Hydrogen Diffusion and Stabilization in Single-Crystal VO2 Micro/Nanobeams by Direct Atomic Hydrogenation

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dc.citation.firstpage5445en_US
dc.citation.issueNumber9en_US
dc.citation.journalTitleNano Lettersen_US
dc.citation.lastpage5451en_US
dc.citation.volumeNumber14en_US
dc.contributor.authorLin, Jianen_US
dc.contributor.authorJi, Hengen_US
dc.contributor.authorSwift, Michael W.en_US
dc.contributor.authorHardy, Will J.en_US
dc.contributor.authorPeng, Zhiweien_US
dc.contributor.authorFan, Xiujunen_US
dc.contributor.authorNevidomskyy, Andriy H.en_US
dc.contributor.authorTour, James M.en_US
dc.contributor.authorNatelson, Douglasen_US
dc.contributor.orgSmalley Institute for Nanoscale Science and Technologyen_US
dc.date.accessioned2016-06-27T14:14:27Zen_US
dc.date.available2016-06-27T14:14:27Zen_US
dc.date.issued2014en_US
dc.description.abstractWe report measurements of the diffusion of atomic hydrogen in single crystalline VO2 micro/nanobeams by direct exposure to atomic hydrogen, without catalyst. The atomic hydrogen is generated by a hot filament, and the doping process takes place at moderate temperature (373 K). Undoped VO2 has a metal-to-insulator phase transition at ∼340 K between a high-temperature, rutile, metallic phase and a low-temperature, monoclinic, insulating phase with a resistance exhibiting a semiconductor-like temperature dependence. Atomic hydrogenation results in stabilization of the metallic phase of VO2 micro/nanobeams down to 2 K, the lowest point we could reach in our measurement setup. Optical characterization shows that hydrogen atoms prefer to diffuse along the c axis of rutile (a axis of monoclinic) VO2, along the oxygen “channels”. Based on observing the movement of the hydrogen diffusion front in single crystalline VO2 beams, we estimate the diffusion constant for hydrogen along the c axis of the rutile phase to be 6.7 × 10–10 cm2/s at approximately 373 K, exceeding the value in isostructural TiO2 by ∼38×. Moreover, we find that the diffusion constant along the c axis of the rutile phase exceeds that along the equivalent a axis of the monoclinic phase by at least 3 orders of magnitude. This remarkable change in kinetics must originate from the distortion of the “channels” when the unit cell doubles along this direction upon cooling into the monoclinic structure. Ab initio calculation results are in good agreement with the experimental trends in the relative kinetics of the two phases. This raises the possibility of a switchable membrane for hydrogen transport.en_US
dc.identifier.citationLin, Jian, Ji, Heng, Swift, Michael W., et al.. "Hydrogen Diffusion and Stabilization in Single-Crystal VO2 Micro/Nanobeams by Direct Atomic Hydrogenation." <i>Nano Letters,</i> 14, no. 9 (2014) American Chemical Society: 5445-5451. http://dx.doi.org/10.1021/nl5030694.en_US
dc.identifier.doihttp://dx.doi.org/10.1021/nl5030694en_US
dc.identifier.urihttps://hdl.handle.net/1911/90571en_US
dc.language.isoengen_US
dc.publisherAmerican Chemical Societyen_US
dc.rightsThis is an author's peer-reviewed final manuscript, as accepted by the publisher. The published article is copyrighted by the American Chemical Society.en_US
dc.subject.keywordVO2en_US
dc.subject.keywordatomic hydrogenationen_US
dc.subject.keywordhydrogen diffusionen_US
dc.subject.keywordMITen_US
dc.titleHydrogen Diffusion and Stabilization in Single-Crystal VO2 Micro/Nanobeams by Direct Atomic Hydrogenationen_US
dc.typeJournal articleen_US
dc.type.dcmiTexten_US
dc.type.publicationpost-printen_US
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