Wave Packet Dynamics at an Extended Seam of Conical Intersection: Mechanism of the Light-Induced Wolff Rearrangement

Quantum dynamics calculations on a model surface based on CASPT(2)//CASSCF calculations are carried out to probe the traversal of a wave packet through an extended seam of conical intersection during the light-induced Wolff rearrangement of diazonaphtoquinone. The reaction is applied in the fabricat...

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Detalhes bibliográficos
Autores: Li, Quansong, Migani, Annapaola, Blancafort San José, Lluís
Formato: artículo
Estado:Versión publicada
Fecha de publicación:2012
País:España
Recursos:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
Repositorio:Recercat. Dipósit de la Recerca de Catalunya
OAI Identifier:oai:recercat.cat:10256/11481
Acesso em linha:http://hdl.handle.net/10256/11481
Access Level:acceso embargado
Palavra-chave:Dinàmica molecular
Molecular dynamics
Espectroscòpia infraroja
Infrared spectroscopy
Rotació molecular
Molecular rotation
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spelling Wave Packet Dynamics at an Extended Seam of Conical Intersection: Mechanism of the Light-Induced Wolff RearrangementLi, QuansongMigani, AnnapaolaBlancafort San José, LluísDinàmica molecularMolecular dynamicsEspectroscòpia infrarojaInfrared spectroscopyRotació molecularMolecular rotationQuantum dynamics calculations on a model surface based on CASPT(2)//CASSCF calculations are carried out to probe the traversal of a wave packet through an extended seam of conical intersection during the light-induced Wolff rearrangement of diazonaphtoquinone. The reaction is applied in the fabrication of integrated circuits. It consists of nitrogen elimination and ring rearrangement to yield a ketene. After excitation, the wave packet relaxes and reaches the extended seam. A fraction of the wave packet decays to the ground state at a region of the seam connected to a carbene intermediate, while the remaining part decays at a region leading to the ketene. The passage of the wave packet through the extended seam explains the competition between concerted ketene formation and a stepwise mechanism involving a carbene. The two primary photoproducts are formed in the first 100 fs of the simulation, in agreement with recent ultrafast spectroscopy measurementsThis work has been supported by Grants CTQ2008-06696 and CTQ2011-26573 from the Spanish Ministerio de Ciencia e Innovacion (MICINN), SGR0528 from the Catalan Agencia de Gestio d'Ajuts Universitaris i de Recerca (AGAUR), and UNGI08-4E-003 from MICINN and the FEDER fund (European Fund for Regional Development). Q.L. acknowledges a Juan de la Cierva fellowship of the MICINN and A.M. a Beatriu de Pinos fellowship of the Generalitat de Catalunya (Spain)American Chemical Society (ACS)Ministerio de Educación y Ciencia (Espanya)Ministerio de Ciencia e Innovación (Espanya)Generalitat de Catalunya. Agència de Gestió d'Ajuts Universitaris i de Recercainfoinfo2012info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionapplication/pdfhttp://hdl.handle.net/10256/11481http://hdl.handle.net/10256/11481© Journal of Physical Chemistry Letters, 2012, vol. 3, núm. 8, p. 1056-1061Articles publicats (D-Q)reponame:Recercat. Dipósit de la Recerca de Catalunyainstname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)Inglésinfo:eu-repo/semantics/altIdentifier/doi/10.1021/jz300235zinfo:eu-repo/semantics/altIdentifier/issn/1948-7185info:eu-repo/grantAgreement/MICINN//CTQ2008-06696info:eu-repo/grantAgreement/MICINN//CTQ2011-26573info:eu-repo/grantAgreement/MEC//UNGI08-4E-003AGAUR/2009-2014/2009 SGR-528Tots els drets reservatsinfo:eu-repo/semantics/embargoedAccessoai:recercat.cat:10256/114812026-05-29T05:05:01Z
dc.title.none.fl_str_mv Wave Packet Dynamics at an Extended Seam of Conical Intersection: Mechanism of the Light-Induced Wolff Rearrangement
title Wave Packet Dynamics at an Extended Seam of Conical Intersection: Mechanism of the Light-Induced Wolff Rearrangement
spellingShingle Wave Packet Dynamics at an Extended Seam of Conical Intersection: Mechanism of the Light-Induced Wolff Rearrangement
Li, Quansong
Dinàmica molecular
Molecular dynamics
Espectroscòpia infraroja
Infrared spectroscopy
Rotació molecular
Molecular rotation
title_short Wave Packet Dynamics at an Extended Seam of Conical Intersection: Mechanism of the Light-Induced Wolff Rearrangement
title_full Wave Packet Dynamics at an Extended Seam of Conical Intersection: Mechanism of the Light-Induced Wolff Rearrangement
title_fullStr Wave Packet Dynamics at an Extended Seam of Conical Intersection: Mechanism of the Light-Induced Wolff Rearrangement
title_full_unstemmed Wave Packet Dynamics at an Extended Seam of Conical Intersection: Mechanism of the Light-Induced Wolff Rearrangement
title_sort Wave Packet Dynamics at an Extended Seam of Conical Intersection: Mechanism of the Light-Induced Wolff Rearrangement
dc.creator.none.fl_str_mv Li, Quansong
Migani, Annapaola
Blancafort San José, Lluís
author Li, Quansong
author_facet Li, Quansong
Migani, Annapaola
Blancafort San José, Lluís
author_role author
author2 Migani, Annapaola
Blancafort San José, Lluís
author2_role author
author
dc.contributor.none.fl_str_mv Ministerio de Educación y Ciencia (Espanya)
Ministerio de Ciencia e Innovación (Espanya)
Generalitat de Catalunya. Agència de Gestió d'Ajuts Universitaris i de Recerca
dc.subject.none.fl_str_mv Dinàmica molecular
Molecular dynamics
Espectroscòpia infraroja
Infrared spectroscopy
Rotació molecular
Molecular rotation
topic Dinàmica molecular
Molecular dynamics
Espectroscòpia infraroja
Infrared spectroscopy
Rotació molecular
Molecular rotation
description Quantum dynamics calculations on a model surface based on CASPT(2)//CASSCF calculations are carried out to probe the traversal of a wave packet through an extended seam of conical intersection during the light-induced Wolff rearrangement of diazonaphtoquinone. The reaction is applied in the fabrication of integrated circuits. It consists of nitrogen elimination and ring rearrangement to yield a ketene. After excitation, the wave packet relaxes and reaches the extended seam. A fraction of the wave packet decays to the ground state at a region of the seam connected to a carbene intermediate, while the remaining part decays at a region leading to the ketene. The passage of the wave packet through the extended seam explains the competition between concerted ketene formation and a stepwise mechanism involving a carbene. The two primary photoproducts are formed in the first 100 fs of the simulation, in agreement with recent ultrafast spectroscopy measurements
publishDate 2012
dc.date.none.fl_str_mv 2012
info
info
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/10256/11481
http://hdl.handle.net/10256/11481
url http://hdl.handle.net/10256/11481
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/10.1021/jz300235z
info:eu-repo/semantics/altIdentifier/issn/1948-7185
info:eu-repo/grantAgreement/MICINN//CTQ2008-06696
info:eu-repo/grantAgreement/MICINN//CTQ2011-26573
info:eu-repo/grantAgreement/MEC//UNGI08-4E-003
AGAUR/2009-2014/2009 SGR-528
dc.rights.none.fl_str_mv Tots els drets reservats
info:eu-repo/semantics/embargoedAccess
rights_invalid_str_mv Tots els drets reservats
eu_rights_str_mv embargoedAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv American Chemical Society (ACS)
publisher.none.fl_str_mv American Chemical Society (ACS)
dc.source.none.fl_str_mv © Journal of Physical Chemistry Letters, 2012, vol. 3, núm. 8, p. 1056-1061
Articles publicats (D-Q)
reponame:Recercat. Dipósit de la Recerca de Catalunya
instname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
instname_str Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
reponame_str Recercat. Dipósit de la Recerca de Catalunya
collection Recercat. Dipósit de la Recerca de Catalunya
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15,811543

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