% IMPORTANT: The following is UTF-8 encoded. This means that in the presence
% of non-ASCII characters, it will not work with BibTeX 0.99 or older.
% Instead, you should use an up-to-date BibTeX implementation like “bibtex8” or
% “biber”.
@PHDTHESIS{Karamatskos:427703,
author = {Karamatskos, Evangelos Thomas},
othercontributors = {Küpper, Jochen and Santra, Robin},
title = {{M}olecular-{F}rame {A}ngularly-{R}esolved {P}hotoelectron
{S}pectroscopy},
school = {Universität Hamburg},
type = {Dissertation},
address = {Hamburg},
reportid = {PUBDB-2019-04144},
pages = {1-196},
year = {2019},
note = {please upload the teaser image; Dissertation, Universität
Hamburg, 2019},
abstract = {One of the big technical and scientific challenges today is
to accomplish the ultimate dreamof filming chemical
reactions with atomic spatial and temporal resolution and
recording themolecular movie. Important prerequisites toward
this goal are, on the one hand, methodsto create cold,
controlled molecular samples and, on the other hand, imaging
techniquesthat combine the required spatial and temporal
resolution. In recent years, especially due tothe fast
progress in the development of laser and electron sources,
more and more refinedimaging techniques have become
accessible. The combination of quantum state selectionwith
laser-induced field-free alignment and orientation, allow to
precisely control and preparethe molecules under study,
before being imaged. Using ultrafast, high-intensity laser
sourcesin the mid-infrared spectral range, self-imaging
methods, such as laser-induced electrondiffraction (LIED),
have emerged and their full potential can be explored today
to image thestructure and dynamics of molecules with atomic
spatio-temporal resolution.This work can be divided into two
major parts, the control and the imaging part.In the control
part, the focus lies on the optimization of field-free
alignment using tailoredlight fields. Strong field-free
alignment will be presented for three different molecules,
rangingfrom the relatively simple linear molecule carbonyl
sulfide (OCS) up to the complex asymmetrictop rotor indole,
which lacks rotational symmetries and marker atoms.
Different experimentaland numerical schemes of increasing
complexity will be presented, depending on the complexityof
the molecule under study, that allow to achieve strong
field-free alignment and to accessthe molecule-fixed frame
(MFF).In the imaging part, the LIED method will be employed
to image and to retrieve thestatic structure of molecules
with atomic resolution, applied on the example of OCS.
Theunprecedented degree of field-free alignment of OCS,
achieved in the control part, is employedto record
angularly-resolved photoelectron momentum distributions
(PEMDs) for differentrotational wavepackets and for
different orientations of the molecular axis with respectto
the ionizing laser polarization. These molecular-frame
angularly-resolved photoelectronspectra (MF-ARPES) exhibit
large differences, indicating a dependence of the emitted
electroncontinuum wavepacket and its dynamics on the shape
of the highest occupied molecular orbital(HOMO). In the
low-energy region of the PEMDs, strong-field photoelectron
holography(SFPH) is observed, revealing diverse interference
patterns for different molecular orientations.Moreover,
measurements of angle-dependent ionization yields of direct,
low-energy electronsand of rescattered, high-energy
electrons will be presented, showing clear
alignment-dependentfeatures. From these aforementioned
observations, conclusions will be drawn about the impactof
the underlying molecular orbital on strong-field ionization
and field-driven recollisions.},
cin = {UNI/CUI / UNI/EXP / FS-CFEL-1 / FS-CFEL-CMI},
cid = {$I:(DE-H253)UNI_CUI-20121230$ /
$I:(DE-H253)UNI_EXP-20120731$ /
I:(DE-H253)FS-CFEL-1-20120731 /
I:(DE-H253)FS-CFEL-CMI-20220405},
pnm = {6211 - Extreme States of Matter: From Cold Ions to Hot
Plasmas (POF3-621) / DFG project 255652344 - SPP 1840:
Quantum Dynamics in Tailored Intense Fields (QUTIF)
(255652344) / DFG project 281310165 - Abbildung chemischer
Dynamik mittels laserinduzierter Elektronenbeugung im
Molekülkoordinatensystem (281310165) / PHGS, VH-GS-500 -
PIER Helmholtz Graduate School $(2015_IFV-VH-GS-500)$},
pid = {G:(DE-HGF)POF3-6211 / G:(GEPRIS)255652344 /
G:(GEPRIS)281310165 / $G:(DE-HGF)2015_IFV-VH-GS-500$},
experiment = {EXP:(DE-MLZ)NOSPEC-20140101},
typ = {PUB:(DE-HGF)11},
doi = {10.3204/PUBDB-2019-04144},
url = {https://bib-pubdb1.desy.de/record/427703},
}