Systematic study of Oxygen vacancy tunable transport properties of few-layer MoO3- x enabled by vapor-based synthesis

Bulk and nanoscale molybdenum trioxide (MoO3) has shown impressive technologically relevant properties, but deeper investigation into 2D MoO3 has been prevented by the lack of reliable vapor-based synthesis and doping techniques. Herein, the successful synthesis of high-quality, few-layer MoO3 down...

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Autores: Hanson, E.D., Lajaunie, L., Hao, S., Myers, B.D., Shi, F., Murthy, A.A., Wolverton, C., Arenal, R., Dravid, V.P.
Tipo de recurso: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2017
País:España
Institución:Universidad de Zaragoza
Repositorio:Zaguán. Repositorio Digital de la Universidad de Zaragoza
OAI Identifier:oai:zaguan.unizar.es:70171
Acceso en línea:http://zaguan.unizar.es/record/70171
Access Level:acceso abierto
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spelling Systematic study of Oxygen vacancy tunable transport properties of few-layer MoO3- x enabled by vapor-based synthesisHanson, E.D.Lajaunie, L.Hao, S.Myers, B.D.Shi, F.Murthy, A.A.Wolverton, C.Arenal, R.Dravid, V.P.Bulk and nanoscale molybdenum trioxide (MoO3) has shown impressive technologically relevant properties, but deeper investigation into 2D MoO3 has been prevented by the lack of reliable vapor-based synthesis and doping techniques. Herein, the successful synthesis of high-quality, few-layer MoO3 down to bilayer thickness via physical vapor deposition is reported. The electronic structure of MoO3 can be strongly modified by introducing oxygen substoichiometry (MoO3- x), which introduces gap states and increases conductivity. A dose-controlled electron irradiation technique to introduce oxygen vacancies into the few-layer MoO3 structure is presented, thereby adding n-type doping. By combining in situ transport with core-loss and monochromated low-loss scanning transmission electron microscopy–electron energy-loss spectroscopy studies, a detailed structure–property relationship is developed between Mo-oxidation state and resistance. Transport properties are reported for MoO3- x down to three layers thick, the most 2D-like MoO3- x transport hitherto reported. Combining these results with density functional theory calculations, a radiolysis-based mechanism for the irradiation-induced oxygen vacancy introduction is developed, including insights into favorable configurations of oxygen defects. These systematic studies represent an important step forward in bringing few-layer MoO3 and MoO3- x into the 2D family, as well as highlight the promise of MoO3- x as a functional, tunable electronic material.2017info:eu-repo/semantics/articleinfo:eu-repo/semantics/acceptedVersionapplication/pdfhttp://zaguan.unizar.es/record/70171reponame:Zaguán. Repositorio Digital de la Universidad de Zaragozainstname:Universidad de ZaragozaInglésinfo:eu-repo/grantAgreement/ES/MINECO/MAT2016-79776-Pinfo:eu-repo/grantAgreement/ES/MINECO/FIS2013-46159-C3-3-PThis project has received funding from the European Union’s Horizon 2020 research and innovation program under grant agreement No H2020 696656-GrapheneCore1info:eu-repo/grantAgreement/EC/H2020/696656This project has received funding from the European Union’s Horizon 2020 research and innovation program under grant agreement No H2020 642742-Enabling Excellenceinfo:eu-repo/grantAgreement/EC/H2020/642742info:eu-repo/grantAgreement/EC/FP7/312483info:eu-repo/semantics/openAccessoai:zaguan.unizar.es:701712026-05-29T13:59:51Z
dc.title.none.fl_str_mv Systematic study of Oxygen vacancy tunable transport properties of few-layer MoO3- x enabled by vapor-based synthesis
title Systematic study of Oxygen vacancy tunable transport properties of few-layer MoO3- x enabled by vapor-based synthesis
spellingShingle Systematic study of Oxygen vacancy tunable transport properties of few-layer MoO3- x enabled by vapor-based synthesis
Hanson, E.D.
title_short Systematic study of Oxygen vacancy tunable transport properties of few-layer MoO3- x enabled by vapor-based synthesis
title_full Systematic study of Oxygen vacancy tunable transport properties of few-layer MoO3- x enabled by vapor-based synthesis
title_fullStr Systematic study of Oxygen vacancy tunable transport properties of few-layer MoO3- x enabled by vapor-based synthesis
title_full_unstemmed Systematic study of Oxygen vacancy tunable transport properties of few-layer MoO3- x enabled by vapor-based synthesis
title_sort Systematic study of Oxygen vacancy tunable transport properties of few-layer MoO3- x enabled by vapor-based synthesis
dc.creator.none.fl_str_mv Hanson, E.D.
Lajaunie, L.
Hao, S.
Myers, B.D.
Shi, F.
Murthy, A.A.
Wolverton, C.
Arenal, R.
Dravid, V.P.
author Hanson, E.D.
author_facet Hanson, E.D.
Lajaunie, L.
Hao, S.
Myers, B.D.
Shi, F.
Murthy, A.A.
Wolverton, C.
Arenal, R.
Dravid, V.P.
author_role author
author2 Lajaunie, L.
Hao, S.
Myers, B.D.
Shi, F.
Murthy, A.A.
Wolverton, C.
Arenal, R.
Dravid, V.P.
author2_role author
author
author
author
author
author
author
author
description Bulk and nanoscale molybdenum trioxide (MoO3) has shown impressive technologically relevant properties, but deeper investigation into 2D MoO3 has been prevented by the lack of reliable vapor-based synthesis and doping techniques. Herein, the successful synthesis of high-quality, few-layer MoO3 down to bilayer thickness via physical vapor deposition is reported. The electronic structure of MoO3 can be strongly modified by introducing oxygen substoichiometry (MoO3- x), which introduces gap states and increases conductivity. A dose-controlled electron irradiation technique to introduce oxygen vacancies into the few-layer MoO3 structure is presented, thereby adding n-type doping. By combining in situ transport with core-loss and monochromated low-loss scanning transmission electron microscopy–electron energy-loss spectroscopy studies, a detailed structure–property relationship is developed between Mo-oxidation state and resistance. Transport properties are reported for MoO3- x down to three layers thick, the most 2D-like MoO3- x transport hitherto reported. Combining these results with density functional theory calculations, a radiolysis-based mechanism for the irradiation-induced oxygen vacancy introduction is developed, including insights into favorable configurations of oxygen defects. These systematic studies represent an important step forward in bringing few-layer MoO3 and MoO3- x into the 2D family, as well as highlight the promise of MoO3- x as a functional, tunable electronic material.
publishDate 2017
dc.date.none.fl_str_mv 2017
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/acceptedVersion
format article
status_str acceptedVersion
dc.identifier.none.fl_str_mv http://zaguan.unizar.es/record/70171
url http://zaguan.unizar.es/record/70171
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv info:eu-repo/grantAgreement/ES/MINECO/MAT2016-79776-P
info:eu-repo/grantAgreement/ES/MINECO/FIS2013-46159-C3-3-P
This project has received funding from the European Union’s Horizon 2020 research and innovation program under grant agreement No H2020 696656-GrapheneCore1
info:eu-repo/grantAgreement/EC/H2020/696656
This project has received funding from the European Union’s Horizon 2020 research and innovation program under grant agreement No H2020 642742-Enabling Excellence
info:eu-repo/grantAgreement/EC/H2020/642742
info:eu-repo/grantAgreement/EC/FP7/312483
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv
publisher.none.fl_str_mv
dc.source.none.fl_str_mv reponame:Zaguán. Repositorio Digital de la Universidad de Zaragoza
instname:Universidad de Zaragoza
instname_str Universidad de Zaragoza
reponame_str Zaguán. Repositorio Digital de la Universidad de Zaragoza
collection Zaguán. Repositorio Digital de la Universidad de Zaragoza
repository.name.fl_str_mv
repository.mail.fl_str_mv
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