Hydrogen‐Associated Filling‐Controlled Mottronics Within Thermodynamically Metastable Vanadium Dioxide

作者：Xuanchi Zhou, Yongjie Jiao, Wentian Lu, Jinjian Guo, Xiaohui Yao, Jiahui Ji, Guowei Zhou, Huihui Ji, Zhe Yuan, Xiaohong Xu · 发表于：Advanced Science · 年份：2025 · DOI：10.1002/advs.202414991 · 被引用次数：12 · 研究领域：Transition Metal Oxide Nanomaterials、Gas Sensing Nanomaterials and Sensors、Copper-based nanomaterials and applications

Abstract The discovery of hydrogen‐associated topotactic phase modulations in correlated oxide system has emerged as a promising paradigm to explore exotic electronic states and physical functionality. Here hydrogen‐induced Mott phase transitions are demonstrated for metastable VO 2 (B) toward new electron‐itinerant hydrogenated phases via introducing non‐equilibrium condition, delicately delivering a rich spectrum of hydrogen‐associated electronic states. Of particular interest, the highly robust but reversible hydrogenated phase achievable in metastable VO 2 (B) significantly benefits protonic device applications, which is in contrast with well‐known VO 2 (M1), where the metallic hydrogenated phase readily turns into insulating state with extensive hydrogen doping. Establishing correlated VO 2 at metastable status fundamentally surpasses the thermodynamic restrictions to expand the adjustability in their electronic structure, giving rise to new electronic states and a superior resistive switching of 10 2 –10 5 to the counterparts in widely‐reported VO 2 (M1). Utilizing the theoretical calculations and synchrotron radiation analysis, the hydrogen‐associated phase modulation in metastable VO 2 (B) is dominantly driven by band‐filling‐controlled orbital reconfiguration, while the concurrent structural evolution unveils a strong ion‐electron‐lattice coupling. The present work provides fundamentally new tuning knob for adjusting the energy landscape of electron‐correlated system...