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Advances in CdZnTeSe for Radiation Detector Applications
Detection of X- and gamma-rays is essential to a wide range of applications from medical imaging to high energy physics, astronomy, and homeland security. Cadmium zinc telluride (CZT) is the most widely used material for room-temperature detector applications and has been fulfilling the requirements for growing detection demands over the last three decades. However, CZT still suffers from the presence of a high density of performance-limiting defects, such as sub-grain boundary networks and Te inclusions. Cadmium zinc telluride selenide (CZTS) is an emerging material with compelling properties that mitigate some of the long-standing issues seen in CZT. This new quaternary is free from sub-grain boundary networks and possesses very few Te inclusions. In addition, the material offers a high degree of compositional homogeneity. The advancement of CZTS has accelerated through investigations of the material properties and virtual Frisch-grid (VFG) detector performance. The excellent material quality with highly reduced performance-limiting defects elevates the importance of CZTS as a potential replacement to CZT at a substantially lower cost.
Characterizing the X-Ray Emission of Intermediate-mass Pre-main-sequence Stars
We use X-ray and infrared observations to study the properties of three classes of young stars in the Carina Nebula: intermediate-mass (2–5 M {sub ⊙}) pre-main-sequence stars (IMPS; i.e., intermediate-mass T Tauri stars), late-B and A stars on the zero-age main sequence (AB), and lower-mass T Tauri stars (TTS). We divide our sources among these three subclassifications and further identify disk-bearing young stellar objects versus diskless sources with no detectable infrared (IR) excess emission using IR (1–8 μm) spectral energy distribution modeling. We then perform X-ray spectral fitting to determine the hydrogen-absorbing column density (N {sub H}), absorption-corrected X-ray luminosity (L {sub X}), and coronal plasma temperature (kT) for each source. We find that the X-ray spectra of both IMPS and TTS are characterized by similar kT and N {sub H}, and on average L {sub X}/L {sub bol} ~ 4 × 10{sup -4}. IMPS are systematically more luminous in X-rays (by ~0.3 dex) than all other subclassifications, with median L {sub X} = 2.5 × 10{sup 31} erg s{sup -1}, while AB stars of similar masses have X-ray emission consistent with TTS companions. These lines of evidence converge on a magnetocoronal flaring source for IMPS X-ray emission, a scaled-up version of the TTS emission mechanism. IMPS therefore provide powerful probes of isochronal ages for the first ~10 Myr in the evolution of a massive stellar population, because their intrinsic, coronal X-ray emission decays rapidly after they commence evolving along radiative tracks. We suggest that the most luminous (in both X-rays and IR) IMPS could be used to place empirical constraints on the location of the intermediate-mass stellar birth line.
Gamma, electron beam and X-ray irradiation effects on polymers in an advanced bone cement mixer device
The medical device industry has been investigating ways to increase the use of alternatives to cobalt-60 gamma radiation and ethylene-oxide gas sterilization, such as electron beam (E-beam) and X-ray radiation, due to regulatory and market pressures. One impediment to switching to E-beam or X-ray technology for sterilization is the lack of data on the effects of these radiation sources on medical device polymers. To provide such data this work considers irradiation and testing of a common single-use medical bone cement mixing system, the Stryker Advanced Cement Mixer (ACM®), that is composed of seven polymer materials. The ACM® devices considered here were processed to sterilization-relevant doses (15, 25, 50, and 70 kGy) using three radiation technologies: gamma, E-beam, and X-ray. The system and its polymer components were tested for product functionality, as well as mechanical and visual properties to determine how exposure effects may be influenced by radiation technology and dose level. We found that although there were instances of statistically significant differences in effects between the gamma-irradiated products and those irradiated with E-beam and X-ray, those effects were negligible in terms of retained functionality of the product and retained mechanical properties of the polymer components. Overall, results of this study demonstrate that, for of the effects studied, E-beam and X-ray are viable alternatives to cobalt-60 gamma radiation for sterilization of the polymer-based device investigated.
Radiation damage and dose limits in serial synchrotron crystallography at cryo- and room temperatures
Radiation damage limits the accuracy of macromolecular structures in X-ray crystallography. Cryogenic (cryo-) cooling reduces the global radiation damage rate and, therefore, became the method of choice over the past decades. The recent advent of serial crystallography, which spreads the absorbed energy over many crystals, thereby reducing damage, has rendered room temperature (RT) data collection more practical and also extendable to microcrystals, both enabling and requiring the study of specific and global radiation damage at RT. Here, we performed sequential serial raster-scanning crystallography using a microfocused synchrotron beam that allowed for the collection of two series of 40 and 90 full datasets at 2- and 1.9-Å resolution at a dose rate of 40.3 MGy/s on hen egg white lysozyme (HEWL) crystals at RT and cryotemperature, respectively. The diffraction intensity halved its initial value at average doses ( D 1/2 ) of 0.57 and 15.3 MGy at RT and 100 K, respectively. Specific radiation damage at RT was observed at disulfide bonds but not at acidic residues, increasing and then apparently reversing, a peculiar behavior that can be modeled by accounting for differential diffraction intensity decay due to the nonuniform illumination by the X-ray beam. Specific damage to disulfide bonds is evident early on at RT and proceeds at a fivefold higher rate than global damage. The decay modeling suggests it is advisable not to exceed a dose of 0.38 MGy per dataset in static and time-resolved synchrotron crystallography experiments at RT. This rough yardstick might change for proteins other than HEWL and at resolutions other than 2 Å.
Ptychographic X-ray speckle tracking with multi-layer Laue lens systems
The ever-increasing brightness of synchrotron radiation sources demands improved X-ray optics to utilize their capability for imaging and probing biological cells, nano-devices and functional matter on the nanometre scale with chemical sensitivity. Hard X-rays are ideal for high-resolution imaging and spectroscopic applications owing to their short wavelength, high penetrating power and chemical sensitivity. The penetrating power that makes X-rays useful for imaging also makes focusing them technologically challenging. Recent developments in layer deposition techniques have enabled the fabrication of a series of highly focusing X-ray lenses, known as wedged multi-layer Laue lenses. Improvements to the lens design and fabrication technique demand an accurate, robust, in situ and at-wavelength characterization method. To this end, a modified form of the speckle tracking wavefront metrology method has been developed. The ptychographic X-ray speckle tracking method is capable of operating with highly divergent wavefields. A useful by-product of this method is that it also provides high-resolution and aberration-free projection images of extended specimens. Three separate experiments using this method are reported, where the ray path angles have been resolved to within 4 nrad with an imaging resolution of 45 nm (full period). This method does not require a high degree of coherence, making it suitable for laboratory-based X-ray sources. Likewise, it is robust to errors in the registered sample positions, making it suitable for X-ray free-electron laser facilities, where beam-pointing fluctuations can be problematic for wavefront metrology.
Advanced Instrumentation for Metal Additive Manufacturing
Laser powder bed fusion (LPBF) is the most widely used process for metal additive manufacturing (AM), particularly where complex geometries provide performance advantages unattainable with traditional manufacturing techniques. However, LPBF is highly sensitive to innate variability in both the powder spreading and fusion steps, often leading to defects such as pores that are difficult to detect yet significantly impair component mechanical properties and fatigue life. This thesis presents a range of novel instruments enabling both precise assessment of powder layer characteristics and in-situ thermal metrology of metal AM to advance the quality control of LPBF. First, leveraging a custom X-ray microscope and a radiation-transport model developed through this work, transmission X-ray imaging is used to study spreading of thin metal powder layers. Effective layer depth is directly mapped at a process-relevant size scale, surpassing optical techniques that can only estimate local deposition from layer surface topography. Layer packing density and quality are shown to be influenced by powder flowability and particle size relative to nominal powder layer thickness. Layer quality is additionally connected to the geometry of the spreading implement and its velocity. This technique and its presented findings enable pairing feedstocks with spreading strategies that create layers with consistent packing density and uniformity. Second, a twofold approach is employed to optically interrogate the laser fusion step of LPBF for observing signatures of defect formation. Aperture division multiplexing is conceptualized, providing for simultaneous laser delivery and high-fidelity infrared (IR) process monitoring through a common optic. In-situ microscopy at 50 μm spatial resolution and at mid-wave IR wavelengths is proven readily achievable with the first purpose-built optic of this type. Next, a bespoke imaging spectrometer, along with a temperature-emissivity separation technique, is used to retrieve accurate process temperatures over a 1000 K range. Data from these instruments are correlated to porosity as fine as 4.3 μm in two LPBF test artifacts, as verified using computed tomography (CT), establishing the viability of robust optically-based component qualification.
LDRD 227829: Multifunctional Composite LDRD: Radiation Effect on CeO 2 -HDPE Composites
Commercial high-density polyethylene (HDPE) is lightweight with excellent mechanical properties but has limited thermal stability. To enhance this, lanthanide-based nanomaterials like CeO 2 were mixed with HDPE. Using a twin-screw extruder improved dispersion. This study examines the effects of neutron, X-rays and gamma radiation on the crystallinity of polymer of CeO 2 -HDPE composites.
Statistical data analysis of x-ray spectroscopy data enabled by neural network accelerated Bayesian inference
Bayesian inference applied to x-ray spectroscopy data analysis enables uncertainty quantification necessary to rigorously test theoretical models. However, when comparing to data, detailed atomic physics and radiation transfer calculations of x-ray emission from non-uniform plasma conditions are typically too slow to be performed in line with statistical sampling methods, such as Markov Chain Monte Carlo sampling. Furthermore, differences in transition energies and x-ray opacities often make direct comparisons between simulated and measured spectra unreliable. Here, we present a spectral decomposition method that allows for corrections to line positions and bound–bound opacities to best fit experimental data, with the goal of providing quantitative feedback to improve the underlying theoretical models and guide future experiments. In this work, we use a neural network (NN) surrogate model to replace spectral calculations of isobaric hot-spots created in Kr-doped implosions at the National Ignition Facility. The NN was trained on calculations of x-ray spectra using an isobaric hot-spot model post-processed with Cretin, a multi-species atomic kinetics and radiation code. The speedup provided by the NN model to generate x-ray emission spectra enables statistical analysis of parameterized models with sufficient detail to accurately represent the physical system and extract the plasma parameters of interest.
Perspectives on UV and x-ray photoelectron spectroscopy
Atomic photoionization using electron spectroscopy was one of the scientific topics in which Professor David A. Shirley excelled and established a research legacy. We discuss selected highlights of atomic photoionization research done by the Shirley group beginning in the 1970s. Our main topics are electron correlation satellites, photoelectron angular distributions with tunable synchrotron radiation, and developments of theory. We also discuss examples of more recent research that extends the earlier work, including double K-shell photoionization, nondipole interactions, and the pervasive role of interchannel coupling. Furthermore, we conclude with examples of current experimental and theoretical research.
A portable X-pinch design for x-ray diagnostics of warm dense matter
We describe the design and x-ray emission properties (temporal, spatial, and spectral) of Dry Pinch I, a portable X-pinch driver developed at Imperial College London. Dry Pinch I is a direct capacitor discharge device, 300 × 300 × 700 mm3 in size and ∼50 kg in mass, that can be used as an external driver for x-ray diagnostics in high-energy-density physics experiments. Among key findings, the device is shown to reliably produce 1.1 ± 0.3 ns long x-ray bursts that couple ∼50 mJ of energy into photon energies from 1 to 10 keV. The average shot-to-shot jitter of these bursts is found to be 10 ± 4.6 ns using a combination of x-ray and current diagnostics. The spatial extent of the x-ray hot spot from which the radiation emanates agrees with previously published results for X-pinches—suggesting a spot size of 10 ± 6 µm in the soft energy region (1–10 keV) and 190 ± 100 µm in the hard energy region (>10 keV). These characteristics mean that Dry Pinch I is ideally suited for use as a probe in experiments driven in the laboratory or at external facilities when more conventional sources of probing radiation are not available. At the same time, this is also the first detailed investigation of an X-pinch operating reliably at current rise rates of less than 1 kA/ns.
Toward fully coherent soft x-ray free-electron laser via echo-enabled harmonic generation in fourth generation synchrotron light sources
Having previously reported on bunching via echo-enabled harmonic generation (EEHG) as an effective way to improve the longitudinal coherence in the NSLS-II storage ring [X. Yang et al., Sci. Rep. 12, 9437 (2022)], we demonstrate that this EEHG scheme can be easily adopted to any fourth generation diffraction-limited synchrotron light source with significant benefits. The advantage of the scheme is that it requires no change of the lattice and is fully compatible with other beamlines. Since the EEHG performance is mainly determined by the momentum compaction, beam emittances, and beta functions of a SR lattice, we have identified these crucial parameters and successfully built a generalized model, which can predict the performance of nearly any SLS. Regarding the fourth generation SLSs, momentum compactions are often significantly smaller; thus, to cover the x rays with a photon energy of up to 1 keV, we utilize a specific design, including a 250 nm seed-laser wavelength. Our model predicts that for most of the current and future fourth generation SLSs, the EEHG scheme can produce significant prebunching up to harmonic 200 and, thus, generate a few MW scale peak power at 1.25 nm wavelength.
Metal Halide Scintillators with Fast and Self‐Absorption‐Free Defect‐Bound Excitonic Radioluminescence for Dynamic X‐Ray Imaging
Abstract Scintillators for radiation detection are of great significance in medical imaging, security, and nondestructive inspection. The current challenge for scintillators is to simultaneously achieve high scintillation light yield, fast radioluminescence, simple film fabrication, large X‐ray attenuation efficiency as well as stable and nontoxic compositions; no previous scintillators fulfill all the above requirements. Here, metal halide Rb 2 AgBr 3 , possessing defect‐bound excitonic radioluminescence, is shown as efficient and fast scintillators. This nontoxic and stable scintillator emits from excitons bound to neutral bromine vacancies, enjoying an efficient and spin‐allowed fast emission with minimized self‐absorption. Rb 2 AgBr 3 thus has a high light yield (25 600 photons MeV −1 ), fast scintillation decay time (5.31 ns), and a record value of light yield versus decay time (4821 photons MeV −1 ns −1 ). The close‐space sublimation method is developed for fast and scalable fabrication of oriented Rb 2 AgBr 3 films. The scintillator film is further integrated with commercial flat‐panel imagers, and the spatial resolution reaches 10.2 line pairs per millimeter at the modulation transfer function of 0.2, doubling the resolution of conventional CsI:Tl flat‐panel detectors. The dynamic X‐ray imaging and its use to real‐time monitoring of bone movement without ghosting effect is also demonstrated.
Photon-In/Photon-Out X-ray Free-Electron Laser Studies of Radiolysis
Understanding the origin of reactive species following ionization in aqueous systems is an important aspect of radiation–matter interactions as the initial reactive species lead to production of radicals and subsequent long-term radiation damage. Tunable ultrafast X-ray free-electron pulses provide a new window to probe events occurring on the sub-picosecond timescale, supplementing other methodologies, such as pulse radiolysis, scavenger studies, and stop flow that capture longer timescale chemical phenomena. We review initial work capturing the fastest chemical processes in liquid water radiolysis using optical pump/X-ray probe spectroscopy in the water window and discuss how ultrafast X-ray pump/X-ray probe spectroscopies can examine ionization-induced processes more generally and with better time resolution. Ultimately, these methods will be applied to understanding radiation effects in complex aqueous solutions present in high-level nuclear waste.
Density evolution after shock release from laser-driven polystyrene (CH) targets in inertial confinement fusion
The evolution of the plasma density in the rarefaction wave formed after a laser-driven shock is released from a CH foil was measured using optical interferometry. Here, it was found that the plasma density profile is very sensitive to the conditions at the back surface of the foil before the shock release. Dedicated experiments demonstrated that radiation preheat by coronal x-rays caused early expansion of the back surface and faster expansion of the rarefaction wave. Radiation-hydrodynamics simulations with accurate modeling of radiation preheat from the plasma corona are in good agreement with the experimental results. The early expansion of material interfaces due to coronal x-ray preheat must be evaluated in designing and interpreting laser-driven inertial confinement fusion experiments.
Limits on Leptonic TeV Emission from the Cygnus Cocoon with Swift-XRT
$\gamma$-ray observations of the Cygnus Cocoon, an extended source surrounding the Cygnus X star-forming region, suggest the presence of a cosmic ray accelerator reaching energies up to a few PeV. The very-high-energy (VHE; 0.1-100~TeV) $\gamma$-ray emission may be explained by the interaction of cosmic-ray hadrons with matter inside the Cocoon, but an origin of inverse Compton radiation by relativistic electrons cannot be ruled out. Inverse Compton $\gamma$-rays at VHE are accompanied by synchrotron radiation peaked in X-rays. Hence, X-ray observations may probe the electron population and magnetic field of the source. We observed eleven fields in or near the Cygnus Cocoon with the Neil Gehrels Swift Observatory's X-Ray Telescope (Swift-XRT) totaling 110 ksec. We fit the fields to a Galactic and extra-galactic background model and performed a log-likelihood ratio test for an additional diffuse component. We found no significant additional emission and established upper limits in each field. By assuming that the X-ray intensity traces the TeV intensity and follows an dN/dE ∝ E -2.5 spectrum, we obtained a 90% upper limit of F X < 8.7 x 10 -11 erg cm -2 s -1 or 5.2 x10 -11 erg cm -2 s -1 on the X-ray flux of the entire Cygnus Cocoon between 2 and 10 keV depending on the choice of hydrogen column density model. This suggests that no more than one quarter of the $\gamma$-ray flux at 1 TeV is produced by inverse Compton scattering, when assuming an equipartition magnetic field of ~20 μG.
Ku-band electron linac for battery-powered hand-portable 2-MeV X-ray generator
X-ray generators, producing radiation in MeV range, are a critical tool for radiography, non-destructive testing and security applications. Field operation of such source requires them to be hand-portable, autonomous and allow parameter adjustability. RF linear accelerators can serve as a flexible, reliable, and robust radiation generator alternative to dangerous radioisotopes and bulky betatrons that are currently used for field radiography if their size, weight, cost, and imaging performance are matched to these sources. Here, in this paper, we present the design and test results of a 2 MeV Ku-band electron linac for a hand-portable X-ray generator system for field radiography being developed by RadiaBeam. The dramatic scale of miniaturization and cost-reduction is achieved thanks to the implementation of innovative technologies such as air-cooled Ku-band air-traffic control magnetrons, a split accelerating structure fabrication technique, and solid-state Marx modulators. This paper presents the design of the first prototype of the accelerator, its operation from Li-Ion batteries, as well as high-power and beam measurements.