Cutting a chemical bond with demon's scissors: Mode- and bond-selective reactivity of methane on metal surfaces

Autores
Lozano, Ariel; Shen, X. J.; Moiraghi, Raquel; Dong, W.; Busnengo, Heriberto Fabio
Año de publicación
2015
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
In this paper we discuss several aspects of methane reactive sticking on Pt(111) in the light of supersonic molecular beam experiments (including state-resolved measurements) and quasi-classical trajectory calculations based on an accurate reaction specific reactive force field constructed from Density Functional Theory (DFT) data. With the aim of understanding the origin of the full bond selectivity recently achieved experimentally and to predict how selectivity depends on the collision conditions, we discuss in detail, the role of initial translational and (mode-specific) vibrational energy of CH4 and all its deuterated isotopomers, as well as surface temperature effects. Last but not least, the systematic and detailed theoretical analysis presented here serves as an illustration of the possibilities and usefulness of accurate reaction specific reactive force fields built from DFT data. This approach allows investigating dynamical aspects of the interaction of polyatomic molecules on surfaces through quasi-classical trajectory calculations accounting for the full dimensionality of the system (including both molecular and surface degrees of freedom): something that a few years ago was just a dream for the gas-surface dynamics community.
Fil: Lozano, Ariel. 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: Shen, X. J.. Ecole Normale Superieure de Lyon; Francia. Chinese Academy of Sciences; República de China
Fil: Moiraghi, Raquel. 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: Dong, W.. Ecole Normale Superieure de Lyon; Francia
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
Materia
Adsorption
Bond Selectivity
Methane
Molecular Dynamics
Reactive Force Fields
Surfaces
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc-nd/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/51095
Acceder
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network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling Cutting a chemical bond with demon's scissors: Mode- and bond-selective reactivity of methane on metal surfacesLozano, ArielShen, X. J.Moiraghi, RaquelDong, W.Busnengo, Heriberto FabioAdsorptionBond SelectivityMethaneMolecular DynamicsReactive Force FieldsSurfaceshttps://purl.org/becyt/ford/1.3https://purl.org/becyt/ford/1In this paper we discuss several aspects of methane reactive sticking on Pt(111) in the light of supersonic molecular beam experiments (including state-resolved measurements) and quasi-classical trajectory calculations based on an accurate reaction specific reactive force field constructed from Density Functional Theory (DFT) data. With the aim of understanding the origin of the full bond selectivity recently achieved experimentally and to predict how selectivity depends on the collision conditions, we discuss in detail, the role of initial translational and (mode-specific) vibrational energy of CH4 and all its deuterated isotopomers, as well as surface temperature effects. Last but not least, the systematic and detailed theoretical analysis presented here serves as an illustration of the possibilities and usefulness of accurate reaction specific reactive force fields built from DFT data. This approach allows investigating dynamical aspects of the interaction of polyatomic molecules on surfaces through quasi-classical trajectory calculations accounting for the full dimensionality of the system (including both molecular and surface degrees of freedom): something that a few years ago was just a dream for the gas-surface dynamics community.Fil: Lozano, Ariel. 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: Shen, X. J.. Ecole Normale Superieure de Lyon; Francia. Chinese Academy of Sciences; República de ChinaFil: Moiraghi, Raquel. 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: Dong, W.. Ecole Normale Superieure de Lyon; FranciaFil: 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; ArgentinaElsevier Science2015-04info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/51095Lozano, Ariel; Shen, X. J.; Moiraghi, Raquel; Dong, W.; Busnengo, Heriberto Fabio; Cutting a chemical bond with demon's scissors: Mode- and bond-selective reactivity of methane on metal surfaces ; Elsevier Science; Surface Science; 640; 4-2015; 25-350039-6028CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/http://www.sciencedirect.com/science/article/pii/S0039602815000916info:eu-repo/semantics/altIdentifier/doi/10.1016/j.susc.2015.04.002info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-nd/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T09:34:24Zoai:ri.conicet.gov.ar:11336/51095instacron: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:34982025-09-29 09:34:25.221CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv Cutting a chemical bond with demon's scissors: Mode- and bond-selective reactivity of methane on metal surfaces
title Cutting a chemical bond with demon's scissors: Mode- and bond-selective reactivity of methane on metal surfaces
spellingShingle Cutting a chemical bond with demon's scissors: Mode- and bond-selective reactivity of methane on metal surfaces
Lozano, Ariel
Adsorption
Bond Selectivity
Methane
Molecular Dynamics
Reactive Force Fields
Surfaces
title_short Cutting a chemical bond with demon's scissors: Mode- and bond-selective reactivity of methane on metal surfaces
title_full Cutting a chemical bond with demon's scissors: Mode- and bond-selective reactivity of methane on metal surfaces
title_fullStr Cutting a chemical bond with demon's scissors: Mode- and bond-selective reactivity of methane on metal surfaces
title_full_unstemmed Cutting a chemical bond with demon's scissors: Mode- and bond-selective reactivity of methane on metal surfaces
title_sort Cutting a chemical bond with demon's scissors: Mode- and bond-selective reactivity of methane on metal surfaces
dc.creator.none.fl_str_mv Lozano, Ariel
Shen, X. J.
Moiraghi, Raquel
Dong, W.
Busnengo, Heriberto Fabio
author Lozano, Ariel
author_facet Lozano, Ariel
Shen, X. J.
Moiraghi, Raquel
Dong, W.
Busnengo, Heriberto Fabio
author_role author
author2 Shen, X. J.
Moiraghi, Raquel
Dong, W.
Busnengo, Heriberto Fabio
author2_role author
author
author
author
dc.subject.none.fl_str_mv Adsorption
Bond Selectivity
Methane
Molecular Dynamics
Reactive Force Fields
Surfaces
topic Adsorption
Bond Selectivity
Methane
Molecular Dynamics
Reactive Force Fields
Surfaces
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.3
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv In this paper we discuss several aspects of methane reactive sticking on Pt(111) in the light of supersonic molecular beam experiments (including state-resolved measurements) and quasi-classical trajectory calculations based on an accurate reaction specific reactive force field constructed from Density Functional Theory (DFT) data. With the aim of understanding the origin of the full bond selectivity recently achieved experimentally and to predict how selectivity depends on the collision conditions, we discuss in detail, the role of initial translational and (mode-specific) vibrational energy of CH4 and all its deuterated isotopomers, as well as surface temperature effects. Last but not least, the systematic and detailed theoretical analysis presented here serves as an illustration of the possibilities and usefulness of accurate reaction specific reactive force fields built from DFT data. This approach allows investigating dynamical aspects of the interaction of polyatomic molecules on surfaces through quasi-classical trajectory calculations accounting for the full dimensionality of the system (including both molecular and surface degrees of freedom): something that a few years ago was just a dream for the gas-surface dynamics community.
Fil: Lozano, Ariel. 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: Shen, X. J.. Ecole Normale Superieure de Lyon; Francia. Chinese Academy of Sciences; República de China
Fil: Moiraghi, Raquel. 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: Dong, W.. Ecole Normale Superieure de Lyon; Francia
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
description In this paper we discuss several aspects of methane reactive sticking on Pt(111) in the light of supersonic molecular beam experiments (including state-resolved measurements) and quasi-classical trajectory calculations based on an accurate reaction specific reactive force field constructed from Density Functional Theory (DFT) data. With the aim of understanding the origin of the full bond selectivity recently achieved experimentally and to predict how selectivity depends on the collision conditions, we discuss in detail, the role of initial translational and (mode-specific) vibrational energy of CH4 and all its deuterated isotopomers, as well as surface temperature effects. Last but not least, the systematic and detailed theoretical analysis presented here serves as an illustration of the possibilities and usefulness of accurate reaction specific reactive force fields built from DFT data. This approach allows investigating dynamical aspects of the interaction of polyatomic molecules on surfaces through quasi-classical trajectory calculations accounting for the full dimensionality of the system (including both molecular and surface degrees of freedom): something that a few years ago was just a dream for the gas-surface dynamics community.
publishDate 2015
dc.date.none.fl_str_mv 2015-04
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/11336/51095
Lozano, Ariel; Shen, X. J.; Moiraghi, Raquel; Dong, W.; Busnengo, Heriberto Fabio; Cutting a chemical bond with demon's scissors: Mode- and bond-selective reactivity of methane on metal surfaces ; Elsevier Science; Surface Science; 640; 4-2015; 25-35
0039-6028
CONICET Digital
CONICET
url http://hdl.handle.net/11336/51095
identifier_str_mv Lozano, Ariel; Shen, X. J.; Moiraghi, Raquel; Dong, W.; Busnengo, Heriberto Fabio; Cutting a chemical bond with demon's scissors: Mode- and bond-selective reactivity of methane on metal surfaces ; Elsevier Science; Surface Science; 640; 4-2015; 25-35
0039-6028
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://www.sciencedirect.com/science/article/pii/S0039602815000916
info:eu-repo/semantics/altIdentifier/doi/10.1016/j.susc.2015.04.002
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc-nd/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc-nd/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
dc.publisher.none.fl_str_mv Elsevier Science
publisher.none.fl_str_mv Elsevier Science
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 13.070432

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