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
- Institución
- Consejo Nacional de Investigaciones Científicas y Técnicas
- OAI Identificador
- oai:ri.conicet.gov.ar:11336/5974
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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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1844613306641285120 |
score |
13.070432 |