Analysis and control of transient spectra using time-dependent density functional theory.

215 p.

Detalles Bibliográficos
Autor: Walkenhorst, Jessica
Tipo de recurso: tesis doctoral
Fecha de publicación:2016
País:España
Institución:Universidad del País Vasco
Repositorio:Addi. Archivo Digital para la Docencia y la Investigación
OAI Identifier:oai:addi.ehu.eus:10810/18453
Acceso en línea:http://hdl.handle.net/10810/18453
Access Level:acceso abierto
id ES_3104f4cfcad1ea155eb9284d9fa45ccf
oai_identifier_str oai:addi.ehu.eus:10810/18453
network_acronym_str ES
network_name_str España
repository_id_str
spelling Analysis and control of transient spectra using time-dependent density functional theory.Walkenhorst, Jessica215 p.Attosecond-transient absorption spectroscopy and attosecond time-resolved photoelectronspectroscopy based on pump-probe setups have recently become possibledue to the availability of ultra-fast pulsed laser sources. These experiments allow tofollow the electronic motion on its natural time-scale, allowing the characterizationof electronic excited states and transitions while neglecting the influence of thenuclear degrees of freedom. Molecular absorption and photo-electron spectra can beefficiently predicted with real-time time-dependent density-functional theory, whichis normally used for the description of systems in their ground state. In this thesis, Ishow how these techniques can be extended to study time-resolved pump-probeexperiments in an excited state providing a tool for the interpretation of fastevolving attosecond time-resolved spectroscopic experiments. I show how the extradegrees of freedom (pump pulse duration, intensity, frequency, and time-delay),which are absent in a conventional steady state experiment, provide additionalinformation about the electronic structure and the dynamics, which can be used toimprove a system characterization. As an extension of this approach, timedependent2D spectroscopies can also be simulated, in principle, for large-scalestructures and extended systems. In addition to numerical modelling, a theoreticalunderstanding of the processes would be useful. In this thesis, I reexamine theLehmann representation of the response function of a pump-driven system in thenon-overlapping regime, deriving some general properties of the excited statespectra, including position and shape of their resonance peaks. I demonstrate, howas a consequence, this Lehmann representation can be used to understand laserinducedline shape changes. Measurement and control of ultrafast processes areinherently intertwined. In this work, I assess the possibility of using tailored pumpsin order to enhance (or reduce) some given features of the probe absorption (forexample, absorption in the visible range of otherwise transparent samples). Thistype of manipulation of the system response could be helpful for its fullcharacterization, since it would allow to visualize transitions that are obscured whenusing un-shaped pulses. In order to investigate this possibility, I firstly combine theLehmann representation with a simple numerical model of the Hydrogen atom toshow, how Hydrogen can be manipulated to loose its transparency in the visible. Ithen proceed to investigate the feasibility of using time-dependent densityfunctionaltheory as a means to implement, theoretically, this absorptionoptimizationidea, for more complex atoms or molecules.Rubio Secades, AngelCastro Barrigón, AlbertoFísica de Materiales;;Materialen Fisika2016201620162016info:eu-repo/semantics/doctoralThesisapplication/pdfhttp://hdl.handle.net/10810/18453reponame:Addi. Archivo Digital para la Docencia y la Investigacióninstname:Universidad del País VascoInglésinfo:eu-repo/semantics/openAccesshttp://creativecommons.org/licenses/by-nc/4.0/(cc)2016 JESSICA WALKENHORST (cc by-nc 4.0)oai:addi.ehu.eus:10810/184532026-06-18T09:23:17Z
dc.title.none.fl_str_mv Analysis and control of transient spectra using time-dependent density functional theory.
title Analysis and control of transient spectra using time-dependent density functional theory.
spellingShingle Analysis and control of transient spectra using time-dependent density functional theory.
Walkenhorst, Jessica
title_short Analysis and control of transient spectra using time-dependent density functional theory.
title_full Analysis and control of transient spectra using time-dependent density functional theory.
title_fullStr Analysis and control of transient spectra using time-dependent density functional theory.
title_full_unstemmed Analysis and control of transient spectra using time-dependent density functional theory.
title_sort Analysis and control of transient spectra using time-dependent density functional theory.
dc.creator.none.fl_str_mv Walkenhorst, Jessica
author Walkenhorst, Jessica
author_facet Walkenhorst, Jessica
author_role author
dc.contributor.none.fl_str_mv Rubio Secades, Angel
Castro Barrigón, Alberto
Física de Materiales;;Materialen Fisika
description 215 p.
publishDate 2016
dc.date.none.fl_str_mv 2016
2016
2016
2016
dc.type.none.fl_str_mv info:eu-repo/semantics/doctoralThesis
format doctoralThesis
dc.identifier.none.fl_str_mv http://hdl.handle.net/10810/18453
url http://hdl.handle.net/10810/18453
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
http://creativecommons.org/licenses/by-nc/4.0/
(cc)2016 JESSICA WALKENHORST (cc by-nc 4.0)
eu_rights_str_mv openAccess
rights_invalid_str_mv http://creativecommons.org/licenses/by-nc/4.0/
(cc)2016 JESSICA WALKENHORST (cc by-nc 4.0)
dc.format.none.fl_str_mv application/pdf
dc.source.none.fl_str_mv reponame:Addi. Archivo Digital para la Docencia y la Investigación
instname:Universidad del País Vasco
instname_str Universidad del País Vasco
reponame_str Addi. Archivo Digital para la Docencia y la Investigación
collection Addi. Archivo Digital para la Docencia y la Investigación
repository.name.fl_str_mv
repository.mail.fl_str_mv
_version_ 1869405583899099136
score 15.301629

Similares en LA Referencia