This Thesis describes the development of hard X-ray zone plates intended for focusing radiation at X-ray free-electron lasers (XFELs). XFELs provide unprecedented brightness and zone plates which are put in the intense X-ray beam are at risk of being damaged. Therefore, it is crucial to perform damage tests in order to design zone plates which can survive the XFEL beam. Zone plates are diffractive nanofocusing optics and are regularly used at high brightness synchrotron beamlines in the soft and hard X-ray regime. The resolution of a zone plate is proportional to its outermost zonewidth and thus depends on the smallest feature that can be fabricated. State-of-the-art nanofabrication processes developed for zone plates are able to produce zonewidths down to 10 nm. However, for hard X-rays, the zone plates need to be of sufficient thickness to efficiently focus the radiation. Thus, the limit in the fabrication of hard X-ray zone plates lies in the high aspect-ratios. This Thesis describes two processes developed for high aspect-ratio nanostructuring. The first process uses tungsten as diffractive material. Aspect-ratios up to 1:15 have been accomplished. Furthermore, a mounting method of a central stop directly on the zone plate is also presented. The other fabrication process uses diamond, in which aspect-ratios of 1:30 have been demonstrated. Both processes rely on thin-film deposition techniques, electron-beam lithography, and reactive ion etching. Thanks to the materials’ excellent thermal properties these types of zone plates should be suitable for XFEL applications. Tungsten and diamond diffractive optics have been tested at an XFEL at Stanford (LCLS), and damage investigations were performed in order to determine the maximum fluence that could be imposed on the optics before degradation occured. The conclusion of these damage tests is that tungsten and diamond diffractive optics can survive the XFEL beam and could potentially be used in beamline experiments relying on nanofocused X-ray beams. Finally in this Thesis, characterization of two zone plates using an interferometer is presented, where it is also shown that the interferometric method can be used to pin-point beamline instabilities. / <p>QC 20150112</p>

The advances achieved using X-ray Free Electron Lasers such as the Linac Coherent Light Source (LCLS), have revolutionised the routine production of uniform solid-density plasmas. Pulses of X-rays above 1 keV and with durations shorter than 100 fs attaining intensities on target of around 10¹⁷ Wcm^-2 are now routinely created. Through simple single-photon photoionization events with atoms in ambient solid conditions, it is possible to create uniform samples that are simultaneously hot, dense, and highly ionized which may be easily modelled. This thesis describes measurements of the spectrally-resolved X-rays emitted from solid-density magnesium targets of varying sub-&mu;m thicknesses isochorically heated by an X-ray laser. The data exhibit a thickness-independent source function, allowing the extraction of a measure of the opacity to K-shell X-rays within well-defined regimes of electron density and temperature, extremely close to Local Thermodynamic Equilibrium conditions by fitting to the simple 1D slab solution of the equation of radiative transfer. The deduced opacities at the peak of the K-&alpha; transitions of the ions are consistent with those predicted by detailed atomic-kinetics calculations. The extracted opacities transpire to be robust to a plethora of variations in X-ray drive conditions, including the shape, pulse-length, and energy content. Furthermore the approximations in using the 1D slab solution are examined in detail and found to be good. A full three-dimensional model of the plasma is advanced which includes attenuation, line-of-sight effects, full longitudinal and transverse gradients, and photon time-of-flight effects. The results from this model are found to also agree with the simpler 1D slab solution. This novel method of elucidating opacities may complement other methods based on absorption and could be important for further benchmarking of opacities in solar-interior relevant conditions.

Koherent Diffraktionsavbildning med en intensiv röntgenpuls från en Frielektronlaser har möjliggjort strukturbestämning av isolerade nanopartiklar som inte går att studera med hjälp av konventionella metoder, så som elektronmikroskopi. En mycket kort pulslängd tillsammans med spridningssignalens beroende av objektets elektroniska struktur medför också möjligheten att studera inducerad ultrasnabb dynamik med denna teknik. I detta projekt studerades joniseringspåverkan av Xe hos Xe-Ar core-shell-nanokluster. Enligt teorin har neutral Xe lägre spridningstvärsnitt under dess 3d-resonans än det motsvarande för fotonenergier över 3d-resonansen. Därför var en hög kontrast i klustren förväntad vid energier över dess 3d-resonans. I stället observerades mörkare regioner liknande hål i rekonstruktioner från de experimentella resultaten vid energier över 3d-resonansen hos Xe. En möjlig förklaring var jonisering av neutral Xe. För att undersöka detta skapades 3D modeller av Xe-Ar nanokluster för att simulera den interaktionen mellan intensiva röntgenpulser och nanokluster. Diffraktionsmönstren som genererades med hjälp av 3D-modellerna användes sedan för att utföra Iterativ fasrekonstruktion och rekonstruera partikeldensiteten. Brytningsindex av neutral Xe och de första tio jontillstånden hos Xe beräknades med hjälp av en modell konstruerad i detta projekt, kallad för step-model. Följaktligen introducerades samtliga jontillstånden hos Xe från 0 till 10 in i 3D modeller av Xe-Ar nanoklustren med brytningsindexen av jontillstånden uppskattade med hjälp av Kramers-Kronig-relationerna. Här antogs det att samtidigt som resonansen för varje Xe-jon förflyttas visar 𝛽 (det vill säga den imaginära komponenten i det komplexa brytningsindexet) som en funktion av fotonenergin, ett icke-monotoniskt beteende med en förändring i fotonenergin. Simuleringsresultaten erhållna med hjälp av Kramers-Kronig-relationerna visade en avtagande trend för 𝛽 i Xe-joner med en laddning&gt; 4+ till skillnad från en ökning i 𝛽 för joner med en laddning &lt;4+ relativt dess motsvarande för neutral Xe. Denna metod ansågs tillräcklig för att användas som en första approximation. Dessa resultat visade att ju mer Xe joniseras (och därför minskar 𝛽) desto mer transparenta blir Xe-jonerna under en laserpuls och därför ser de mörkare ut jämfört med Ar som har sin resonans långt ifrån fotonenergierna relevanta för detta projekt (660–760 eV). Vidare simulerades temporära förändringar i Xe-jonpopulationer för att bekräfta de erhållna simuleringsresultaten via step-model. En massiv energideposition då den intensiva röntgenpulsen träffar Xe-kärnorna initierar en serie av joniseringsmekanismer under de första få femtosekunderna av pulsen. Simuleringar för de jonpopulationer som uppstår och försvinner under förloppet av en 100 femtosekunder-lång röntgenpuls visade att jontillstånd mellan 1+ och 10+ är redan förbrukade efter några få femtosekunder vid 1016 W/cm2. Vid slutet av pulsen observerades endast högt laddade Xe-joner (upp till 35+). Den slutsats som drogs var därför att mörkare regioner som liknade hål och observerades i rekonstruktioner från experimentella data var en konsekvens av en förflyttning av resonansen hos de högt laddade Xe-joner (&gt;4+) relativt dess motsvarande i en neutral Xe så att deras spridning minskar. / Coherent Diffraction Imaging with intense x-ray pulses from X-ray Free-Electron Lasers has enabled structure determination of isolated nanoparticles, that cannot be studied with conventional methods, such as electron microscopy. The very short pulse durations and the intrinsic dependence of the scattering signal on the electronic structure of the scattering object also allow studying ultrafast light-induced dynamics with this technique. In this project, the ionization impact of Xe on Xe-Ar core-shell nanoclusters was studied. Theory predicts that neutral Xe has a lower scattering cross-section below its 3d resonance than that at photon energies above its 3d resonance. Therefore, a high contrast in clusters above the neutral Xe’s 3d resonance is expected. However, in the experimental data, unusual dark features resembling holes were observed at energies above Xe’s 3d resonance. As possible explanation, ionization of neutral Xe was suggested. To investigate this, 3D models of Xe-Ar nanoclusters were created to simulate the interaction of intense x-ray pulses and nanoclusters. The diffraction patterns generated by these 3D models were used to perform Iterative Phase Retrieval to reconstruct the particle densities. The refractive indices of neutral Xe and Xe’s first ten ionic states were computed using a model designed in this project, called the step-model. Hence, each and every ionic state of Xe from 0 to 10 were introduced into the 3D models of the Xe-Ar nanoclusters with refractive indices of the ionic states estimated based on the Kramers-Kronig relations. Here, it was assumed that as the resonance is shifting for every ionic state of Xe, 𝛽 (i.e the imaginary component of the complex refractive index) as a function of photon energy shows a nonmonotonic behavior as the photon energy is varied. The simulation results by Kramers-Kronig relations showed a decrease in 𝛽 for ionic states &gt; 4+ in contrast to an increase in 𝛽 for ions with charges &lt; 4+ relative to that of neutral Xe. This approach was sufficient to be used as a first approximation. The results showed that Xe ions become more transparent to the laser pulse as their charge increases (and 𝛽 thereby decreases) and therefore they appear darker than Ar, which has its resonance far away from photon energies relevant for this project (660–760 eV). Furthermore, temporal changes in ionic populations of Xe were simulated to confirm the simulation results obtained by the step-model. The massive energy deposition upon interaction with the intense laser pulse launches a series of ionization events in the Xe cores during the first few fs of the x-ray pulse. The simulation of ionic populations emerging and depleting during the 100-fs-long 1016 W/cm2 x-ray pulse showed that ionic states 1+ to 10+ are depleted already after a few fs. By the end of the pulse, only highly charged (up to 35+) Xe ions are observed. Therefore, it was concluded that the dark features resembling holes in reconstructions from the experimental data were a consequence of a shift in the resonance of highly charged Xe ions (&gt;4+) relative to that of neutral Xe so that their scattering decreases.