Non-adiabatic effects in F + CHD3 reactive scattering
- Autores
- Palma, Juliana Isabel; Manthe, Uwe
- Año de publicación
- 2017
- Idioma
- inglés
- Tipo de recurso
- artículo
- Estado
- versión publicada
- Descripción
- The effect of non-adiabatic transitions on the F(2P) + CHD3(ν1) → DF + CHD2 and F(2P) + CHD3(ν1) → HF + CD3 reactions is investigated. The dynamics of the nuclei was simulated using trajectory surface hopping and a vibronically and spin-orbit coupled diabatic potential energy matrix. To facilitate the calculations, the fewest switching algorithm of Tully was adapted to the use of a complex diabatic potential energy matrix. For reactions of CHD3 with ground state fluorine atoms, F(2P3/2), the ratio between the previously computed adiabatic cross sections and the non-adiabatic ones was found to range from 1.4 to 2.1. The actual ratio depends on the translational energy and the initial vibrational state of CHD3. The total reactivity of CHD3(ν1 = 1) was found to be always larger than that of CHD3(ν1=0) mainly because of the increase in the cross sections for the HF + CD3 channel. Thus, the inclusion of non-adiabatic transitions in the theoretical treatment cannot resolve the existing disagreement between theory and experiment. Cross sections for the reaction of CHD3 with spin-orbit excited fluorine atoms, F(2P1/2), were found to be significantly smaller than the ones for reaction with F(2P3/2).
Fil: Palma, Juliana Isabel. Universidad Nacional de Quilmes. Departamento de Ciencia y Tecnología; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Manthe, Uwe. Universitat Bielefeld; Alemania - Materia
-
Reaction dynamics
Non-adiabatic effects
F+CH4
F+CHD3 - 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:11336/72613
Ver los metadatos del registro completo
id |
CONICETDig_cf361c8ca8e2777d1271263e6de031b8 |
---|---|
oai_identifier_str |
oai:ri.conicet.gov.ar:11336/72613 |
network_acronym_str |
CONICETDig |
repository_id_str |
3498 |
network_name_str |
CONICET Digital (CONICET) |
spelling |
Non-adiabatic effects in F + CHD3 reactive scatteringPalma, Juliana IsabelManthe, UweReaction dynamicsNon-adiabatic effectsF+CH4F+CHD3https://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1The effect of non-adiabatic transitions on the F(2P) + CHD3(ν1) → DF + CHD2 and F(2P) + CHD3(ν1) → HF + CD3 reactions is investigated. The dynamics of the nuclei was simulated using trajectory surface hopping and a vibronically and spin-orbit coupled diabatic potential energy matrix. To facilitate the calculations, the fewest switching algorithm of Tully was adapted to the use of a complex diabatic potential energy matrix. For reactions of CHD3 with ground state fluorine atoms, F(2P3/2), the ratio between the previously computed adiabatic cross sections and the non-adiabatic ones was found to range from 1.4 to 2.1. The actual ratio depends on the translational energy and the initial vibrational state of CHD3. The total reactivity of CHD3(ν1 = 1) was found to be always larger than that of CHD3(ν1=0) mainly because of the increase in the cross sections for the HF + CD3 channel. Thus, the inclusion of non-adiabatic transitions in the theoretical treatment cannot resolve the existing disagreement between theory and experiment. Cross sections for the reaction of CHD3 with spin-orbit excited fluorine atoms, F(2P1/2), were found to be significantly smaller than the ones for reaction with F(2P3/2).Fil: Palma, Juliana Isabel. Universidad Nacional de Quilmes. Departamento de Ciencia y Tecnología; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; ArgentinaFil: Manthe, Uwe. Universitat Bielefeld; AlemaniaAmerican Institute of Physics2017-06info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/72613Palma, Juliana Isabel; Manthe, Uwe; Non-adiabatic effects in F + CHD3 reactive scattering; American Institute of Physics; Journal of Chemical Physics; 146; 21; 6-2017; 1-9; 2141170021-9606CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1063/1.4984593info:eu-repo/semantics/altIdentifier/url/https://aip.scitation.org/doi/10.1063/1.4984593info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-10-15T15:01:24Zoai:ri.conicet.gov.ar:11336/72613instacron: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:34982025-10-15 15:01:24.485CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse |
dc.title.none.fl_str_mv |
Non-adiabatic effects in F + CHD3 reactive scattering |
title |
Non-adiabatic effects in F + CHD3 reactive scattering |
spellingShingle |
Non-adiabatic effects in F + CHD3 reactive scattering Palma, Juliana Isabel Reaction dynamics Non-adiabatic effects F+CH4 F+CHD3 |
title_short |
Non-adiabatic effects in F + CHD3 reactive scattering |
title_full |
Non-adiabatic effects in F + CHD3 reactive scattering |
title_fullStr |
Non-adiabatic effects in F + CHD3 reactive scattering |
title_full_unstemmed |
Non-adiabatic effects in F + CHD3 reactive scattering |
title_sort |
Non-adiabatic effects in F + CHD3 reactive scattering |
dc.creator.none.fl_str_mv |
Palma, Juliana Isabel Manthe, Uwe |
author |
Palma, Juliana Isabel |
author_facet |
Palma, Juliana Isabel Manthe, Uwe |
author_role |
author |
author2 |
Manthe, Uwe |
author2_role |
author |
dc.subject.none.fl_str_mv |
Reaction dynamics Non-adiabatic effects F+CH4 F+CHD3 |
topic |
Reaction dynamics Non-adiabatic effects F+CH4 F+CHD3 |
purl_subject.fl_str_mv |
https://purl.org/becyt/ford/1.4 https://purl.org/becyt/ford/1 |
dc.description.none.fl_txt_mv |
The effect of non-adiabatic transitions on the F(2P) + CHD3(ν1) → DF + CHD2 and F(2P) + CHD3(ν1) → HF + CD3 reactions is investigated. The dynamics of the nuclei was simulated using trajectory surface hopping and a vibronically and spin-orbit coupled diabatic potential energy matrix. To facilitate the calculations, the fewest switching algorithm of Tully was adapted to the use of a complex diabatic potential energy matrix. For reactions of CHD3 with ground state fluorine atoms, F(2P3/2), the ratio between the previously computed adiabatic cross sections and the non-adiabatic ones was found to range from 1.4 to 2.1. The actual ratio depends on the translational energy and the initial vibrational state of CHD3. The total reactivity of CHD3(ν1 = 1) was found to be always larger than that of CHD3(ν1=0) mainly because of the increase in the cross sections for the HF + CD3 channel. Thus, the inclusion of non-adiabatic transitions in the theoretical treatment cannot resolve the existing disagreement between theory and experiment. Cross sections for the reaction of CHD3 with spin-orbit excited fluorine atoms, F(2P1/2), were found to be significantly smaller than the ones for reaction with F(2P3/2). Fil: Palma, Juliana Isabel. Universidad Nacional de Quilmes. Departamento de Ciencia y Tecnología; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina Fil: Manthe, Uwe. Universitat Bielefeld; Alemania |
description |
The effect of non-adiabatic transitions on the F(2P) + CHD3(ν1) → DF + CHD2 and F(2P) + CHD3(ν1) → HF + CD3 reactions is investigated. The dynamics of the nuclei was simulated using trajectory surface hopping and a vibronically and spin-orbit coupled diabatic potential energy matrix. To facilitate the calculations, the fewest switching algorithm of Tully was adapted to the use of a complex diabatic potential energy matrix. For reactions of CHD3 with ground state fluorine atoms, F(2P3/2), the ratio between the previously computed adiabatic cross sections and the non-adiabatic ones was found to range from 1.4 to 2.1. The actual ratio depends on the translational energy and the initial vibrational state of CHD3. The total reactivity of CHD3(ν1 = 1) was found to be always larger than that of CHD3(ν1=0) mainly because of the increase in the cross sections for the HF + CD3 channel. Thus, the inclusion of non-adiabatic transitions in the theoretical treatment cannot resolve the existing disagreement between theory and experiment. Cross sections for the reaction of CHD3 with spin-orbit excited fluorine atoms, F(2P1/2), were found to be significantly smaller than the ones for reaction with F(2P3/2). |
publishDate |
2017 |
dc.date.none.fl_str_mv |
2017-06 |
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/11336/72613 Palma, Juliana Isabel; Manthe, Uwe; Non-adiabatic effects in F + CHD3 reactive scattering; American Institute of Physics; Journal of Chemical Physics; 146; 21; 6-2017; 1-9; 214117 0021-9606 CONICET Digital CONICET |
url |
http://hdl.handle.net/11336/72613 |
identifier_str_mv |
Palma, Juliana Isabel; Manthe, Uwe; Non-adiabatic effects in F + CHD3 reactive scattering; American Institute of Physics; Journal of Chemical Physics; 146; 21; 6-2017; 1-9; 214117 0021-9606 CONICET Digital CONICET |
dc.language.none.fl_str_mv |
eng |
language |
eng |
dc.relation.none.fl_str_mv |
info:eu-repo/semantics/altIdentifier/doi/10.1063/1.4984593 info:eu-repo/semantics/altIdentifier/url/https://aip.scitation.org/doi/10.1063/1.4984593 |
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 |
_version_ |
1846083154272583680 |
score |
13.22299 |