Simulating pump-probe photoelectron and absorption spectroscopy on the attosecond timescale with time-dependent density functional theory

Molecular absorption and photoelectron spectra can be efficiently predicted with real-time time-dependent density functional theory. We show herein how these techniques can be easily extended to study time-resolved pump-probe experiments, in which a system response (absorption or electron emission)...

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Detalhes bibliográficos
Autores: Giovannini, Umberto de, Brunetto, Gustavo, Castro, Alberto, Walkenhorst, Jessica, Rubio, Angel
Formato: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2013
País:España
Recursos:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/95064
Acesso em linha:http://hdl.handle.net/10261/95064
Access Level:acceso abierto
Palavra-chave:Ab initio calculations
Time-resolved spectroscopy
Attosecond dynamics
Single-molecule studies
Laser spectroscopy
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spelling Simulating pump-probe photoelectron and absorption spectroscopy on the attosecond timescale with time-dependent density functional theoryGiovannini, Umberto deBrunetto, GustavoCastro, AlbertoWalkenhorst, JessicaRubio, AngelAb initio calculationsTime-resolved spectroscopyAttosecond dynamicsSingle-molecule studiesLaser spectroscopyMolecular absorption and photoelectron spectra can be efficiently predicted with real-time time-dependent density functional theory. We show herein how these techniques can be easily extended to study time-resolved pump-probe experiments, in which a system response (absorption or electron emission) to a probe pulse is measured in an excited state. This simulation tool helps with the interpretation of fast-evolving attosecond time-resolved spectroscopic experiments, in which electronic motion must be followed at its natural timescale. We show how the extra degrees of freedom (pump-pulse duration, intensity, frequency, and time delay), which are absent in a conventional steady-state experiment, provide additional information about electronic structure and dynamics that improve characterization of a system. As an extension of this approach, time-dependent 2D spectroscopy can also be simulated, in principle, for large-scale structures and extended systems. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.Funded by: European Research Council. Grant Numbers: ERC-2010-AdG-Proposal No. 267374, FIS2011-65702-C02-01, PIB2010US-00652; ACI. Grant Number: ACI2009-1036; Gobierno Vasco. Grant Number: IT-319-07; European Commission. Grant Numbers: 280879-2 CRONOS CP-FP7, FP7-NMP-2008-SMALL-2, 228539; CAPES Foundation and Ministry of Education of Brazil. Grant Number: 2287/110.Peer ReviewedWiley-VCHEuropean Research CouncilEuropean CommissionMinistério da Educação (Brasil)Fundaçao Capes (Brasil)2014201420132014info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Postprintinfo:eu-repo/semantics/acceptedVersionhttp://hdl.handle.net/10261/95064reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)Inglés#PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE#info:eu-repo/grantAgreement/EC/FP7/267374info:eu-repo/grantAgreement/EC/FP7/280879http://dx.doi.org/10.1002/cphc.201201007info:eu-repo/semantics/openAccessoai:digital.csic.es:10261/950642026-05-22T06:33:51Z
dc.title.none.fl_str_mv Simulating pump-probe photoelectron and absorption spectroscopy on the attosecond timescale with time-dependent density functional theory
title Simulating pump-probe photoelectron and absorption spectroscopy on the attosecond timescale with time-dependent density functional theory
spellingShingle Simulating pump-probe photoelectron and absorption spectroscopy on the attosecond timescale with time-dependent density functional theory
Giovannini, Umberto de
Ab initio calculations
Time-resolved spectroscopy
Attosecond dynamics
Single-molecule studies
Laser spectroscopy
title_short Simulating pump-probe photoelectron and absorption spectroscopy on the attosecond timescale with time-dependent density functional theory
title_full Simulating pump-probe photoelectron and absorption spectroscopy on the attosecond timescale with time-dependent density functional theory
title_fullStr Simulating pump-probe photoelectron and absorption spectroscopy on the attosecond timescale with time-dependent density functional theory
title_full_unstemmed Simulating pump-probe photoelectron and absorption spectroscopy on the attosecond timescale with time-dependent density functional theory
title_sort Simulating pump-probe photoelectron and absorption spectroscopy on the attosecond timescale with time-dependent density functional theory
dc.creator.none.fl_str_mv Giovannini, Umberto de
Brunetto, Gustavo
Castro, Alberto
Walkenhorst, Jessica
Rubio, Angel
author Giovannini, Umberto de
author_facet Giovannini, Umberto de
Brunetto, Gustavo
Castro, Alberto
Walkenhorst, Jessica
Rubio, Angel
author_role author
author2 Brunetto, Gustavo
Castro, Alberto
Walkenhorst, Jessica
Rubio, Angel
author2_role author
author
author
author
dc.contributor.none.fl_str_mv European Research Council
European Commission
Ministério da Educação (Brasil)
Fundaçao Capes (Brasil)
dc.subject.none.fl_str_mv Ab initio calculations
Time-resolved spectroscopy
Attosecond dynamics
Single-molecule studies
Laser spectroscopy
topic Ab initio calculations
Time-resolved spectroscopy
Attosecond dynamics
Single-molecule studies
Laser spectroscopy
description Molecular absorption and photoelectron spectra can be efficiently predicted with real-time time-dependent density functional theory. We show herein how these techniques can be easily extended to study time-resolved pump-probe experiments, in which a system response (absorption or electron emission) to a probe pulse is measured in an excited state. This simulation tool helps with the interpretation of fast-evolving attosecond time-resolved spectroscopic experiments, in which electronic motion must be followed at its natural timescale. We show how the extra degrees of freedom (pump-pulse duration, intensity, frequency, and time delay), which are absent in a conventional steady-state experiment, provide additional information about electronic structure and dynamics that improve characterization of a system. As an extension of this approach, time-dependent 2D spectroscopy can also be simulated, in principle, for large-scale structures and extended systems. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
publishDate 2013
dc.date.none.fl_str_mv 2013
2014
2014
2014
dc.type.none.fl_str_mv info:eu-repo/semantics/article
http://purl.org/coar/resource_type/c_6501
Postprint
info:eu-repo/semantics/acceptedVersion
format article
status_str acceptedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/10261/95064
url http://hdl.handle.net/10261/95064
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv #PLACEHOLDER_PARENT_METADATA_VALUE#
#PLACEHOLDER_PARENT_METADATA_VALUE#
info:eu-repo/grantAgreement/EC/FP7/267374
info:eu-repo/grantAgreement/EC/FP7/280879
http://dx.doi.org/10.1002/cphc.201201007
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.publisher.none.fl_str_mv Wiley-VCH
publisher.none.fl_str_mv Wiley-VCH
dc.source.none.fl_str_mv reponame:DIGITAL.CSIC. Repositorio Institucional del CSIC
instname:Consejo Superior de Investigaciones Científicas (CSIC)
instname_str Consejo Superior de Investigaciones Científicas (CSIC)
reponame_str DIGITAL.CSIC. Repositorio Institucional del CSIC
collection DIGITAL.CSIC. Repositorio Institucional del CSIC
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15,811543

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