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Rare-gas clusters in intense VUV laser fieldsGeorgescu, Ionut 28 July 2008 (has links)
A hybrid quantum-classical approach to the interaction of atomic clusters with intense laser fields in the vacuum ultra-violet (VUV) has been developed. Much emphasis is put on localized electrons, those quasi-free electrons which localize about the ions and screen them. These electrons set a time scale, which is used to interpolate between the quantum, rate based description of photon absorption by bound electrons and the classical, deterministic description of the cluster nano-plasma. Typical observables such as total energy absorption, electron and ion spectra are in very good agreement with the experimental findings. A scheme to probe the multi-electron motion in clusters with attosecond laser pulses is introduced. Conventional final state measurements in the energy domain cannot provide information about earlier states of the system due to the incoherent nature of the dynamics. Time-delayed attosecond pulses in the extreme ultra-violet (XUV) are used to probe the transient charging of the cluster ions during the interaction with the laser by measuring the kinetic energy of the electrons detached by the probe pulse. This information is otherwise lost at later times due to recombination. Knowledge about the transient charging would also shed more light on the still controversial subject of the energy absorption mechanisms in the VUV regime. Moving to shorter duration of the excitation, the characteristic time-scales for ionization and plasma equilibration are inversed. An attosecond laser pulse in the VUV regime creates a dense, warm nano-plasma far from equilibrium. Time-delayed attosecond pulses in the XUV probe then both the creation and the relaxation. The latter shows the breakup of the Bogoliubov hierarchy of characteristic times, indicating strongly-coupled plasma dynamics and drawing parallels to the relaxation of extended ultra-cold neutral plasmas with millions of particles.
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Imagerie ultrarapide à l’échelle nanométrique par diffraction XUV cohérente / Ultrafast coherent XUV diffractive imaging at nanometer scaleGe, Xunyou 11 December 2012 (has links)
Imager des objets non-périodiques à une échelle nanométrique et à une échelle femto seconde est un vrai challenge à notre époque. Les techniques d’imagerie « sans lentille » sont des moyens puissants pour répondre à ce besoin. En utilisant des sources ultrarapide (~fs) et cohérente (ex. laser à électron libre ou harmoniques d’ordres élevés), ces techniques nous permettent de reconstruire des objets à partir de leur figure de diffraction, remplaçant les optiques conventionnelles du système d’imagerie par un algorithme informatique. Dans ce travail de thèse, je présent des expériences d’imageries en utilisant un rayonnement extrême-UV (15~40 nm) produit par la génération d’harmoniques d’ordre élevé d’un laser infrarouge puissant. Ce manuscrit est constitué d’une introduction, un chapitre de background théorique, trois chapitres de travail de thèse et une conclusion générale avec perspectives. La première partie du travail de thèse porte sur les développements et caractérisations de la ligne de lumière avec l’objectif de générer maximum de photons harmoniques cohérents avec un front d’onde plat. La deuxième partie est consacrée aux expériences et analyses de trois techniques d’imageries « sans lentille » : Imagerie par diffraction cohérente (CDI), Holographie par la transformée de Fourier (FTH) et Holographie avec références étendues (HERALDO). Ces derniers nous permettent de reconstruire des objets avec une résolution spatiale de 78 nm dans le cas de CDI et de 112 nm dans le cas de HERALDO, tous les deux avec une résolution temporaire de 20 fs. La troisième partie est une première application physique de l’imagerie sur la ligne harmonique. Il s’agit des études statiques et dynamiques de nano-domaines magnétique avec une résolution spatiale sub-100 nm à l’échelle femto seconde. Perspective des techniques d’imagerie 3D et développement potentiel de la ligne d’harmoniques sont présentés à la fin. / Ultrafast imaging of isolated objects with nanometric spatial resolution is a great challenge in our time. The lensless imaging techniques have shown great potential to answer this challenge. In lensless imaging, one can reconstruct sample images from their diffraction patterns with computational algorithms, which replace the conventional lens systems. Using ultrafast and coherent light sources, such as free electron laser and high order harmonics, one can investigate dynamic phenomena at the femtosecond time scale. In this thesis work, I present the lenless imaging experiments using XUV radiation provided by a laser driven high order harmonic beamline. The manuscript is composed of an introduction, a chapter of theoretical background, three chapters of main research work and a general conclusion with perspectives. The first part of this work concerns the development of the harmonic beamline to optimize the illumination condition for lensless imaging. The second part concentrates on the imaging techniques: the Coherent Diffraction Imaging (CDI), the Fourier Transform Holography (FTH) and the Holography using extended references (HERALDO). The reconstructions have achieved 78 nm spatial resolution in case of CDI and 112 nm resolution in case of HERALDO, both in single-shot regime corresponding to a temporal resolution of 20 fs. The third part presents the first physical application on the harmonic beamline using the lensless imaging. Samples with magnetic nano-domains have been studied with sub-100 nm spatial resolution, which paves the way for ultrafast magnetic dynamic studies. At the end, single-shot 3D imaging and further beamline development have been discussed.
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Constructing and Commissioning HELIOS – A High Harmonic Generation Source for Pump-Probe Measurements with sub 50 fs Temporal Resolution : The Development of Experimental Equipment for Extreme Ultraviolet SpectroscopyTerschlüsen, Joachim A. January 2016 (has links)
This thesis presents HELIOS, an in-house laboratory for time-resolved pump-probe spectroscopy with extreme-ultraviolet (XUV) probe radiation. A wide span of pump wavelengths can be generated using commercial laser equipment while XUV probe radiation is generated via a high harmonic generation process in a noble gas delivering probe photons with energies between 20 eV and 72 eV. The XUV beam path features a time-preserving monochromator and was constructed and built in-house. HELIOS features an overall time resolution of about 50 fs when using 800 nm pump and 41 eV probe photons. An energy resolution of 110 meV at 41 eV photon energy can be achieved. HELIOS features two beamlines. One µ-focus beamline with an XUV focal size of about 20 µm can be used with experiments that require such a small XUV focal size as well as with different end stations. The other beamline features a semi-permanently mounted end station for angle-resolved photoelectron spectroscopy under ultra-high vacuum conditions. Experiments demonstrating the usability of HELIOS and the two beamlines are presented. A pump-probe measurement on graphene demonstrates the capability of determining a large part of the k-space in only one measurement due to the use of an ARTOF angle-resolved time-of-flight electron spectrometer. A non-angle-resolved pump-probe measurement on the conducting polymer PCPDTBT demonstrates the high signal-to-noise ratio achievable at this beamline in non-angle-resolved photoelectron-spectroscopy pump-probe measurements. The usability of the µ-focus beamline is demonstrated with time-resolved measurements on magnetic samples employing an in-house-designed spectrometer. These experiments allow the retrieval of element-specific information on the magnetization within a sample employing the transversal magneto-optical Kerr effect (T-MOKE). Additionally, a Fourier transform spectrometer for the XUV is presented, the concept was tested at a synchrotron and it was used to determine the longitudinal coherence of the XUV radiation at HELIOS.
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