Direct evidence of Fe2+ - Fe3+ charge ordering in the ferrimagnetic hematite-ilmenite Fe1.35Ti0.65O3−δ thin films

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dc.contributor.authorBocher, L.
dc.contributor.authorPopova, Elena
dc.contributor.authorNolan, Michael
dc.contributor.authorGloter, Alexandre
dc.contributor.authorChikoidze, Ekaterina
dc.contributor.authorMarch, K.
dc.contributor.authorWarot-Fonrose, B.
dc.contributor.authorBerini, B.
dc.contributor.authorStephan, Odile
dc.contributor.authorKeller, Niels
dc.contributor.authorDumont, Yves
dc.contributor.funderEuropean Commission
dc.contributor.funderSeventh Framework Programme
dc.contributor.funderUniversité Paris-Saclay
dc.contributor.funderIrish Centre for High-End Computing
dc.contributor.funderScience Foundation Ireland
dc.contributor.funderCentre de Compétences Nanosciences Ile-de-France
dc.contributor.funderCommissariat à l'Énergie Atomique et aux Énergies Alternatives
dc.contributor.funderCentre National de la Recherche Scientifique
dc.contributor.funderEuropean Cooperation in Science and Technology
dc.date.accessioned2017-09-04T09:02:30Z
dc.date.available2017-09-04T09:02:30Z
dc.date.issued2013-10-14
dc.description.abstractIn this Letter we highlight direct experimental evidence of Fe2+-Fe3+ charge ordering at room temperature in hematite-ilmenite Fe1.35Ti0.65O3-delta epitaxial thin films grown by pulsed laser deposition, using aberration-corrected scanning transmission electron microscopy coupled to high-resolution energy electron-loss spectroscopy. These advanced spectromicroscopy techniques demonstrate a strong modulation of the Fe2+ valence state along the c axis. Density functional theory calculations provide crucial information on the key role of oxygen vacancies in the observed charge distributions. Their presence at significant levels leads to the localization of extra electrons onto reduced Fe2+ sites, while Ti remains solely +4. The magnetic and transport properties of these films are reviewed in the light of the present results regarding their ferrimagnetic character correlated with the Fe2+ modulation and their semi-conducting behavior interpreted by an Efros-Shklovskii variable-range hopping conduction regime via Fe2+ and Fe3+ centers. The experimental evidence of only one type of mixed valence state, i.e., Fe2+ and Fe3+, in the Fe2-xTixO3-delta system will thus help to interpret further the origin of its geomagnetic properties and to illuminate fundamental issues regarding its spintronic potential.en
dc.description.sponsorshipCentre de Compétences Nanosciences Ile-de-France (Project No. IF-08-1453/R); Université Paris-Saclay (LabEx CHARM3AT (Invited Professor grant); European Commission (COST Action CM1104 "Reducible Oxide Chemistry, Structure and Functions)en
dc.description.statusPeer revieweden
dc.description.versionPublished Versionen
dc.format.mimetypeapplication/pdfen
dc.identifier.articleid167202
dc.identifier.citationBocher, L., Popova, E., Nolan, M., Gloter, A., Chikoidze, E., March, K., Warot-Fonrose, B., Berini, B., Stéphan, O., Keller, N. and Dumont, Y. (2013) ‘Direct evidence of Fe2+ - Fe3+ charge ordering in the ferrimagnetic hematite-ilmenite Fe1.35Ti0.65O3−δ thin films’, Physical Review Letters, 111(16), 167202 (6pp). doi: 10.1103/PhysRevLett.111.167202en
dc.identifier.doi10.1103/PhysRevLett.111.167202
dc.identifier.issn0031-9007
dc.identifier.issn1079-7114
dc.identifier.issued16
dc.identifier.journaltitlePhysical Review Lettersen
dc.identifier.urihttps://hdl.handle.net/10468/4615
dc.identifier.volume111
dc.language.isoenen
dc.publisherAmerican Physical Societyen
dc.relation.projectinfo:eu-repo/grantAgreement/EC/FP7::SP4::INFRA/312483/EU/Enabling Science and Technology through European Electron Microscopy/ESTEEM 2
dc.relation.projectinfo:eu-repo/grantAgreement/SFI/SFI Starting Investigator Research Grant (SIRG)/09/SIRG/I1620/IE/EMOIN: Engineering Metal Oxide Interfaces For Renewable Energy Photocatalysis/
dc.relation.urihttps://journals.aps.org/prl/abstract/10.1103/PhysRevLett.111.167202
dc.rights© 2013, American Physical Societyen
dc.subjectSolid solution seriesen
dc.subjectWeak ferromagnetismen
dc.subjectElectrical propertiesen
dc.subjectElectronic structureen
dc.subjectMagnetic propertiesen
dc.subjectCrystal structureen
dc.subjectHigh temperatureen
dc.subjectFetio3en
dc.subjectInterfaceen
dc.subjectSystemen
dc.titleDirect evidence of Fe2+ - Fe3+ charge ordering in the ferrimagnetic hematite-ilmenite Fe1.35Ti0.65O3−δ thin filmsen
dc.typeArticle (peer-reviewed)en
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