Vibrational dynamics of the FCH4(-) complex
- Autores
- Wodraszka, Robert; Palma, Juliana Isabel; Manthe, Uwe
- Año de publicación
- 2012
- Idioma
- inglés
- Tipo de recurso
- artículo
- Estado
- versión publicada
- Descripción
- Motivated by recent photodetachment experiments studying resonance structures in the transition-state region of the F + CH4 → HF + CH3 reaction, the vibrational dynamics of the precursor complex CH4•F- is investigated. Delocalized vibrational eigenstates of CH4•F- are computed in full dimensionality employing the multiconfigurational time-dependent Hartree (MCTDH) approach and a recently developed iterative diagonalization approach for general multiwell systems. Different types of stereographic coordinates are used, and a corresponding general N-body kinetic energy operator is given. The calculated tunneling splittings of the ground and the lower vibrational excited states of the CH4•F- complex do not significantly exceed 1 cm-1. Comparing the converged MCTDH results for localized vibrational excitations with existing results obtained by normal-mode-based (truncated) vibrational configuration interaction calculations, significantly lower frequencies are found for excitations in the intermolecular modes.
Fil: Wodraszka, Robert. Universitat Bielefeld; Alemania
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
-
MCTDH
Multidymensional quantum dynamics
Vibrational spectrum - Nivel de accesibilidad
- acceso abierto
- Condiciones de uso
- https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
- Repositorio
.jpg)
- Institución
- Consejo Nacional de Investigaciones Científicas y Técnicas
- OAI Identificador
- oai:ri.conicet.gov.ar:11336/189007
Ver los metadatos del registro completo
| id |
CONICETDig_3855675a13609b4fd4d3049c5ee99278 |
|---|---|
| oai_identifier_str |
oai:ri.conicet.gov.ar:11336/189007 |
| network_acronym_str |
CONICETDig |
| repository_id_str |
3498 |
| network_name_str |
CONICET Digital (CONICET) |
| spelling |
Vibrational dynamics of the FCH4(-) complexWodraszka, RobertPalma, Juliana IsabelManthe, UweMCTDHMultidymensional quantum dynamicsVibrational spectrumhttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1Motivated by recent photodetachment experiments studying resonance structures in the transition-state region of the F + CH4 → HF + CH3 reaction, the vibrational dynamics of the precursor complex CH4•F- is investigated. Delocalized vibrational eigenstates of CH4•F- are computed in full dimensionality employing the multiconfigurational time-dependent Hartree (MCTDH) approach and a recently developed iterative diagonalization approach for general multiwell systems. Different types of stereographic coordinates are used, and a corresponding general N-body kinetic energy operator is given. The calculated tunneling splittings of the ground and the lower vibrational excited states of the CH4•F- complex do not significantly exceed 1 cm-1. Comparing the converged MCTDH results for localized vibrational excitations with existing results obtained by normal-mode-based (truncated) vibrational configuration interaction calculations, significantly lower frequencies are found for excitations in the intermolecular modes.Fil: Wodraszka, Robert. Universitat Bielefeld; AlemaniaFil: 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 Chemical Society2012-06info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/189007Wodraszka, Robert; Palma, Juliana Isabel; Manthe, Uwe; Vibrational dynamics of the FCH4(-) complex; American Chemical Society; Journal of Physical Chemistry A; 116; 46; 6-2012; 11249-112591089-5639CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/http://pubs.acs.org/doi/abs/10.1021/jp3052642info:eu-repo/semantics/altIdentifier/doi/10.1021/jp3052642info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-10-22T11:43:01Zoai:ri.conicet.gov.ar:11336/189007instacron: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:34982025-10-22 11:43:01.428CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse |
| dc.title.none.fl_str_mv |
Vibrational dynamics of the FCH4(-) complex |
| title |
Vibrational dynamics of the FCH4(-) complex |
| spellingShingle |
Vibrational dynamics of the FCH4(-) complex Wodraszka, Robert MCTDH Multidymensional quantum dynamics Vibrational spectrum |
| title_short |
Vibrational dynamics of the FCH4(-) complex |
| title_full |
Vibrational dynamics of the FCH4(-) complex |
| title_fullStr |
Vibrational dynamics of the FCH4(-) complex |
| title_full_unstemmed |
Vibrational dynamics of the FCH4(-) complex |
| title_sort |
Vibrational dynamics of the FCH4(-) complex |
| dc.creator.none.fl_str_mv |
Wodraszka, Robert Palma, Juliana Isabel Manthe, Uwe |
| author |
Wodraszka, Robert |
| author_facet |
Wodraszka, Robert Palma, Juliana Isabel Manthe, Uwe |
| author_role |
author |
| author2 |
Palma, Juliana Isabel Manthe, Uwe |
| author2_role |
author author |
| dc.subject.none.fl_str_mv |
MCTDH Multidymensional quantum dynamics Vibrational spectrum |
| topic |
MCTDH Multidymensional quantum dynamics Vibrational spectrum |
| purl_subject.fl_str_mv |
https://purl.org/becyt/ford/1.4 https://purl.org/becyt/ford/1 |
| dc.description.none.fl_txt_mv |
Motivated by recent photodetachment experiments studying resonance structures in the transition-state region of the F + CH4 → HF + CH3 reaction, the vibrational dynamics of the precursor complex CH4•F- is investigated. Delocalized vibrational eigenstates of CH4•F- are computed in full dimensionality employing the multiconfigurational time-dependent Hartree (MCTDH) approach and a recently developed iterative diagonalization approach for general multiwell systems. Different types of stereographic coordinates are used, and a corresponding general N-body kinetic energy operator is given. The calculated tunneling splittings of the ground and the lower vibrational excited states of the CH4•F- complex do not significantly exceed 1 cm-1. Comparing the converged MCTDH results for localized vibrational excitations with existing results obtained by normal-mode-based (truncated) vibrational configuration interaction calculations, significantly lower frequencies are found for excitations in the intermolecular modes. Fil: Wodraszka, Robert. Universitat Bielefeld; Alemania 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 |
Motivated by recent photodetachment experiments studying resonance structures in the transition-state region of the F + CH4 → HF + CH3 reaction, the vibrational dynamics of the precursor complex CH4•F- is investigated. Delocalized vibrational eigenstates of CH4•F- are computed in full dimensionality employing the multiconfigurational time-dependent Hartree (MCTDH) approach and a recently developed iterative diagonalization approach for general multiwell systems. Different types of stereographic coordinates are used, and a corresponding general N-body kinetic energy operator is given. The calculated tunneling splittings of the ground and the lower vibrational excited states of the CH4•F- complex do not significantly exceed 1 cm-1. Comparing the converged MCTDH results for localized vibrational excitations with existing results obtained by normal-mode-based (truncated) vibrational configuration interaction calculations, significantly lower frequencies are found for excitations in the intermolecular modes. |
| publishDate |
2012 |
| dc.date.none.fl_str_mv |
2012-06 |
| 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/11336/189007 Wodraszka, Robert; Palma, Juliana Isabel; Manthe, Uwe; Vibrational dynamics of the FCH4(-) complex; American Chemical Society; Journal of Physical Chemistry A; 116; 46; 6-2012; 11249-11259 1089-5639 CONICET Digital CONICET |
| url |
http://hdl.handle.net/11336/189007 |
| identifier_str_mv |
Wodraszka, Robert; Palma, Juliana Isabel; Manthe, Uwe; Vibrational dynamics of the FCH4(-) complex; American Chemical Society; Journal of Physical Chemistry A; 116; 46; 6-2012; 11249-11259 1089-5639 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://pubs.acs.org/doi/abs/10.1021/jp3052642 info:eu-repo/semantics/altIdentifier/doi/10.1021/jp3052642 |
| 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 Chemical Society |
| publisher.none.fl_str_mv |
American Chemical Society |
| 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_ |
1846782119788937216 |
| score |
12.982451 |