Advanced spectroscopic investigation of colour centres in LiF crystals irradiated with monochromatic hard x-rays.

Nominally-pure lithium fluoride (LiF) crystals were irradiated with monochromatic hard x-rays of energy 5, 7, 9 and 12 keV at the METROLOGIE beamline of the SOLEIL synchrotron facility, in order to understand the role of the selected x-ray energy on their visible photoluminescence (PL) response, which is used for high spatial resolution 2D x-ray imaging detectors characterized by a wide dynamic range. At the energies of 7 and 12 keV the irradiations were performed at five different doses corresponding to five uniformly irradiated areas, while at 5 and 9 keV only two irradiations at two different doses were carried out. The doses were planned in a range between 4 and 1.4 × 103Gy (10.5 mJ cm-3to 3.7 J cm-3), depending on the x-ray energy. After irradiation at the energies of 7 and 12 keV, the spectrally-integrated visible PL intensity of the F2and F3+colour centres (CCs) generated in the LiF crystals, carefully measured by fluorescence microscopy under blue excitation, exhibits a linear dependence on the irradiation dose in the investigated dose range. This linear behaviour was confirmed by the optical absorption spectra of the irradiated spots, which shows a similar linear behaviour for both the F2and F3+CCs, as derived from their overlapping absorption band at around 450 nm. At the highest x-ray energy, the average concentrations of the radiation-induced F, F2and F3+CCs were also estimated. The volume distributions of F2defects in the crystals irradiated with 5 and 9 keV x-rays were reconstructed in 3D by measuring their PL signal using a confocal laser scanning microscope operating in fluorescence mode. On-going investigations are focusing on the results obtained through thisz-scanning technique to explore the potential impact of absorption effects at the excitation laser wavelength.

Bright and fast scintillations of an inorganic halide perovskite CsPbBr3 crystal at cryogenic temperatures.

Highly efficient scintillation crystals with short decay times are indispensable for improving the performance of numerous detection and imaging instruments that use- X-rays, gamma-quanta, ionising particles or neutrons. Halide perovskites emerged recently as very promising materials for detection of ionising radiation that motivated further exploration of the materials. In this work, we report on excellent scintillation properties of CsPbBr3 crystals when cooled to cryogenic temperatures. The temperature dependence of luminescence spectra, decay kinetics and light yield under excitation with X-rays and α-particles was investigated. It is shown that the observed changes of spectral and kinetic characteristics of the crystal with temperature can be consistently explained by radiative decay of free excitons, bound and trapped excitons as well as electron-hole pairs originating from their disintegration. It has been found that the crystal exhibits a fast decay time constant of 1 ns at 7 K. The scintillation light yield of CsPbBr3 at 7 K is assessed to be 50,000 ± 10,000 ph/MeV at excitation with 12 keV X-rays and 109,000 ± 22,000 ph/MeV at excitation with α-particles of 241Am. This finding places CsPbBr3 in an excellent position for the development of a new generation of cryogenic, efficient scintillation detectors with nanosecond response time, marking a step-change in opportunities for scintillator-based applications.

SOLEIL shining on the solution-state structure of biomacromolecules by synchrotron X-ray footprinting at the Metrology beamline.

Synchrotron X-ray footprinting complements the techniques commonly used to define the structure of molecules such as crystallography, small-angle X-ray scattering and nuclear magnetic resonance. It is remarkably useful in probing the structure and interactions of proteins with lipids, nucleic acids or with other proteins in solution, often better reflecting the in vivo state dynamics. To date, most X-ray footprinting studies have been carried out at the National Synchrotron Light Source, USA, and at the European Synchrotron Radiation Facility in Grenoble, France. This work presents X-ray footprinting of biomolecules performed for the first time at the X-ray Metrology beamline at the SOLEIL synchrotron radiation source. The installation at this beamline of a stopped-flow apparatus for sample delivery, an irradiation capillary and an automatic sample collector enabled the X-ray footprinting study of the structure of the soluble protein factor H (FH) from the human complement system as well as of the lipid-associated hydrophobic protein S3 oleosin from plant seed. Mass spectrometry analysis showed that the structural integrity of both proteins was not affected by the short exposition to the oxygen radicals produced during the irradiation. Irradiated molecules were subsequently analysed using high-resolution mass spectrometry to identify and locate oxidized amino acids. Moreover, the analyses of FH in its free state and in complex with complement C3b protein have allowed us to create a map of reactive solvent-exposed residues on the surface of FH and to observe the changes in oxidation of FH residues upon C3b binding. Studies of the solvent accessibility of the S3 oleosin show that X-ray footprinting offers also a unique approach to studying the structure of proteins embedded within membranes or lipid bodies. All the biomolecular applications reported herein demonstrate that the Metrology beamline at SOLEIL can be successfully used for synchrotron X-ray footprinting of biomolecules.

X-ray broadband Ni/SiC multilayers: improvement with W barrier layers.

We present an experimental study and performance improvement of periodic and aperiodic Ni/SiC multilayer coatings. Periodic Ni/SiC multilayer mirrors have been coated and characterized by grazing incidence X-ray reflectometry at 8.048 keV (Cu Kα radiation) and by measurements at 3 keV and 5 keV on synchrotron radiation facilities. An interdiffusion effect is found between Ni and SiC layers. A two-material model, Ni(x)Si(y)/SiC, using a silicide instead of Ni, was used to fit the measurements. The addition of 0.6 nm W barrier layers at the interfaces allows a significant reduction of the interdiffusion between Ni and SiC. In order to obtain a specific reflectivity profile in the 2 - 8 keV energy range, we have designed and coated aperiodic multilayer mirrors by using Ni/SiC with and without W barrier layers. The experimental reflectivity profiles as a function of the photon energy were measured on a synchrotron radiation facility in both cases. Adding W barrier layers in Ni/SiC multilayers provides a better precision on the layer thicknesses and a very good agreement between the experimental data and the targeted spectral profile.

X-ray phase contrast imaging and noise evaluation using a single phase grating interferometer.

In this paper we present some quantitative measurements of X-ray phase contrast images and noise evaluation obtained with a recent grating based X-ray phase contrast interferometer. This device is built using a single phase grating and a large broadband X-ray source. It was calibrated using a reference sample and finally used to perform measurements of a biological fossil: a mosquito trapped in amber. As phase images, noise was evaluated from the measured interferograms.

Wavefront analysis of nonlinear self-amplified spontaneous-emission free-electron laser harmonics in the single-shot regime.

The single-shot spatial characteristics of the vacuum ultraviolet self-amplified spontaneous emission of a free electron laser (FEL) is measured at different stages of amplification up to saturation with a Hartmann wavefront sensor. We show that the fundamental radiation at 61.5 nm tends towards a single-mode behavior as getting closer to saturation. The measurements are found in good agreement with simulations and theory. A near diffraction limited wavefront was measured. The analysis of Fresnel diffraction through the Hartmann wavefront sensor hole array also provides some further insight for the evaluation of the FEL transverse coherence, of high importance for various applications.

A high-intensity highly coherent soft X-ray femtosecond laser seeded by a high harmonic beam.

Synchrotrons have for decades provided invaluable sources of soft X-rays, the application of which has led to significant progress in many areas of science and technology. But future applications of soft X-rays--in structural biology, for example--anticipate the need for pulses with much shorter duration (femtoseconds) and much higher energy (millijoules) than those delivered by synchrotrons. Soft X-ray free-electron lasers should fulfil these requirements but will be limited in number; the pressure on beamtime is therefore likely to be considerable. Laser-driven soft X-ray sources offer a comparatively inexpensive and widely available alternative, but have encountered practical bottlenecks in the quest for high intensities. Here we establish and characterize a soft X-ray laser chain that shows how these bottlenecks can in principle be overcome. By combining the high optical quality available from high-harmonic laser sources (as a seed beam) with a highly energetic soft X-ray laser plasma amplifier, we produce a tabletop soft X-ray femtosecond laser operating at 10 Hz and exhibiting full saturation, high energy, high coherence and full polarization. This technique should be readily applicable on all existing laser-driven soft X-ray facilities.

Imaging and quality assessment of high-harmonic focal spots.

We present a direct method of studying the focusability of an intense, short-pulse extreme-ultraviolet (XUV) beam obtained by high-harmonic generation. We perform near-field imaging of the focal spot of five high-harmonic orders strongly focused by a broadband toroidal mirror. To visualize the focal spot directly, we image the fluorescence induced by an XUV beam on a cerium-doped YAG crystal on a visible CCD camera. We can thus measure the harmonic spot size on a single image, together with the Strehl ratio, to evaluate the quality of focusing. Such techniques should become instrumental in optimizing the focusing conditions and reaching intensities required for exploring attosecond nonlinear optics in the XUV range.