X-ray Near Field Speckle: Implementation and Critical Analysis

We have implemented the newly-introduced, coherence-based technique of x-ray near-field speckle (XNFS) at 8-ID-I at the Advanced Photon Source. In the near field regime of high-brilliance synchrotron x-rays scattered from a sample of interest, it turns out, that, when the scattered radiation and the main beam both impinge upon an x-ray area detector, the measured intensity shows low-contrast speckles, resulting from interference between the incident and scattered beams. We built a micrometer-resolution XNFS detector with a high numerical aperture microscope objective and demonstrate its capability for studying static structures and dynamics at longer length scales than traditional far field x-ray scattering techniques. Specifically, we characterized the structure and dynamics of dilute silica and polystyrene colloidal samples. Our study reveals certain limitations of the XNFS technique, which we discuss.Comment: 53 pages, 16 figure

Effects of Impurity Content on the Sintering Characteristics of Plasma-Sprayed Zirconia

Yttria-stabilized zirconia powders, containing different levels of SiO2 and Al2O3, have been plasma sprayed onto metallic substrates. The coatings were detached from their substrates and a dilatometer was used to monitor the dimensional changes they exhibited during prolonged heat treatments. It was found that specimens containing higher levels of silica and alumina exhibited higher rates of linear contraction, in both in-plane and through-thickness directions. The in-plane stiffness and the through-thickness thermal conductivity were also measured after different heat treatments and these were found to increase at a greater rate for specimens with higher impurity (silica and alumina) levels. Changes in the pore architecture during heat treatments were studied using Mercury Intrusion Porosimetry (MIP). Fine scale porosity (<_50 nm) was found to be sharply reduced even by relatively short heat treatments. This is correlated with improvements in inter-splat bonding and partial healing of intra-splat microcracks, which are responsible for the observed changes in stiffness and conductivity, as well as the dimensional changes

Low temperature structural phase transition and incommensurate lattice modulation in the spin gap compound BaCuSi2O6

Results of high resolution x-ray diffraction experiments are presented for single crystals of the spin gap compound BaCuSi$_2$O$_6$ in the temperature range from 16 to 300 K. The data show clear evidence of a transition from the room temperature tetragonal phase into an incommensurately modulated orthorhombic structure below $\sim$100 K. This lattice modulation is characterized by a resolution limited wave vector {\bf q}$_{IC}$=(0,$\sim$0.13,0) and its 2$^{nd}$ and 3$^{rd}$ harmonics. The phase transition is first order and exhibits considerable hysteresis. This observation implies that the spin Hamiltonian representing the system is more complex than originally thought.Comment: 4 pages, 4 figure

Three-dimensional coherent X-ray diffraction imaging of a ceramic nanofoam: determination of structural deformation mechanisms

Ultra-low density polymers, metals, and ceramic nanofoams are valued for their high strength-to-weight ratio, high surface area and insulating properties ascribed to their structural geometry. We obtain the labrynthine internal structure of a tantalum oxide nanofoam by X-ray diffractive imaging. Finite element analysis from the structure reveals mechanical properties consistent with bulk samples and with a diffusion limited cluster aggregation model, while excess mass on the nodes discounts the dangling fragments hypothesis of percolation theory.Comment: 8 pages, 5 figures, 30 reference

Measurements of droplet size in shear-driven atomization using ultra-small angle x-ray scattering

[EN] Measurements of droplet size in optically-thick, non-evaporating, shear-driven sprays have been made using ultra-small angle x-ray scattering (USAXS). The sprays are produced by orifice-type nozzles coupled to diesel injectors, with measurements conducted from 1 - 24 mm from the orifice, spanning from the optically-dense near-nozzle region to more dilute regions where optical diagnostics are feasible. The influence of nozzle diameter, liquid injection pressure, and ambient density were examined. The USAXS measurements reveal few if any nanoscale droplets, in conflict with a popular computational model of diesel spray breakup. The average droplet diameter rapidly decreases with downstream distance from the nozzle until a plateau value is reached, after which only small changes are seen in droplet diameter. This plateau droplet size is consistent with the droplets being small enough to be stable with respect to further breakup. Liquid injection pressure and nozzle diameter have the biggest impact on droplet size, while ambient density has a smaller effect. (C) 2017 Published by Elsevier Ltd.X-ray spray research at Argonne is supported by the DOE Advanced Combustion Program. We acknowledge team leaders Gurpreet Singh and Leo Breton for their support. These experiments were performed at the 7-BM, 9-ID, and 15-ID beamlines of the Advanced Photon Source, Argonne National Laboratory. ChemMatCARS Sector 15 is principally supported by the Divisions of Chemistry (CHE) and Materials Research (DMR), National Science Foundation, under grant number NSF/CHE-1346572. Use of the Advanced Photon Source, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science by Argonne National Laboratory, was supported by the U.S. DOE under Contract No. DE-ACO2-06CH11357. R. Payri was funded by a Fulbright visiting scholar grant in collaboration with the Ministry of Education, Culture and Sports of Spain (reference PRX14/00331) while performing this work. J.P. Viera was funded by the Spanish MINECO grant EEBB-I-15-0976 under project TRA2012-36932.Kastengren, A.; Ilavsky, J.; Viera-Sotillo, JP.; Payri, R.; Duke, DJ.; Swantek, A.; Tilocco, FZ.... (2017). Measurements of droplet size in shear-driven atomization using ultra-small angle x-ray scattering. International Journal of Multiphase Flow. 92:131-139. https://doi.org/10.1016/j.ijmultiphaseflow.2017.03.005S1311399

Enhancement of scattering and reflectance properties of plasma-sprayed alumina coatings by controlling the porosity

nombre de pages = 5International audienceThe plasma-spraying process generates materials with typical, porous and complex, microstructures. Inspired by Dielectric Multilayer Mirrors (DMMs), thermal sprayed media may be used in the field of optics, particularly for making scattering and reflecting coatings suitable for a large range of wavelengths. In fact, pores inside plasma sprayed matrix create numerous optical index discontinuities, similarly to the gaps created in DMMs, in order to obtain high reflectivity. The porosity of coatings microstructure can be customized by selection of plasma sprayed process parameters. This study aimed to optimize scattering and reflectance properties in porous alumina by the control of spray parameters resulting in the optimized porosity. A self-supporting bi-layer with a diffuse reflectance over 90% over a large band of wavelengths was obtained. The first layer (micro-structured), which is thick enough to support the free standing, was prepared by atmospheric plasma spraying (APS). The second layer (nanostructured) was manufactured by suspension plasma spraying (SPS) over the first layer in order to enhance the reflectance at short wavelengths

Use of small-angle X-ray scattering to resolve intracellular structure changes of Escherichia coli cells induced by antibiotic treatment.

The application of small-angle X-ray scattering (SAXS) to whole Escherichia coli cells is challenging owing to the variety of internal constituents. To resolve their contributions, the outer shape was captured by ultra-small-angle X-ray scattering and combined with the internal structure resolved by SAXS. Building on these data, a model for the major structural components of E. coli was developed. It was possible to deduce information on the occupied volume, occurrence and average size of the most important intracellular constituents: ribosomes, DNA and proteins. E. coli was studied after treatment with three different antibiotic agents (chloramphenicol, tetracycline and rifampicin) and the impact on the intracellular constituents was monitored

Experimental and Computational Investigation of Subcritical Near-Nozzle Spray Structure and Primary Atomization in the Engine Combustion Network Spray D

[EN] In order to improve understanding of the primary atomization process for diesel-like sprays, a collaborative experimental and computational study was focused on the near-nozzle spray structure for the Engine Combustion Network (ECN) Spray D single-hole injector. These results were presented at the 5th Workshop of the ECN in Detroit, Michigan. Application of x-ray diagnostics to the Spray D standard cold condition enabled quantification of distributions of mass, phase interfacial area, and droplet size in the near-nozzle region from 0.1 to 14 mm from the nozzle exit. Using these data, several modeling frameworks, from Lagrangian-Eulerian to Eulerian-Eulerian and from Reynolds-Averaged Navier-Stokes (RANS) to Direct Numerical Simulation (DNS), were assessed in their ability to capture and explain experimentally observed spray details. Due to its computational efficiency, the Lagrangian-Eulerian approach was able to provide spray predictions across a broad range of conditions. In general, this "engineering-level" simulation was able to reproduce the details of the droplet size distribution throughout the spray after calibration of the spray breakup model constants against the experimental data. Complementary to this approach, higher-fidelity modeling techniques were able to provide detailed insight into the experimental trends. For example, interface-capturing multiphase simulations were able to capture the experimentally observed bimodal behavior in the transverse interfacial area distributions in the near-nozzle region. Further analysis of the spray predictions suggests that peaks in the interfacial area distribution may coincide with regions of finely atomized droplets, whereas local minima may coincide with regions of continuous liquid structures. The results from this study highlight the potential of x-ray diagnostics to reveal salient details of the near-nozzle spray structure and to guide improvements to existing primary atomization modeling approaches.Battistoni, M.; Magnotti, GM.; Genzale, CL.; Arienti, M.; Matusik, KE.; Duke, DJ.; Giraldo-Valderrama, JS.... (2018). Experimental and Computational Investigation of Subcritical Near-Nozzle Spray Structure and Primary Atomization in the Engine Combustion Network Spray D. SAE International Journal of Fuel and Lubricants. 11(4):337-352. https://doi.org/10.4271/2018-01-0277S33735211