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At least 235 records · Page 13

Radiation Effects on the Performance of Advanced Sulfur Monochloride Chlorination Processes

Advanced sulfur chloride-based chlorination technologies are being developed to enable efficient recycling of aluminum and zirconium-based materials used in the nuclear industry. However, the impacts of ionizing radiation on the performance of these sulfur chloride compounds are not well established, despite this being critical knowledge for assessing their feasibility and longevity under envisioned process conditions. Here, in the present article, we report on the effects of cobalt-60 gamma irradiation (≤ 5 MGy) on the aluminum alloy 6061 (AA6061-T6) chlorination yield in sulfur monochloride (S 2 Cl 2 ). Our findings indicate that, compared to nonirradiated solvent, radiation-induced changes in the chemical composition of S 2 Cl 2 —identified using Raman spectroscopy—afford an additional, dose-dependent exothermic process prior to the chlorination reaction’s typical thermodynamic behavior. We attribute this new process to reactions involving aluminum species (metal, oxide, or [oxy]hydroxides) and sulfur dichloride (SCl 2 ), an S 2 Cl 2 radiolysis product that accumulates with absorbed gamma dose, but is absent following an AA6061-T6 chlorination study. Despite the exothermicity of this new process, the overall yield of chlorination decreased with increasing preirradiation dose. Consequently, the chemical reactivity, specificity (aluminum metal vs aluminum passivation and corrosion layer constituents), and byproducts of SCl 2 must be more thoroughly evaluated to support the continued development of advanced S 2 Cl 2 chlorination technologies.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Increased importance of aerosol–cloud interactions for surface PM 2.5 pollution relative to aerosol–radiation interactions in China with the anthropogenic emission reductions

Surface fine particulate matter (PM 2.5 ) pollution can be enhanced by feedback processes induced by aerosol–radiation interactions (ARIs) and aerosol–cloud interactions (ACIs). Many previous studies have reported enhanced PM 2.5 concentrations induced by ARIs and ACIs for episodic events in China. However, few studies have examined the changes in the ARI- and ACI-induced PM 2.5 enhancements over a long period, though the anthropogenic emissions have changed substantially in the last decade. In this study, we quantify the ARI- and ACI-induced PM 2.5 changes for 2013–2021 under different meteorology and emission scenarios using the Weather Research and Forecasting model with Chemistry (WRF-Chem), and we investigate the driving factors behind the changes. Our results show that, in January 2013, when China suffered from the worst PM 2.5 pollution, the PM 2.5 enhancement induced by ARIs in eastern China (5.59 µg m −3 ) was larger than that induced by ACIs (3.96 µg m −3 ). However, the ACI-induced PM 2.5 enhancement showed a significantly smaller decrease ratio (51 %) than the ARI-induced enhancement (75 %) for 2013–2021, making ACIs more important for enhancing PM 2.5 concentrations in January 2021. Our analyses suggest that the anthropogenic emission reductions played a key role in this shift. Owing to only anthropogenic emission reductions, the ACI-induced PM 2.5 enhancement decreased by 43 % in January, which was lower than the decrease ratio of the ARI-induced enhancement (57 %). The relative change in ARI- and ACI-induced PM 2.5 enhancement in July was similar to the pattern observed in January, caused by anthropogenic emission reductions. The primary reason for this phenomenon is that the decrease in ambient PM 2.5 for 2013–2021 caused a disproportionately small decrease in the liquid water path (LWP) and an increase in the cloud effective radius (Re) under the condition of high PM 2.5 concentrations. Therefore, the surface solar radiation attenuation (and, hence, the boundary layer height reduction) caused by ACIs decreased slower than that caused by ARIs. Moreover, the lower decrease ratio of the ACI-induced PM 2.5 enhancement was dominated by the lower decrease ratio of ACI-induced secondary PM 2.5 component enhancement, which was additionally caused by the smaller decrease ratio of the air temperature reduction and the relative humidity (RH) increase. Our findings indicate that, with the decrease in ambient PM 2.5 , the ACI-induced PM 2.5 enhancement inevitably becomes more important. This needs to be considered in the formulation of control policies to meet the national PM 2.5 air quality standard.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Low temperature process for diode termination of fully depleted high resistivity silicon radiation detectors that can be used for shallow entrance windows and thinned sensors

Fabrication of vertical diodes for radiation sensing using a low temperature microwave anneal is provided. This kind of anneal allows the back side processing to be performed after the front side processing is done without damaging the front side structures. This enables a simplified fabrication of thinned detectors compared to a conventional silicon on insulator process. Another feature that this technology enables is a thin entrance window for a detector that also serves as the doped diode termination. Such thin entrance windows are especially suitable for detection of low energy radiation.

Kenney, Christopher J.↗

Comprehensive Analysis of the Relative Dispersion of Droplet-Size Distributions and Their Relationships to Key Physical Fog Processes Under Different Aerosol Conditions and Evolutionary Stages

The relative dispersion of cloud and fog droplets has significant impacts on aerosol indirect effects, radiative transfer, and microphysical processes. However, previous studies have been mostly concerned with clouds, with limited studies on fog, particularly those that examine the combined influences of all key physical processes and their roles during fog evolution. As such, this study aims to conduct a comprehensive investigation by examining the relationships between relative dispersion and other microphysical variables, as well as the underlying microphysical and dynamic processes, based on field fog campaigns in polluted and clean conditions. In polluted fog, droplet concentrations are higher, leading to smaller droplets and increased dispersion. The correlation between dispersion and droplet volume-mean radius is positive in the polluted fog, but shifts to negative in clean fog. Here, we attribute the difference to various microphysical processes like aerosol activation, condensation, collision-coalescence, and entrainment-mixing. In polluted fog, high aerosol concentrations, low supersaturations, and strong turbulence (entrainment-mixing) provide suitable conditions for the simultaneous occurrence of droplet condensation and aerosol activation, resulting in a positive correlation between dispersion and volume-mean radius, especially during the fog formation stage. In contrast, during the mature stage in clean fog, condensation is dominant with weak aerosol activation leading to a negative correlation between relative dispersion and volume-mean radius. The collision-coalescence process is more active in the mature stage, increasing radii and leading to the negative correlation between dispersion and volume-mean radius. This result sheds new light on understanding the relative dispersion and mechanisms in fog under different aerosol backgrounds.

54 ENVIRONMENTAL SCIENCES↗

New approach to QCD final-state evolution in processes with massive partons

We present an algorithm for massive parton evolution which is based on the differentially accurate simulation of soft-gluon radiation by means of a nontrivial azimuthal angle dependence of the splitting functions. The kinematics mapping is chosen such as to reflect the symmetry of the final state in soft-gluon radiation and collinear splitting processes. We compute the counterterms needed for a fully differential next-to-leading order matching and discuss the analytic structure of the parton shower in the next-to-leading logarithmic limit. We implement the new algorithm in the numerical code Alaric and present a first comparison to experimental data. Published by the American Physical Society 2024

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Droplet collection efficiencies inferred from satellite retrievals constrain effective radiative forcing of aerosol–cloud interactions

Abstract. Process-oriented observational constraints for the anthropogenic effective radiative forcing due to aerosol–cloud interactions (ERFaci) are highly desirable because the uncertainty associated with ERFaci poses a significant challenge to climate prediction. The contoured frequency by optical depth diagram (CFODD) analysis supports the evaluation of model representation of cloud liquid-to-rain conversion processes because the slope of a CFODD, generated from joint MODerate Resolution Imaging Spectroradiometer (MODIS)-CloudSat cloud retrievals, provides an estimate of cloud droplet collection efficiency in single-layer warm liquid clouds. Here, we present an updated CFODD analysis as an observational constraint on the ERFaci due to warm rain processes and apply it to the U.S. Department of Energy's Energy Exascale Earth System Model version 2 (E3SMv2). A series of sensitivity experiments shows that E3SMv2 droplet collection efficiencies and ERFaci are highly sensitive to autoconversion, i.e., the rate of mass transfer from cloud liquid to rain, yielding a strong correlation between the CFODD slope and the shortwave component of ERFaci (ERFaciSW; Pearson's R=-0.91). E3SMv2's CFODD slope (0.20 ± 0.04) is in agreement with observations (0.20 ± 0.03). The strong sensitivity of ERFaciSW to the CFODD slope provides a useful constraint on highly uncertain warm rain processes, whereby ERFaciSW, constrained by MODIS-CloudSat, is estimated by calculating the intercept of the linear association between the ERFaciSW and the CFODD slopes, using the MODIS-CloudSat CFODD slope as a reference.

Beall, Charlotte M. (ORCID:0000000311370835)↗

The U.S. DOE ARM User Facility Establishes a New Site for Studies of Land–Aerosol–Cloud Interactions in the Southeastern United States

The U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) user facility has established a new site in the Bankhead National Forest (BNF) in northern Alabama that will gather data on how clouds, the land surface, and aerosols interact at a hierarchy of scales important to understanding and simulating the Earth system. Starting its operations in October 2024, the BNF site provides a multi-year opportunity for scientists to unravel complex land-atmosphere interactions. A suite of ground-based sensors, elevated tower-based instrumentation, and aerial facilities will enable scientists to investigate those interactions from within the canopy to the clouds. The Southeastern United States was recommended by the DOE ARM and its collaborators in the broader community as an important region to address their common scientific questions given the region’s abundant surface-forced convective clouds and mesoscale convective systems that pose ongoing challenges in Earth system models. The region is also home to significant terrain complexity and land-use heterogeneity that will unleash new understanding of anthropogenic and biogenic aerosol processes, boundary-layer aerosol-cloud interactions, and the interactions between the terrestrial ecosystem and coupled aerosol-cloud-radiation processes.

Aerosols↗

Reconstructions from randomly generated longitudinal electron bunch profiles with Gaussian envelopes using the Gerchberg–Saxton algorithm

Knowledge of longitudinal electron bunch profiles is vital to optimize the performance of plasma wakefield accelerators and x-ray free electron laser linacs. Because of their importance to these novel applications, noninvasive frequency domain techniques are often employed to reconstruct longitudinal bunch profiles from coherent synchrotron, transition, or undulator radiation measurements. In this paper, we detail several common reconstruction techniques involving the Kramers–Kronig phase relationship and Gerchberg–Saxton algorithm. Additionally, through statistical analysis, we draw general conclusions about the accuracy of these reconstruction techniques and the most suitable candidate for reconstructing well-isolated longitudinal bunch profiles from spectroscopic data.

47 OTHER INSTRUMENTATION↗

Scanning Probe Microscope to Map Thermal and Thermoelectric Properties of Combinatorial Materials

The combinatorial methodology offers a high-throughput process for developing radiation-resistant sensor materials for nuclear energy applications through the synthesis and screening of large numbers of compositions and processing conditions in a single process. The combinatorial materials fabrication coupled with an automated screening process enables us to identify the optimal materials composition and processing conditions that yield both desired properties and required irradiation resistance in the most efficient and economic manner. The report focuses on the development of scanning probe technique to map with high resolution the thermal conductivity, Seebeck coefficient and electrical conductivity of combinatory materials with gradient compositions, which has been a key challenge in combinatory materials science. The above three properties play important roles in many sensor materials for nuclear energy applications.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Multiscale Modeling of Plutonium Radiation Chemistry in Nitric Acid Solutions. 1. Cobalt-60 Gamma Irradiation of Pu(IV)

We report careful manipulation of the plutonium oxidation states is essential in the study and utilization of its rich redox chemistry. To achieve this level of control, a comprehensive mechanistic understanding of radiation-induced plutonium redox chemistry is critical due to the unavoidable exposure of plutonium to ionizing radiation fields, both inherent and from in-process applications. To this end, we have developed an experimentally evaluated multiscale computer model for the prediction of gamma radiation-induced Pu(IV) redox chemistry in concentrated nitric acid solutions (1.0, 3.0, and 6.0 M). Under these acidic, aqueous solution conditions, cobalt-60 gamma irradiation afforded marginal net conversion of Pu(IV) to Pu(VI), the extent of which was dependent on the concentration of HNO 3 and absorbed gamma dose. Multiscale calculations, which are in excellent agreement with experimental data, indicate that this observation is due to a combination of inherent plutonium disproportionation reactions and several radiation-induced processes, including redox cycling between Pu(IV) and Pu(III), as achieved by the reduction of Pu(IV) by nitrous acid and hydrogen peroxide, the oxidation of Pu(III) by nitrate and hydroxyl radicals, and the sequential oxidation of Pu(IV) to Pu(V) and Pu(VI) by the remaining available yield of nitrate radicals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

The Study of TRR Radial Thermal Shielding Dismantling Process - 20063

The decommissioning of nuclear facilities has become an important worldwide topic because many nuclear power facilities will permanently cease operation in the foreseeable future. Taiwan Research Reactor (TRR) has stepped into the decommissioning phase in 2004, and the dismantling processes will start in 2022. TRR is a heavy water reactor designed by Canatom Company with output thermal power 40 MW. On January 3, 1973, it reaches criticality. TRR had been operated for 15 years and was permanently shut down in early 1988. The decommissioning plan of TRR was approved in 2004. According to the Nuclear Reactor Facilities Regulation Act in Taiwan, a nuclear facility must be dismantled in 25 years after stepping into the decommissioning phase. Therefore, TRR decommissioning must be completed before 2029. One of the most important tasks of TRR decommissioning is to dismantle reactor body. In the task of TRR decommissioning, mechanical cutting with remote handling is used to dismantle radial thermal shielding, which are the internal components of the TRR. This study outlines the internal components of the TRR and explains the difficulties encountered during the dismantling processes. Considering the structure and radiation dose rate of TRR and its internal components, the dismantling method and packaging method are properly arranged to complete the TRR dismantling task. This study describes the process of dismantling the radial thermal shielding during the dismantling processes and considers the impact of the radiation dose on the staff during the operation. The calculation of the radiation dose rate for the personnel during the segmentation process is based on the evaluation result by using VRdose. If the calculation of personnel working dose rate is too high, we will increase the shielding or use remote handling to reduce the operator's exposure dose in the dismantling processes to comply with the As Low As Reasonably Achievable (ALARA) principle. In this study, the latest developments in the TRR decommissioning program are described. It also provides usable experience and information regarding the future decommissioning of other nuclear facilities or nuclear power plants in Taiwan. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Closures and Simulation for Thermal Radiation Transport in Stochastic Media with Nonlinear Temperature Dependence

Because of the practical challenge of rendering very complex realistic spatial structures for numerical work, it is common practice to resort to characterizing such media as stochastic mixtures of materials, ideally parametrized with low order statistics such as the mean, variance, and correlation functions of the now random material properties. This enables realizations of the medium to be repeatedly generated and radiation transport computations to, in principle, be performed for a large ensemble of these realizations to obtain a statistically well-characterized radiation field. Statistical post-processing yields desired quantities such as conditional and unconditional mean radiation flux and probability distributions of transmitted radiation. However, such computations prove expensive for all but the simplest stochastic geometries and are most suited for benchmarking approximate models. The most common approximations lead to homogenized media so that transport computations are required only on a single medium realization but by construct provide only limited statistical information on the radiation field. Almost all approximate approaches to this problem attempt to develop equations for low order moments of the radiation intensity (mean, second moment, correlation function) but inevitably encounter a closure problem: the equation for any statistical moment will contain terms depending on unknown higher-order moments. Thus, the challenge shifts to one of developing closure relations that relate the unknown moments to the lower order moments. Under very special conditions, an exact closure can be derived but in general closures are heuristically stated constitutive relations. Also, closure approaches depend on whether the mixing statistics are spatially and/or temporally continuous as in fluctuating turbulent fields, or discontinuous as in randomly mixed solid chunks of material. Thus, unconditional averaging is generally applied in the former case but conditional averaging is more appropriate when the mixing is discontinuous. In this work, the emphasis is on binary statistical mixtures of immiscible fluids as as such the quantities of interest are averages (flux, temperature) conditioned on the material type.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Radioactive Source Localization via Bayesian Particle Filter

In the event of a misplaced radioactive source or other emergency situation, measuring a radiation field, mapping its distribution, and determining a source location are essential tasks to ameliorating the situation. However, radiation fields may be extremely hazardous to human surveyors and minimizing received radiation doses is just as essential. Robots appear to be a potential solution to these problems. Beyond simply measuring radiation, the robot's computer processing capabilities offer a way to apply complex data analysis methods to radiation measurements in real-time. Methods which predict likely source locations can then feed this information into other processes, potentially improving path planning and enabling more efficient measurements. Given a robot mounted with a gamma-ray detector, can we: develop a methodology to account for detector performance across a wide range of source angles, distances, and photon energies? operate an autonomously navigating robot to effectively survey and characterize an area of interest? implement a data analysis method, conventionally used in measurements of motion, for source localization purposes? An open-source TurtleBot 3 robot, running Robot Operating System (ROS) on Ubuntu 16.04 LTS, was fitted with a Kromek GR1{sup R} Cadmium Zinc Telluride (CZT) solid-state gamma-ray detector. As a part of ROS, the packages OpenSlam, gmapping, and amcl were used to perform Simultaneous Localization and Mapping (SLAM), determining the robot's position and mapping the surrounding area. Data was acquired via Lidar mounted on top the TurtleBot 3. Detector Calibration Fit: The equation was fit to 365 counts of various energies, distances, and angles. A MATLAB{sup R} program was written to simulate measurements taken a robot on a random walk, with count data and positions discretized into finite element pixels. Using this program, a sample of 100 runs was performed on a map with a simulated source at the center, with a total of 200 of 2 pixels each. Similarly, multiple runs of the filter were performed on recorded robot measurement data. In both simulation and real tests, when corrected for errors (particles placed outside of bounds or on the robot, and simulation-specific errors), corresponding t-tests of predicted x and y-coordinates were within a 95% confidence interval of the actual position. For the real trial, these positions are slightly skewed right in the x-axis as the robot remained mainly to the left side of the source within the sample area. These simulations demonstrate potential validity for the usage of a particle filter as method of radioactive source localization. In the future, true real-time implementation and data fusion may further augment the performance of the robot to localize lost sources. Additionally, identification of multiple sources, determination of source types, and usage of a collimator are areas to potentially be explored.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

CoURAGE KAZR b1 Processing: Corrections, Calibrations, and Processing Report

The U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) User Facility supports atmospheric and earth system research through a comprehensive network of fixed and mobile observatories. These facilities provide long-term and intensive campaign-based observations of clouds, aerosols, precipitation, radiation, and meteorological state variables. ARM observations are designed to improve the physical understanding and numerical representation of atmospheric processes in earth system models, with particular emphasis on cloud-radiation interactions and precipitation processes. The Coast-Urban-Rural Atmospheric Gradient Experiment (CoURAGE) deploys one of the ARM Mobile Facilities (AMF) to the Mid-Atlantic region surrounding Baltimore, Maryland, for the period 1 December 2024 through 30 November 2025. This deployment focuses on characterizing atmospheric structure, cloud properties, and precipitation processes across strong land-use and surface heterogeneity gradients associated with urban, rural, and coastal (Chesapeake Bay) environments. The CoURAGE deployment complements the Baltimore Social-Environmental Collaborative (BSEC), a DOE Urban Integrated Field Laboratory (UIFL), by providing high-quality atmospheric observations needed to connect urban surface processes, emissions, and meteorology to cloud and precipitation responses. In addition to the central urban site, ancillary observing sites were deployed to rural Maryland northwest of Baltimore and to an island site in Chesapeake Bay. These measurements further complement a long-term atmospheric observatory operated in Beltsville, Maryland, by Howard University in collaboration with the Maryland Department of the Environment. Together, these assets form a four-node regional atmospheric observatory network representing Baltimore and its three primary surrounding environments—urban, rural, and coastal/bay. This coordinated observational strategy enables investigation of spatial gradients in boundary-layer structure, cloud occurrence, precipitation evolution, and aerosol-cloud interactions across complex surface regimes. Within this network, vertically pointing cloud radars play a critical role by providing continuous, high-resolution measurements of cloud and precipitation vertical structure.

54 ENVIRONMENTAL SCIENCES↗

Defect Generation and Evolution in Irradiated Epitaxial Films and Heterostructures of Fe 3 O 4 and Cr 2 O 3

Abstract The functionality of nuclear structural materials, sensors, and microelectronics in harsh environments such as radiation relies on understanding defect generation and evolution processes in oxide layers. The initial radiation response of epitaxial thin films of Fe 3 O 4 (111), Cr 2 O 3 (0001), and Fe 3 O 4 (111)/Cr 2 O 3 (0001) heterostructures deposited on Al 2 O 3 (0001) by oxygen‐assisted molecular beam epitaxy and irradiated with 200 keV He + is characterized. X‐ray diffraction and X‐ray absorption near edge spectroscopy showed that the Cr 2 O 3 layers underwent significant lattice expansion and disordering under irradiation, whereas the Fe 3 O 4 layers do not exhibit noticeable changes. In contrast, positron annihilation spectroscopy revealed an evolution of cation vacancy point defects in the Fe 3 O 4 layers into larger vacancy clusters with increasing irradiation, while the cation vacancies in Cr 2 O 3 remained primarily as single vacancies and small clusters. The results suggest that the Fe 3 O 4 lattice can utilize the free volume of the larger vacancy clusters to relax but the small vacancies in the Cr 2 O 3 lattice do not facilitate relaxation. Comparing defect concentrations in the single layer films versus the heterostructure suggests that point defects may cross the interface from Fe 3 O 4 into Cr 2 O 3 . Together, these results enhance the understanding of the initial defect evolution mechanisms in oxide layers in harsh irradiation environments.

36 MATERIALS SCIENCE↗

A model for radiative heating of a high-Z pusher

Several approaches to Inertial Confinement Fusion (ICF), including double-shell, pushered-single-shell, and the Revolver designs, have fuel surrounded by pushers made from high-Z materials. An advantage of these designs is that radiation emitted by the hot fuel will be absorbed and re-radiated into the fuel to reduce cooling. This process is referred to as radiation-trapping, and it lowers the fuel temperature required for ignition. To elucidate the physics of radiation trapping, a simplified model comprising a set of coupled differential equations has been developed to model the arbitrary time-dependent wall temperature from the Hammer and Rosen solution [J. H. Hammer and M. D. Rosen, Phys. Plasmas 10, 1829 (2003)] to a Marshak wave. The derivation of the model and a set of analytical power-law solutions will be presented. A discussion on numerical implementation of the differential equations into a model for burn in ICF capsules is also included.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗