High-resolution X-ray Research Articles

DEM simulation of the compression of crushable sand: does the initial particle shape matter?

Advances in DEM modeling, combined with high-resolution X-ray tomography, opened the way for computer models based on virtual replicas of the particles to preserve nearly all facets of their geometry. This leads to simulation advantages, but also high computational costs. Here we tackle a question stemming from this trend: how accurate should particle models be to ensure accuracy? We address this question for the case of the compression of crushable sand. LS-DEM was used to generate three models of Ottawa sand (exact replicas, ellipsoids, and spheres) from digital images of its grains. Compression-induced crushing was simulated for all sets by tracking evolving size and shape distribution. The results confirm that exact replicas provide the closest match of the measurements. However, intermediate degrees of rendering (e.g., ellipsoids preserving volume and aspect ratio of the real grains) led to satisfactory results only marginally different from those of exact replicas. These findings provide an example of the protocols that may be followed to identify the optimal degree of particle approximation which should be regarded as mandatory to achieve a conscious, sustainable use of computational resources.

The way to high transmission and high-resolution tender x-ray monochromator/spectrometer using high- order multilayer coated blazed gratings

The way to high transmission and high-resolution tender x-ray monochromator/spectrometer using high- order multilayer coated blazed gratings

Large-field high-resolution X-ray AKB microscope for measuring hydrodynamic instabilities at the SG-III prototype laser facility.

X-ray imaging with a large field of view (FOV) and high resolution is extremely important for Rayleigh-Taylor instability measurement with a small amplitude and high spatial frequency in laser inertial confinement fusion. We developed an advanced Kirkpatrick-Baez (AKB) microscope based on the quadratic-aberration theory to realize a large FOV and high resolution. This microscope was assembled and tested in a laboratory, and it was then successfully applied for imaging the hydrodynamic instability of a perturbation target in implosion experiments at the Shenguang-III prototype laser facility. Imaging results demonstrate that the AKB microscope can achieve an optimal resolution of ~ 0.53μm and ~ 0.40μm and a spatial resolution of < 1.5μm within a 300-µm FOV and < 4.5μm in a 1-mm FOV.

Impact of Temperature and Substrate Type on the Optical and Structural Properties of AlN Epilayers: A Cross-Sectional Analysis Using Advanced Characterization Techniques

AlN, with its ultra-wide bandgap, is highly attractive for modern applications in deep ultraviolet light-emitting diodes and electronic devices. In this study, the surface and cross-sectional properties of AlN films grown on flat and nano-patterned sapphire substrates are characterized by a variety of techniques, including photoluminescence spectroscopy, high-resolution X-ray diffraction, X-ray photoelectron spectroscopy, ultraviolet photoelectron spectroscopy, and Raman spectroscopy. The results indicate that different sapphire substrates have minimal impact on the photoluminescence spectrum of the epitaxial films. As the temperature increased, the radius of curvature of the AlN films increased, while the warpage decreased. The AlN films grown on nano-patterned substrates exhibited superior quality with less surface oxidation. During the growth of AlN thin films on different types of substrates, slight shifts in the energy bands occurred due to differences in the introduction of carbon-related impurities and intrinsic defects. The Raman shift and full width at half maximum (FWHM) of the E2(low), A1(TO), E2(high), E1(TO), and E1(LO) phonon modes for the cross-sectional AlN films varied with the depth and temperature. The stress state within the film was precisely determined with specific depths and temperatures. The FWHM of the E2(high) phonon mode suggests that the films grown on nano-patterned substrates exhibited better crystalline quality.

Superlattice effects and limitations of non-destructive measurement of advanced Si/Si1−xGex superlattice structures using Mueller matrix scatterometry and high-resolution X-ray diffraction

Superlattice effects and limitations of non-destructive measurement of advanced Si/Si1−xGex superlattice structures using Mueller matrix scatterometry and high-resolution X-ray diffraction

High Resolution X-ray Diffraction Studies of the Natural Minerals of Gas Hydrates and Occurrence of Mixed Phases

The types and concentrations of gas hydrates collected from four different geological sites were analyzed using high-resolution angular dispersive X-ray powder diffraction, with synchrotron radiation as the source. Measurements were taken across a temperature range of 80 to 300 K and a pressure range of 0.1 to 80 MPa. All four gas hydrate samples showed the presence of three mixed crystal structures: structures I, II, and H. Additionally, the ice Ih structure was inherently present in all the natural gas hydrate minerals. The variation in the types and concentrations of gas hydrates can be attributed to the diversity of natural gases at different geographic locations.

Deep Ultraviolet Excitation Photoluminescence Characteristics and Correlative Investigation of Al-Rich AlGaN Films on Sapphire.

AlGaN is attractive for fabricating deep ultraviolet (DUV) optoelectronic and electronic devices of light-emitting diodes (LEDs), photodetectors, high-electron-mobility field-effect transistors (HEMTs), etc. We investigated the quality and optical properties of AlxGa1-xN films with high Al fractions (60-87%) grown on sapphire substrates, including AlN nucleation and buffer layers, by metal-organic chemical vapor deposition (MOCVD). They were initially investigated by high-resolution X-ray diffraction (HR-XRD) and Raman scattering (RS). A set of formulas was deduced to precisely determine x(Al) from HR-XRD data. Screw dislocation densities in AlGaN and AlN layers were deduced. DUV (266 nm) excitation RS clearly exhibits AlGaN Raman features far superior to visible RS. The simulation on the AlGaN longitudinal optical (LO) phonon modes determined the carrier concentrations in the AlGaN layers. The spatial correlation model (SCM) analyses on E2(high) modes examined the AlGaN and AlN layer properties. These high-x(Al) AlxGa1-xN films possess large energy gaps Eg in the range of 5.0-5.6 eV and are excited by a DUV 213 nm (5.8 eV) laser for room temperature (RT) photoluminescence (PL) and temperature-dependent photoluminescence (TDPL) studies. The obtained RTPL bands were deconvoluted with two Gaussian bands, indicating cross-bandgap emission, phonon replicas, and variation with x(Al). TDPL spectra at 20-300 K of Al0.87Ga0.13N exhibit the T-dependences of the band-edge luminescence near 5.6 eV and the phonon replicas. According to the Arrhenius fitting diagram of the TDPL spectra, the activation energy (19.6 meV) associated with the luminescence process is acquired. In addition, the combined PL and time-resolved photoluminescence (TRPL) spectroscopic system with DUV 213 nm pulse excitation was applied to measure a typical AlGaN multiple-quantum well (MQW). The RT TRPL decay spectra were obtained at four wavelengths and fitted by two exponentials with fast and slow decay times of ~0.2 ns and 1-2 ns, respectively. Comprehensive studies on these Al-rich AlGaN epi-films and a typical AlGaN MQW are achieved with unique and significant results, which are useful to researchers in the field.

Quantifying the Hydration-Dependent Dynamics of Cu Migration and Activity in Zeolite Omega for the Partial Oxidation of Methane.

Copper-exchanged zeolite omega (Cu-omega) is a potent material for the selective conversion of methane-to-methanol (MtM) via the oxygen looping approach. However, its performance exhibits substantial variation depending on the operational conditions. Under an isothermal temperature regime, Cu-omega demonstrates subdued activity below 230 °C, but experiences a remarkable increase in activity at 290 °C. Applying a high-temperature activation protocol at 450 °C causes a rapid deactivation of the material. This behavioral divergence is investigated by combining reactivity studies, neutron diffraction and in situ high-resolution anomalous X-ray powder diffraction (HR-AXRPD), as well as electron paramagnetic resonance spectroscopy, to reveal that the migration of Cu throughout the framework is the primary cause of these behaviors, which in turn is predominantly governed by the degree of hydration of the system. This work suggests that control over the Cu migration throughout the zeolite framework may be harnessed to significantly increase the activity of Cu-omega by generating more active sites for the MtM conversion. These results underscore the power of in situ HR-AXRPD for unraveling the behavior of materials under reaction conditions and suggest that a re-evaluation of Cu-zeolites priorly deemed inactive for the MtM conversion across a broader range of conditions and looping protocols may be warranted.

Enhancing stability of industrial Cu-based catalysts under harsh reduction reaction conditions with silica armor protection

Cu-based catalysts are widely employed in various industrial processes, yet they are susceptible to deactivation due to sintering. Inhibiting the sintering deactivation of Cu nanoparticles has been a long-standing challenge for Cu-based catalysts. In this study, we propose a novel silica armor strategy to effectively protect Cu-based catalysts from sintering. Bioethanol dehydrogenation was selected as the test reaction, with the resulting products of acetaldehyde and hydrogen displaying strong reducing properties. After a 160-hour reaction period, the Cu nanoparticles in Cu/ZnO protected by a silica armor demonstrated exceptional stability, as the sintering of the Cu nanoparticles was effectively prevented. High resolution transmission electron microscope (HRTEM), X-ray absorption (XAS), and theoretical calculations were carried out to disclose the reasons for the stabilization of Cu nanoparticles by silica armor. The physical confinement created by the silica armor and the interactions between silicon species and Cu species efficiently suppressed the sintering of Cu particles. Furthermore, our research has showcased the potential application of the silica armor strategy on commercially available catalysts, highlighting its ability to effectively prevent the sintering of Cu particles on high-Cu content Cu/ZnO/Al2O3 industrial catalysts.

Altered post-fracture systemic bone loss in a mouse model of osteocyte dysfunction

Abstract Femur fracture leads to loss of bone at uninjured skeletal sites, which may increase risk of subsequent fracture. Osteocytes, the most abundant bone cells, can directly resorb bone matrix and regulate osteoclast and osteoblast activity, but their role in systemic bone loss after fracture remains poorly understood. In this study we used a transgenic (TG+) mouse model that overexpresses human B-cell lymphoma 2 (BCL-2) in osteoblasts and osteocytes. This causes enhanced osteoblast proliferation, followed by disruption in lacunar-canalicular connectivity and massive osteocyte death by 10 weeks of age. We hypothesized that reduced viable osteocyte density would decrease the magnitude of systemic bone loss after femur fracture, reduce perilacunar remodeling, and alter callus formation. Bone remodeling was assessed using serum biomarkers of bone formation and resorption at 5 days post-fracture. We used micro-computed tomography, high resolution x-ray microscopy, mechanical testing, and Raman spectroscopy to quantify the magnitude of systemic bone loss, as well as changes in osteocyte lacunar volume, bone strength, and bone composition 2 weeks post-fracture. Fracture was associated with a reduction in circulating markers of bone resorption in non-transgenic (TG-) animals. TG+ mice exhibited high bone mass in the limbs, greater cortical elastic modulus and reduced post-yield displacement. After fracture, TG+ mice lost less trabecular bone than TG- mice, but conversely TG+ mice exhibited trends towards a lower yield point and reduced femoral cortical thickness after fracture, though these were not statistically significant. Lacunar density was greater in TG+ mice, but fracture did not alter lacunar volume in TG+ or TG- mice. These findings suggest that osteocytes potentially play a significant role in the post-traumatic systemic response to fracture, though the effects differ between trabecular and cortical bone.

Forecasting Constraints from Surface Brightness Fluctuations in Galaxy Clusters

Studies of surface brightness (SB) fluctuations in the intracluster medium present an indirect estimate of turbulent pressure support and associated Mach numbers. While high-resolution X-ray spectroscopy can directly constrain line-of-sight gas motions, including those due to turbulence, such observations are relatively expensive and will be limited to nearby, bright clusters. In this respect, SB fluctuations are the most economical means to constrain turbulent motions at large cluster radii across a range of redshifts and masses. To forecast what current and future X-ray and Sunyaev–Zel’dovich facilities may achieve in SB fluctuation studies, I review and synthesize matters of accuracy and precision with respect to calculating power spectra of SB fluctuations, from which turbulent properties are derived. Balancing concerns of power spectrum accuracy and precision across a range of spatial scales, I propose the use of three annuli with [0, 0.4]R 500, [0.4, 1]R 500, and [1, 1.5]R 500. Adopting these three regions, I calculate the uncertainty in the hydrostatic mass bias, σbM , that can be achieved for various instruments in several scenarios. I find that Lynx and AtLAST are competitive in their constraints at R 500, while AtLAST should perform better when constraining σbM at R 200.

Coherent Epitaxy of HfxZr1-xO2 Thin Films by High-pressure Magnetron Sputtering

Due to remarkable high-k and ferroelectric properties in CMOS devices, the study of crystalline HfxZr1-xO2 (HZO) thin films has attracted tremendous interest recently. However, up to now, the epitaxial growth of HZO films has only been achieved by pulse laser deposition, a technique scarcely utilized in CMOS devices. Therefore, developing appropriate epitaxial methods of HZO films (such as sputtering) is fairly necessary, but a challenge at present. In this work, high-quality single-crystalline HZO films were synthesized by high-pressure magnetron sputtering. The epitaxial growth of HZO films on yttria-stabilized zirconia (YSZ) substrate was demonstrated by a combination of high-resolution X-ray diffraction, atom force microscope, and scanning transmission electron microscope. In addition, good insulating characteristics were obtained by replacing insulating substrates with conductive substrates as electrodes. Our results provide a novel way for the epitaxial growth of the single-crystalline structure of HZO thin films towards the high performance of high-k and ferroelectric devices.

Correlation of interface structure and optical properties of Ga(N,As) and Ga(As,Bi) based type-II hetero structures

The type-II band alignment of particular III/V heterostructures is a promising route towards achieving certain wavelengths on specific substrates, which would not be possible with type-I structures. One example is telecommunication lasers on GaAs substrates. This study reports on the progress in combining dilute nitrides and dilute bismides in W-type hetero structures to improve the luminescence intensity, which is a fundamental prerequisite for future incorporation in a laser structure. Increasing the emission wavelength of these structures is challenging and the interface formation is critical, especially as two metastable materials are combined. Here, we investigate the impact of different interface configurations by growing Ga(N,As)/Ga(As,Bi) and Ga(As,Bi)/Ga(N,As) type-II structures. We employ metal–organic vapor phase epitaxy (MOVPE) to grow Ga(N,As) and Ga(As,Bi) layers and investigate the effects of interlayer thicknesses on the structural and optical properties of the hetero structures. The results indicate that − while the introduction of a GaAs interlayer can affect the direct and indirect transitions intensities − it does not significantly improve the interface quality. However, this is strongly influenced by the order in which the materials are grown. The growth of Ga(N,As) on Ga(As,Bi) shows no peculiarities, while the type II transition energy is shifted to lower energies when Ga(As,Bi) is grown on Ga(N,As). High-resolution X-ray diffraction (HR-XRD), photoluminescence (PL) spectroscopy, atomic force microscopy (AFM), and scanning transmission electron microscopy (STEM) were used to characterize the samples.

High-Performance Sol-Gel-Derived CNT-ZnO Nanocomposite-Based Photodetectors with Controlled Surface Wrinkles.

We investigate the effects of incorporating single-walled carbon nanotubes (CNTs) into sol-gel-derived ZnO thin films to enhance their optoelectronic properties for photodetector applications. ZnO thin films were fabricated on c-plane sapphire substrates with varying CNT concentrations ranging from 0 to 2.0 wt%. Characterization techniques, including high-resolution X-ray diffraction, photoluminescence, and atomic force microscopy, demonstrated the preferential growth of the ZnO (002) facet and improved optical properties with the increase in the CNT content. Electrical measurements revealed that the optimal CNT concentration of 1.5 wt% resulted in a significant increase in the dark current (from 0.34 mA to 1.7 mA) and peak photocurrent (502.9 µA), along with enhanced photoresponsivity. The rising and falling times of the photocurrent were notably reduced at this concentration, indicating improved charge dynamics due to the formation of a p-CNT/n-ZnO heterojunction. The findings suggest that the incorporation of CNTs not only modifies the structural and optical characteristics of ZnO thin films but also significantly enhances their electrical performance, positioning CNT-ZnO composites as promising candidates for advanced photodetector technologies in optoelectronic applications.

Structure-Photoluminescence Relationship in Ce3+-Doped K5Y(P2O7)2 and Its Sensitization to Dy3+ with Enhanced White Light Emission.

From a fundamental point of view, the structure-photoluminescence relationship is vitally important for developing efficient phosphors and rationally improving their performances. In this work, Rietveld refinements on high-resolution powder X-ray diffraction (XRD) data were conducted to verify the Ce3+ distribution in K5Y(P2O7)2 (KYPO). Ce3+ ions are located at both M1 and M2 sites, with occupation factors of 0.31(2) and 0.19(2), respectively. Importantly, the crystal field strength (CFS) is stronger at the former site due to the larger bond valence sum. Correspondingly, the Ce3+ emission can be deconvoluted into four Gaussian-type bands centered at ∼353, ∼383, ∼343, and ∼369 nm, where the former two belong to Ce3+ at the M1 site and the latter two are assigned to Ce3+ at the M2 site. Ce3+ in KYPO is a highly efficient activator, with optimal internal and external quantum efficiencies of 98.9 and 74.6%, respectively, and was thus utilized to sensitize the Dy3+ emission. Indeed, energy transfer from Ce3+ to Dy3+ was confirmed by fluorescent decay curves for Ce3+/Dy3+ codoped KYPO, and the mechanism was supposed to be dominated by dipole-dipole interactions. Indeed, it can be pumped by a 310 nm LED chip and emits a bright white light. Ce3+ photoluminescence exhibits high resistance to thermal quenching, and it can be further enhanced by codoping Dy3+, i.e. the emission intensity remains 96.3% at 423 K.

Breakup dynamics in a pressure-swirl injector for urea-water solution applications: A computational study

The co-optimization of in-cylinder combustion and after-treatment technology has become a major aspect in engine design and development, with the goal of meeting the increasingly restrictive emission regulations in the transportation industry. Selective Catalytic Reduction is a robust technology to control the emission of NOx, and the injection of urea in water solution is the exhaust tailpipe is a key aspect of its operation. The proposed work uses high-fidelity Computational Fluid Dynamics to characterize the atomization dynamics of the liquid jet in relevant cross-flow conditions. The study focuses on a commercial low-pressure (9 bar) pressure-swirl injector which is characterized in its internal geometry through high-resolution X-ray micro-computational tomography. The internal two-phase flow has been modeled according to the volume-of-fluid approach in a large eddy simulation framework and validated against near-nozzle X-ray radiography measurement. Moreover, characterizing the breakup dynamics for the swirling hollow cone formation, and assessing the influence of the cross-flow in the breakup dynamics was completed. The results have been reported proposing Re-Oh maps and probability density functions of the spray kinematics. Higher cross-flow momentum generates an increase in the jet intact length and a reduction of the liquid droplet diameters. The axial momentum of the jet is affected by the cross-flow already in the near-nozzle region, determining a relevant deviation of the spray velocities. This work aims to inform the initialization of Eulerian-Lagrangian spray models through the assignment of droplet kinematics and static one-way coupling between volume-of-fluid results and Lagrangian spray parcels, to be used for system-size domain simulations.

Into the spongy-verse: structural differences between leaf and flower mesophyll.

As the site of almost all terrestrial carbon fixation, the mesophyll tissue is critical to leaf function. However, mesophyll tissue is not restricted only to leaves but also occurs in the laminar, heterotrophic organs of the floral perianth, providing a powerful test of how metabolic differences are linked to differences in tissue structure. Here, we compared mesophyll tissues of leaves and flower perianths of six species using high-resolution X-ray computed microtomography (microCT) imaging. Consistent with previous studies, stomata were nearly absent from flowers, and flowers had a significantly lower vein density compared to leaves. However, mesophyll porosity was significantly higher in flowers than in leaves, and higher mesophyll porosity was associated with more aspherical mesophyll cells. Despite these differences in cell and tissue structure between leaf and flower mesophyll, modeled intercellular airspace conductance did not differ significantly between organs, regardless of differences in stomatal density between organs. These results suggest that in addition to differences between leaves and flowers in vein and stomatal densities, the mesophyll cells and tissues inside these organs also exhibit marked differences that may allow for flowers to be relatively cheaper in terms of biomass investment per unit of flower surface area.

Probing atomic-scale processes at the ferrihydrite-water interface with reactive molecular dynamics

Interfacial processes involving metal (oxyhydr)oxide phases are important for the mobility and bioavailability of nutrients and contaminants in soils, sediments, and water. Consequently, these processes influence ecosystem health and functioning, and have shaped the biological and environmental co-evolution of Earth over geologic time. Here we employ reactive molecular dynamics simulations, supported by synchrotron X-ray spectroscopy to study the molecular-scale interfacial processes that influence surface complexation in ferrihydrite-water systems containing aqueous MoO42-\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$${\ ext {MoO}_4}^{2-}$$\\end{document}. We validate the utility of this approach by calculating surface complexation models directly from simulations. The reactive force-field captures the realistic dynamics of surface restructuring, surface charge equilibration, and the evolution of the interfacial water hydrogen bond network in response to adsorption and proton transfer. We find that upon hydration and adsorption, ferrihydrite restructures into a more disordered phase through surface charge equilibration, as revealed by simulations and high-resolution X-ray diffraction. We observed how this restructuring leads to a different interfacial hydrogen bond network compared to bulk water by monitoring water dynamics. Using umbrella sampling, we constructed the free energy landscape of aqueous MoO42-\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$${\ ext {MoO}_4}^{2-}$$\\end{document} adsorption at various concentrations and the deprotonation of the ferrihydrite surface. The results demonstrate excellent agreement with the values reported by experimental surface complexation models. These findings are important as reactive molecular dynamics opens new avenues to study mineral-water interfaces, enriching and refining surface complexation models beyond their foundational assumptions.Graphic

Multifunctional GAN-based optimization for X-ray tomography under different conditions

Based on the generative adversarial network (GAN), we present a multifunctional X-ray tomographic protocol for artifact correction, noise suppression, and super-resolution of reconstruction. The protocol mainly consists of a data preprocessing module and multifunctional GAN-based loss function simultaneously dealing with ring artifacts and super-resolution. The experimental protocol removes ring artifacts and improves the contrast-to-noise ratio (CNR) and spatial resolution (SR) of reconstructed images successfully, which shows the capability to adaptively rectify ring artifacts with varying intensities and types while achieving super-resolution. Compared with the main existing deep learning models or conventional tomographic correction methods, it also enables higher processing speed and minimal information loss, especially for images of smaller dimensions. This study provides a robust optimization tool for the equivalent realization of large fields of view and high-resolution X-ray tomography. The experimental datasets were collected from a series of X-ray cone-beam computed tomography scans of biological samples.

Crystal structure, Chemical Bonding, and Magnetism of α-Fe6Ga5: How Local Interactions Shape the Structure and Properties of Intermetallic Compounds.

α-Fe6Ga5 was synthesized from the elements as a polycrystalline powder. Its crystal structure was redetermined by high-resolution powder X-ray diffraction, which showed a complex monoclinic structure of the Fe6Ge5 type. The determined lattice parameters (a = 10.08380(6) Å, b = 7.97071(5) Å, c = 7.70489(5) Å, and β = 108.3062(2)°) differ notably from the previous reports. Despite possessing the same structure type as Fe6Ge5, α-Fe6Ga5 displays several distinctive features, such as short Ga-Ga bonds and distorted Fe layers. According to magnetization measurements, α-Fe6Ga5 is a soft ferromagnet with a high Curie temperature of 760 K, which is in stark contrast to the antiferromagnetic behavior of Fe6Ge5 reported in the literature. The electronic structure of α-Fe6Ga5 was studied theoretically using density functional theory-calculations, which showed the pronouncedly covalent character of the short Fe-Ga and Ga-Ga bonds. Similar calculations were performed for Fe6Ge5, which revealed stronger Fe-Ge interactions, which preclude the formation of short Ge-Ge bonds. In both cases, the theoretical calculations showed ferromagnetic instability, which leads to ferromagnetic ordering only in the case of α-Fe6Ga5, likely due to the different nature of Fe-Ga-Fe and Fe-Ge-Fe superexchange interactions.