X-ray Laminography and SAXS on Beryllium Grades and Lenses and Wavefront Propagation through Imperfect Compound Refractive Lenses

Hard X-ray free electron lasers provide almost fully transverse coherent X-rays. Though the natural divergence of these X-rays is a few micro-radians, they still need to be collimated or focused while traveling up to 1km towards the sample. This can be done with beryllium compound refractive lenses (CRLs). Due to the coherence of the beam, it is important that the impurities or granular boundaries in these CRLs do not distort the wavefront of the X-ray beam to a measurable extend. We measured the SAXS signal of various beryllium grades and of 2D parabolic lenses made of IF-1 beryllium. Then, we imaged these samples using X-ray computed laminography at a resolution of around 1 micrometer. Computed laminography is a 3D imaging technique similar to computed tomography, but particularly adapted for at extended objects. These measurements are used to characterize the voids and granular boundaries in the beryllium samples. Boundaries between the former powder particles are easily seen for beryllium grades produced via powder metallurgy methods. This is not the case for cast ingots. Common to all samples are voids with diameters in the 10 micrometer range as well as smaller sized, denser impurities. Finally, we use wavefront propagation simulations in order to analyze the effect of voids in the CRLs on the wavefront of the XFEL beam. If the distance "lens to focus and sample" is large enough, the diffraction patterns emerging from the voids smoothen ou

Design and Throughput Simulations of a Hard X-Ray Split and Delay Line for the MID Station at the European XFEL

A hard X-ray Split and Delay Line (SDL) under development for the Materials Imaging and Dynamics (MID) station at the European X-Ray Free-Electron Laser (XFEL.EU) is presented. This device will provide pairs of X-ray pulses with a variable time delay ranging from-10 ps to 800 ps in a photon energy range from 5 to 10 keV. Throughput simulations in the SASE case indicate a total transmission of 1.1% or 3.5% depending on the operation mode. In the self-seeded case of XFEL.EU operation simulations indicate that the transmission can be improved to more than 11%

Implications of disturbed photon-counting statistics of Eiger detectors for X-ray speckle visibility experiments

This paper reports on coherent scattering experiments in the low-count regime with less than one photon per pixel per acquisition on average, conducted with two detectors based on the Eiger single-photon-counting chip. The obtained photon-count distributions show systematic deviations from the expected Poisson–gamma distribution, which result in a strong overestimation of the measured speckle contrast. It is shown that these deviations originate from an artificial increase of double-photon events, which is proportional to the detected intensity and inversely proportional to the exposure time. The observed miscounting effect may have important implications for new coherent scattering experiments emerging with the advent of high-brilliance X-ray sources. Different correction schemes are discussed in order to obtain the correct photon distributions from the data. A successful correction is demonstrated with the measurement of Brownian motion from colloidal particles using X-ray speckle visibility spectroscop

Ultrafast time dynamics studies of periodic lattices with free electron laser radiation

It has been proposed that radiation from free electron laser(FEL) at Hamburg (FLASH) can be used for ultrafast time-resolved x-ray diffraction experiments based on the near-infrared (NIR) pump/FEL probe scheme. Here, investigation probing the ultrafast structural dynamics of periodic nano-crystalline organic matter (silver behenate) with such a scheme is reported. Excitation with a femtosecond NIR laser leads to an ultrafast lattice modification which time evolution has been studied through the scattering of vacuum ultraviolet FEL pulses. The found effect last for 6 ps and underpins the possibility for studying nanoperiodic dynamics down to the FEL source time resolution. Furthermore, the possibility of extending the use of silver behenate (AgBh) as a wavelength and temporal calibration tool for experiments with soft x-ray/FEL sources is suggested

Coherence properties from speckle contrast analysis at the European XFEL

We show the results of speckle contrast analysis at the MID instrument of European XFEL in the hard X-ray regime. Speckle patterns measured from static colloidal samples are compared to results previously obtained at the SPB/SFX instrument. A high degree of coherence of 0.79 is obtained by modelling the q-dependence of the speckle contrast, that corresponds to a number of coherent modes of M = 1.7. Furthermore, the variation of contrast over many pulse trains is exceptional low, resulting in a degree of coherence with a relative standard deviation below 0.1. Our results demonstrate the high stability of coherence properties at European XFEL over many X-ray pulses and pulse trains which is a prerequisite for coherence-based techniques such as MHz X-ray photon correlation spectroscopy

Single-pulse phase-contrast imaging at free-electron lasers in the hard X-ray regime

X-ray free-electron lasers (XFELs) have opened up unprecedented opportunities for time-resolved nano-scale imaging with X-rays. Near-field propagation-based imaging, and in particular near-field holography (NFH) in its high-resolution implementation in cone-beam geometry, can offer full-field views of a specimen's dynamics captured by single XFEL pulses. To exploit this capability, for example in optical-pump/X-ray-probe imaging schemes, the stochastic nature of the self-amplified spontaneous emission pulses, i.e. the dynamics of the beam itself, presents a major challenge. In this work, a concept is presented to address the fluctuating illumination wavefronts by sampling the configuration space of SASE pulses before an actual recording, followed by a principal component analysis. This scheme is implemented at the MID (Materials Imaging and Dynamics) instrument of the European XFEL and time-resolved NFH is performed using aberration-corrected nano-focusing compound refractive lenses. Specifically, the dynamics of a micro-fluidic water-jet, which is commonly used as sample delivery system at XFELs, is imaged. The jet exhibits rich dynamics of droplet formation in the break-up regime. Moreover, pump–probe imaging is demonstrated using an infrared pulsed laser to induce cavitation and explosion of the jet

Pump-probe X-ray holographic imaging of laser-induced cavitation bubbles with femtosecond FEL pulses

Cavitation bubbles can be seeded from a plasma following optical breakdown, by focusing an intense laser in water. The fast dynamics are associated with extreme states of gas and liquid, especially in the nascent state. This offers a unique setting to probe water and water vapor far-from equilibrium. However, current optical techniques cannot quantify these early states due to contrast and resolution limitations. X-ray holography with single X-ray free-electron laser pulses has now enabled a quasi-instantaneous high resolution structural probe with contrast proportional to the electron density of the object. In this work, we demonstrate cone-beam holographic flash imaging of laser-induced cavitation bubbles in water with nanofocused X-ray free-electron laser pulses. We quantify the spatial and temporal pressure distribution of the shockwave surrounding the expanding cavitation bubble at time delays shortly after seeding and compare the results to numerical simulations

Resonant X-ray excitation of the nuclear clock isomer 45Sc

Resonant oscillators with stable frequencies and large quality factors help us to keep track of time with high precision. Examples range from quartz crystal oscillators in wristwatches to atomic oscillators in atomic clocks, which are, at present, our most precise time measurement devices1. The search for more stable and convenient reference oscillators is continuing2,3,4,5,6. Nuclear oscillators are better than atomic oscillators because of their naturally higher quality factors and higher resilience against external perturbations7,8,9. One of the most promising cases is an ultra-narrow nuclear resonance transition in 45Sc between the ground state and the 12.4-keV isomeric state with a long lifetime of 0.47 s (ref. 10). The scientific potential of 45Sc was realized long ago, but applications require 45Sc resonant excitation, which in turn requires accelerator-driven, high-brightness X-ray sources11 that have become available only recently. Here we report on resonant X-ray excitation of the 45Sc isomeric state by irradiation of Sc-metal foil with 12.4-keV photon pulses from a state-of-the-art X-ray free-electron laser and subsequent detection of nuclear decay products. Simultaneously, the transition energy was determined as with an uncertainty that is two orders of magnitude smaller than the previously known values. These advancements enable the application of this isomer in extreme metrology, nuclear clock technology, ultra-high-precision spectroscopy and similar applications

Microsecond hydrodynamic interactions in dense colloidal dispersions probed at the European XFEL

Many soft-matter systems are composed of macromolecules or nanoparticles suspended in water. The characteristic times at intrinsic length scales of a few nanometres fall therefore in the microsecond and sub-microsecond time regimes. With the development of free-electron lasers (FELs) and fourth-generation synchrotron light-sources, time-resolved experiments in such time and length ranges will become routinely accessible in the near future. In the present work we report our findings on prototypical soft-matter systems, composed of charge-stabilized silica nanoparticles dispersed in water, with radii between 12 and 15 nm and volume fractions between 0.005 and 0.2. The sample dynamics were probed by means of X-ray photon correlation spectroscopy, employing the megahertz pulse repetition rate of the European XFEL and the Adaptive Gain Integrating Pixel Detector. We show that it is possible to correctly identify the dynamical properties that determine the diffusion constant, both for stationary samples and for systems driven by XFEL pulses. Remarkably, despite the high photon density the only observable induced effect is the heating of the scattering volume, meaning that all other X-ray induced effects do not influence the structure and the dynamics on the probed timescales. This work also illustrates the potential to control such induced heating and it can be predicted with thermodynamic models

On the use of multilayer Laue lenses with X-ray Free Electron Lasers

Multilayer Laue lenses were used for the first time to focus x-rays from an X-ray Free Electron Laser (XFEL). In an experiment, which was performed at the European XFEL, we demonstrated focusing to a spot size of a few tens of nanometers. A series of runs in which the number of pulses per train was increased from 1 to 2, 3, 4, 5, 6, 7, 10, 20 and 30 pulses per train, all with a pulse separation of 3.55 us, was done using the same set of lenses. The increase in the number of pulses per train was accompanied with an increase of x-ray intensity (transmission) from 9% to 92% at 5 pulses per train, and then the transmission was reduced to 23.5 % when the pulses were increased further. The final working condition was 30 pulses per train and 23.5% transmission. Only at this condition we saw that the diffraction efficiency of the MLLs changed over the course of a pulse train, and this variation was reproducible from train to train. We present the procedure to align and characterize these lenses and discuss challenges working with the pulse trains from this unique x-ray source