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At least 37 records · Page 2

Advances in ultrafast gas-phase x-ray scattering

Recent developments of x-ray free electron lasers and pulsed electron sources have enabled ultrafast scattering to become an increasingly powerful tool for exploring molecular dynamics. Here, this article describes our recent experimental and methodological advances in ultrafast gas-phase x-ray scattering experiments at the LCLS. A re-designed short-pathlength windowless diffractometer is coupled with careful optimization of sample density and independent normalization of x-ray intensity fluctuations to provide gas-phase scattering patterns with exceptionally high signal-to-noise ratios. These advances, coupled with careful geometry optimization and data treatment, provide both ground- and excited-state signals in excellent agreement with high level ab initio total scattering patterns.

74 ATOMIC AND MOLECULAR PHYSICS↗

Comparative time-resolved photoemission from the Cu(100) and Cu(111) surfaces

Motivated by the striking dependence of the valence electronic structure of transition metal surfaces on their crystallographic orientation, and by emerging experiments on laser-assisted extended ultraviolet (XUV) photoemission from solid surfaces, we calculate photoemission spectra from Cu(100) and Cu(111) surfaces as a function of the photoelectron final kinetic energy and the delay between the ionizing attosecond XUV pulse train and assisting infrared (IR) laser pulse. Our numerical simulations predict distinct differences in delay-dependent photoelectron energy distributions and photoemission time delays for Cu(100) and Cu(111) surfaces. Furthermore, these differences can be scrutinized experimentally with existing technology in a suggested in situ comparative RABBITT (reconstruction of attosecond beating by interference of two-photon transitions) configuration by placing the two surfaces on a sliding platform while keeping all optical components and pathlengths fixed. Our calculations also show that the inclusion of the Fresnel-reflected incident IR pulse at the metal-vacuum interface modifies photoelectron spectra and photoemission time delays in a characteristic way that reveals the degree of spatial location of the initial electronic states.

74 ATOMIC AND MOLECULAR PHYSICS↗

Sub-Bandgap Features in CdSeTe Solar Cells: Parsing the Roles of Material Properties and Cell Optics

In this contribution, we investigate why different dopant species and back-contact architectures lead to different sub-bandgap behaviors in CdSeTe solar cells. Through extraction of the absorptance from photoluminescence spectra, we parse the contributions from material properties and from cell optics. We show that, as expected, arsenic doping leads to an increase in sub-bandgap features over traditional copper doping, and that this is a material property of arsenic-doped CdSeTe. Conversely, the increase in sub-bandgap absorption and emission using alternative back contact architectures can be attributed to the cell optics, and more specifically to the increased reflectance of the back interface, leading to at least a doubling of the pathlength for sub-bandgap photons.

arsenic doping↗

Granal thylakoid structure and function: explaining an enduring mystery of higher plants

Summary In higher plants, photosystems II and I are found in grana stacks and unstacked stroma lamellae, respectively. To connect them, electron carriers negotiate tortuous multi‐media paths and are subject to macromolecular blocking. Why does evolution select an apparently unnecessary, inefficient bipartition? Here we systematically explain this perplexing phenomenon. We propose that grana stacks, acting like bellows in accordions, increase the degree of ultrastructural control on photosynthesis through thylakoid swelling/shrinking induced by osmotic water fluxes. This control coordinates with variations in stomatal conductance and the turgor of guard cells, which act like an accordion's air button. Thylakoid ultrastructural dynamics regulate macromolecular blocking/collision probability, direct diffusional pathlengths, division of function of Cytochrome b 6 f complex between linear and cyclic electron transport, luminal pH via osmotic water fluxes, and the separation of pH dynamics between granal and lamellar lumens in response to environmental variations. With the two functionally asymmetrical photosystems located distantly from each other, the ultrastructural control, nonphotochemical quenching, and carbon‐reaction feedbacks maximally cooperate to balance electron transport with gas exchange, provide homeostasis in fluctuating light environments, and protect photosystems in drought. Grana stacks represent a dry/high irradiance adaptation of photosynthetic machinery to improve fitness in challenging land environments. Our theory unifies many well‐known but seemingly unconnected phenomena of thylakoid structure and function in higher plants.

59 BASIC BIOLOGICAL SCIENCES↗

Optical constants measurements of liquids for modeling aerosolized threats

Spectroscopic identification of aerosolized chemical threats is challenging due to the complex nature of the photon/particle interaction, as well as the diversity of possible particle sizes, morphologies, and compositions. Constructing a database of laboratory - measured transmittance spectra that covers each permutation is not practical. However, calculation of the spectra using the measured optical constants as a function of wavenumber, n(?) and k(?), for each of the liquids and/or solids composing the aerosol particles provides a viable alternative. These synthetic spectra (vis-à-vis laboratory-measured spectra) can be used to identify chemicals of interest and subtract out background interferents in field measurements. Using a well-established multiple pathlength approach, we measure the optical constants n/k for liquids that may be found as chemical species of interest or common background interferents aerosolized in plumes. These measurements are also used to generate several test case aerosol synthetic spectra.

Lockwood, Schuyler↗

The effects of gantry tilt on breast dose and image noise in cardiac CT

Purpose: This study investigated the effects of tilted-gantry acquisition on image noise and glandular breast dose in females during cardiac computed tomography (CT) scans. Reducing the dose to glandular breast tissue is important due to its high radiosensitivity and limited diagnostic significance in cardiac CT scans.Methods: Tilted-gantry acquisition was investigated through computer simulations and experimental measurements. Upon IRB approval, eight voxelized phantoms were constructed from previously acquired cardiac CT datasets. Monte Carlo simulations quantified the dose deposited in glandular breast tissue over a range of tilt angles. The effects of tilted-gantry acquisition on breast dose were measured on a clinical CT scanner (CT750HD, GE Healthcare) using an anthropomorphic phantom with MOSFET dosimeters in the breast regions. In both simulations and experiments, scans were performed at gantry tilt angles of 0°–30°, in 5° increments. The percent change in breast dose was calculated relative to the nontilted scan for all tilt angles. The percent change in noise standard deviation due to gantry tilt was calculated in all reconstructed simulated and experimental images.Results: Tilting the gantry reduced the breast dose in all simulated and experimental phantoms, with generally greater dose reduction at increased gantry tilts. For example, at 30° gantry tilt, the dosimeters located in the superior, middle, and inferior breast regions measured dose reductions of 74%, 61%, and 9%, respectively. The simulations estimated 0%–30% total breast dose reduction across the eight phantoms and range of tilt angles. However, tilted-gantry acquisition also increased the noise standard deviation in the simulated phantoms by 2%–50% due to increased pathlength through the iodine-filled heart. The experimental phantom, which did not contain iodine in the blood, demonstrated decreased breast dose and decreased noise at all gantry tilt angles.Conclusions: Tilting the gantry reduced the dose to the breast, while also increasing noise standard deviation. Overall, the noise increase outweighed the dose reduction for the eight voxelized phantoms, suggesting that tilted gantry acquisition may not be beneficial for reducing breast dose while maintaining image quality.

61 RADIATION PROTECTION AND DOSIMETRY↗

Task-based detectability in CT image reconstruction by filtered backprojection and penalized likelihood estimation

Purpose: Nonstationarity is an important aspect of imaging performance in CT and cone-beam CT (CBCT), especially for systems employing iterative reconstruction. This work presents a theoretical framework for both filtered-backprojection (FBP) and penalized-likelihood (PL) reconstruction that includes explicit descriptions of nonstationary noise, spatial resolution, and task-based detectability index. Potential utility of the model was demonstrated in the optimal selection of regularization parameters in PL reconstruction. Methods: Analytical models for local modulation transfer function (MTF) and noise-power spectrum (NPS) were investigated for both FBP and PL reconstruction, including explicit dependence on the object and spatial location. For FBP, a cascaded systems analysis framework was adapted to account for nonstationarity by separately calculating fluence and system gains for each ray passing through any given voxel. For PL, the point-spread function and covariance were derived using the implicit function theorem and first-order Taylor expansion according toFessler [“Mean and variance of implicitly defined biased estimators (such as penalized maximum likelihood): Applications to tomography,” IEEE Trans. Image Process. 5(3), 493–506 (1996)]. Detectability index was calculated for a variety of simple tasks. The model for PL was used in selecting the regularization strength parameter to optimize task-based performance, with both a constant and a spatially varying regularization map. Results: Theoretical models of FBP and PL were validated in 2D simulated fan-beam data and found to yield accurate predictions of local MTF and NPS as a function of the object and the spatial location. The NPS for both FBP and PL exhibit similar anisotropic nature depending on the pathlength (and therefore, the object and spatial location within the object) traversed by each ray, with the PL NPS experiencing greater smoothing along directions with higher noise. The MTF of FBP is isotropic and independent of location to a first order approximation, whereas the MTF of PL is anisotropic in a manner complementary to the NPS. Task-based detectability demonstrates dependence on the task, object, spatial location, and smoothing parameters. A spatially varying regularization “map” designed from locally optimal regularization can improve overall detectability beyond that achievable with the commonly used constant regularization parameter. Conclusions: Analytical models for task-based FBP and PL reconstruction are predictive of nonstationary noise and resolution characteristics, providing a valuable framework for understanding and optimizing system performance in CT and CBCT.

62 RADIOLOGY AND NUCLEAR MEDICINE↗

Effects of refractive index mismatch in optical CT imaging of polymer gel dosimeters

Purpose: Proposing an image reconstruction technique, algebraic reconstruction technique-refraction correction (ART-rc). The proposed method takes care of refractive index mismatches present in gel dosimeter scanner at the boundary, and also corrects for the interior ray refraction. Polymer gel dosimeters with high dose regions have higher refractive index and optical density compared to the background medium, these changes in refractive index at high dose results in interior ray bending. Methods: The inclusion of the effects of refraction is an important step in reconstruction of optical density in gel dosimeters. The proposed ray tracing algorithm models the interior multiple refraction at the inhomogeneities. Jacob’s ray tracing algorithm has been modified to calculate the pathlengths of the ray that traverses through the higher dose regions. The algorithm computes the length of the ray in each pixel along its path and is used as the weight matrix. Algebraic reconstruction technique and pixel based reconstruction algorithms are used for solving the reconstruction problem. The proposed method is tested with numerical phantoms for various noise levels. The experimental dosimetric results are also presented. Results: The results show that the proposed scheme ART-rc is able to reconstruct optical density inside the dosimeter better than the results obtained using filtered backprojection and conventional algebraic reconstruction approaches. The quantitative improvement using ART-rc is evaluated using gamma-index. The refraction errors due to regions of different refractive indices are discussed. The effects of modeling of interior refraction in the dose region are presented. Conclusions: The errors propagated due to multiple refraction effects have been modeled and the improvements in reconstruction using proposed model is presented. The refractive index of the dosimeter has a mismatch with the surrounding medium (for dry air or water scanning). The algorithm reconstructs the dose profiles by estimating refractive indices of multiple inhomogeneities having different refractive indices and optical densities embedded in the dosimeter. This is achieved by tracking the path of the ray that traverses through the dosimeter. Extensive simulation studies have been carried out and results are found to be matching that of experimental results.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

SU-C-204-04: Patient Specific Proton Stopping Powers Estimation by Combining Proton Radiography and Prior-Knowledge X-Ray CT Information

Purpose: The material relative stopping power (RSP) uncertainty is the highest contributor to the range uncertainty in proton therapy. The purpose of this work is to develop a robust and systematic method that yields accurate, patient specific, RSP by combining 1) pre-treatment x-ray CT and 2) daily proton radiograph of the patient. Methods: The method is formulated as a linear least-square optimization problem (min||Ax-B||2). The parameter A represents the pathlength crossed by the proton in each material. The RSPs for the materials (water equivalent thickness (WET)/physical thickness) are denoted by x. B is the proton radiograph expressed as WET crossed. The problem is minimized using a convex-conic optimization algorithm with xi<xi+1 constraint. The Gammex RMI-465 phantom, with 13 material inserts, is used to investigate the optimal RSPs. The proton radiograph (B) is produced using Geant4 simulation. The matrix A is computed by calculating proton trajectories through the CT with the cubic-spline approach. Geant4 RSPs are used as reference and the clinical HU-RSP calibration curve is used as comparison. The convergence is investigated as a function of the number of angles and protons used. The radiographs angle which yield the most accurate RSPs are investigated. Results: Optimization with 9 angles and 104 protons/angle yields precise RSP (<0.75%) for all materials, except plastic lung (1.5%). Average deviation relative to Geant4 RSP is 0.5% and 3.5% using HU-RSP. Using more than two angles or more than 4×103 proton does not further increase the RSP estimate accuracy. The insert distance to the beam initial plane is related to the RSP error for this insert material. Specific filters are applied on the proton angle and energy loss to remove nuclear interaction artefacts. Conclusion: The proposed formulation of the problem with prior knowledge x-ray CT demonstrates serious potential to increase the accuracy of present RSP estimates.

60 APPLIED LIFE SCIENCES↗

Revealing the Nanostructure of Mesoporous Fuel Cell Catalyst Supports for Durable, High-Power Performance

Achieving high power performance and durability with low Pt loadings are critical challenges for proton exchange membrane fuel cells. PtCo catalysts developed on new carbon black supports show promise by simultaneously providing good oxygen reduction kinetics and local oxygen transport. We investigate the role of nanoscale morphology in the performance of these catalysts supported on accessible (HSC-e and HSC-f) and conventional (Ketjen Black) porous carbons using 3D electron tomography, nitrogen sorption, and electrochemical performance measurements. We find that the accessible porous carbons have hollow interiors with mesopores that are larger and more numerous than conventional porous carbons. However, mesopore-sized openings (>2 nm width) are too rare to account for significant oxygen transport. Instead we propose the primary oxygen transport pathway into the interior is through 1–2 nm microporous channels permeating the carbon. The increased mesoporosity in the accessible porous carbons results in a shorter diffusion pathlength through constrictive, tortuous micropores in the support shell leading to lower local oxygen transport resistance. In durability testing, the accessible porous carbons show faster rates of electrochemical surface area loss, likely from fewer constrictive pores that would mitigate coarsening, but maintain superior high current density performance at end of test from the improved local oxygen transport.

Electrochemistry↗

Design of a Molten Salt Flow Cell for Combined Absorbance and Laser-Induced Breakdown Spectroscopy for Online Measurements

A novel flow cell allowing for multiple optical spectroscopy measurements on flowing molten salts was designed, and demonstrative calibrations of impurities in aqueous samples were performed. Online compositional measurements of molten salts are of high interest to monitor the state of relevant solar and nuclear systems. Here, the Spectroscopic Configuration for Optical Real-Time Characterization of High-Temperature (SCORCH) fluids cell was designed to meet this need by providing optical access to a high-temperature molten salt sample stream without physical contact between the sample and window materials. Laser-induced breakdown spectroscopy (LIBS) was utilized to quantify Li, Cr, Fe, Ni, Sr, and Pr at concentrations ranging nominally from 0 to 315 mmol L −1 . Laser power, frequency, and plasma position were optimized to mitigate challenges associated with sample splashing. Univariate calibration models were built with R 2 > 0.98, percent root mean square error of cross-validation (%RMSECV) as low as 2.7%, and limits of quantification (LOQs) down to 4.1 mmol L −1 . Simultaneously, absorbance calibrations were developed for the applicable analytes (Cr, Ni, and Pr) using Beer’s law with a pathlength of 4.41 ± 0.10 mm. These models provide excellent quantification performance with R 2 > 0.999, %RMSECV as low as 0.6%, and LODs down to 0.08 mmol L −1 . Although these calibrations were performed for each spectroscopic technique separately, the two methods may be combined in the future through multivariate modeling and sensor fusion to provide more robust models with the benefits of both techniques (e.g., absorbance: oxidation state concentrations, LIBS: elemental concentration). Additionally, optimized spectrometers may be deployed to enhance sensitivity.

absorbance spectroscopy↗

Exploration of Water Jets in Supersonic Crossflow Using X-Ray Diagnostics

Here, near-field structures of pure- and aerated-liquid jets injected into Mach 2 crossflow environments were experimentally investigated at the 7-BM beamline of the Advanced Photon Source at Argonne National Laboratory using high-speed shadowgraph imaging, high-speed x-ray imaging, and pathlength-integrated x-ray fluorescence. Liquid was flush injected into a blowdown supersonic wind tunnel. Test section top and side windows were fitted with a polycarbonate plate for high x-ray transmittance. An axisymmetric aerated-liquid injector was fitted with an exchangeable nozzle adaptor to generate a liquid jet. Water and nitrogen, the gas used for aerated-liquid jets, were doped with specially selected dopants to facilitate x-ray measurements. Liquid column structures for a pure-liquid jet, typically masked by dense droplet clouds in a supersonic crossflow environment, were visualized with the present x-ray imaging setup. Surface-wave formation, movement, and transformation on the column windward surface of the pure-liquid jet, along with column deformation and breakup processes, were qualitatively characterized. We measured time-averaged line-of-sight (LOS) liquid mass distributions within the liquid jet near fields. Cross-sectional liquid column contours of pure-liquid jets at various deformation stages were reconstructed from LOS liquid mass distributions. The pure-liquid jet deformed liquid column reached a maximum width of 1.47 times the orifice diameter before exhibiting rapid mass removal. We also observed the plume-crossing phenomenon in the aerated-liquid jet.

47 OTHER INSTRUMENTATION↗

Investigation of Thermal Radiation under Pressurized Oxy-combustion Conditions

Thermal radiation of the gaseous and particle phases in a pilot-scale pressurized oxy-combustor is computationally studied. In particular, the radiation characteristics of gases and particles are estimated by employing the statistical narrow-band model and the large-particle model. It is found that thermal radiation of the particle cloud dominates in the combustor under a furnace temperature of 1500 K and when there is no substantial loss of particles to the walls. Another important observation is that radiation from the gas and particles can be approximately treated as a graybody under these conditions. More specifically, the results on the spectral radiation intensity of a gas comprising 40% (vol) H 2 O and 60% CO 2 show that when the pressure is increased to 15 bar, and the radiation pathlength is 100 cm, the spectral radiation profile of the gas phase approaches that of a blackbody at the respective temperature. In addition, the emissivity of the particulate cloud has been evaluated as a function of the particle concentration and diameter by employing the large-particle model. It is shown that the emissivity grows with the particle concentration but decreases with the particle size for the same mass of the particles. Finally, this outcome of the present study is expected to be used to validate the assumption of the gray-gas model adopted in the numerical simulations of pressurized oxy-combustion.

large-particle model↗

New measurement techniques for gear-changing research using DESIREE

In this work we cover some of the newer techniques developed to measure the effects of a gear changing system maintained in DESIREE at Stockholm University. Gear-changing is a collider synchronization method where two rings with different harmonic numbers in them maintain collisions through different velocities, pathlengths or a combination of the two. This system has been demonstrated using the low energy ion collider DESIREE at Stockholm university. We have not only continued our previous methods of studying the beam using a repeating pattern technique where one bucket in each ring is intentionally left empty, but we now also use recently installed pickups outside of the merger region to study the beams separately while they collide.

Accelerator Physics↗

Solution of the Generalized Linear Boltzmann Equation for Multidimensional Stochastic Media

The generalized linear Boltzmann equation is a recently developed framework based on non-classical transport theory for modeling the expected value of particle flux in an arbitrary stochastic medium. Provided with a non-classical cross-section for a given statistical description of a medium, any transport problem in that medium may be solved. Previous work has only considered one-dimensional media without finite boundary conditions and discrete binary mixtures of materials. In this work the solution approach for the GLBE in multidimensional media with finite boundaries is outlined. The discrete ordinates method with an implicit discretization of the pathlength variable is used to leverage sweeping methods for the transport operator. In addition, several convenient approximations for non-classical cross-sections are introduced. The solution approach is verified against random realizations of a Gaussian process medium in a square enclosure.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

A formaldehyde and nitrogen dioxide toxics monitor for environmental justice

DOE’s Integrated Field Laboratories (IFLs) require a vast array of measurements to measure urban air quality. Nitrogen dioxide (NO2) and formaldehyde (HCHO) are ubiquitous pollutants with numerous sources, most notably vehicle exhaust. High-spatial density measurements are critical to understanding how certain neighborhoods are more adversely impacted by pollutants. This report describes the results of a Phase I SBIR project to develop and demonstrate a rapid, affordable, low-power monitor to provide high spatial resolution mobile measurements of formaldehyde and nitrogen dioxide at street-level, where people live and walk. The spatial density will be achieved via rapid measurements on a mobile platform. This sensor will quantify spatial disparities in cities of the toxics, HCHO and NO2, as well as carbon monoxide and carbon dioxide for better source identification. These species are detected in the mid infrared by laser absorption spectroscopy, and fiberoptics are used. Tasks accomplished include identification and testing of the appropriate spectroscopic regions; coupling of laser light into a fiberoptic system; development of software to control miniature electronics to scan and control two lasers simultaneously; coupling of the mid infrared fiber into a multipass cell for enhanced pathlength and sensitivity; characterization of sources of instrument noise; and design work for a Phase II prototype.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

T-1075: Large Area Fast Timing Beam Time of Flight (LAFTBToF) for ProtoDUNE

Large-area Picosecond Photodetectors (LAPPDs), developed at Argonne National Laboratory (ANL), present an opportunity to provide identification of charged particles in the 2-10 GeV/c range. Traditional methods using ionization or Cherenkov detectors require large amounts of material or pathlength for the particle to traverse in order to get a clean measurement, and are ill suited for particle beam identification in fixed-target experiments. The 6x6 cm 2 LAPPD uses mm-thick borosilicate glass micro-channel plates with a resistive surface coating added via atomic layer deposition. An electrical connection schematic of the LAPPD is shown in Figure 1. Electrons emitted by the photocathode are accelerated through the MCPs, which have µm-sized capillaries, and an avalanche of electrons is created as the electrons collide against the walls of the capillaries of the MCPs. The resulting electron avalanche is collected on anode strip lines and the signal may be read out on both ends of the stipline. The resistive coating of the thin MCPs and the short path length of the electrons to the readout results in fast rise times, gains of greater than 10 6 and typical timing resolutions of 50 ps. Differential timing on the ends of the strip lines can provide mm-level position measurements. The material of the bare LAPPD presents less than 0.05 of an interaction length and approximately 0.12 of a radiation length for a charged particle of I GeV/c. In our application, two large-area photodetectors separated by 5-10 meters can be used in a time-of-flight (ToF) measurement for 3σ separation of2-7 GeV/c charged pions, kaons and protons with minimal impact on the particle's trajectory and momentum.

43 PARTICLE ACCELERATORS↗

Analysis of thermal radiation of a gas-particulate-cloud in a pressurized oxy-coal combustor

Pressurized oxy-combustion (POC) aims to reduce carbon emissions from coal-fired power plants. In the POC process, pulverized coal is burned at elevated pressure in an O2-CO2 environment. The elevated pressure and high CO2 and H2O concentrations strongly impact thermal radiation, thereby significantly distinguishing POC system from conventional atmospheric-pressure air-fired and oxy-fuel combustion. Consequently, a thorough understanding of thermal radiation in POC is required to promote the development of novel combustors. The present computational work analyzes thermal radiation of the gaseous and particle phases in the pilot-scale POC combustor in Washington University in St. Louis. Particularly, the radiation characteristics of the gaseous and particulate cloud were estimated by employing the statistical narrow band model and the large-particle model. It is found that thermal radiation of a particulate cloud dominates in the combustor under the conditions of a furnace temperature of 1500 K and no substantial particle loss. Another important result is that the gas-and-particulate cloud can be approximately treated as a graybody under the same conditions. To be more specific, the results of spectral radiation intensity of a gas comprised of 40% (vol) H2O and 60% CO2 show that when the pressure is increased to 15 bar, and the radiation pathlength to 100 cm, the spectral radiation profile of the gas phase approaches that of a blackbody at the respective temperature. In addition, the emissivity of the particulate cloud has been evaluated as a function of the particle concentration and diameter by means of the large particle model. It is shown that the emissivity grows with the particle concentration but decreases with the particle size for the same mass of a particulate cloud. The emissivity of a particulate cloud in oxy- combustion exceeds that in air-fired combustion. This work could be used to validate the assumption of the gray gas model adopted in numerical simulations.

Li, Lei↗