Vibrationally resolved two-photon electronic spectra including vibrational pre-excitation: Theory and application to VIPER spectroscopy with two-photon excitation

Following up on our previous work on vibrationally resolved electronic absorption spectra including the effect of vibrational pre-excitation [von Cosel et al., J. Chem. Phys. 147, 164116 (2017)], we present a combined theoretical and experimental study of two-photon-induced vibronic transitions in p...

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Autores: Horz, Maximiliane, Masood, Hafiz M.A., Brunst, Hendrik, Cerezo Bastida, Javier, Picconi, David, Vormann, Hannah, Niraghatam, Madhava Shyam, Wilderen, Luuk J.G.W., Van, Bredenbeck, Jens, Santoro, Fabrizio, Burghardt, Irene
Tipo de recurso: artículo
Fecha de publicación:2023
País:España
Institución:Universidad Autónoma de Madrid
Repositorio:Biblos-e Archivo. Repositorio Institucional de la UAM
Idioma:inglés
OAI Identifier:oai:repositorio.uam.es:10486/708738
Acceso en línea:http://hdl.handle.net/10486/708738
https://dx.doi.org/10.1063/5.0132608
Access Level:acceso abierto
Palabra clave:Absorption Spectroscopy
Chemical Bonds
Molecular Orbitals
Fourier Transforms
Excited States
Química
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spelling Vibrationally resolved two-photon electronic spectra including vibrational pre-excitation: Theory and application to VIPER spectroscopy with two-photon excitationHorz, MaximilianeMasood, Hafiz M.A.Brunst, HendrikCerezo Bastida, JavierPicconi, DavidVormann, HannahNiraghatam, Madhava ShyamWilderen, Luuk J.G.W., VanBredenbeck, JensSantoro, FabrizioBurghardt, IreneAbsorption SpectroscopyChemical BondsMolecular OrbitalsFourier TransformsExcited StatesQuímicaFollowing up on our previous work on vibrationally resolved electronic absorption spectra including the effect of vibrational pre-excitation [von Cosel et al., J. Chem. Phys. 147, 164116 (2017)], we present a combined theoretical and experimental study of two-photon-induced vibronic transitions in polyatomic molecules that are probed in the VIbrationally Promoted Electronic Resonance experiment using two-photon excitation (2P-VIPER). In order to compute vibronic spectra, we employ time-independent and time-dependent methods based on the evaluation of Franck-Condon overlap integrals and Fourier transformations of time-domain correlation functions, respectively. The time-independent approach uses a generalized version of the FCclasses method, while the time-dependent approach relies on the analytical evaluation of Gaussian moments within the harmonic approximation, including Duschinsky rotation effects. For the Coumarin 6 dye, two-dimensional 2P-VIPER experiments involving excitation to the lowest-lying singlet excited state (S1) are presented and compared with corresponding one-photon VIPER spectra. In both cases, coumarin ring modes and a CO stretch mode show VIPER activity, albeit with different relative intensities. Selective pre-excitation of these modes leads to a pronounced redshift of the low-frequency edge of the electronic absorption spectrum, which is a prerequisite for the VIPER experiment. Theoretical analysis underscores the role of interference between Franck-Condon and Herzberg-Teller effects in the two-photon experiment, which is at the root of the observed intensity distributionAmerican Institute of PhysicsDepartamento de QuímicaFacultad de Ciencias20232023-02-08research articlehttp://purl.org/coar/resource_type/c_2df8fbb1VoRhttp://purl.org/coar/version/c_970fb48d4fbd8a85info:eu-repo/semantics/articleapplication/pdfhttp://hdl.handle.net/10486/708738https://dx.doi.org/10.1063/5.0132608reponame:Biblos-e Archivo. Repositorio Institucional de la UAMinstname:Universidad Autónoma de MadridInglésengopen accesshttp://purl.org/coar/access_right/c_abf2info:eu-repo/semantics/openAccessoai:repositorio.uam.es:10486/7087382026-06-23T12:46:27Z
dc.title.none.fl_str_mv Vibrationally resolved two-photon electronic spectra including vibrational pre-excitation: Theory and application to VIPER spectroscopy with two-photon excitation
title Vibrationally resolved two-photon electronic spectra including vibrational pre-excitation: Theory and application to VIPER spectroscopy with two-photon excitation
spellingShingle Vibrationally resolved two-photon electronic spectra including vibrational pre-excitation: Theory and application to VIPER spectroscopy with two-photon excitation
Horz, Maximiliane
Absorption Spectroscopy
Chemical Bonds
Molecular Orbitals
Fourier Transforms
Excited States
Química
title_short Vibrationally resolved two-photon electronic spectra including vibrational pre-excitation: Theory and application to VIPER spectroscopy with two-photon excitation
title_full Vibrationally resolved two-photon electronic spectra including vibrational pre-excitation: Theory and application to VIPER spectroscopy with two-photon excitation
title_fullStr Vibrationally resolved two-photon electronic spectra including vibrational pre-excitation: Theory and application to VIPER spectroscopy with two-photon excitation
title_full_unstemmed Vibrationally resolved two-photon electronic spectra including vibrational pre-excitation: Theory and application to VIPER spectroscopy with two-photon excitation
title_sort Vibrationally resolved two-photon electronic spectra including vibrational pre-excitation: Theory and application to VIPER spectroscopy with two-photon excitation
dc.creator.none.fl_str_mv Horz, Maximiliane
Masood, Hafiz M.A.
Brunst, Hendrik
Cerezo Bastida, Javier
Picconi, David
Vormann, Hannah
Niraghatam, Madhava Shyam
Wilderen, Luuk J.G.W., Van
Bredenbeck, Jens
Santoro, Fabrizio
Burghardt, Irene
author Horz, Maximiliane
author_facet Horz, Maximiliane
Masood, Hafiz M.A.
Brunst, Hendrik
Cerezo Bastida, Javier
Picconi, David
Vormann, Hannah
Niraghatam, Madhava Shyam
Wilderen, Luuk J.G.W., Van
Bredenbeck, Jens
Santoro, Fabrizio
Burghardt, Irene
author_role author
author2 Masood, Hafiz M.A.
Brunst, Hendrik
Cerezo Bastida, Javier
Picconi, David
Vormann, Hannah
Niraghatam, Madhava Shyam
Wilderen, Luuk J.G.W., Van
Bredenbeck, Jens
Santoro, Fabrizio
Burghardt, Irene
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 Absorption Spectroscopy
Chemical Bonds
Molecular Orbitals
Fourier Transforms
Excited States
Química
topic Absorption Spectroscopy
Chemical Bonds
Molecular Orbitals
Fourier Transforms
Excited States
Química
description Following up on our previous work on vibrationally resolved electronic absorption spectra including the effect of vibrational pre-excitation [von Cosel et al., J. Chem. Phys. 147, 164116 (2017)], we present a combined theoretical and experimental study of two-photon-induced vibronic transitions in polyatomic molecules that are probed in the VIbrationally Promoted Electronic Resonance experiment using two-photon excitation (2P-VIPER). In order to compute vibronic spectra, we employ time-independent and time-dependent methods based on the evaluation of Franck-Condon overlap integrals and Fourier transformations of time-domain correlation functions, respectively. The time-independent approach uses a generalized version of the FCclasses method, while the time-dependent approach relies on the analytical evaluation of Gaussian moments within the harmonic approximation, including Duschinsky rotation effects. For the Coumarin 6 dye, two-dimensional 2P-VIPER experiments involving excitation to the lowest-lying singlet excited state (S1) are presented and compared with corresponding one-photon VIPER spectra. In both cases, coumarin ring modes and a CO stretch mode show VIPER activity, albeit with different relative intensities. Selective pre-excitation of these modes leads to a pronounced redshift of the low-frequency edge of the electronic absorption spectrum, which is a prerequisite for the VIPER experiment. Theoretical analysis underscores the role of interference between Franck-Condon and Herzberg-Teller effects in the two-photon experiment, which is at the root of the observed intensity distribution
publishDate 2023
dc.date.none.fl_str_mv 2023
2023-02-08
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/10486/708738
https://dx.doi.org/10.1063/5.0132608
url http://hdl.handle.net/10486/708738
https://dx.doi.org/10.1063/5.0132608
dc.language.none.fl_str_mv Inglés
eng
language_invalid_str_mv Inglés
language eng
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 Institute of Physics
publisher.none.fl_str_mv American Institute of Physics
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 15,301603

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