In situ diffraction study of catalytic hydrogenation of VO2: Stable phases and origins of metallicity

Yaroslav Filinchuk, Nikolay A. Tumanov, Voraksmy Ban, Heng Ji, Jiang Wei, Michael W. Swift, Andriy H. Nevidomskyy, Douglas Natelson

Résultats de recherche: Contribution à un journal/une revueArticle

Résumé

Controlling electronic population through chemical doping is one way to tip the balance between competing phases in materials with strong electronic correlations. Vanadium dioxide exhibits a first-order phase transition at around 338 K between a high-temperature, tetragonal, metallic state (T) and a low-temperature, monoclinic, insulating state (M1), driven by electron-electron and electron-lattice interactions. Intercalation of VO2 with atomic hydrogen has been demonstrated, with evidence that this doping suppresses the transition. However, the detailed effects of intercalated H on the crystal and electronic structure of the resulting hydride have not been previously reported. Here we present synchrotron and neutron diffraction studies of this material system, mapping out the structural phase diagram as a function of temperature and hydrogen content. In addition to the original T and M1 phases, we find two orthorhombic phases, O1 and O2, which are stabilized at higher hydrogen content. We present density functional calculations that confirm the metallicity of these states and discuss the physical basis by which hydrogen stabilizes conducting phases, in the context of the metal-insulator transition.

langue originaleAnglais
Pages (de - à)8100-8109
Nombre de pages10
journalJournal of the American Chemical Society
Volume136
Numéro de publication22
Les DOIs
étatPublié - 4 juin 2014
Modification externeOui

Empreinte digitale

Hydrogenation
Hydrogen
Diffraction
Electrons
Temperature
Doping (additives)
Neutron Diffraction
Synchrotrons
Metal insulator transition
Phase Transition
Neutron diffraction
Intercalation
Hydrides
Vanadium
Phase diagrams
Electronic structure
Density functional theory
Crystal structure
Phase transitions
Metals

Citer ceci

Filinchuk, Yaroslav ; Tumanov, Nikolay A. ; Ban, Voraksmy ; Ji, Heng ; Wei, Jiang ; Swift, Michael W. ; Nevidomskyy, Andriy H. ; Natelson, Douglas. / In situ diffraction study of catalytic hydrogenation of VO2 : Stable phases and origins of metallicity. Dans: Journal of the American Chemical Society. 2014 ; Vol 136, Numéro 22. p. 8100-8109.
@article{cae1bc19cc704301b8ca14c9db3a7988,
title = "In situ diffraction study of catalytic hydrogenation of VO2: Stable phases and origins of metallicity",
abstract = "Controlling electronic population through chemical doping is one way to tip the balance between competing phases in materials with strong electronic correlations. Vanadium dioxide exhibits a first-order phase transition at around 338 K between a high-temperature, tetragonal, metallic state (T) and a low-temperature, monoclinic, insulating state (M1), driven by electron-electron and electron-lattice interactions. Intercalation of VO2 with atomic hydrogen has been demonstrated, with evidence that this doping suppresses the transition. However, the detailed effects of intercalated H on the crystal and electronic structure of the resulting hydride have not been previously reported. Here we present synchrotron and neutron diffraction studies of this material system, mapping out the structural phase diagram as a function of temperature and hydrogen content. In addition to the original T and M1 phases, we find two orthorhombic phases, O1 and O2, which are stabilized at higher hydrogen content. We present density functional calculations that confirm the metallicity of these states and discuss the physical basis by which hydrogen stabilizes conducting phases, in the context of the metal-insulator transition.",
author = "Yaroslav Filinchuk and Tumanov, {Nikolay A.} and Voraksmy Ban and Heng Ji and Jiang Wei and Swift, {Michael W.} and Nevidomskyy, {Andriy H.} and Douglas Natelson",
year = "2014",
month = "6",
day = "4",
doi = "10.1021/ja503360y",
language = "English",
volume = "136",
pages = "8100--8109",
journal = "J. Am. Chem. Soc.",
issn = "0002-7863",
publisher = "American Chemical Society",
number = "22",

}

Filinchuk, Y, Tumanov, NA, Ban, V, Ji, H, Wei, J, Swift, MW, Nevidomskyy, AH & Natelson, D 2014, 'In situ diffraction study of catalytic hydrogenation of VO2: Stable phases and origins of metallicity', Journal of the American Chemical Society, VOL. 136, Numéro 22, p. 8100-8109. https://doi.org/10.1021/ja503360y

In situ diffraction study of catalytic hydrogenation of VO2 : Stable phases and origins of metallicity. / Filinchuk, Yaroslav; Tumanov, Nikolay A.; Ban, Voraksmy; Ji, Heng; Wei, Jiang; Swift, Michael W.; Nevidomskyy, Andriy H.; Natelson, Douglas.

Dans: Journal of the American Chemical Society, Vol 136, Numéro 22, 04.06.2014, p. 8100-8109.

Résultats de recherche: Contribution à un journal/une revueArticle

TY - JOUR

T1 - In situ diffraction study of catalytic hydrogenation of VO2

T2 - Stable phases and origins of metallicity

AU - Filinchuk, Yaroslav

AU - Tumanov, Nikolay A.

AU - Ban, Voraksmy

AU - Ji, Heng

AU - Wei, Jiang

AU - Swift, Michael W.

AU - Nevidomskyy, Andriy H.

AU - Natelson, Douglas

PY - 2014/6/4

Y1 - 2014/6/4

N2 - Controlling electronic population through chemical doping is one way to tip the balance between competing phases in materials with strong electronic correlations. Vanadium dioxide exhibits a first-order phase transition at around 338 K between a high-temperature, tetragonal, metallic state (T) and a low-temperature, monoclinic, insulating state (M1), driven by electron-electron and electron-lattice interactions. Intercalation of VO2 with atomic hydrogen has been demonstrated, with evidence that this doping suppresses the transition. However, the detailed effects of intercalated H on the crystal and electronic structure of the resulting hydride have not been previously reported. Here we present synchrotron and neutron diffraction studies of this material system, mapping out the structural phase diagram as a function of temperature and hydrogen content. In addition to the original T and M1 phases, we find two orthorhombic phases, O1 and O2, which are stabilized at higher hydrogen content. We present density functional calculations that confirm the metallicity of these states and discuss the physical basis by which hydrogen stabilizes conducting phases, in the context of the metal-insulator transition.

AB - Controlling electronic population through chemical doping is one way to tip the balance between competing phases in materials with strong electronic correlations. Vanadium dioxide exhibits a first-order phase transition at around 338 K between a high-temperature, tetragonal, metallic state (T) and a low-temperature, monoclinic, insulating state (M1), driven by electron-electron and electron-lattice interactions. Intercalation of VO2 with atomic hydrogen has been demonstrated, with evidence that this doping suppresses the transition. However, the detailed effects of intercalated H on the crystal and electronic structure of the resulting hydride have not been previously reported. Here we present synchrotron and neutron diffraction studies of this material system, mapping out the structural phase diagram as a function of temperature and hydrogen content. In addition to the original T and M1 phases, we find two orthorhombic phases, O1 and O2, which are stabilized at higher hydrogen content. We present density functional calculations that confirm the metallicity of these states and discuss the physical basis by which hydrogen stabilizes conducting phases, in the context of the metal-insulator transition.

UR - http://www.scopus.com/inward/record.url?scp=84901918896&partnerID=8YFLogxK

U2 - 10.1021/ja503360y

DO - 10.1021/ja503360y

M3 - Article

AN - SCOPUS:84901918896

VL - 136

SP - 8100

EP - 8109

JO - J. Am. Chem. Soc.

JF - J. Am. Chem. Soc.

SN - 0002-7863

IS - 22

ER -