Toward Functionalized Ultrathin Oxide Films: The Impact of Surface Apical Oxygen

Abstract Thin films of transition metal oxides open up a gateway to nanoscale electronic devices beyond silicon characterized by novel electronic functionalities. While such films are commonly prepared in an oxygen atmosphere, they are typically considered to be ideally terminated with the stoichiom...

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Main Authors: Judith Gabel, Matthias Pickem, Philipp Scheiderer, Lenart Dudy, Berengar Leikert, Marius Fuchs, Martin Stübinger, Matthias Schmitt, Julia Küspert, Giorgio Sangiovanni, Jan M. Tomczak, Karsten Held, Tien‐Lin Lee, Ralph Claessen, Michael Sing
Format: Article
Language:English
Published: Wiley-VCH 2022-04-01
Series:Advanced Electronic Materials
Subjects:
Online Access:https://doi.org/10.1002/aelm.202101006
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author Judith Gabel
Matthias Pickem
Philipp Scheiderer
Lenart Dudy
Berengar Leikert
Marius Fuchs
Martin Stübinger
Matthias Schmitt
Julia Küspert
Giorgio Sangiovanni
Jan M. Tomczak
Karsten Held
Tien‐Lin Lee
Ralph Claessen
Michael Sing
author_facet Judith Gabel
Matthias Pickem
Philipp Scheiderer
Lenart Dudy
Berengar Leikert
Marius Fuchs
Martin Stübinger
Matthias Schmitt
Julia Küspert
Giorgio Sangiovanni
Jan M. Tomczak
Karsten Held
Tien‐Lin Lee
Ralph Claessen
Michael Sing
author_sort Judith Gabel
collection DOAJ
description Abstract Thin films of transition metal oxides open up a gateway to nanoscale electronic devices beyond silicon characterized by novel electronic functionalities. While such films are commonly prepared in an oxygen atmosphere, they are typically considered to be ideally terminated with the stoichiometric composition. Using the prototypical correlated metal SrVO3 as an example, it is demonstrated that this idealized description overlooks an essential ingredient: oxygen adsorbing at the surface apical sites. The oxygen adatoms, which are present even if the films are kept in an ultrahigh vacuum environment and not explicitly exposed to air, are shown to severely affect the intrinsic electronic structure of a transition metal oxide film. Their presence leads to the formation of an electronically dead surface layer but also alters the band filling and the electron correlations in the thin films. These findings highlight that it is important to take into account surface apical oxygen or—mutatis mutandis—the specific oxygen configuration imposed by a capping layer to predict the behavior of ultrathin films of transition metal oxides near the single unit‐cell limit.
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spelling doaj.art-d4808f2921684ca5b6a5b4a46ca40f2c2023-11-21T07:01:06ZengWiley-VCHAdvanced Electronic Materials2199-160X2022-04-0184n/an/a10.1002/aelm.202101006Toward Functionalized Ultrathin Oxide Films: The Impact of Surface Apical OxygenJudith Gabel0Matthias Pickem1Philipp Scheiderer2Lenart Dudy3Berengar Leikert4Marius Fuchs5Martin Stübinger6Matthias Schmitt7Julia Küspert8Giorgio Sangiovanni9Jan M. Tomczak10Karsten Held11Tien‐Lin Lee12Ralph Claessen13Michael Sing14Diamond Light Source Didcot OX11 0DE UKInstitute of Solid State Physics TU Wien Vienna 1040 AustriaPhysikalisches Institut and Würzburg‐Dresden Cluster of Excellence ct.qmat Universität Würzburg 97074 Würzburg GermanySynchrotron SOLEIL Saint‐Aubin 91190 FrancePhysikalisches Institut and Würzburg‐Dresden Cluster of Excellence ct.qmat Universität Würzburg 97074 Würzburg GermanyInstitut für Theoretische Physik and Würzburg‐Dresden Cluster of Excellence ct.qmat Universität Würzburg 97074 Würzburg GermanyPhysikalisches Institut and Würzburg‐Dresden Cluster of Excellence ct.qmat Universität Würzburg 97074 Würzburg GermanyPhysikalisches Institut and Würzburg‐Dresden Cluster of Excellence ct.qmat Universität Würzburg 97074 Würzburg GermanyPhysikalisches Institut and Würzburg‐Dresden Cluster of Excellence ct.qmat Universität Würzburg 97074 Würzburg GermanyInstitut für Theoretische Physik and Würzburg‐Dresden Cluster of Excellence ct.qmat Universität Würzburg 97074 Würzburg GermanyInstitute of Solid State Physics TU Wien Vienna 1040 AustriaInstitute of Solid State Physics TU Wien Vienna 1040 AustriaDiamond Light Source Didcot OX11 0DE UKPhysikalisches Institut and Würzburg‐Dresden Cluster of Excellence ct.qmat Universität Würzburg 97074 Würzburg GermanyPhysikalisches Institut and Würzburg‐Dresden Cluster of Excellence ct.qmat Universität Würzburg 97074 Würzburg GermanyAbstract Thin films of transition metal oxides open up a gateway to nanoscale electronic devices beyond silicon characterized by novel electronic functionalities. While such films are commonly prepared in an oxygen atmosphere, they are typically considered to be ideally terminated with the stoichiometric composition. Using the prototypical correlated metal SrVO3 as an example, it is demonstrated that this idealized description overlooks an essential ingredient: oxygen adsorbing at the surface apical sites. The oxygen adatoms, which are present even if the films are kept in an ultrahigh vacuum environment and not explicitly exposed to air, are shown to severely affect the intrinsic electronic structure of a transition metal oxide film. Their presence leads to the formation of an electronically dead surface layer but also alters the band filling and the electron correlations in the thin films. These findings highlight that it is important to take into account surface apical oxygen or—mutatis mutandis—the specific oxygen configuration imposed by a capping layer to predict the behavior of ultrathin films of transition metal oxides near the single unit‐cell limit.https://doi.org/10.1002/aelm.202101006correlated oxideselectronic phase transitionsphotoelectron spectroscopythin filmstransition metal oxides
spellingShingle Judith Gabel
Matthias Pickem
Philipp Scheiderer
Lenart Dudy
Berengar Leikert
Marius Fuchs
Martin Stübinger
Matthias Schmitt
Julia Küspert
Giorgio Sangiovanni
Jan M. Tomczak
Karsten Held
Tien‐Lin Lee
Ralph Claessen
Michael Sing
Toward Functionalized Ultrathin Oxide Films: The Impact of Surface Apical Oxygen
Advanced Electronic Materials
correlated oxides
electronic phase transitions
photoelectron spectroscopy
thin films
transition metal oxides
title Toward Functionalized Ultrathin Oxide Films: The Impact of Surface Apical Oxygen
title_full Toward Functionalized Ultrathin Oxide Films: The Impact of Surface Apical Oxygen
title_fullStr Toward Functionalized Ultrathin Oxide Films: The Impact of Surface Apical Oxygen
title_full_unstemmed Toward Functionalized Ultrathin Oxide Films: The Impact of Surface Apical Oxygen
title_short Toward Functionalized Ultrathin Oxide Films: The Impact of Surface Apical Oxygen
title_sort toward functionalized ultrathin oxide films the impact of surface apical oxygen
topic correlated oxides
electronic phase transitions
photoelectron spectroscopy
thin films
transition metal oxides
url https://doi.org/10.1002/aelm.202101006
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