Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 58, Issue 39, Pages 13711-13716Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201904148
Keywords
first-principle simulations; hydrogenation; metal-insulator phase transition; synchrotron characterization
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Funding
- National Key Research and Development Program of China [2016YFA0401004, 2018YFA0208603]
- National Natural Science Foundation of China [11404095, 11574279, 11704362]
- Youth Innovation Promotion Association CAS
- Major/Innovative Program of Development Foundation of Hefei Center for Physical Science and Technology
- China Postdoctoral Science Foundation [2017M622002]
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Charge doping is an effective way to induce the metal-insulator transition (MIT) in correlated materials for many important utilizations, which is however practically limited by problem of low stability. An electron-proton co-doping mechanism is used to achieve pronounced phase modulation of monoclinic vanadium dioxide (VO2) at room temperature. Using l-ascorbic acid (AA) solution to treat VO2, the ionized AA(-) species donate electrons to the adsorbed VO2 surface. Charges then electrostatically attract surrounding protons to penetrate, and eventually results in stable hydrogen-doped metallic VO2. The variations of electronic structures, especially the electron occupancy of V 3d/O 2p hybrid orbitals, were examined by synchrotron characterizations and first-principle theoretical simulations. The adsorbed molecules protect hydrogen dopants from escaping out of lattice and thereby stabilize the metallic phase for VO2.
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