Characterization of Pt-coated twin paraboloidal laboratory capillary high energy X-ray optics.

Novel focusing optics composed of twin paraboloidal capillaries coated with Pt, for laboratory X-ray sources are presented and characterized. The optics are designed to focus the X-rays, resulting in an achromatic focused beam with photon energies up to 40 keV. The performance of the optics under different operational conditions is studied by comparing the energy-photon count spectra of the direct and focused beams. Based on these analyses, the optics gain and efficiency as a function of photon energy are determined. A focal spot of 8.5 µm with a divergence angle of 0.59° is observed. The obtained characteristics are discussed and related to theoretical considerations. Moreover, the suitability and advantages of the present optics for X-ray microdiffraction is demonstrated using polycrystalline aluminium. Finally, possibilities for further developments are suggested.

Single-shot, omni-directional x-ray scattering imaging with a laboratory source and single-photon localization.

Omni-directional, ultra-small-angle x-ray scattering imaging provides a method to measure the orientation of micro-structures without having to resolve them. In this letter, we use single-photon localization with the Timepix3 chip to demonstrate, to the best of our knowledge, the first laboratory-based implementation of single-shot, omni-directional x-ray scattering imaging using the beam-tracking technique. The setup allows a fast and accurate retrieval of the scattering signal using a simple absorption mask. We suggest that our new approach may enable faster laboratory-based tensor tomography and could be used for energy-resolved x-ray scattering imaging.

Evolution of intermetallic GaPd2/SiO2 catalyst and optimization for methanol synthesis at ambient pressure.

The CO2 hydrogenation to methanol is efficiently catalyzed at ambient pressure by nanodispersed intermetallic GaPd2/SiO2 catalysts prepared by incipient wetness impregnation. Here we optimize the catalyst in terms of metal content and reduction temperature in relation to its catalytic activity. We find that the intrinsic activity is higher for the GaPd2/SiO2 catalyst with a metal loading of 13 wt.% compared to catalysts with 23 wt.% and 7 wt.%, indicating that there is an optimum particle size for the reaction of around 8 nm. The highest catalytic activity is measured on catalysts reduced at 550°C. To unravel the formation of the active phase, we studied calcined GaPd2/SiO2 catalysts with 23 wt.% and 13 wt.% using a combination of in situ techniques: X-ray diffraction (XRD), X-ray absorption near edge fine structure (XANES) and extended X-ray absorption fine structure (EXAFS). We find that the catalyst with higher metal content reduces to metallic Pd in a mixture of H2/Ar at room temperature, while the catalyst with lower metal content retains a mixture of PdO and Pd up to 140°C. Both catalysts form the GaPd2 phase above 300°C, albeit the fraction of crystalline intermediate Pd nanoparticles of the catalyst with higher metal loading reduces at higher temperature. In the final state, the catalyst with higher metal loading contains a fraction of unalloyed metallic Pd, while the catalyst with lower metal loading is phase pure. We discuss the alloying mechanism leading to the catalyst active phase formation selecting three temperatures: 25°C, 320°C and 550°C.

Subpixel resolution in CdTe Timepix3 pixel detectors.

Timepix3 (256 × 256 pixels with a pitch of 55 µm) is a hybrid-pixel-detector readout chip that implements a data-driven architecture and is capable of simultaneous time-of-arrival (ToA) and energy (ToT: time-over-threshold) measurements. The ToA information allows the unambiguous identification of pixel clusters belonging to the same X-ray interaction, which allows for full one-by-one detection of photons. The weighted mean of the pixel clusters can be used to measure the subpixel position of an X-ray interaction. An experiment was performed at the European Synchrotron Radiation Facility in Grenoble, France, using a 5 µm × 5 µm pencil beam to scan a CdTe-ADVAPIX-Timepix3 pixel (55 µm × 55 µm) at 8 × 8 matrix positions with a step size of 5 µm. The head-on scan was carried out at four monochromatic energies: 24, 35, 70 and 120 keV. The subpixel position of every single photon in the beam was constructed using the weighted average of the charge spread of single interactions. Then the subpixel position of the total beam was found by calculating the mean position of all photons. This was carried out for all points in the 8 × 8 matrix of beam positions within a single pixel. The optimum conditions for the subpixel measurements are presented with regards to the cluster sizes and beam subpixel position, and the improvement of this technique is evaluated (using the charge sharing of each individual photon to achieve subpixel resolution) versus alternative techniques which compare the intensity ratio between pixels. The best result is achieved at 120 keV, where a beam step of 4.4 µm ± 0.86 µm was measured.

Novel micro-reactor flow cell for investigation of model catalysts using in situ grazing-incidence X-ray scattering.

The design, fabrication and performance of a novel and highly sensitive micro-reactor device for performing in situ grazing-incidence X-ray scattering experiments of model catalyst systems is presented. The design of the reaction chamber, etched in silicon on insulator (SIO), permits grazing-incidence small-angle X-ray scattering (GISAXS) in transmission through 10 µm-thick entrance and exit windows by using micro-focused beams. An additional thinning of the Pyrex glass reactor lid allows simultaneous acquisition of the grazing-incidence wide-angle X-ray scattering (GIWAXS). In situ experiments at synchrotron facilities are performed utilizing the micro-reactor and a designed transportable gas feed and analysis system. The feasibility of simultaneous in situ GISAXS/GIWAXS experiments in the novel micro-reactor flow cell was confirmed with CO oxidation over mass-selected Ru nanoparticles.

Introducing a standard method for experimental determination of the solvent response in laser pump, X-ray probe time-resolved wide-angle X-ray scattering experiments on systems in solution.

In time-resolved laser pump, X-ray probe wide-angle X-ray scattering experiments on systems in solution the structural response of the system is accompanied by a solvent response. The solvent response is caused by reorganization of the bulk solvent following the laser pump event, and in order to extract the structural information of the solute, the solvent response has to be treated. Methodologies capable of doing so include both theoretical modelling and experimental determination of the solvent response. In the work presented here, we have investigated how to obtain a reproducible solvent response-the solvent term-experimentally when applying laser pump, X-ray probe time-resolved wide-angle X-ray scattering. The solvent term describes difference scattering arising from the structural response of the solvent to changes in the hydrodynamic parameters: pressure, temperature and density. We present results based on NIR and dye mediated solvent heating, and demonstrate that the solvent response is independent of the heating method. The NIR heating is shown to be rendered unusable by higher order effects under certain experimental conditions, while the dye mediated solvent heating is demonstrated to exhibit first order behaviour with respect to the amount of energy deposited in the solution. We introduce a standardized method for recording solvent responses in laser pump, X-ray probe time-resolved X-ray wide-angle scattering experiments by using dye mediated solvent heating. Furthermore, we have generated a library of solvent terms, which can be used to describe the solvent term in any TRWAXS experiment, and made it available online.