Mapping and controlling ultrafast dynamics of highly excited H2 molecules by VUV-IR pump-probe schemes

We used ultrashort femtosecond vacuum ultraviolet (VUV) and infrared (IR) pulses in a pump-probe scheme to map the dynamics and nonequilibrium dissociation channels of excited neutral H2 molecules. A nuclear wave packet is created in the BΣu+1 state of the neutral H2 molecule by absorption of the ni...

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Autores: Sturm, F. P., Tong, X. M., Palacios Cañas, Alicia, Wright, T. W., Zalyubovskaya, I., Ray, D., Shivaram, N., Martín García, Fernando, Belkacem, A., Ranitovic, P., Weber, Th
Tipo de documento: artigo
Data de publicação:2017
País:España
Recursos:Universidad Autónoma de Madrid
Repositório:Biblos-e Archivo. Repositorio Institucional de la UAM
Idioma:inglês
OAI Identifier:oai:repositorio.uam.es:10486/679858
Acesso em linha:http://hdl.handle.net/10486/679858
https://dx.doi.org/10.1103/PhysRevA.95.012501
Access Level:Acceso aberto
Palavra-chave:Dissociation
Excited states
Ionization
Multiphoton processes
Química
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spelling Mapping and controlling ultrafast dynamics of highly excited H2 molecules by VUV-IR pump-probe schemesSturm, F. P.Tong, X. M.Palacios Cañas, AliciaWright, T. W.Zalyubovskaya, I.Ray, D.Shivaram, N.Martín García, FernandoBelkacem, A.Ranitovic, P.Weber, ThDissociationExcited statesIonizationMultiphoton processesQuímicaWe used ultrashort femtosecond vacuum ultraviolet (VUV) and infrared (IR) pulses in a pump-probe scheme to map the dynamics and nonequilibrium dissociation channels of excited neutral H2 molecules. A nuclear wave packet is created in the BΣu+1 state of the neutral H2 molecule by absorption of the ninth harmonic of the driving infrared laser field. Due to the large stretching amplitude of the molecule excited in the BΣu+1 electronic state, the effective H2+ ionization potential changes significantly as the nuclear wave packet vibrates in the bound, highly electronically and vibrationally excited B potential-energy curve. We probed such dynamics by ionizing the excited neutral molecule using time-delayed VUV-or-IR radiation. We identified the nonequilibrium dissociation channels by utilizing three-dimensional momentum imaging of the ion fragments. We found that different dissociation channels can be controlled, to some extent, by changing the IR laser intensity and by choosing the wavelength of the probe laser light. Furthermore, we concluded that even in a benchmark molecular system such as H2∗, the interpretation of the nonequilibrium multiphoton and multicolor ionization processes is still a challenging task, requiring intricate theoretical analysisWe acknowledge many fruitful discussions and advice from R. Dorner, M. S. Schoffler, L. Ph. Schmidt, and Wei Cao. We are indebted to O. Jagutzki and A. Czasch from Roentdek GmbH and T. Jahnke from Cronologic GmbH for outstanding support for their momentum imaging detectors readout and software. F.S. acknowledges financial support by Studienstiftung des deutschen Volkes. A.P. and F.M.acknowledge the European COST Action XLIC CM1204, the European Research Council Advanced Grant XCHEM No. 290853, and the MINECO Project No. FIS2013-42002-R. X.M.T. was supported by a Grand-in-Aid for Scientific Research from the Japan Society for the Promotion of Science and Interdisciplinary Computational Science Program in Center for Computational Sciences, University of Tsukuba. This work was supported by the Director, Office of Science, Office of Basic Energy Sciences, and by the Division of Chemical Sciences, Geosciences, and Biosciences of the U.S. Department of Energy at LBNL under Contract No. DE-AC02-05CH11231American Physical SocietyDepartamento de QuímicaFacultad de Ciencias20172017-01-09research articlehttp://purl.org/coar/resource_type/c_2df8fbb1VoRhttp://purl.org/coar/version/c_970fb48d4fbd8a85info:eu-repo/semantics/articleapplication/pdfhttp://hdl.handle.net/10486/679858https://dx.doi.org/10.1103/PhysRevA.95.012501reponame:Biblos-e Archivo. Repositorio Institucional de la UAMinstname:Universidad Autónoma de MadridInglésengEuropean Commission http://dx.doi.org/10.13039/501100000780 Framework Programme Seven 290853European Commission http://dx.doi.org/10.13039/501100000780 Framework Programme Seven 321971open accesshttp://purl.org/coar/access_right/c_abf2info:eu-repo/semantics/openAccessoai:repositorio.uam.es:10486/6798582026-06-23T12:46:27Z
dc.title.none.fl_str_mv Mapping and controlling ultrafast dynamics of highly excited H2 molecules by VUV-IR pump-probe schemes
title Mapping and controlling ultrafast dynamics of highly excited H2 molecules by VUV-IR pump-probe schemes
spellingShingle Mapping and controlling ultrafast dynamics of highly excited H2 molecules by VUV-IR pump-probe schemes
Sturm, F. P.
Dissociation
Excited states
Ionization
Multiphoton processes
Química
title_short Mapping and controlling ultrafast dynamics of highly excited H2 molecules by VUV-IR pump-probe schemes
title_full Mapping and controlling ultrafast dynamics of highly excited H2 molecules by VUV-IR pump-probe schemes
title_fullStr Mapping and controlling ultrafast dynamics of highly excited H2 molecules by VUV-IR pump-probe schemes
title_full_unstemmed Mapping and controlling ultrafast dynamics of highly excited H2 molecules by VUV-IR pump-probe schemes
title_sort Mapping and controlling ultrafast dynamics of highly excited H2 molecules by VUV-IR pump-probe schemes
dc.creator.none.fl_str_mv Sturm, F. P.
Tong, X. M.
Palacios Cañas, Alicia
Wright, T. W.
Zalyubovskaya, I.
Ray, D.
Shivaram, N.
Martín García, Fernando
Belkacem, A.
Ranitovic, P.
Weber, Th
author Sturm, F. P.
author_facet Sturm, F. P.
Tong, X. M.
Palacios Cañas, Alicia
Wright, T. W.
Zalyubovskaya, I.
Ray, D.
Shivaram, N.
Martín García, Fernando
Belkacem, A.
Ranitovic, P.
Weber, Th
author_role author
author2 Tong, X. M.
Palacios Cañas, Alicia
Wright, T. W.
Zalyubovskaya, I.
Ray, D.
Shivaram, N.
Martín García, Fernando
Belkacem, A.
Ranitovic, P.
Weber, Th
author2_role author
author
author
author
author
author
author
author
author
author
dc.contributor.none.fl_str_mv Departamento de Química
Facultad de Ciencias
dc.subject.none.fl_str_mv Dissociation
Excited states
Ionization
Multiphoton processes
Química
topic Dissociation
Excited states
Ionization
Multiphoton processes
Química
description We used ultrashort femtosecond vacuum ultraviolet (VUV) and infrared (IR) pulses in a pump-probe scheme to map the dynamics and nonequilibrium dissociation channels of excited neutral H2 molecules. A nuclear wave packet is created in the BΣu+1 state of the neutral H2 molecule by absorption of the ninth harmonic of the driving infrared laser field. Due to the large stretching amplitude of the molecule excited in the BΣu+1 electronic state, the effective H2+ ionization potential changes significantly as the nuclear wave packet vibrates in the bound, highly electronically and vibrationally excited B potential-energy curve. We probed such dynamics by ionizing the excited neutral molecule using time-delayed VUV-or-IR radiation. We identified the nonequilibrium dissociation channels by utilizing three-dimensional momentum imaging of the ion fragments. We found that different dissociation channels can be controlled, to some extent, by changing the IR laser intensity and by choosing the wavelength of the probe laser light. Furthermore, we concluded that even in a benchmark molecular system such as H2∗, the interpretation of the nonequilibrium multiphoton and multicolor ionization processes is still a challenging task, requiring intricate theoretical analysis
publishDate 2017
dc.date.none.fl_str_mv 2017
2017-01-09
dc.type.none.fl_str_mv research article
http://purl.org/coar/resource_type/c_2df8fbb1
VoR
http://purl.org/coar/version/c_970fb48d4fbd8a85
dc.type.openaire.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.none.fl_str_mv http://hdl.handle.net/10486/679858
https://dx.doi.org/10.1103/PhysRevA.95.012501
url http://hdl.handle.net/10486/679858
https://dx.doi.org/10.1103/PhysRevA.95.012501
dc.language.none.fl_str_mv Inglés
eng
language_invalid_str_mv Inglés
language eng
dc.relation.none.fl_str_mv European Commission http://dx.doi.org/10.13039/501100000780 Framework Programme Seven 290853

European Commission http://dx.doi.org/10.13039/501100000780 Framework Programme Seven 321971
dc.rights.none.fl_str_mv open access
http://purl.org/coar/access_right/c_abf2
dc.rights.openaire.fl_str_mv info:eu-repo/semantics/openAccess
rights_invalid_str_mv open access
http://purl.org/coar/access_right/c_abf2
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv American Physical Society
publisher.none.fl_str_mv American Physical Society
dc.source.none.fl_str_mv reponame:Biblos-e Archivo. Repositorio Institucional de la UAM
instname:Universidad Autónoma de Madrid
instname_str Universidad Autónoma de Madrid
reponame_str Biblos-e Archivo. Repositorio Institucional de la UAM
collection Biblos-e Archivo. Repositorio Institucional de la UAM
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15.300724

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