Angle-Resolved Observation of X-Ray Second Harmonic Generation in Diamond

This thesis reports angularly-resolved observation of X-ray second harmonic generation (XSHG) in diamond at several phase-matching geometries. The XSHG signal was produced by ultra-short, highly intense X-ray pulses with a photon energy of 9.831 keV generated by a free-electron laser. In some geometries for high pulse energies more than 10 second harmonic photons per pulse were generated. Different phase-matched geometries were used for XSHG to investigate the angular dependence of the efficiency of the process. Furthermore, for each phase-matching condition, the quadratic dependence for second harmonic generation at each geometry was verified and the crystal rocking curves were measured. The results for the angular dependence of the efficiency are in good agreement with the theory as shown by simulations (done by Priyanka Chakraborti). Improved interpretations of the data are enabled by a new analysis algorithm (developed within the framework of this thesis) that interprets the detected photon signal using a deeper understanding of the used 2D detector. Further an extensive analysis on established interpretation methods is presented. Adviser: Matthias Fuch

Thin-disk laser-pumped OPCPA system delivering 4.4 TW few-cycle pulses

We present an optical parametric chirped pulse amplification (OPCPA) system delivering 4.4 TW pulses centered at 810 nm with a sub-9 fs duration and a carrier-envelope phase stability of 350 mrad. The OPCPA setup pumped by sub-10 ps pulses from two Yb:YAG thin-disk lasers at 100 Hz repetition rate is optimized for a high conversion-efficiency. The terawatt pulses of the OPCPA are utilized for generating intense extreme ultraviolet (XUV) pulses by high-order harmonic generation, achieving XUV pulse energies approaching the microjoule level. © 2020 Optical Society of America under the terms of the OSA Open Access Publishing Agreemen

XUV double-pulses with femtosecond to 650 ps separation from a multilayer-mirror-based split-and-delay unit at FLASH

Extreme ultraviolet (XUV) and X-ray free-electron lasers enable new scientific opportunities. Their ultra-intense coherent femtosecond pulses give unprecedented access to the structure of undepositable nanoscale objects and to transient states of highly excited matter. In order to probe the ultrafast complex light-induced dynamics on the relevant time scales, the multi-purpose end-station CAMP at the free-electron laser FLASH has been complemented by the novel multilayer-mirror-based split-and-delay unit DESC (DElay Stage for CAMP) for time-resolved experiments. XUV double-pulses with delays adjustable from zero femtoseconds up to 650 picoseconds are generated by reflecting under near-normal incidence, exceeding the time range accessible with existing XUV split-and-delay units. Procedures to establish temporal and spatial overlap of the two pulses in CAMP are presented, with emphasis on the optimization of the spatial overlap at long time-delays via time-dependent features, for example in ion spectra of atomic clusters

Angle-Resolved Observation of X-Ray Second Harmonic Generation in Diamond

This thesis reports angularly-resolved observation of X-ray second harmonic generation (XSHG) in diamond at several phase-matching geometries. The XSHG signal was produced by ultra-short, highly intense X-ray pulses with a photon energy of 9.831 keV generated by a free-electron laser. In some geometries for high pulse energies more than 10 second harmonic photons per pulse were generated. Different phase-matched geometries were used for XSHG to investigate the angular dependence of the efficiency of the process. Furthermore, for each phase-matching condition, the quadratic dependence for second harmonic generation at each geometry was verified and the crystal rocking curves were measured. The results for the angular dependence of the efficiency are in good agreement with the theory as shown by simulations (done by Priyanka Chakraborti). Improved interpretations of the data are enabled by a new analysis algorithm (developed within the framework of this thesis) that interprets the detected photon signal using a deeper understanding of the used 2D detector. Further an extensive analysis on established interpretation methods is presented. Adviser: Matthias Fuch

Thin-disk laser-pumped OPCPA system delivering 44 TW few-cycle pulses

ISSN:1094-408

Propagation-assisted generation of intense few-femtosecond high-harmonic pulses

The ongoing development of intense high-harmonic generation (HHG) sources has recently enabled highly non-linear ionization of atoms by the absorption of at least 10 extreme-ultraviolet (XUV) photons within a single atom (Senfftlebenet al, arXiv:). Here we investigate how the generation of these very intense HHG pulses in our 18-m-long beamline is aided by the reshaping of the fundamental, few-cycle, near-infrared (NIR) driving laser within a 30-cm-long HHG Xe medium. Using an incident NIR intensity that is higher than what is required for phase-matched HHG, signatures of reshaping are found by measuring the NIR blueshift and the fluorescence from the HHG medium along the propagation axis. These results are well reproduced by numerical calculations that show temporal compression of the NIR pulses in the HHG medium. The simulations predict that after refocusing an XUV beam waist radius of 320 nm and a clean attosecond pulse train can be obtained in the focal plane, with an estimated XUV peak intensity of 9 x 10(15)W cm(-2). Our results show that XUV intensities that were previously only available at large-scale facilities can now be obtained using moderately powerful table-top light sources

XUV double-pulses with femtosecond to 650 ps separation from a multilayer-mirror-based split-and-delay unit at FLASH

Extreme ultraviolet (XUV) and X-ray free-electron lasers enable new scientific opportunities. Their ultra-intense coherent femtosecond pulses give unprecedented access to the structure of undepositable nanoscale objects and to transient states of highly excited matter. In order to probe the ultrafast complex light-induced dynamics on the relevant time scales, the multi-purpose end-station CAMP at the free-electron laser FLASH has been complemented by the novel multilayer-mirror-based split-and-delay unit DESC (DElay Stage for CAMP) for time-resolved experiments. XUV double-pulses with delays adjustable from zero femtoseconds up to 650 picoseconds are generated by reflecting under near-normal incidence, exceeding the time range accessible with existing XUV split-and-delay units. Procedures to establish temporal and spatial overlap of the two pulses in CAMP are presented, with emphasis on the optimization of the spatial overlap at long time-delays via time-dependent features, for example in ion spectra of atomic clusters

XUV double-pulses with femtosecond to 650 picoseconds separation from a multilayer mirror based split-and-delay unit at FLASH

Extreme ultraviolet (XUV) and X-ray free-electron lasers enable new scientific opportunities. Their ultra-intense coherent femtosecond pulses give unprecedented access to the structure of undepositable nanoscale objects and to transient states of highly excited matter. In order to probe the ultrafast complex light-induced dynamics on the relevant time scales, the multi-purpose end-station CAMP at the free-electron laser FLASH has been complemented by the novel multilayer-mirror-based split-and-delay unit DESC (DElay Stage for CAMP) for time-resolved experiments. XUV double-pulses with delays adjustable from zero femtoseconds up to 650 picoseconds are generated by reflecting under near-normal incidence, exceeding the time range accessible with existing XUV split-and-delay units. Procedures to establish temporal and spatial overlap of the two pulses in CAMP are presented, with emphasis on the optimization of the spatial overlap at long time-delays via time-dependent features, for example in ion spectra of atomic clusters.ISSN:0909-0495ISSN:1600-577

Generation of Large Vortex-Free Superfluid Helium Nanodroplets

Superfluid helium nanodroplets are an ideal environment for the formation of metastable, self-organized dopant nanostructures. However, the presence of vortices often hinders their formation. Here, we demonstrate the generation of vortex-free helium nanodroplets and explore the size range in which they can be produced. From x-ray diffraction images of xenon-doped droplets, we identify that single compact structures, assigned to vortex-free aggregation, prevail up to 10 8 atoms per droplet. This finding builds the basis for exploring the assembly of far-from-equilibrium nanostructures at low temperatures.ISSN:0031-9007ISSN:1079-711

X-ray diffractive imaging of highly ionized helium nanodroplets

Finding the lowest energy configuration of N unit charges on a sphere, known as Thomson's problem, is a long-standing query which has only been studied via numerical simulations. We present its physical realization using multiply charged He nanodroplets. The charge positions are determined by x-ray coherent diffractive imaging with Xe as a contrast agent. In neutral droplets, filaments resulting from Xe atoms condensing on quantum vortices are observed. Unique to charged droplets, however, Xe clusters that condense on charges are distributed on the surface in lattice-like structures, introducing He droplets as experimental model systems for the study of Thomson's problem.ISSN:2643-156