Hydrogen‐Associated Filling‐Controlled Mottronics Within Thermodynamically Metastable Vanadium Dioxide
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 VO2 (B) toward new el...
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Wiley
2025-04-01
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| Series: | Advanced Science |
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| Online Access: | https://doi.org/10.1002/advs.202414991 |
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| author | Xuanchi Zhou Yongjie Jiao Wentian Lu Jinjian Guo Xiaohui Yao Jiahui Ji Guowei Zhou Huihui Ji Zhe Yuan Xiaohong Xu |
| author_facet | Xuanchi Zhou Yongjie Jiao Wentian Lu Jinjian Guo Xiaohui Yao Jiahui Ji Guowei Zhou Huihui Ji Zhe Yuan Xiaohong Xu |
| author_sort | Xuanchi Zhou |
| collection | DOAJ |
| description | 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 VO2 (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 VO2 (B) significantly benefits protonic device applications, which is in contrast with well‐known VO2 (M1), where the metallic hydrogenated phase readily turns into insulating state with extensive hydrogen doping. Establishing correlated VO2 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 102–105 to the counterparts in widely‐reported VO2 (M1). Utilizing the theoretical calculations and synchrotron radiation analysis, the hydrogen‐associated phase modulation in metastable VO2 (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, advancing the rational design of unachievable electronic states in hydrogen‐related equilibrium phase diagram. |
| format | Article |
| id | doaj-art-dba9625bd637422fa74c60f64f1e8a53 |
| institution | DOAJ |
| issn | 2198-3844 |
| language | English |
| publishDate | 2025-04-01 |
| publisher | Wiley |
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| series | Advanced Science |
| spelling | doaj-art-dba9625bd637422fa74c60f64f1e8a532025-08-20T03:09:08ZengWileyAdvanced Science2198-38442025-04-011214n/an/a10.1002/advs.202414991Hydrogen‐Associated Filling‐Controlled Mottronics Within Thermodynamically Metastable Vanadium DioxideXuanchi Zhou0Yongjie Jiao1Wentian Lu2Jinjian Guo3Xiaohui Yao4Jiahui Ji5Guowei Zhou6Huihui Ji7Zhe Yuan8Xiaohong Xu9Key Laboratory of Magnetic Molecules and Magnetic Information Materials of Ministry of Education & School of Chemistry and Materials Science Shanxi Normal University Taiyuan 030031 ChinaKey Laboratory of Magnetic Molecules and Magnetic Information Materials of Ministry of Education & School of Chemistry and Materials Science Shanxi Normal University Taiyuan 030031 ChinaKey Laboratory of Magnetic Molecules and Magnetic Information Materials of Ministry of Education & School of Chemistry and Materials Science Shanxi Normal University Taiyuan 030031 ChinaKey Laboratory of Magnetic Molecules and Magnetic Information Materials of Ministry of Education & School of Chemistry and Materials Science Shanxi Normal University Taiyuan 030031 ChinaKey Laboratory of Magnetic Molecules and Magnetic Information Materials of Ministry of Education & School of Chemistry and Materials Science Shanxi Normal University Taiyuan 030031 ChinaKey Laboratory of Magnetic Molecules and Magnetic Information Materials of Ministry of Education & School of Chemistry and Materials Science Shanxi Normal University Taiyuan 030031 ChinaKey Laboratory of Magnetic Molecules and Magnetic Information Materials of Ministry of Education & School of Chemistry and Materials Science Shanxi Normal University Taiyuan 030031 ChinaKey Laboratory of Magnetic Molecules and Magnetic Information Materials of Ministry of Education & School of Chemistry and Materials Science Shanxi Normal University Taiyuan 030031 ChinaInstitute for Nanoelectronic Devices and Quantum Computing Fudan University Shanghai 200433 ChinaKey Laboratory of Magnetic Molecules and Magnetic Information Materials of Ministry of Education & School of Chemistry and Materials Science Shanxi Normal University Taiyuan 030031 ChinaAbstract 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 VO2 (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 VO2 (B) significantly benefits protonic device applications, which is in contrast with well‐known VO2 (M1), where the metallic hydrogenated phase readily turns into insulating state with extensive hydrogen doping. Establishing correlated VO2 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 102–105 to the counterparts in widely‐reported VO2 (M1). Utilizing the theoretical calculations and synchrotron radiation analysis, the hydrogen‐associated phase modulation in metastable VO2 (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, advancing the rational design of unachievable electronic states in hydrogen‐related equilibrium phase diagram.https://doi.org/10.1002/advs.202414991correlated oxideshydrogenationmetal‐insulator transitionmetastable materialtopotactic phase modulation |
| spellingShingle | Xuanchi Zhou Yongjie Jiao Wentian Lu Jinjian Guo Xiaohui Yao Jiahui Ji Guowei Zhou Huihui Ji Zhe Yuan Xiaohong Xu Hydrogen‐Associated Filling‐Controlled Mottronics Within Thermodynamically Metastable Vanadium Dioxide Advanced Science correlated oxides hydrogenation metal‐insulator transition metastable material topotactic phase modulation |
| title | Hydrogen‐Associated Filling‐Controlled Mottronics Within Thermodynamically Metastable Vanadium Dioxide |
| title_full | Hydrogen‐Associated Filling‐Controlled Mottronics Within Thermodynamically Metastable Vanadium Dioxide |
| title_fullStr | Hydrogen‐Associated Filling‐Controlled Mottronics Within Thermodynamically Metastable Vanadium Dioxide |
| title_full_unstemmed | Hydrogen‐Associated Filling‐Controlled Mottronics Within Thermodynamically Metastable Vanadium Dioxide |
| title_short | Hydrogen‐Associated Filling‐Controlled Mottronics Within Thermodynamically Metastable Vanadium Dioxide |
| title_sort | hydrogen associated filling controlled mottronics within thermodynamically metastable vanadium dioxide |
| topic | correlated oxides hydrogenation metal‐insulator transition metastable material topotactic phase modulation |
| url | https://doi.org/10.1002/advs.202414991 |
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