Reactive scattering of H2 from Cu(100): comparison of dynamics calculations based on the specific reaction parameter approach to density functional theory with experiment
- Autores
- Sementa, L.; Wijzenbroek, M.; Van Kolck, B. J.; Somers, M. F.; Al-Halabi, A.; Busnengo, Heriberto Fabio; Olsen, R. A.; Kroes, G. J.; Rutkowski, M.; Thewes, C.; Kleimeier, N. F.; Zacharias, H.
- Año de publicación
- 2013
- Idioma
- inglés
- Tipo de recurso
- artículo
- Estado
- versión publicada
- Descripción
- We present new experimental and theoretical results for reactive scattering of dihydrogen from Cu(100). In the new experiments, the associative desorption of H2 is studied in a velocity resolved and final rovibrational state selected manner, using time-of-flight techniques in combination with resonance-enhanced multi-photon ionization laser detection. Average desorption energies and rota- tional quadrupole alignment parameters were obtained in this way for a number of (v = 0, 1) ro- tational states, v being the vibrational quantum number. Results of quantum dynamics calculations based on a potential energy surface computed with a specific reaction parameter (SRP) density func- tional, which was derived earlier for dihydrogen interacting with Cu(111), are compared with the results of the new experiments and with the results of previous molecular beam experiments on sticking of H2 and on rovibrationally elastic and inelastic scattering of H2 and D2 from Cu(100). The calculations use the Born-Oppenheimer and static surface approximations. With the functional derived semi-empirically for dihydrogen + Cu(111), a chemically accurate description is obtained of the molecular beam experiments on sticking of H2 on Cu(100), and a highly accurate descrip- tion is obtained of rovibrationally elastic and inelastic scattering of D2 from Cu(100) and of the orientational dependence of the reaction of (v = 1, j = 2 − 4) H2 on Cu(100). This suggests that a SRP density functional derived for H2 interacting with a specific low index face of a metal will yield accurate results for H2 reactively scattering from another low index face of the same metal, and that it may also yield accurate results for H2 interacting with a defected (e.g., stepped) surface of that same metal, in a system of catalytic interest. However, the description that was obtained of the average desorption energies, of rovibrationally elastic and inelastic scattering of H2 from Cu(100), and of the orientational dependence of reaction of (v = 0, j = 3 − 5, 8) H2 on Cu(100) compares less well with the available experiments. More research is needed to establish whether more accurate SRP-density functional theory dynamics results can be obtained for these observables if surface atom motion is added to the dynamical model. The experimentally and theoretically found dependence of the rotational quadrupole alignment parameter on the rotational quantum number provides evidence for rotational enhancement of reaction at low translational energies.
Fil: Sementa, L.. Leiden University; Países Bajos. Istituto per i Processi Chimico-Fisici of the Consiglio Nazionale delle Ricerche; Italia
Fil: Wijzenbroek, M.. Leiden University; Países Bajos
Fil: Van Kolck, B. J.. Leiden University; Países Bajos
Fil: Somers, M. F.. Leiden University; Países Bajos
Fil: Al-Halabi, A.. Leiden University; Países Bajos
Fil: Busnengo, Heriberto Fabio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Rosario. Instituto de Física de Rosario (i); Argentina
Fil: Olsen, R. A.. Leiden University; Países Bajos. SINTEF Materials and Chemistry; Noruega
Fil: Kroes, G. J.. Leiden University; Países Bajos
Fil: Rutkowski, M.. Westfalische Wilhelms Universitat; Alemania
Fil: Thewes, C.. Westfalische Wilhelms Universitat; Alemania
Fil: Kleimeier, N. F.. Westfalische Wilhelms Universitat; Alemania
Fil: Zacharias, H.. Westfalische Wilhelms Universitat; Alemania - Materia
-
SURFACES
HYDROGEN
DFT - Nivel de accesibilidad
- acceso abierto
- Condiciones de uso
- https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
- Repositorio
- Institución
- Consejo Nacional de Investigaciones Científicas y Técnicas
- OAI Identificador
- oai:ri.conicet.gov.ar:11336/5971
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Reactive scattering of H2 from Cu(100): comparison of dynamics calculations based on the specific reaction parameter approach to density functional theory with experimentSementa, L.Wijzenbroek, M.Van Kolck, B. J.Somers, M. F.Al-Halabi, A.Busnengo, Heriberto FabioOlsen, R. A.Kroes, G. J.Rutkowski, M.Thewes, C.Kleimeier, N. F.Zacharias, H.SURFACESHYDROGENDFThttps://purl.org/becyt/ford/1.3https://purl.org/becyt/ford/1We present new experimental and theoretical results for reactive scattering of dihydrogen from Cu(100). In the new experiments, the associative desorption of H2 is studied in a velocity resolved and final rovibrational state selected manner, using time-of-flight techniques in combination with resonance-enhanced multi-photon ionization laser detection. Average desorption energies and rota- tional quadrupole alignment parameters were obtained in this way for a number of (v = 0, 1) ro- tational states, v being the vibrational quantum number. Results of quantum dynamics calculations based on a potential energy surface computed with a specific reaction parameter (SRP) density func- tional, which was derived earlier for dihydrogen interacting with Cu(111), are compared with the results of the new experiments and with the results of previous molecular beam experiments on sticking of H2 and on rovibrationally elastic and inelastic scattering of H2 and D2 from Cu(100). The calculations use the Born-Oppenheimer and static surface approximations. With the functional derived semi-empirically for dihydrogen + Cu(111), a chemically accurate description is obtained of the molecular beam experiments on sticking of H2 on Cu(100), and a highly accurate descrip- tion is obtained of rovibrationally elastic and inelastic scattering of D2 from Cu(100) and of the orientational dependence of the reaction of (v = 1, j = 2 − 4) H2 on Cu(100). This suggests that a SRP density functional derived for H2 interacting with a specific low index face of a metal will yield accurate results for H2 reactively scattering from another low index face of the same metal, and that it may also yield accurate results for H2 interacting with a defected (e.g., stepped) surface of that same metal, in a system of catalytic interest. However, the description that was obtained of the average desorption energies, of rovibrationally elastic and inelastic scattering of H2 from Cu(100), and of the orientational dependence of reaction of (v = 0, j = 3 − 5, 8) H2 on Cu(100) compares less well with the available experiments. More research is needed to establish whether more accurate SRP-density functional theory dynamics results can be obtained for these observables if surface atom motion is added to the dynamical model. The experimentally and theoretically found dependence of the rotational quadrupole alignment parameter on the rotational quantum number provides evidence for rotational enhancement of reaction at low translational energies.Fil: Sementa, L.. Leiden University; Países Bajos. Istituto per i Processi Chimico-Fisici of the Consiglio Nazionale delle Ricerche; ItaliaFil: Wijzenbroek, M.. Leiden University; Países BajosFil: Van Kolck, B. J.. Leiden University; Países BajosFil: Somers, M. F.. Leiden University; Países BajosFil: Al-Halabi, A.. Leiden University; Países BajosFil: Busnengo, Heriberto Fabio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Rosario. Instituto de Física de Rosario (i); ArgentinaFil: Olsen, R. A.. Leiden University; Países Bajos. SINTEF Materials and Chemistry; NoruegaFil: Kroes, G. J.. Leiden University; Países BajosFil: Rutkowski, M.. Westfalische Wilhelms Universitat; AlemaniaFil: Thewes, C.. Westfalische Wilhelms Universitat; AlemaniaFil: Kleimeier, N. F.. Westfalische Wilhelms Universitat; AlemaniaFil: Zacharias, H.. Westfalische Wilhelms Universitat; AlemaniaAmerican Institute of Physics2013-01-25info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/5971Sementa, L.; Wijzenbroek, M.; Van Kolck, B. J.; Somers, M. F.; Al-Halabi, A.; et al.; Reactive scattering of H2 from Cu(100): comparison of dynamics calculations based on the specific reaction parameter approach to density functional theory with experiment; American Institute of Physics; Journal of Chemical Physics; 138; 4; 25-1-2013; 44708-447270021-9606enginfo:eu-repo/semantics/altIdentifier/doi/info:eu-repo/semantics/altIdentifier/doi/10.1063/1.4776224info:eu-repo/semantics/altIdentifier/url/http://scitation.aip.org/content/aip/journal/jcp/138/4/10.1063/1.4776224info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T10:15:49Zoai:ri.conicet.gov.ar:11336/5971instacron: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 10:15:49.433CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse |
dc.title.none.fl_str_mv |
Reactive scattering of H2 from Cu(100): comparison of dynamics calculations based on the specific reaction parameter approach to density functional theory with experiment |
title |
Reactive scattering of H2 from Cu(100): comparison of dynamics calculations based on the specific reaction parameter approach to density functional theory with experiment |
spellingShingle |
Reactive scattering of H2 from Cu(100): comparison of dynamics calculations based on the specific reaction parameter approach to density functional theory with experiment Sementa, L. SURFACES HYDROGEN DFT |
title_short |
Reactive scattering of H2 from Cu(100): comparison of dynamics calculations based on the specific reaction parameter approach to density functional theory with experiment |
title_full |
Reactive scattering of H2 from Cu(100): comparison of dynamics calculations based on the specific reaction parameter approach to density functional theory with experiment |
title_fullStr |
Reactive scattering of H2 from Cu(100): comparison of dynamics calculations based on the specific reaction parameter approach to density functional theory with experiment |
title_full_unstemmed |
Reactive scattering of H2 from Cu(100): comparison of dynamics calculations based on the specific reaction parameter approach to density functional theory with experiment |
title_sort |
Reactive scattering of H2 from Cu(100): comparison of dynamics calculations based on the specific reaction parameter approach to density functional theory with experiment |
dc.creator.none.fl_str_mv |
Sementa, L. Wijzenbroek, M. Van Kolck, B. J. Somers, M. F. Al-Halabi, A. Busnengo, Heriberto Fabio Olsen, R. A. Kroes, G. J. Rutkowski, M. Thewes, C. Kleimeier, N. F. Zacharias, H. |
author |
Sementa, L. |
author_facet |
Sementa, L. Wijzenbroek, M. Van Kolck, B. J. Somers, M. F. Al-Halabi, A. Busnengo, Heriberto Fabio Olsen, R. A. Kroes, G. J. Rutkowski, M. Thewes, C. Kleimeier, N. F. Zacharias, H. |
author_role |
author |
author2 |
Wijzenbroek, M. Van Kolck, B. J. Somers, M. F. Al-Halabi, A. Busnengo, Heriberto Fabio Olsen, R. A. Kroes, G. J. Rutkowski, M. Thewes, C. Kleimeier, N. F. Zacharias, H. |
author2_role |
author author author author author author author author author author author |
dc.subject.none.fl_str_mv |
SURFACES HYDROGEN DFT |
topic |
SURFACES HYDROGEN DFT |
purl_subject.fl_str_mv |
https://purl.org/becyt/ford/1.3 https://purl.org/becyt/ford/1 |
dc.description.none.fl_txt_mv |
We present new experimental and theoretical results for reactive scattering of dihydrogen from Cu(100). In the new experiments, the associative desorption of H2 is studied in a velocity resolved and final rovibrational state selected manner, using time-of-flight techniques in combination with resonance-enhanced multi-photon ionization laser detection. Average desorption energies and rota- tional quadrupole alignment parameters were obtained in this way for a number of (v = 0, 1) ro- tational states, v being the vibrational quantum number. Results of quantum dynamics calculations based on a potential energy surface computed with a specific reaction parameter (SRP) density func- tional, which was derived earlier for dihydrogen interacting with Cu(111), are compared with the results of the new experiments and with the results of previous molecular beam experiments on sticking of H2 and on rovibrationally elastic and inelastic scattering of H2 and D2 from Cu(100). The calculations use the Born-Oppenheimer and static surface approximations. With the functional derived semi-empirically for dihydrogen + Cu(111), a chemically accurate description is obtained of the molecular beam experiments on sticking of H2 on Cu(100), and a highly accurate descrip- tion is obtained of rovibrationally elastic and inelastic scattering of D2 from Cu(100) and of the orientational dependence of the reaction of (v = 1, j = 2 − 4) H2 on Cu(100). This suggests that a SRP density functional derived for H2 interacting with a specific low index face of a metal will yield accurate results for H2 reactively scattering from another low index face of the same metal, and that it may also yield accurate results for H2 interacting with a defected (e.g., stepped) surface of that same metal, in a system of catalytic interest. However, the description that was obtained of the average desorption energies, of rovibrationally elastic and inelastic scattering of H2 from Cu(100), and of the orientational dependence of reaction of (v = 0, j = 3 − 5, 8) H2 on Cu(100) compares less well with the available experiments. More research is needed to establish whether more accurate SRP-density functional theory dynamics results can be obtained for these observables if surface atom motion is added to the dynamical model. The experimentally and theoretically found dependence of the rotational quadrupole alignment parameter on the rotational quantum number provides evidence for rotational enhancement of reaction at low translational energies. Fil: Sementa, L.. Leiden University; Países Bajos. Istituto per i Processi Chimico-Fisici of the Consiglio Nazionale delle Ricerche; Italia Fil: Wijzenbroek, M.. Leiden University; Países Bajos Fil: Van Kolck, B. J.. Leiden University; Países Bajos Fil: Somers, M. F.. Leiden University; Países Bajos Fil: Al-Halabi, A.. Leiden University; Países Bajos Fil: Busnengo, Heriberto Fabio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Rosario. Instituto de Física de Rosario (i); Argentina Fil: Olsen, R. A.. Leiden University; Países Bajos. SINTEF Materials and Chemistry; Noruega Fil: Kroes, G. J.. Leiden University; Países Bajos Fil: Rutkowski, M.. Westfalische Wilhelms Universitat; Alemania Fil: Thewes, C.. Westfalische Wilhelms Universitat; Alemania Fil: Kleimeier, N. F.. Westfalische Wilhelms Universitat; Alemania Fil: Zacharias, H.. Westfalische Wilhelms Universitat; Alemania |
description |
We present new experimental and theoretical results for reactive scattering of dihydrogen from Cu(100). In the new experiments, the associative desorption of H2 is studied in a velocity resolved and final rovibrational state selected manner, using time-of-flight techniques in combination with resonance-enhanced multi-photon ionization laser detection. Average desorption energies and rota- tional quadrupole alignment parameters were obtained in this way for a number of (v = 0, 1) ro- tational states, v being the vibrational quantum number. Results of quantum dynamics calculations based on a potential energy surface computed with a specific reaction parameter (SRP) density func- tional, which was derived earlier for dihydrogen interacting with Cu(111), are compared with the results of the new experiments and with the results of previous molecular beam experiments on sticking of H2 and on rovibrationally elastic and inelastic scattering of H2 and D2 from Cu(100). The calculations use the Born-Oppenheimer and static surface approximations. With the functional derived semi-empirically for dihydrogen + Cu(111), a chemically accurate description is obtained of the molecular beam experiments on sticking of H2 on Cu(100), and a highly accurate descrip- tion is obtained of rovibrationally elastic and inelastic scattering of D2 from Cu(100) and of the orientational dependence of the reaction of (v = 1, j = 2 − 4) H2 on Cu(100). This suggests that a SRP density functional derived for H2 interacting with a specific low index face of a metal will yield accurate results for H2 reactively scattering from another low index face of the same metal, and that it may also yield accurate results for H2 interacting with a defected (e.g., stepped) surface of that same metal, in a system of catalytic interest. However, the description that was obtained of the average desorption energies, of rovibrationally elastic and inelastic scattering of H2 from Cu(100), and of the orientational dependence of reaction of (v = 0, j = 3 − 5, 8) H2 on Cu(100) compares less well with the available experiments. More research is needed to establish whether more accurate SRP-density functional theory dynamics results can be obtained for these observables if surface atom motion is added to the dynamical model. The experimentally and theoretically found dependence of the rotational quadrupole alignment parameter on the rotational quantum number provides evidence for rotational enhancement of reaction at low translational energies. |
publishDate |
2013 |
dc.date.none.fl_str_mv |
2013-01-25 |
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/11336/5971 Sementa, L.; Wijzenbroek, M.; Van Kolck, B. J.; Somers, M. F.; Al-Halabi, A.; et al.; Reactive scattering of H2 from Cu(100): comparison of dynamics calculations based on the specific reaction parameter approach to density functional theory with experiment; American Institute of Physics; Journal of Chemical Physics; 138; 4; 25-1-2013; 44708-44727 0021-9606 |
url |
http://hdl.handle.net/11336/5971 |
identifier_str_mv |
Sementa, L.; Wijzenbroek, M.; Van Kolck, B. J.; Somers, M. F.; Al-Halabi, A.; et al.; Reactive scattering of H2 from Cu(100): comparison of dynamics calculations based on the specific reaction parameter approach to density functional theory with experiment; American Institute of Physics; Journal of Chemical Physics; 138; 4; 25-1-2013; 44708-44727 0021-9606 |
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/10.1063/1.4776224 info:eu-repo/semantics/altIdentifier/url/http://scitation.aip.org/content/aip/journal/jcp/138/4/10.1063/1.4776224 |
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 |
American Institute of Physics |
publisher.none.fl_str_mv |
American Institute of Physics |
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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13.070432 |