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  Composition-dependent charge transfer and phase separation in the V1-xRexO2 solid solution

Mikhailova, D., Kuratieva, N. N., Utsumi, Y., Tsirlin, A. A., Abakumov, A. M., Schmidt, M., et al. (2017). Composition-dependent charge transfer and phase separation in the V1-xRexO2 solid solution. Dalton Transactions, 46(5), 1606-1617. doi:10.1039/c6dt04389e.

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Item Permalink: http://hdl.handle.net/11858/00-001M-0000-002D-0A2A-C Version Permalink: http://hdl.handle.net/21.11116/0000-0000-6E5B-0
Genre: Journal Article

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 Creators:
Mikhailova, D.1, Author              
Kuratieva, N. N.2, Author
Utsumi, Y.3, Author              
Tsirlin, A. A.2, Author
Abakumov, A. M.2, Author
Schmidt, M.4, Author              
Oswald, S.2, Author
Fuess, H.2, Author
Ehrenberg, H.2, Author
Affiliations:
1Daria Mikhailova, Physics of Correlated Matter, Max Planck Institute for Chemical Physics of Solids, Max Planck Society, ou_1863448              
2External Organizations, ou_persistent22              
3Physics of Correlated Matter, Max Planck Institute for Chemical Physics of Solids, Max Planck Society, ou_1863445              
4Marcus Schmidt, Chemical Metal Science, Max Planck Institute for Chemical Physics of Solids, Max Planck Society, ou_1863415              

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 Abstract: The substitution of vanadium in vanadium dioxide VO2 influences the critical temperatures of structural and metal-to-insulator transitions in different ways depending on the valence of the dopant. Rhenium adopts valence states between + 4 and + 7 in an octahedral oxygen surrounding and is particularly interesting in this context. Structural investigation of V1-xRexO2 solid solutions (0.01 <= x <= 0.30) between 80 and 1200 K using synchrotron X-ray powder diffraction revealed only two polymorphs that resemble VO2: the low-temperature monoclinic MoO2-type form (space group P2(1)/c), and the tetragonal rutile-like form (space group P4(2)/mnm). However, for compositions with 0.03 < x <= 0.15 a phase separation in the solid solution was observed below 1000 K upon cooling down from 1200 K, giving rise to two isostructural phases with slightly different lattice parameters. This is reflected in the appearance of two metal-toinsulator transition temperatures detected by magnetization and specific heat measurements. Comprehensive X-ray photoelectron spectroscopy studies showed that an increased amount of Re leads to a change in the Re valence state from solely Re6+ at a low doping level (<= 3 at% Re) via mixed-valence states Re4+/Re6+ for at least 0.03 < x <= 0.10, up to nearly pure Re4+ in V0.70Re0.30O2. Thus, compositions V1-xRexO2 with only one valence state of Re in the material (Re6+ or Re4+) can be obtained as a single phase, while intermediate compositions are subjected to a phase separation, presumably due to different valence states of Re.

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Language(s): eng - English
 Dates: 2017-02-072017-02-07
 Publication Status: Published in print
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 Table of Contents: -
 Rev. Method: -
 Identifiers: ISI: 000395442700030
DOI: 10.1039/c6dt04389e
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Title: Dalton Transactions
  Abbreviation : Dalton Trans.
Source Genre: Journal
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Publ. Info: Cambridge, UK : Royal Society of Chemistry
Pages: - Volume / Issue: 46 (5) Sequence Number: - Start / End Page: 1606 - 1617 Identifier: ISSN: 1477-9226
CoNE: /journals/resource/954925269323