Normal and off-normal incidence dissociative dynamics of O 2 ( v , J ) on ultrathin Cu films grown on Ru(0001)

Autores
Fallaque, J. G.; Ramos Acevedo, Maximiliano; Busnengo, Heriberto Fabio; Martín, F.; Díaz, C.
Año de publicación
2020
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
The dissociative adsorption of molecular oxygen on metal surfaces has long been controversial, mostly due to the spin-triplet nature of its ground state, to possible non-adiabatic effects, such as an abrupt charge transfer from the metal to the molecule, or even to the role played by the surface electronic state. Here, we have studied the dissociative adsorption of O2on CuML/Ru(0001) at normal and off-normal incidence, from thermal to super-thermal energies, using quasi-classical dynamics, in the framework of the generalized Langevin oscillator model, and density functional theory based on a multidimensional potential energy surface. Our simulations reveal a rather intriguing behavior of dissociative adsorption probabilities, which exhibit normal energy scaling at incidence energies below the reaction barriers and total energy scaling above, irrespective of the reaction channel, either direct dissociation, trapping dissociation, or molecular adsorption. We directly compare our results with existing scanning tunneling spectroscopy and microscopy measurements. From this comparison, we infer that the observed experimental behavior at thermal energies may be due to ligand and strain effects, as already found for super-thermal incidence energies.
Fil: Fallaque, J. G.. Universidad Autónoma de Madrid; España. Instituto Madrileño de Estudios Avanzados en Nanociencia; España
Fil: Ramos Acevedo, Maximiliano. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Rosario. Instituto de Física de Rosario. Universidad Nacional de Rosario. Instituto de Física de Rosario; Argentina
Fil: Busnengo, Heriberto Fabio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Rosario. Instituto de Física de Rosario. Universidad Nacional de Rosario. Instituto de Física de Rosario; Argentina
Fil: Martín, F.. Universidad Autónoma de Madrid; España. Instituto Madrileño de Estudios Avanzados en Nanociencia; España
Fil: Díaz, C.. Universidad Complutense de Madrid; España
Materia
SURFACES
MOLECULE
MOLECULAR DYNAMICS
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/183640
Acceder
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network_name_str CONICET Digital (CONICET)
spelling Normal and off-normal incidence dissociative dynamics of O 2 ( v , J ) on ultrathin Cu films grown on Ru(0001)Fallaque, J. G.Ramos Acevedo, MaximilianoBusnengo, Heriberto FabioMartín, F.Díaz, C.SURFACESMOLECULEMOLECULAR DYNAMICShttps://purl.org/becyt/ford/1.3https://purl.org/becyt/ford/1The dissociative adsorption of molecular oxygen on metal surfaces has long been controversial, mostly due to the spin-triplet nature of its ground state, to possible non-adiabatic effects, such as an abrupt charge transfer from the metal to the molecule, or even to the role played by the surface electronic state. Here, we have studied the dissociative adsorption of O2on CuML/Ru(0001) at normal and off-normal incidence, from thermal to super-thermal energies, using quasi-classical dynamics, in the framework of the generalized Langevin oscillator model, and density functional theory based on a multidimensional potential energy surface. Our simulations reveal a rather intriguing behavior of dissociative adsorption probabilities, which exhibit normal energy scaling at incidence energies below the reaction barriers and total energy scaling above, irrespective of the reaction channel, either direct dissociation, trapping dissociation, or molecular adsorption. We directly compare our results with existing scanning tunneling spectroscopy and microscopy measurements. From this comparison, we infer that the observed experimental behavior at thermal energies may be due to ligand and strain effects, as already found for super-thermal incidence energies.Fil: Fallaque, J. G.. Universidad Autónoma de Madrid; España. Instituto Madrileño de Estudios Avanzados en Nanociencia; EspañaFil: Ramos Acevedo, Maximiliano. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Rosario. Instituto de Física de Rosario. Universidad Nacional de Rosario. Instituto de Física de Rosario; ArgentinaFil: Busnengo, Heriberto Fabio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Rosario. Instituto de Física de Rosario. Universidad Nacional de Rosario. Instituto de Física de Rosario; ArgentinaFil: Martín, F.. Universidad Autónoma de Madrid; España. Instituto Madrileño de Estudios Avanzados en Nanociencia; EspañaFil: Díaz, C.. Universidad Complutense de Madrid; EspañaRoyal Society of Chemistry2020-09info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/183640Fallaque, J. G.; Ramos Acevedo, Maximiliano; Busnengo, Heriberto Fabio; Martín, F.; Díaz, C.; Normal and off-normal incidence dissociative dynamics of O 2 ( v , J ) on ultrathin Cu films grown on Ru(0001); Royal Society of Chemistry; Physical Chemistry Chemical Physics; 23; 13; 9-2020; 7768-77761463-9076CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/http://xlink.rsc.org/?DOI=D0CP03979Ainfo:eu-repo/semantics/altIdentifier/doi/10.1039/D0CP03979Ainfo:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-17T10:57:20Zoai:ri.conicet.gov.ar:11336/183640instacron:CONICETInstitucionalhttp://ri.conicet.gov.ar/Organismo científico-tecnológicoNo correspondehttp://ri.conicet.gov.ar/oai/requestdasensio@conicet.gov.ar; lcarlino@conicet.gov.arArgentinaNo correspondeNo correspondeNo correspondeopendoar:34982025-09-17 10:57:20.702CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Normal and off-normal incidence dissociative dynamics of O 2 ( v , J ) on ultrathin Cu films grown on Ru(0001)
title Normal and off-normal incidence dissociative dynamics of O 2 ( v , J ) on ultrathin Cu films grown on Ru(0001)
spellingShingle Normal and off-normal incidence dissociative dynamics of O 2 ( v , J ) on ultrathin Cu films grown on Ru(0001)
Fallaque, J. G.
SURFACES
MOLECULE
MOLECULAR DYNAMICS
title_short Normal and off-normal incidence dissociative dynamics of O 2 ( v , J ) on ultrathin Cu films grown on Ru(0001)
title_full Normal and off-normal incidence dissociative dynamics of O 2 ( v , J ) on ultrathin Cu films grown on Ru(0001)
title_fullStr Normal and off-normal incidence dissociative dynamics of O 2 ( v , J ) on ultrathin Cu films grown on Ru(0001)
title_full_unstemmed Normal and off-normal incidence dissociative dynamics of O 2 ( v , J ) on ultrathin Cu films grown on Ru(0001)
title_sort Normal and off-normal incidence dissociative dynamics of O 2 ( v , J ) on ultrathin Cu films grown on Ru(0001)
dc.creator.none.fl_str_mv Fallaque, J. G.
Ramos Acevedo, Maximiliano
Busnengo, Heriberto Fabio
Martín, F.
Díaz, C.
author Fallaque, J. G.
author_facet Fallaque, J. G.
Ramos Acevedo, Maximiliano
Busnengo, Heriberto Fabio
Martín, F.
Díaz, C.
author_role author
author2 Ramos Acevedo, Maximiliano
Busnengo, Heriberto Fabio
Martín, F.
Díaz, C.
author2_role author
author
author
author
dc.subject.none.fl_str_mv SURFACES
MOLECULE
MOLECULAR DYNAMICS
topic SURFACES
MOLECULE
MOLECULAR DYNAMICS
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.3
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv The dissociative adsorption of molecular oxygen on metal surfaces has long been controversial, mostly due to the spin-triplet nature of its ground state, to possible non-adiabatic effects, such as an abrupt charge transfer from the metal to the molecule, or even to the role played by the surface electronic state. Here, we have studied the dissociative adsorption of O2on CuML/Ru(0001) at normal and off-normal incidence, from thermal to super-thermal energies, using quasi-classical dynamics, in the framework of the generalized Langevin oscillator model, and density functional theory based on a multidimensional potential energy surface. Our simulations reveal a rather intriguing behavior of dissociative adsorption probabilities, which exhibit normal energy scaling at incidence energies below the reaction barriers and total energy scaling above, irrespective of the reaction channel, either direct dissociation, trapping dissociation, or molecular adsorption. We directly compare our results with existing scanning tunneling spectroscopy and microscopy measurements. From this comparison, we infer that the observed experimental behavior at thermal energies may be due to ligand and strain effects, as already found for super-thermal incidence energies.
Fil: Fallaque, J. G.. Universidad Autónoma de Madrid; España. Instituto Madrileño de Estudios Avanzados en Nanociencia; España
Fil: Ramos Acevedo, Maximiliano. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Rosario. Instituto de Física de Rosario. Universidad Nacional de Rosario. Instituto de Física de Rosario; Argentina
Fil: Busnengo, Heriberto Fabio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Rosario. Instituto de Física de Rosario. Universidad Nacional de Rosario. Instituto de Física de Rosario; Argentina
Fil: Martín, F.. Universidad Autónoma de Madrid; España. Instituto Madrileño de Estudios Avanzados en Nanociencia; España
Fil: Díaz, C.. Universidad Complutense de Madrid; España
description The dissociative adsorption of molecular oxygen on metal surfaces has long been controversial, mostly due to the spin-triplet nature of its ground state, to possible non-adiabatic effects, such as an abrupt charge transfer from the metal to the molecule, or even to the role played by the surface electronic state. Here, we have studied the dissociative adsorption of O2on CuML/Ru(0001) at normal and off-normal incidence, from thermal to super-thermal energies, using quasi-classical dynamics, in the framework of the generalized Langevin oscillator model, and density functional theory based on a multidimensional potential energy surface. Our simulations reveal a rather intriguing behavior of dissociative adsorption probabilities, which exhibit normal energy scaling at incidence energies below the reaction barriers and total energy scaling above, irrespective of the reaction channel, either direct dissociation, trapping dissociation, or molecular adsorption. We directly compare our results with existing scanning tunneling spectroscopy and microscopy measurements. From this comparison, we infer that the observed experimental behavior at thermal energies may be due to ligand and strain effects, as already found for super-thermal incidence energies.
publishDate 2020
dc.date.none.fl_str_mv 2020-09
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
http://purl.org/coar/resource_type/c_6501
info:ar-repo/semantics/articulo
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/11336/183640
Fallaque, J. G.; Ramos Acevedo, Maximiliano; Busnengo, Heriberto Fabio; Martín, F.; Díaz, C.; Normal and off-normal incidence dissociative dynamics of O 2 ( v , J ) on ultrathin Cu films grown on Ru(0001); Royal Society of Chemistry; Physical Chemistry Chemical Physics; 23; 13; 9-2020; 7768-7776
1463-9076
CONICET Digital
CONICET
url http://hdl.handle.net/11336/183640
identifier_str_mv Fallaque, J. G.; Ramos Acevedo, Maximiliano; Busnengo, Heriberto Fabio; Martín, F.; Díaz, C.; Normal and off-normal incidence dissociative dynamics of O 2 ( v , J ) on ultrathin Cu films grown on Ru(0001); Royal Society of Chemistry; Physical Chemistry Chemical Physics; 23; 13; 9-2020; 7768-7776
1463-9076
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/http://xlink.rsc.org/?DOI=D0CP03979A
info:eu-repo/semantics/altIdentifier/doi/10.1039/D0CP03979A
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
dc.publisher.none.fl_str_mv Royal Society of Chemistry
publisher.none.fl_str_mv Royal Society of Chemistry
dc.source.none.fl_str_mv reponame:CONICET Digital (CONICET)
instname:Consejo Nacional de Investigaciones Científicas y Técnicas
reponame_str CONICET Digital (CONICET)
collection CONICET Digital (CONICET)
instname_str Consejo Nacional de Investigaciones Científicas y Técnicas
repository.name.fl_str_mv CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicas
repository.mail.fl_str_mv dasensio@conicet.gov.ar; lcarlino@conicet.gov.ar
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score 13.001348

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