7D Quantum Dynamicsof H2 scattering form Cu(111): the accuracy of the phonon sudden approximation

Autores
Bonfanti, Matteo; Somers, Mark F.; Díaz, Cristina; Busnengo, Heriberto Fabio; Kroes, Geert Jan
Año de publicación
2013
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
The correct prediction of elementary processes occurring when H 2 scatters from a metal surface is one of the main challenges of surface science. In the field, the scattering of H 2 from Cu(111) has been considered a prototype system for activated dissociative chemisorption. Experimental and theoretical work suggested that a proper description of some scattering experiments on this system might require going beyond the static surface approximation, to consider how the motion of the Cu atoms affects the scattering event. Previous work suggested that important effects of phonons on the dynamics can be incorporated in the Potential Energy Surface (PES) by including four degrees of freedom, that have approximately additive couplings with the hydrogen molecule: the 3 dimensional motion of the nearest 1st layer copper atom and the displacement of the nearest 2nd layer copper atom along the direction perpendicular to the surface [3]. In the present work, we extend the 6D dynamical model by including the perpendicular motion of the 2nd layer surface atom and we study this novel dynamical model with two techniques: an approximate method based on the Phonon Sudden Approximation (PSA) and an exact description using 7D wavepacket quantum dynamics. We consider how the inclusion and the excitation of the lattice degree of freedom affect some relevant processes: dissociative chemisorption, vibrational excitation of H2 and state-to-state scattering probabilities fully resolved with respect to the vibrational states of the surface. We show that the PSA works in an excellent way for the system, thereby suggesting that this might be a viable way to study higher dimensional quantum models, incorporating four surface degrees of freedom that appear to be most relevant for H2 scattering.
Fil: Bonfanti, Matteo. Leiden University; Países Bajos
Fil: Somers, Mark F.. Leiden University; Países Bajos
Fil: Díaz, Cristina. Universidad Autónoma de Madrid; España
Fil: Busnengo, Heriberto Fabio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Rosario. Instituto de Física de Rosario (i); Argentina. Universidad Nacional de Rosario. Facultad de Ciencias Exactas, Ingeniería y Agrimensura; Argentina
Fil: Kroes, Geert Jan. Leiden University; Países Bajos
Materia
SURFACES
DFT
HYDROGEN
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/5974

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network_name_str CONICET Digital (CONICET)
spelling 7D Quantum Dynamicsof H2 scattering form Cu(111): the accuracy of the phonon sudden approximationBonfanti, MatteoSomers, Mark F.Díaz, CristinaBusnengo, Heriberto FabioKroes, Geert JanSURFACESDFTHYDROGENhttps://purl.org/becyt/ford/1.3https://purl.org/becyt/ford/1The correct prediction of elementary processes occurring when H 2 scatters from a metal surface is one of the main challenges of surface science. In the field, the scattering of H 2 from Cu(111) has been considered a prototype system for activated dissociative chemisorption. Experimental and theoretical work suggested that a proper description of some scattering experiments on this system might require going beyond the static surface approximation, to consider how the motion of the Cu atoms affects the scattering event. Previous work suggested that important effects of phonons on the dynamics can be incorporated in the Potential Energy Surface (PES) by including four degrees of freedom, that have approximately additive couplings with the hydrogen molecule: the 3 dimensional motion of the nearest 1st layer copper atom and the displacement of the nearest 2nd layer copper atom along the direction perpendicular to the surface [3]. In the present work, we extend the 6D dynamical model by including the perpendicular motion of the 2nd layer surface atom and we study this novel dynamical model with two techniques: an approximate method based on the Phonon Sudden Approximation (PSA) and an exact description using 7D wavepacket quantum dynamics. We consider how the inclusion and the excitation of the lattice degree of freedom affect some relevant processes: dissociative chemisorption, vibrational excitation of H2 and state-to-state scattering probabilities fully resolved with respect to the vibrational states of the surface. We show that the PSA works in an excellent way for the system, thereby suggesting that this might be a viable way to study higher dimensional quantum models, incorporating four surface degrees of freedom that appear to be most relevant for H2 scattering.Fil: Bonfanti, Matteo. Leiden University; Países BajosFil: Somers, Mark F.. Leiden University; Países BajosFil: Díaz, Cristina. Universidad Autónoma de Madrid; EspañaFil: Busnengo, Heriberto Fabio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Rosario. Instituto de Física de Rosario (i); Argentina. Universidad Nacional de Rosario. Facultad de Ciencias Exactas, Ingeniería y Agrimensura; ArgentinaFil: Kroes, Geert Jan. Leiden University; Países BajosOldenbourg Verlag2013-06info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/5974Bonfanti, Matteo; Somers, Mark F.; Díaz, Cristina; Busnengo, Heriberto Fabio; Kroes, Geert Jan; 7D Quantum Dynamicsof H2 scattering form Cu(111): the accuracy of the phonon sudden approximation; Oldenbourg Verlag; Zeitschrift Für Physikalische Chemie; 227; 9-11; 6-2013; 1397-14200942-9352enginfo:eu-repo/semantics/altIdentifier/doi/info:eu-repo/semantics/altIdentifier/doi/10.1524/zpch.2013.0405info:eu-repo/semantics/altIdentifier/url/http://www.degruyter.com/view/j/zpch.2013.227.issue-9-11/zpch-2013-0405/zpch-2013-0405.xmlinfo:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T09:41:21Zoai:ri.conicet.gov.ar:11336/5974instacron: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 09:41:21.893CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv 7D Quantum Dynamicsof H2 scattering form Cu(111): the accuracy of the phonon sudden approximation
title 7D Quantum Dynamicsof H2 scattering form Cu(111): the accuracy of the phonon sudden approximation
spellingShingle 7D Quantum Dynamicsof H2 scattering form Cu(111): the accuracy of the phonon sudden approximation
Bonfanti, Matteo
SURFACES
DFT
HYDROGEN
title_short 7D Quantum Dynamicsof H2 scattering form Cu(111): the accuracy of the phonon sudden approximation
title_full 7D Quantum Dynamicsof H2 scattering form Cu(111): the accuracy of the phonon sudden approximation
title_fullStr 7D Quantum Dynamicsof H2 scattering form Cu(111): the accuracy of the phonon sudden approximation
title_full_unstemmed 7D Quantum Dynamicsof H2 scattering form Cu(111): the accuracy of the phonon sudden approximation
title_sort 7D Quantum Dynamicsof H2 scattering form Cu(111): the accuracy of the phonon sudden approximation
dc.creator.none.fl_str_mv Bonfanti, Matteo
Somers, Mark F.
Díaz, Cristina
Busnengo, Heriberto Fabio
Kroes, Geert Jan
author Bonfanti, Matteo
author_facet Bonfanti, Matteo
Somers, Mark F.
Díaz, Cristina
Busnengo, Heriberto Fabio
Kroes, Geert Jan
author_role author
author2 Somers, Mark F.
Díaz, Cristina
Busnengo, Heriberto Fabio
Kroes, Geert Jan
author2_role author
author
author
author
dc.subject.none.fl_str_mv SURFACES
DFT
HYDROGEN
topic SURFACES
DFT
HYDROGEN
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 correct prediction of elementary processes occurring when H 2 scatters from a metal surface is one of the main challenges of surface science. In the field, the scattering of H 2 from Cu(111) has been considered a prototype system for activated dissociative chemisorption. Experimental and theoretical work suggested that a proper description of some scattering experiments on this system might require going beyond the static surface approximation, to consider how the motion of the Cu atoms affects the scattering event. Previous work suggested that important effects of phonons on the dynamics can be incorporated in the Potential Energy Surface (PES) by including four degrees of freedom, that have approximately additive couplings with the hydrogen molecule: the 3 dimensional motion of the nearest 1st layer copper atom and the displacement of the nearest 2nd layer copper atom along the direction perpendicular to the surface [3]. In the present work, we extend the 6D dynamical model by including the perpendicular motion of the 2nd layer surface atom and we study this novel dynamical model with two techniques: an approximate method based on the Phonon Sudden Approximation (PSA) and an exact description using 7D wavepacket quantum dynamics. We consider how the inclusion and the excitation of the lattice degree of freedom affect some relevant processes: dissociative chemisorption, vibrational excitation of H2 and state-to-state scattering probabilities fully resolved with respect to the vibrational states of the surface. We show that the PSA works in an excellent way for the system, thereby suggesting that this might be a viable way to study higher dimensional quantum models, incorporating four surface degrees of freedom that appear to be most relevant for H2 scattering.
Fil: Bonfanti, Matteo. Leiden University; Países Bajos
Fil: Somers, Mark F.. Leiden University; Países Bajos
Fil: Díaz, Cristina. Universidad Autónoma de Madrid; España
Fil: Busnengo, Heriberto Fabio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Rosario. Instituto de Física de Rosario (i); Argentina. Universidad Nacional de Rosario. Facultad de Ciencias Exactas, Ingeniería y Agrimensura; Argentina
Fil: Kroes, Geert Jan. Leiden University; Países Bajos
description The correct prediction of elementary processes occurring when H 2 scatters from a metal surface is one of the main challenges of surface science. In the field, the scattering of H 2 from Cu(111) has been considered a prototype system for activated dissociative chemisorption. Experimental and theoretical work suggested that a proper description of some scattering experiments on this system might require going beyond the static surface approximation, to consider how the motion of the Cu atoms affects the scattering event. Previous work suggested that important effects of phonons on the dynamics can be incorporated in the Potential Energy Surface (PES) by including four degrees of freedom, that have approximately additive couplings with the hydrogen molecule: the 3 dimensional motion of the nearest 1st layer copper atom and the displacement of the nearest 2nd layer copper atom along the direction perpendicular to the surface [3]. In the present work, we extend the 6D dynamical model by including the perpendicular motion of the 2nd layer surface atom and we study this novel dynamical model with two techniques: an approximate method based on the Phonon Sudden Approximation (PSA) and an exact description using 7D wavepacket quantum dynamics. We consider how the inclusion and the excitation of the lattice degree of freedom affect some relevant processes: dissociative chemisorption, vibrational excitation of H2 and state-to-state scattering probabilities fully resolved with respect to the vibrational states of the surface. We show that the PSA works in an excellent way for the system, thereby suggesting that this might be a viable way to study higher dimensional quantum models, incorporating four surface degrees of freedom that appear to be most relevant for H2 scattering.
publishDate 2013
dc.date.none.fl_str_mv 2013-06
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/11336/5974
Bonfanti, Matteo; Somers, Mark F.; Díaz, Cristina; Busnengo, Heriberto Fabio; Kroes, Geert Jan; 7D Quantum Dynamicsof H2 scattering form Cu(111): the accuracy of the phonon sudden approximation; Oldenbourg Verlag; Zeitschrift Für Physikalische Chemie; 227; 9-11; 6-2013; 1397-1420
0942-9352
url http://hdl.handle.net/11336/5974
identifier_str_mv Bonfanti, Matteo; Somers, Mark F.; Díaz, Cristina; Busnengo, Heriberto Fabio; Kroes, Geert Jan; 7D Quantum Dynamicsof H2 scattering form Cu(111): the accuracy of the phonon sudden approximation; Oldenbourg Verlag; Zeitschrift Für Physikalische Chemie; 227; 9-11; 6-2013; 1397-1420
0942-9352
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/
info:eu-repo/semantics/altIdentifier/doi/10.1524/zpch.2013.0405
info:eu-repo/semantics/altIdentifier/url/http://www.degruyter.com/view/j/zpch.2013.227.issue-9-11/zpch-2013-0405/zpch-2013-0405.xml
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
dc.publisher.none.fl_str_mv Oldenbourg Verlag
publisher.none.fl_str_mv Oldenbourg Verlag
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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