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@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},
}