Tailoring the physical and chemical properties of Sn1-xCoxO2 nanoparticles: an experimental and theoretical approach
Autor(a) principal: | |
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Data de Publicação: | 2020 |
Outros Autores: | , , , , , , , , , , , |
Tipo de documento: | Artigo |
Idioma: | eng |
Título da fonte: | Repositório Institucional da UNESP |
Texto Completo: | http://dx.doi.org/10.1039/c9cp05928h http://hdl.handle.net/11449/196658 |
Resumo: | In this work, we present a coupled experimental and theoretical first-principles investigation on one of the more promising oxide-diluted magnetic semiconductors, the Sn1-xCoxO2 nanoparticle system, in order to see the effect of cobalt doping on the physical and chemical properties. Our findings suggest that progressive surface enrichment with dopant ions plays an essential role in the monotonous quenching of the surface disorder modes. That weakening is associated with the passivation of the oxygen vacancies as the Co excess at the surface becomes larger. Room-temperature Sn-119 Mossbauer spectroscopy data analysis revealed the occurrence of a distribution of isomer shifts, related to the different non-equivalent surroundings of Sn4+ ions and the coexistence of Sn2+/Sn4+ at the particle surfaces provoked by the inhomogeneous distribution of Co ions, in agreement with the X-ray photoelectron spectroscopy measurements. Magnetic measurements revealed a paramagnetic behavior of the Co ions dispersed in the rutile-type matrix with antiferromagnetic correlations, which become stronger as the Co content is increased. Theoretical calculations show that a defect with two Co mediated by a nearby oxygen vacancy is the most likely defect. The predicted effects of this defect complex are in accordance with the experimental results. |
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Tailoring the physical and chemical properties of Sn1-xCoxO2 nanoparticles: an experimental and theoretical approachIn this work, we present a coupled experimental and theoretical first-principles investigation on one of the more promising oxide-diluted magnetic semiconductors, the Sn1-xCoxO2 nanoparticle system, in order to see the effect of cobalt doping on the physical and chemical properties. Our findings suggest that progressive surface enrichment with dopant ions plays an essential role in the monotonous quenching of the surface disorder modes. That weakening is associated with the passivation of the oxygen vacancies as the Co excess at the surface becomes larger. Room-temperature Sn-119 Mossbauer spectroscopy data analysis revealed the occurrence of a distribution of isomer shifts, related to the different non-equivalent surroundings of Sn4+ ions and the coexistence of Sn2+/Sn4+ at the particle surfaces provoked by the inhomogeneous distribution of Co ions, in agreement with the X-ray photoelectron spectroscopy measurements. Magnetic measurements revealed a paramagnetic behavior of the Co ions dispersed in the rutile-type matrix with antiferromagnetic correlations, which become stronger as the Co content is increased. Theoretical calculations show that a defect with two Co mediated by a nearby oxygen vacancy is the most likely defect. The predicted effects of this defect complex are in accordance with the experimental results.Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq)Coordenação de Aperfeiçoamento de Pessoal de Nível Superior (CAPES)Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP)Brazilian Agency Fundacao de Amparo a Pesquisa do Distrito Federal (FAP/DF)Univ Brasilia, Inst Fis, Nucleo Fis Aplicada, BR-70910900 Brasilia, DF, BrazilUniv Nacl San Agustin Arequipa, Lab Peliculas Delgadas, Escuela Profes Fis, Av Independencia S-N, Arequipa, PeruUniv Estadual Paulista, Dept Fis, IGCE, BR-13506900 Rio Claro, SP, BrazilUniv Fed Sao Carlos, Ctr Ciencias Exatas & Tecnol, Dept Fis, BR-13565905 Sao Carlos, SP, BrazilUniv Sao Paulo, Inst Fis, BR-05508090 Sao Paulo, BrazilCDTN, BR-3127901 Belo Horizonte, MG, BrazilUniv Estadual Paulista, Dept Fis, IGCE, BR-13506900 Rio Claro, SP, BrazilCNPq: 305.647/2015-6FAPESP: 2016/21371-5FAPESP: 2014/19142-2FAPESP: 2017/02317-2Brazilian Agency Fundacao de Amparo a Pesquisa do Distrito Federal (FAP/DF): 0193.001.345/2016Brazilian Agency Fundacao de Amparo a Pesquisa do Distrito Federal (FAP/DF): 0193001.196/2016Royal Soc ChemistryUniversidade de Brasília (UnB)Univ Nacl San Agustin ArequipaUniversidade Estadual Paulista (Unesp)Universidade Federal de São Carlos (UFSCar)Universidade de São Paulo (USP)CDTNAragon, F. F. H.Villegas-Lelovsky, L. [UNESP]Cabral, L.Lima, M. P.Aquino, J. C. R.Mathpal, M. C.Coaquira, J. A. H.Silva, S. W. daNagamine, L. C. C. M.Parreiras, S. O.Gastelois, P. L.Marques, G. E.Macedo, W. A. A.2020-12-10T19:52:01Z2020-12-10T19:52:01Z2020-02-14info:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/article3702-3714http://dx.doi.org/10.1039/c9cp05928hPhysical Chemistry Chemical Physics. Cambridge: Royal Soc Chemistry, v. 22, n. 6, p. 3702-3714, 2020.1463-9076http://hdl.handle.net/11449/19665810.1039/c9cp05928hWOS:000518683800052Web of Sciencereponame:Repositório Institucional da UNESPinstname:Universidade Estadual Paulista (UNESP)instacron:UNESPengPhysical Chemistry Chemical Physicsinfo:eu-repo/semantics/openAccess2021-10-23T08:59:49Zoai:repositorio.unesp.br:11449/196658Repositório InstitucionalPUBhttp://repositorio.unesp.br/oai/requestopendoar:29462021-10-23T08:59:49Repositório Institucional da UNESP - Universidade Estadual Paulista (UNESP)false |
dc.title.none.fl_str_mv |
Tailoring the physical and chemical properties of Sn1-xCoxO2 nanoparticles: an experimental and theoretical approach |
title |
Tailoring the physical and chemical properties of Sn1-xCoxO2 nanoparticles: an experimental and theoretical approach |
spellingShingle |
Tailoring the physical and chemical properties of Sn1-xCoxO2 nanoparticles: an experimental and theoretical approach Aragon, F. F. H. |
title_short |
Tailoring the physical and chemical properties of Sn1-xCoxO2 nanoparticles: an experimental and theoretical approach |
title_full |
Tailoring the physical and chemical properties of Sn1-xCoxO2 nanoparticles: an experimental and theoretical approach |
title_fullStr |
Tailoring the physical and chemical properties of Sn1-xCoxO2 nanoparticles: an experimental and theoretical approach |
title_full_unstemmed |
Tailoring the physical and chemical properties of Sn1-xCoxO2 nanoparticles: an experimental and theoretical approach |
title_sort |
Tailoring the physical and chemical properties of Sn1-xCoxO2 nanoparticles: an experimental and theoretical approach |
author |
Aragon, F. F. H. |
author_facet |
Aragon, F. F. H. Villegas-Lelovsky, L. [UNESP] Cabral, L. Lima, M. P. Aquino, J. C. R. Mathpal, M. C. Coaquira, J. A. H. Silva, S. W. da Nagamine, L. C. C. M. Parreiras, S. O. Gastelois, P. L. Marques, G. E. Macedo, W. A. A. |
author_role |
author |
author2 |
Villegas-Lelovsky, L. [UNESP] Cabral, L. Lima, M. P. Aquino, J. C. R. Mathpal, M. C. Coaquira, J. A. H. Silva, S. W. da Nagamine, L. C. C. M. Parreiras, S. O. Gastelois, P. L. Marques, G. E. Macedo, W. A. A. |
author2_role |
author author author author author author author author author author author author |
dc.contributor.none.fl_str_mv |
Universidade de Brasília (UnB) Univ Nacl San Agustin Arequipa Universidade Estadual Paulista (Unesp) Universidade Federal de São Carlos (UFSCar) Universidade de São Paulo (USP) CDTN |
dc.contributor.author.fl_str_mv |
Aragon, F. F. H. Villegas-Lelovsky, L. [UNESP] Cabral, L. Lima, M. P. Aquino, J. C. R. Mathpal, M. C. Coaquira, J. A. H. Silva, S. W. da Nagamine, L. C. C. M. Parreiras, S. O. Gastelois, P. L. Marques, G. E. Macedo, W. A. A. |
description |
In this work, we present a coupled experimental and theoretical first-principles investigation on one of the more promising oxide-diluted magnetic semiconductors, the Sn1-xCoxO2 nanoparticle system, in order to see the effect of cobalt doping on the physical and chemical properties. Our findings suggest that progressive surface enrichment with dopant ions plays an essential role in the monotonous quenching of the surface disorder modes. That weakening is associated with the passivation of the oxygen vacancies as the Co excess at the surface becomes larger. Room-temperature Sn-119 Mossbauer spectroscopy data analysis revealed the occurrence of a distribution of isomer shifts, related to the different non-equivalent surroundings of Sn4+ ions and the coexistence of Sn2+/Sn4+ at the particle surfaces provoked by the inhomogeneous distribution of Co ions, in agreement with the X-ray photoelectron spectroscopy measurements. Magnetic measurements revealed a paramagnetic behavior of the Co ions dispersed in the rutile-type matrix with antiferromagnetic correlations, which become stronger as the Co content is increased. Theoretical calculations show that a defect with two Co mediated by a nearby oxygen vacancy is the most likely defect. The predicted effects of this defect complex are in accordance with the experimental results. |
publishDate |
2020 |
dc.date.none.fl_str_mv |
2020-12-10T19:52:01Z 2020-12-10T19:52:01Z 2020-02-14 |
dc.type.status.fl_str_mv |
info:eu-repo/semantics/publishedVersion |
dc.type.driver.fl_str_mv |
info:eu-repo/semantics/article |
format |
article |
status_str |
publishedVersion |
dc.identifier.uri.fl_str_mv |
http://dx.doi.org/10.1039/c9cp05928h Physical Chemistry Chemical Physics. Cambridge: Royal Soc Chemistry, v. 22, n. 6, p. 3702-3714, 2020. 1463-9076 http://hdl.handle.net/11449/196658 10.1039/c9cp05928h WOS:000518683800052 |
url |
http://dx.doi.org/10.1039/c9cp05928h http://hdl.handle.net/11449/196658 |
identifier_str_mv |
Physical Chemistry Chemical Physics. Cambridge: Royal Soc Chemistry, v. 22, n. 6, p. 3702-3714, 2020. 1463-9076 10.1039/c9cp05928h WOS:000518683800052 |
dc.language.iso.fl_str_mv |
eng |
language |
eng |
dc.relation.none.fl_str_mv |
Physical Chemistry Chemical Physics |
dc.rights.driver.fl_str_mv |
info:eu-repo/semantics/openAccess |
eu_rights_str_mv |
openAccess |
dc.format.none.fl_str_mv |
3702-3714 |
dc.publisher.none.fl_str_mv |
Royal Soc Chemistry |
publisher.none.fl_str_mv |
Royal Soc Chemistry |
dc.source.none.fl_str_mv |
Web of Science reponame:Repositório Institucional da UNESP instname:Universidade Estadual Paulista (UNESP) instacron:UNESP |
instname_str |
Universidade Estadual Paulista (UNESP) |
instacron_str |
UNESP |
institution |
UNESP |
reponame_str |
Repositório Institucional da UNESP |
collection |
Repositório Institucional da UNESP |
repository.name.fl_str_mv |
Repositório Institucional da UNESP - Universidade Estadual Paulista (UNESP) |
repository.mail.fl_str_mv |
|
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1799965731255746560 |