Ground- and excited-state properties of M-center oxygen vacancy aggregates in the bulk and the surface of MgO

Aggregates of oxygen vacancies (F centers) represent a particular form of point defects in ionic crystals. In this study we have considered the combination of two oxygen vacancies, the M center, in the bulk and on the surface of MgO by means of cluster model calculations. Both neutral and charged fo...

Descripción completa

Detalles Bibliográficos
Autores: Domínguez-Ariza, David, Sousa Romero, Carmen, Illas i Riera, Francesc, Ricci, Davide, Pacchioni, Gianfranco
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2003
País:España
Institución:Universidad de Barcelona
Repositorio:Dipòsit Digital de la UB
OAI Identifier:oai:diposit.ub.edu:2445/10809
Acceso en línea:https://hdl.handle.net/2445/10809
Access Level:acceso abierto
Palabra clave:Defectes cristal·lins
Química de superfícies
Química computacional
Teoria del funcional de densitat
Crystals defects
Surface chemistry
Computational chemistry
Density functional theory
id ES_237be520b01b2b91eca9cf2d9e345dfa
oai_identifier_str oai:diposit.ub.edu:2445/10809
network_acronym_str ES
network_name_str España
repository_id_str
spelling Ground- and excited-state properties of M-center oxygen vacancy aggregates in the bulk and the surface of MgODomínguez-Ariza, DavidSousa Romero, CarmenIllas i Riera, FrancescRicci, DavidePacchioni, GianfrancoDefectes cristal·linsQuímica de superfíciesQuímica computacionalTeoria del funcional de densitatCrystals defectsSurface chemistryComputational chemistryDensity functional theoryAggregates of oxygen vacancies (F centers) represent a particular form of point defects in ionic crystals. In this study we have considered the combination of two oxygen vacancies, the M center, in the bulk and on the surface of MgO by means of cluster model calculations. Both neutral and charged forms of the defect M and M+ have been taken into account. The ground state of the M center is characterized by the presence of two doubly occupied impurity levels in the gap of the material; in M+ centers the highest level is singly occupied. For the ground-state properties we used a gradient corrected density functional theory approach. The dipole-allowed singlet-to-singlet and doublet-to-doublet electronic transitions have been determined by means of explicitly correlated multireference second-order perturbation theory calculations. These have been compared with optical transitions determined with the time-dependent density functional theory formalism. The results show that bulk M and M+ centers give rise to intense absorptions at about 4.4 and 4.0 eV, respectively. Another less intense transition at 1.3 eV has also been found for the M+ center. On the surface the transitions occur at 1.6 eV (M+) and 2 eV (M). The results are compared with recently reported electron energy loss spectroscopy spectra on MgO thin films.The American Physical Society2003info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionapplication/pdfhttps://hdl.handle.net/2445/10809Articles publicats en revistes (Ciència dels Materials i Química Física)reponame:Dipòsit Digital de la UBinstname:Universidad de BarcelonaInglésReproducció digital del document publicat en format paper, proporcionada per PROLA i http://dx.doi.org/10.1103/PhysRevB.68.054101Physical Review B, 2003, vol. 68, núm. 5, p. 054101-1-054101-9http://dx.doi.org/10.1103/PhysRevB.68.054101(c) The American Physical Society, 2003info:eu-repo/semantics/openAccessoai:diposit.ub.edu:2445/108092026-05-27T06:46:51Z
dc.title.none.fl_str_mv Ground- and excited-state properties of M-center oxygen vacancy aggregates in the bulk and the surface of MgO
title Ground- and excited-state properties of M-center oxygen vacancy aggregates in the bulk and the surface of MgO
spellingShingle Ground- and excited-state properties of M-center oxygen vacancy aggregates in the bulk and the surface of MgO
Domínguez-Ariza, David
Defectes cristal·lins
Química de superfícies
Química computacional
Teoria del funcional de densitat
Crystals defects
Surface chemistry
Computational chemistry
Density functional theory
title_short Ground- and excited-state properties of M-center oxygen vacancy aggregates in the bulk and the surface of MgO
title_full Ground- and excited-state properties of M-center oxygen vacancy aggregates in the bulk and the surface of MgO
title_fullStr Ground- and excited-state properties of M-center oxygen vacancy aggregates in the bulk and the surface of MgO
title_full_unstemmed Ground- and excited-state properties of M-center oxygen vacancy aggregates in the bulk and the surface of MgO
title_sort Ground- and excited-state properties of M-center oxygen vacancy aggregates in the bulk and the surface of MgO
dc.creator.none.fl_str_mv Domínguez-Ariza, David
Sousa Romero, Carmen
Illas i Riera, Francesc
Ricci, Davide
Pacchioni, Gianfranco
author Domínguez-Ariza, David
author_facet Domínguez-Ariza, David
Sousa Romero, Carmen
Illas i Riera, Francesc
Ricci, Davide
Pacchioni, Gianfranco
author_role author
author2 Sousa Romero, Carmen
Illas i Riera, Francesc
Ricci, Davide
Pacchioni, Gianfranco
author2_role author
author
author
author
dc.subject.none.fl_str_mv Defectes cristal·lins
Química de superfícies
Química computacional
Teoria del funcional de densitat
Crystals defects
Surface chemistry
Computational chemistry
Density functional theory
topic Defectes cristal·lins
Química de superfícies
Química computacional
Teoria del funcional de densitat
Crystals defects
Surface chemistry
Computational chemistry
Density functional theory
description Aggregates of oxygen vacancies (F centers) represent a particular form of point defects in ionic crystals. In this study we have considered the combination of two oxygen vacancies, the M center, in the bulk and on the surface of MgO by means of cluster model calculations. Both neutral and charged forms of the defect M and M+ have been taken into account. The ground state of the M center is characterized by the presence of two doubly occupied impurity levels in the gap of the material; in M+ centers the highest level is singly occupied. For the ground-state properties we used a gradient corrected density functional theory approach. The dipole-allowed singlet-to-singlet and doublet-to-doublet electronic transitions have been determined by means of explicitly correlated multireference second-order perturbation theory calculations. These have been compared with optical transitions determined with the time-dependent density functional theory formalism. The results show that bulk M and M+ centers give rise to intense absorptions at about 4.4 and 4.0 eV, respectively. Another less intense transition at 1.3 eV has also been found for the M+ center. On the surface the transitions occur at 1.6 eV (M+) and 2 eV (M). The results are compared with recently reported electron energy loss spectroscopy spectra on MgO thin films.
publishDate 2003
dc.date.none.fl_str_mv 2003
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv https://hdl.handle.net/2445/10809
url https://hdl.handle.net/2445/10809
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv Reproducció digital del document publicat en format paper, proporcionada per PROLA i http://dx.doi.org/10.1103/PhysRevB.68.054101
Physical Review B, 2003, vol. 68, núm. 5, p. 054101-1-054101-9
http://dx.doi.org/10.1103/PhysRevB.68.054101
dc.rights.none.fl_str_mv (c) The American Physical Society, 2003
info:eu-repo/semantics/openAccess
rights_invalid_str_mv (c) The American Physical Society, 2003
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv The American Physical Society
publisher.none.fl_str_mv The American Physical Society
dc.source.none.fl_str_mv Articles publicats en revistes (Ciència dels Materials i Química Física)
reponame:Dipòsit Digital de la UB
instname:Universidad de Barcelona
instname_str Universidad de Barcelona
reponame_str Dipòsit Digital de la UB
collection Dipòsit Digital de la UB
repository.name.fl_str_mv
repository.mail.fl_str_mv
_version_ 1869404643752148992
score 15.300724

Similares en LA Referencia