanced Science, Volume 12, Issue 43, November 20, 2025.