X-ray Microbeam Research Articles

Extraordinarily Time- and Memory-Efficient Large-Scale Canonical Correlation Analysis in Fourier Domain: From Shallow to Deep.

Canonical correlation analysis (CCA) is a correlation analysis technique that is widely used in statistics and the machine-learning community. However, the high complexity involved in the training process lays a heavy burden on the processing units and memory system, making CCA nearly impractical in large-scale data. To overcome this issue, a novel CCA method that tries to carry out analysis on the dataset in the Fourier domain is developed in this article. Appling Fourier transform on the data, we can convert the traditional eigenvector computation of CCA into finding some predefined discriminative Fourier bases that can be learned with only element-wise dot product and sum operations, without complex time-consuming calculations. As the eigenvalues come from the sum of individual sample products, they can be estimated in parallel. Besides, thanks to the data characteristic of pattern repeatability, the eigenvalues can be well estimated with partial samples. Accordingly, a progressive estimate scheme is proposed, in which the eigenvalues are estimated through feeding data batch by batch until the eigenvalues sequence is stable in order. As a result, the proposed method shows its characteristics of extraordinarily fast and memory efficiencies. Furthermore, we extend this idea to the nonlinear kernel and deep models and obtained satisfactory accuracy and extremely fast training time consumption as expected. An extensive discussion on the fast Fourier transform (FFT)-CCA is made in terms of time and memory efficiencies. Experimental results on several large-scale correlation datasets, such as MNIST8M, X-RAY MICROBEAM SPEECH, and Twitter Users Data, demonstrate the superiority of the proposed algorithm over state-of-the-art (SOTA) large-scale CCA methods, as our proposed method achieves almost same accuracy with the training time of our proposed method being 1000 times faster. This makes our proposed models best practice models for dealing with large-scale correlation datasets. The source code is available at https://github.com/Mrxuzhao/FFTCCA.

Microbeam X-ray and Scanning Electron Microscopic Analyses on Sector-Banded Spherulites of Poly(p-dioxanone) Justified with Pixelated Iridescence.

Poly(p-dioxanone) (PPDO) is crystallized with amorphous poly(p-vinyl phenol) (PVPh) and tannic acid (TA) as co-diluents to regulate and induce dendritic-ringed PPDO spherulites, with spoke- or sector-bands, aiming for convenience of analyses on interior lamellar assembly. Morphologies and interior lamellar arrangement leading to the peculiar rings on individual dendrites are evaluated by using polarized-light microscopy (PLM) and scanning electron microscope (SEM). Combinatory microbeam small-/wide-angle X-ray scattering (SAXS/WAXS) analyses further confirm the unique assembly patterns in periodic cycles. Alternate gratings are packed with periodic ridges composed of feather-like branches and the valley is featured with some embossed textures. The periodic gratings in the ringed spokes resemble those in nature's structured coloration and are proven to display light-interference iridescence.

Collimation principles of a hollow X-ray microbeam for high-contrast cytoplasm irradiation.

A Monte Carlo simulation was used to assess the performance of a collimated hollow X-ray microbeam for subcellular cytoplasm irradiation. A high-Z coaxial collimation structure with an inner core for nucleus shielding was investigated. Two key performances, the extraction efficiency (cytoplasm dose per unit incident fluence) and the dose contrast (cytoplasm-to-nucleus dose ratio), were evaluated regarding the influences of the material, geometry and physical arrangements of the collimator, target dish and incident beam source. Simulation results demonstrate that a gold coaxial structure with a practical collimation geometry of a 1-mm length, 10-μm inner diameter and 200-μm outer diameter, with the top exit closely attached (with a minimized air gap) to the bottom of a cell dish with a 3-μm thick Mylar film is recommended for cytoplasm irradiation of adherent mammalian cells. For a synchrotron source in the energy range < 10keV, a dose contrast of approximately 100 can be achieved. For a bremsstrahlung source <30-kV tube voltage, a dose contrast of approximately 50-100 can still be achieved. General principles are summarized with further explanations of the performance of the hollow X-ray microbeam.

Phoneme sequence-to-speech conversion in dynamic phonological models: A survey

This survey is devoted to dynamic models that model how a discrete phoneme sequence becomes converted to the corresponding continuous flow of articulations. The key concepts of modern dynamic models are discussed: articulatory model, articulatory parameters, goals and gestures, pronunciation effort economy principle, etc. The results of research conducted by specialists from Haskins Laboratories (articulatory phonology, task dynamic model), as well as by Japanese scientists (mostly from Waseda University) are presented. The survey is illustrated by both model examples and real articulatory X-ray microbeam measurements.

Spectral intensity drift correction of Spark Mapping Analysis for large-size metal materials

BackgroundSpectral intensity drift is a frequent issue in analytical processes, especially in long time excitation scanning for large size metal materials, which can significantly adversely impact the accuracy and stability of analysis results. Spectral intensity drift correction is the process of preprocessing spectral data using mathematical algorithms in order to facilitate the subsequent qualitative and quantitative analysis of spectra, especially in combination with stoichiometric methods. Up to now, spectral intensity drift correction within prolonged excitation has not been reported yet. ResultsWe propose an intensity drift correction method for element content of large-size samples using the Spark Mapping Analysis for Large Samples (SMALS) technique. By considering the row-by-row and column-by-column mapping modes of the SMALS, this includes curve fitting baseline correction for in-row and in-column correction, as well as total average value correction for inter-row and inter-column correction. The final measurement values are derived by coupling rows with columns. The careful implementation of correction steps can enhance baseline correction performance, effectively reducing measurement errors a drift errors. Application of this method to characterize the cross and longitudinal sections of an oversized steel billet indicates high agreement with composition distribution obtained by micro-beam X-ray fluorescence (μ-XRF). The corrected longitudinal and cross-sectional data also exhibit strong alignment. Comparison of statistical analysis results pre- and post-correction demonstrates significant improvements in the clarity of elements segregation pattern. SignificanceThis intensity drift correction method not only enhances the spectral quality but also improves the accuracy and robustness of quantitative and qualitative spectral analysis. This study contributes to establishing a robust foundation for component characterization of large-size metal materials using the SMALS technique. The novel spectral intensity correction method shows theoretical significance and practical value for large-scale, long-duration excitation scanning analysis.

Neuro-Oncologic Veterinary Trial for the Clinical Transfer of Microbeam Radiation Therapy: Acute to Subacute Radiotolerance after Brain Tumor Irradiation in Pet Dogs.

Synchrotron Microbeam Radiation Therapy (MRT) has repeatedly proven its superiority compared with conventional radiotherapy for glioma control in preclinical research. The clinical transfer phase of MRT has recently gained momentum; seven dogs with suspected glioma were treated under clinical conditions to determine the feasibility and safety of MRT. We administered a single fraction of 3D-conformal, image-guided MRT. Ultra-high-dose rate synchrotron X-ray microbeams (50 µm-wide, 400 µm-spaced) were delivered through five conformal irradiation ports. The PTV received ~25 Gy peak dose (within microbeams) per port, corresponding to a minimal cumulated valley dose (diffusing between microbeams) of 2.8 Gy. The dogs underwent clinical and MRI follow-up, and owner evaluations. One dog was lost to follow-up. Clinical exams of the remaining six dogs during the first 3 months did not indicate radiotoxicity induced by MRT. Quality of life improved from 7.3/10 [±0.7] to 8.9/10 [±0.3]. Tumor-induced seizure activity decreased significantly. A significant tumor volume reduction of 69% [±6%] was reached 3 months after MRT. Our study is the first neuro-oncologic veterinary trial of 3D-conformal Synchrotron MRT and reveals that MRT does not induce acute to subacute radiotoxicity in normal brain tissues. MRT improves quality of life and leads to remarkable tumor volume reduction despite low valley dose delivery. This trial is an essential step towards the forthcoming clinical application of MRT against deep-seated human brain tumors.

Uranium mineralization in the Thrace Basin, NW Türkiye: Evidence from radiation-induced defects in detrital quartz and synchrotron XRF/XANES analysis

The Paleogene-Neogene Thrace Basin in northwestern Türkiye has long been known to host economic gas and oil resources and has recently been reported to potentially host sandstone-type uranium deposits in the Oligocene Süloğlu Formation. The latter discovery raises questions about the source and deposition mechanism of uranium mineralization in the basin. This contribution reports on the results of a detailed electron paramagnetic resonance (EPR) spectroscopic study of detrital quartz from four sandstone and one mudstone samples in the Süloğlu Formation and documents the distribution and speciation of uranium using combined microbeam synchrotron X-ray fluorescence maps (μsXRF) and microbeam X-ray near edge structure spectroscopy (μsXANES). The EPR spectra of quartz separates are characterized by the presence of diagnostic radiation-induced defects (i.e., silicon-vacancy hole centers H′3, H′4, and H′7 with gmax = 2.049, 2.034, and 2.018, respectively, and the oxygen-vacancy electron center E′1), formed by the bombardment of alpha particles emitted from uranium, thorium, and their unstable progenies. Moreover, notable decreases in the intensity of silicon-vacancy hole centers in the EPR spectra of quartz separates after partial dissolution with hydrofluoric acid, provide compelling evidence for the circulation of uranium-bearing fluids in the Thrace Basin. The μsXRF and μsXANES data reveal the occurrences of mixed U6+ and U4+ species in hematite partially replacing pyrite aggregates but dominantly U4+ in disseminated pyrite and illite in sandstones of the Süloğlu Formation. These results provide new insights into uranium transport, reduction, and deposition mechanisms, with important implications for better understanding sandstone-type uranium deposits in general and further exploration in the Thrace Basin.

A new experimental station for microbeam X-ray scattering at the SSRF BL10U1 beamline

Benefiting from the development of high-brilliance synchrotron radiation sources, microbeam X-ray scattering has become a well established scattering-based imaging technology. This article describes the newly constructed time-resolved microbeam small-angle X-ray scattering (µSAXS) experimental station at the BL10U1 beamline at the Shanghai Synchrotron Radiation Facility. The µSAXS endstation provides SAXS/WAXS measurements with a 10 µm hard X-ray beam and a flux of ∼1012 photons s−1. A multi-axis sample stage, an on-axis viewer and in situ experimental apparatus are incorporated to facilitate multi-method scientific experiments in various material fields. As scientific examples, this article explores 1D tomography, 2D mapping and tomographic sectioning based on X-ray scattering to investigate the micro–nanostructures of polymer fiber, spherulite and bamboo samples.

Dose and compositional dependence of irradiation-induced property change in FeCr

Ferritic/martensitic steels will be used as structural components in next generation nuclear reactors. Their successful operation relies on an understanding of irradiation-induced defect behaviour in the material. In this study, Fe and FeCr alloys (3–12%Cr) were irradiated with 20 MeV Fe-ions at 313 K to doses ranging between 0.00008 dpa to 6.0 dpa. This dose range covers six orders of magnitude, spanning low, transition, and high dose regimes. Lattice strain and hardness in the irradiated material were characterised with micro-beam Laue X-ray diffraction and nanoindentation, respectively.Irradiation hardening was observed even at very low doses (0.00008 dpa) and showed a monotonic increase with dose up to 6.0 dpa. Lattice strain measurements of samples at 0.0008 dpa allow the calculation of equivalent Frenkel pair densities and corrections to the Norgett-Robinson-Torrens (NRT) model for Fe and FeCr alloys at low dose. NRT efficiency for FeCr is 0.2, which agrees with literature values for high irradiation energy. Lattice strain increases with dose up to 0.8 dpa and then decreases when the damage dose is further increased. The strains measured in this study are lower and peak at a larger dose than predicted by atomistic simulations. This difference can be explained by taking temperature and impurities into account.

The [s -- &amp;gt; ʃ] sound change in /str-/ contexts: how temporal changes in the acoustic spectrum affect fricative percept

Studies have documented a sound change in some English dialects whereby /s/ in the context /strV/ surfaces as [ʃtrV]. This can be interpreted as /s/ rounding for the rhotic being re-analyzed as [ʃ]. We recently measured F;M, the frequency of the main peak in mid-fricative spectra, in seven adults producing words with /s/ and /ʃ/ across phonetic contexts and compared the acoustics to perceptual rankings on an [ʃ] to [s] scale. One speaker exhibited a perceived sound change; two, partial sound changes. It was shown that F;M was correlated with the perceptual rankings for /strV/ words. However, in all speakers, lowered F;M for /s/ in labial contexts did not affect percepts. The time course of lip rounding and tongue-tip retraction in /strV/ could help differentiate coarticulation versus a phonemic change. Interestingly, however, X-Ray Microbeam data [Iskarous, K. et al. (2011) Articulatory-acoustic kinematics of /s/, J. Acoust. Soc. Am. 129, 944-954] showed that / s/ constriction location was constant over time except in /str-/ context. This study will assess the amount and timing of F;M lowering, its perceptual consequences and likely articulatory causes, to gain more insight into the [strV] -- &amp;gt; [ʃtrV] sound change.

Pioneering preparation and analysis of a clean surface on a microcrystal, mined by a focused ion beam

We demonstrate a series of procedures to prepare a clean surface of micro-sized graphite, mined from a bulk flake and securely affixed onto a macroscopic Si plate by focused ion beam scanning electron microscope. Analyses of structure and electronic (chemical) states were made using micro-beam X-ray photoelectron spectroscopy and angle-resolved photoemission spectroscopy. At the surface of the micro graphite, the band dispersion from a single-domain structure was observed. The proposed methodology showcases its capability to produce clean and high-quality micro samples suitable for surface-sensitive analyses. This technique paves the way to investigate surfaces of unexplored microcrystals embedded in complex materials.

Treatment planning with high-resolution 3D dose maps in preclinical and translational synchrotron microbeam radiation therapy

Background and PurposeMicrobeam Radiation Therapy (MRT) aims to deliver higher doses to the target while minimizing radiation damage to healthy tissues using synchrotron x-ray microbeams. Translational MRT research has now started, driven by promising results from preclinical studies. This study aimed to propose a first dose-outcome model by analyzing micrometric dose distributions obtained with high-resolution 3D dose calculations, accounting for the inherent physical dose distribution complexity in MRT. The feasibility of integrating penMRT, our full Monte Carlo multiscale dose calculation algorithm based on PENELOPE into translational research on veterinary patients was also investigated. Material and MethodsMicrometric dose distributions were calculated in tumor-bearing rats and for a veterinary patient with penMRT, for conformal multi-directional MRT treatment plans. Absorbed dose maps were obtained with 0.005 × 0.005 × 1 mm3 voxel sizes. High-resolution dose-volume histograms were extracted and analyzed against radiobiology studies. ResultsThe complexity of the MRT dose distribution was properly rendered at a micrometer scale on 3D dose maps, with well separated dose regions observed on the differential dose-volume histograms. The median survival time of glioma-bearing rats varied linearly with the volume fraction of the planning target volume that received doses higher than 50 Gy (R2 = 0.98). The feasibility of using penMRT for treatment planning in large volumes has been shown on a veterinary patient. ConclusionsThis study demonstrated the significant added value of penMRT for planning and prescribing MRT treatments. It also shed light on the correlation between the high-resolution 3D dose distributions and the treatment outcome.

A spatially resolved analysis of dislocation loop and nanohardness evolution in proton irradiated Zircaloys

Proton irradiation is increasingly used as a surrogate for neutron irradiation, providing similar damage structures at significantly lower costs and less time compared to neutron irradiation. However, in contrast to neutrons, protons produce a depth dependent damage profile that incorporates a plateau region and a Bragg peak in the tens of microns region depending on the material and proton energy. Here we demonstrate that this depth dependent damage can be utilised to obtain new understanding about irradiation induced damage at different dose levels from a single sample by combining spatially resolved micro-beam synchrotron X-ray diffraction-based dislocation analysis and nanoindentation. For this purpose, and to study the damage evolution starting from very early stages, we have investigated microstructure evolution and hardening behaviour of Zircaloy-2 and Zircaloy-4 proton irradiated samples between 0.01 dpa and 17 dpa at 350 °C. The results highlight good agreements of SRIM-based damage depth predictions with irradiation-induced dislocation appearance and nanohardness. However, at even relatively low damage levels within the plateau region, dislocation line density and nanohardness profiles appear saturated across the entire irradiated region, even when the dpa levels differed significantly. When relating dislocation loop line densities to nanohardness, it was found that from a certain point hardness increased only very slightly with increasing line densities. This apparent discrepancy can be explained by a decreasing loop size for the highest line densities identified by from the diffraction line profile analysis and the application of a Dispersed Barrier Hardening model that relates obstacle strength to dislocation loop size.

Retrieving images from tarnished daguerreotypes using X-ray fluorescence imaging with an X-ray micro beam with tunable energy

We report recent observations using a synchrotron X-ray micro-beam to retrieve images from tarnished 19th century daguerreotypes. We confirm that high quality image can always be retrieved from tarnished plates using Hg Lα XRF as long as the bulk of the image particles and their distribution remains intact. We also report results from using tunable tender X-rays (2 - 7 keV) to conduct imaging in high vacuum at energy above the Ag L-edge and the Hg M-edge, extracting images using Ag Lα and Hg Mα, respectively among others (e.g., S to track corrosion). Images obtained with the surface sensitive total electron yield (TEY) and the bulk sensitive fluorescence yield (FLY) as well as corresponding micro-XANES are reported. Flux tolerance to high intensity X-beam is also explored. These results and their implications for cultural heritage research are discussed.

Characterization of electromigration-induced short-range stress development in Al(0.25 at. % Cu) conductor line

Scanning x-ray microbeam topography and fluorescence experiments were conducted in situ to study the electromigration behavior of a 0.5 μm thick, 10 μm wide, and 200 μm long Al(0.25 at. % Cu) conductor line with 1.5 μm-thick SiO2 passivation on a single crystal Si substrate. The strain sensitivity of x-ray topography measurement allowed detailed examination of the electromigration-induced stress distribution and evolution in the conductor line in response to the depletion of Cu solute early in the electromigration process. Upon electromigration at 0.4 MA/cm2 and 303 °C, a short-range stress gradient was quickly induced by Al migration in the Cu-depleted cathode region to counteract further Al flow. The stress gradient was fully developed during the 5.3 h incubation time, extending over the critical Blech length of about 66 μm from the cathode end. Plastic deformation then occurred at the downstream end of the Cu-depleted region. The preferential electromigration of Cu did not cause detectable stress change outside the Cu-depleted region, except for the significant stress development from the Al2Cu precipitation at the anode end which appeared to initiate the fracture in the passivation. Preliminary finite difference modeling was undertaken to simulate the experimental observations, from which important parameters dictating electromigration in Al(Cu) line were extracted: an apparent effective valence of −5.6 and −1.9 for Cu and Al in Al(Cu), respectively, and a critical Cu concentration of 0.16 at. % above which Al grain boundary diffusion is effectively blocked.

X-ray diffraction recording from a small amount of fibrous protein materials oriented by a micro shear-flow cell.

This paper describes a method for recording X-ray diffraction patterns from a small amount of fibrous protein materials while being oriented by using a micro shear-flow cell. This cell consists of two concentrically arranged glass tubes. The inner tube is stationary, while the outer one rotates at a high speed. The gap between the two tubes is about 100 μm, into which the suspension of fibrous protein materials is injected. By using synchrotron-radiation X-ray microbeams (diameter, 10 μm), clear diffraction images from oriented protein materials can be recorded. The required volume of the sample is only about 10 μl. This method can also be combined with the laser-flash photolysis of caged compounds. Examples of application of this method to the flagella of a green alga Chlamydomonas, and sperm of a tunicate Ciona are presented.

Application of transition-edge sensors for micro-X-ray fluorescence measurements and micro-X-ray absorption near edge structure spectroscopy: a case study of uranium speciation in biotite obtained from a uranium mine.

In this study, we successfully applied a transition-edge sensor (TES) spectrometer as a detector for microbeam X-ray measurements from a synchrotron X-ray light source in the hard X-ray region to determine uranium (U) distribution at the micro-scale and its chemical species in biotite obtained from a U mine. It is difficult to separate the fluorescent X-ray of the U Lα1 line at 13.615 keV from that of the Rb Kα line at 13.395 keV in the X-ray fluorescence spectrum with an energy resolution of approximately 220 eV using a conventional silicon drift detector (SDD). Meanwhile, the fluorescent X-rays of U Lα1 and Rb Kα were fully separated by a TES with 50 eV energy resolution at an energy of around 13 keV. The successful peak separation by the TES led to an accurate mapping analysis of trace U in micro-X-ray fluorescence measurements and a decrease in the signal-to-background ratio in micro-X-ray absorption near edge structure spectroscopy. Thus, it could be a powerful tool for studying the U distribution and speciation in various environmental samples.

Confocal micro-X-ray fluorescence analysis for difference identification of ceramic samples.

A nondestructive analytical method for difference identification is required in the research fields such as forensic science or archeology. An X-ray fluorescence (XRF) analysis is one of feasible techniques for this purpose. Micro-XRF using an X-ray micro-beam gives elemental distributions by scanning the samples. A confocal micro-XRF (CM-XRF) technique is a unique analytical technique to analyze limited volume. CM-XRF enables elemental depth imaging and elemental profiling in depth nondestructively. Therefore, CM-XRF has been applied for various samples such as industrial samples, paintings, forensic samples, food materials, and human hairs. CM-XRF technique would be a suitable method for difference identification because the CM-XRF gives detailed information on elemental distribution not only on the surface of the sample but also in depth. We developed CM-XRF instrument in the laboratory and applied to two very similar ceramics samples. It showed differences in the intensity profiles of Fe and Mn for blue paintings on the ceramics. In addition, depth elemental analysis revealed different depth profiles especially of Co and Zn for both samples. These results suggest that CM-XRF provides useful information for the identification of ceramic samples.

Analysis on bimodal complex permeability spectrum of a noise suppression sheet and single constituent flakes

In recent years, highly integrated active components inside small mobile communication devices have led to serious electromagnetic interference problems. The countermeasure to this problem is covering a noise source with a noise suppression sheet (NSS) which is composed of ferromagnetic flakes and polymers. The NSS absorbs effectively electromagnetic waves due to a large imaginary part of relative permeability μr″ at the specific frequency region. This function is attributed to the bimodal μr″ spectrum of NSS, but its physical origin has not been revealed so far. In this study, the bimodal μr″ spectrum of NSS has been analyzed and its physical mechanism has been discussed. The μr″ spectrum of a constituent single magnetic flake was measured by using a newly developed high-sensitivity permeability measurement system, which showed a bimodal spectrum quite similar to that of NSS. This fact indicates that the physical origin of the bimodal μr″ spectrum is attributed to the magnetization dynamics of each single constituent flake. After measuring the μr″ spectra of single flakes with various materials, such as Fe, Fe-Al, Fe-Co-V, and Fe-Si-Al alloys, these bimodal μr″ spectra were quantitatively explained by the magnetization dynamics of the flux closure states inside the flake. The magnetic domain structure of a single flake was observed by a micro-beam X-ray magnetic circular dichroism microscopy. The result confirmed that the segmented magnetic domains form the local flux closure states inside the flake.

Quantitative Characterization of Elemental Segregation in Inconel 718 Superalloy by Micro-Beam X-ray Fluorescence Spectroscopy and Its Correlation Study.

Inconel 718 (IN718) nickel-based superalloy is widely used in aerospace and nuclear applications owing to its excellent comprehensive mechanical properties, oxidation resistance, and hot corrosion resistance. However, the elemental segregation caused by heterogeneous solidification during casting has great influence on the mechanical properties. Therefore, accurately characterizing the segregation behavior is necessary. Traditional quantitative characterization of elemental segregation uses various sampling methods, in which only macroscopic segregation results are obtained. In this study, micro-beam X-ray fluorescence (μ-XRF) is used for the quantitative characterization of element micro-segregation in IN718 superalloy. The concentration distributions of Cr, Fe, Mo, Nb, and Ti in IN718 alloy are determined with optimized testing parameters, and the degree of elemental segregation in different regions of the analytical area is calculated. It is found that the segregation degree of Nb and Ti in the testing area is larger than other alloying elements. The correlation between the microstructure distribution and the segregation degree of Nb and Ti has been studied using scanning electron microscopy (SEM) combined with energy-dispersive spectrometry (EDS). There is severe segregation of Nb and Ti in areas where Nb-containing precipitates are accumulated. The distribution of abnormal signals of Nb with a high fluorescence intensity has a close relationship with the area of precipitates-enriched Nb.