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At least 217 records · Page 12

Qualitative assessment of uranium ore concentrates and related materials using scanning electron microscopy

Several studies have evaluated the morphology of uranium compounds produced under controlled conditions at the laboratory scale, but it is unclear whether the morphological characteristics of these materials persist in commercially produced uranium ore concentrates (UOCs). To assess the morphology in “real-world” UOCs, we qualitatively evaluated the morphological profile of secondary electron images from over 100 commercial UOCs using a previously published lexicon. We observe differences between samples with differing chemical composition and samples with similar chemical composition and differing provenance. Further, this work contextualizes morphology for commercially produced UOCs and will provide a basis for future machine learning efforts.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Solid-phase extraction microfluidic devices for matrix removal in trace element assay of actinide materials

Advances in sample nebulization and injection technology have significantly reduced the volume of solution required for trace impurity analysis in plutonium and uranium materials. Correspondingly, we have designed and tested a novel chip-based microfluidic platform, containing a 100-µL or 20-µL solid-phase microextraction column, packed by centrifugation, which supports nuclear material mass and solution volume reductions of 90% or more compared to standard methods. Quantitative recovery of 28 trace elements in uranium was demonstrated using a UTEVA chromatographic resin column, and trace element recovery from thorium (a surrogate for plutonium) was similarly demonstrated using anion exchange resin AG MP-1. Of nine materials tested, compatibility of polyvinyl chloride (PVC), polypropylene (PP), and polytetrafluoroethylene (PTFE) chips with the strong nitric acid media was highest. Finally, the microcolumns can be incorporated into a variety of devices and systems, and can be loaded with other solid-phase resins for trace element assay in high-purity metals.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Arecibo Observatory Auxiliary M4N Socket Termination Failure Investigation

The NASA Engineering and Safety Center (NESC) was requested to support the Arecibo Observatory failure investigation in determining the root cause of the Auxiliary M4N cable failure. The NESC and Kennedy Space Center led an integrated NASA investigation with support from Marshall Space Flight Center and The Aerospace Corporation that included forensic investigation of failed hardware, finite element modeling, materials characterization, and root cause analysis. This document contains the outcome of the NESC Assessment.

Zinc Spelter Sockets↗

Thermal Microwave Kinetic Inductance Device, RSLN-023-16, Year 1 of 2

Presentation describes decay-energy spectroscopy as a transformative method for nondestructive isotopic assay of trace-level nuclear materials with potential applications in areas including nuclear forensics. This project concentrates on optimizing this technology for low-energy electron spectroscopy. Measurement of the decay by electron capture of holmium-163 (163Ho) was explored because its low energy decay, which allows accurate study of energy-resolution capabilities of decay-energy spectroscopy.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Characterization Techniques for LiInSe{sub 2} Semiconducting Neutron Detector - Paper 55

As the world supply of helium continues to dwindle, alternatives to neutron detection have been a key focus area of radiation detection research. Solid-state neutron detectors are one possible alternative to the {sup 3}He detectors currently used for neutron detection when large detector areas are not required. Although {sup 6}Li and {sup 10}B are both also commonly used for neutron detection, neither has as high of a thermal cross section as {sup 3}He. The thermal cross sections for {sup 6}Li, {sup 10}B, and {sup 3}He are, respectively, 940 barns, 3840 barns, and 5330 barns. Both boron and helium are used in a gaseous form for neutron detection; however, there is no suitable gaseous form of lithium for neutron detection. Lithium is instead utilized in solid or liquid compounds for neutron detection. In this context, one area of interest is in the development of ternary A{sup I}B{sup III}C{sup IV} semiconductors comprised of isotopically-enriched lithium. Single crystal samples are being prepared through collaboration with the Y12 National Security Complex. This research focuses on the characterization of {sup 6}LiInSe{sub 2} (LISe) crystals, as well as on the development of prototype systems to assess the viability of using LISe crystals as a thermal neutron detector. Data to be obtained will provide previously untested physical parameters to facilitate growth optimization. Eventually, the refined crystals will be developed into solid-state, position-sensitive pixel detectors used for neutron imaging, among a wide array of possible applications including nuclear forensics. For the most part, the research team has been focused on mastering the detector fabrication processes, response tests on the first two batches of crystal samples, and the design of the first iteration detection system (Fig. 2). Response tests using alphas and neutrons have shown sensitivity to both particles. The first iteration detection system developed utilizes a 3-stage filter ladder of resistors and capacitors, similar to an ORTEC 142PC Preamplifier. Ideally, this ladder will reduce the noise associated with the high voltage power supply. The preamplifier is AC coupled to improve its counting rate capability (saturation), and critical components are on insulated posts. The custom circuit is housed in an aluminum box, and initial testing of the circuit has shown expected results. Investigation into further noise reduction is underway and will be the focus of the presented results. Upon completion and successful testing of the final detection system design, further development in spatial resolution and gamma/neutron discrimination will continue. (authors)

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Sensitivity and Uncertainty Analysis of Plutonium and Cesium Isotopes in Modeling of BR3 Reactor Spent Fuel

Nuclear forensics has a broad task to characterize recovered nuclear or radiological material and interpret the results of investigation. One approach to isotopic characterization of nuclear material obtained from a reactor is to chemically separate and perform isotopic measurements on the sample and verify the results with modeling of the sample history, for example, operation of a nuclear reactor. The major actinide plutonium and fission product cesium are commonly measured signatures of the fuel history in a reactor core. This study investigates the uncertainty of the plutonium and cesium isotope ratios of a fuel rod discharged from a research pressurized water reactor when the location of the sample is not known a priori. A sensitivity analysis showed overpredicted values for the 240 Pu/ 239 Pu ratio toward the axial center of the rod and revealed a lower probability of the rod of interest (ROI) being on the periphery of the assembly. The uncertainty analysis found the relative errors due to only the rod position and boron concentration to be 17% to 36% and 7% to 15% for the 240 Pu/ 239 Pu and 137 Cs/ 135 Cs ratios, respectively. Lastly, this study provides a method for uncertainty quantification of isotope concentrations due to the location of the ROI. Similar analyses can be performed to verify future chemical and isotopic analyses.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Batch Extraction Studies to Evaluate Trace Element Behavior in PUREX Conditions

The multilab Intentional Forensics Venture is working to identify which stable elements (i.e., taggants) at trace concentrations relative to U would persist throughout the nuclear fuel cycle in a voluntary fuel tagging scheme. A taggant would provide the nuclear forensics community with a “barcode” to help identify nuclear materials found outside of regulatory control. A portion of this project was focused on reprocessing effects and determining which, if any, elements would coextract with U(VI) in standard Pu–U reduction extraction (PUREX) conditions. Elements with a propensity to coextract could, in theory, be used as taggants from a PUREX perspective. Although retention is not a performance requirement, the taggant signature would need to partition predictably from the U stream after the PUREX process to maintain forensic utility. This report documents results from several batch extraction studies with numerous trace elements from HNO 3 (1.5–5 M), with and without U(VI), into 30% tri-n-butyl phosphate (TBP) in kerosene. Extraction and back-extraction tests were used to evaluate nearly 60 elements in surrogate conditions for PUREX, and distribution coefficients (i.e., D-values) for most species were <0.1, indicating few species are likely to co-extract with U through PUREX. Additional studies are needed to optimize sample volumes and dilutions to dial in these low D-values. The D-values (D) were determined for several of the more promising elements, including Re and Se. Ultimately, we conclude that only a limited number of the ~ 60 elements investigated are extractable in the U stream of PUREX, based on measured D values, meaning most candidate elemental taggants would likely be lost at this stage of the nuclear fuel cycle, even when considering a range of acid concentrations.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Morphology and particle size (MaPS) exercise: testing the applications of image analysis and morphology descriptions for nuclear forensics

Image analysis techniques have been applied and shown to be a valuable tool in nuclear forensics analysis. The interlaboratory exercise reported here has tested quantitative and qualitative approaches for characterizing nuclear materials. Particle size, surface features and morphology descriptions were compared by four laboratories on a common image set generated by Scanning Electron Microscopy and Digital Light Microscopy. Quantitative analysis of the image sets through the Morphological Analysis for MAterials software highlighted the strength of image analysis, but also that the application of the software alone can introduce significant bias in the analysis. Qualitative morphology descriptions following the process outlined by Tamasi et al. (J Radioanal Nuclear Chem 307:1611–1619, 2015) were compared with a discussion on the robustness and reproducibility of the results. Finally, future work should continue to focus on proficiency and standardization of image analysis through continued exercises within the extended nuclear forensics community.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Scanning transmission x-ray microscopy (STXM) of plutonium oxide

Scanning transmission x-ray microscopy was used to examine plutonium oxide particles formed by the corrosion of δ-phase plutonium alloy under high-humidity conditions. O K-edge spectra collected from eight distinct particles displayed significant spectral differences, revealing heterogeneity in oxidation states within a single sample batch. Here, this variation suggests complex chemical environments and formation histories, which are important considerations for nuclear forensic investigations. These findings highlight both the potential of synchrotron-based x-ray microscopy for nondestructive, high-resolution analysis of nuclear materials and the need for expanded reference datasets to improve the interpretation and forensic utility of such measurements.

organic↗

Determination of origin and intended use of plutonium metal using nuclear forensic techniques

Nuclear forensics techniques, including micro-XRF, gamma spectrometry, trace elemental analysis and isotopic/chronometric characterization were used to interrogate two, potentially related plutonium metal foils. These samples were submitted for analysis with only limited production information, and a comprehensive suite of forensic analyses were performed. Resulting analytical data was paired with available reactor model and historical information to provide insight into the materials’ properties, origins, and likely intended uses. Both were super-grade plutonium, containing less than 3% 240 Pu, and age-dating suggested that most recent chemical purification occurred in 1948 and 1955 for the respective metals. Additional consideration of reactor modelling feedback and trace elemental observables indicate plausible U.S. reactor origin associated with the Hanford site production efforts. In conclusion, based on this investigation, the most likely intended use for these plutonium foils was 239 Pu fission foil targets for physics experiments, such as cross-section measurements, etc.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Laser Ablation Plasmas and Spectroscopy for Nuclear Applications

The development of measurement methodologies to detect and monitor nuclear-relevant materials remains a consistent and significant interest across the nuclear energy, nonproliferation, safeguards, and forensics communities. Optical spectroscopy of laser-produced plasmas is becoming an increasingly popular diagnostic technique to measure radiological and nuclear materials in the field without sample preparation, where current capabilities encompass the standoff, isotopically resolved and phase-identifiable (e.g., UO and UO[Formula: see text]) detection of elements across the periodic table. These methods rely on the process of laser ablation (LA), where a high-powered pulsed laser is used to excite a sample (solid, liquid, or gas) into a luminous microplasma that rapidly undergoes de-excitation through the emission of electromagnetic radiation, which serves as a spectroscopic fingerprint for that sample. This review focuses on LA plasmas and spectroscopy for nuclear applications, covering topics from the wide-area environmental sampling and atmospheric sensing of radionuclides to recent implementations of multivariate machine learning methods that work to enable the real-time analysis of spectrochemical measurements with an emphasis on fundamental research and development activities over the past two decades. Background on the physical breakdown mechanisms and interactions of matter with nanosecond and ultrafast laser pulses that lead to the generation of laser-produced microplasmas is provided, followed by a description of the transient spatiotemporal plasma conditions that control the behavior of spectroscopic signatures recorded by analytical methods in atomic and molecular spectroscopy. High-temperature chemical and thermodynamic processes governing reactive LA plasmas are also examined alongside investigations into the condensation pathways of the plasma, which are believed to serve as chemical surrogates for fallout particles formed in nuclear fireballs. Laser-supported absorption waves and laser-induced shockwaves that accompany LA plasmas are also discussed, which could provide insights into atmospheric ionization phenomena from strong shocks following nuclear detonations. Furthermore, the standoff detection of trace radioactive aerosols and fission gases is reviewed in the context of monitoring atmospheric radiation plumes and off-gas streams of molten salt reactors. Finally, concluding remarks will present future outlooks on the role of LA plasma spectroscopy in the nuclear community.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Rare-earth element fractionation in uranium ore and its U(VI) alteration minerals

We developed a cation exchange chromatography method employing sulfonated polysterene cation resin (DOWEX AG50-X8) in order to separate rare-earth elements (REEs) from uranium-rich materials. The chemical separation scheme is designed to reduce matrix effects and consequently yield enhanced ionization efficiencies for concentration determinations of REEs without significant fractionation using solution mode-inductively coupled plasma mass spectrometry (ICP-MS) analysis. This method was then applied to determine REE abundances in four uraninite (ideally UO 2 ) samples and their associated U(VI) alteration minerals. In three of the samples analyzed, the concentration of REEs for primary uraninite are higher than those for their corresponding secondary uranium alteration phases. The results for U(VI) alteration minerals of two samples indicate enrichment of the light REEs (LREEs) over the heavy REEs (HREEs). This differential mobilization is attributed to differences in the mineralogical composition of the U(VI) alteration. There is a lack of fractionation of the LREEs in the uraninite alteration rind that is composed of U(VI) minerals containing Ca 2+ as the interlayer cation (uranophane and bequerelite); contrarily, U(VI) alteration minerals containing K + and Pb 2+ as interlayer cations (fourmarierite, dumontite) indicate fractionation (enrichment) of the LREEs. Our results have implications for nuclear forensic analyses since a comparison is reported between the REE abundances for the CUP-2 (processed uranium ore) certified reference material and previously determined values for uranium ore concentrate (UOC) produced from the same U deposit (Blind River/Elliott Lake, Canada). UOCs represent the most common form of interdicted nuclear material and consequently is material frequently targeted for forensic analysis. The comparison reveals similar chondrite normalized REE signatures but variable absolute abundances. Based on the results reported here, the latter may be attributed to the differing REE abundances between primary ore and associated alteration phases, and/or is related to varying fabrication processes adopted during production of UOC.

58 GEOSCIENCES↗

Laser Driven Hydrothermal Processing (LDHP) for Rapid Dissolution of Glassy Nuclear Debris

Discovered in 2009 on the SLAB laser system at LLNL, Laser-Driven Hydrothermal Processing (LDHP) both spalls and transiently dissolves a wetted surface (e.g., rock, concrete, paint) when that surface is struck by a laser beam pulse under specific conditions. Previous projects have explored the application of LDHP to expediting sample dissolution for post-detonation nuclear forensics. Early results were very promising, indicating that this method could decrease material dissolution time by a factor of 10 or more. However, the large and complicated lasers previously used are impractical for this application. Under the R^3 venture we aimed to benchmark the LDHP capabilities of turn-key commercial off-the-shelf (COTS) lasers, and to establish how this process could be integrated into an analytical workflow for nuclear forensic analysis. We demonstrated that geological rock standards could be quickly processed into fine powder by LDHP followed by complete acid digestion in 15 minutes, without elemental fractionation that would skew analytical results. We determined that the COTS laser can be used for LDHP that could potentially reduce dissolution time for solid nuclear debris samples in post detonation nuclear forensics. One downside to this approach, however, is that the laser interactions are different with every material, so extensive method validation would be required for all likely material compositions. The LDHP processing rates of several materials were tested and determined to be favorable in the beginning with significant slowdown due to particulate scattering. This could be mitigated either by stopping and centrifuging the sample at specific intervals, or through design of a continuous solvent flow through mechanism.

36 MATERIALS SCIENCE↗

Nonproliferation and Arms Control Research and Development (NPAC R&D) [Slides]

NPAC R&D focus areas include: Advancing U.S. capabilities to detect and characterize nuclear weapon development activities globally, including material production, the movement of special nuclear materials and nuclear weapons, and the testing or use of nuclear weapons, Supporting the development and testing of policy options and technical capabilities for international nuclear safeguards, arms control / treaty verification, nuclear export controls, and nonproliferation initiatives consistent with U.S. Government goals and objectives to enable monitoring and verification, Utilizing uranium, lithium, and high explosives (HE) materials expertise to support national-level activities in nuclear forensics and nuclear detection technology testing and evaluation, Providing unique training and capacity-building programs, particularly with the Nuclear Detection and Sensor Testing Center (NDSTC), and Engaging internationally to promote nonproliferation and arms control norms and best practices through bilateral and multilateral work.

36 MATERIALS SCIENCE↗

Developing a GUM Compliant Uncertainty Approach for NDA Gamma Analysis Using FRAM

The Fixed-Energy Response-Function Analysis with Multiple Efficiency (FRAM) code was developed at Los Alamos National Laboratory (LANL) to analyze gamma-ray spectra for the isotopic composition of plutonium or uranium. This software provides means to easily process gamma-ray spectra to obtain isotopic information and is used globally for international safeguards applications. In a recent review of the FRAM code for the use in nuclear forensics applications, it was determined that a more complete understanding and definition of the various sources of uncertainty that contribute to the overall uncertainty of the FRAM measurement process is required. As one of the ISO 17025 accredited Bulk Special Nuclear Materials Analysis Program (BSAP) laboratories, LANL is required to perform an accurate and transparent uncertainty calculation on every analysis it performs. This paper describes a new approach to calculate a Guide to the Expression of Uncertainty in Measurement (GUM) compliant FRAM uncertainty to support nuclear forensics applications.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Isotopic Ratios of Samarium by TIMS for Nuclear Forensic Application

The isotopic ratio of Nd, Sm, and Gd can provide important information regarding fissile material (nuclear devices, reactors), neutron environment, and device yield. These studies require precise measurement of Sm isotope ratios, by either TIMS or MC-ICP-MS. There has been an increasing trend to measure smaller and smaller quantities of Sm bearing samples. In nuclear forensics 10-100 ng of Sm are needed for precise measurement. To measure sub-ng Sm samples using TIMS for nuclear forensic analysis.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Conceptual Design for the Pilot-Scale Plutonium Oxide Processing Unit in the Radiochemical Processing Laboratory

This report describes a conceptual design for a pilot-scale capability to produce plutonium oxide for use as exercise and reference materials, and for use in identifying and validating nuclear forensics signatures associated with plutonium production. This capability is referred to as the Pilot-scale Plutonium oxide Processing Unit (P3U), and it will be located in the Radiochemical Processing Laboratory at the Pacific Northwest National Laboratory. The key unit operations are described, including plutonium dioxide (PuO2) dissolution, purification of the Pu by ion exchange, precipitation, and conversion to oxide by calcination.

plutonium oxide↗

Technical Comparative Analysis of "Best of Breed" Turnkey Si-Based Processes and Equipment, to be Used to Produce a Combined Multi-entity Research and Development Technology Roadmap for Thick and Thin Silicon PV

A side-by-side analysis was done on then currently available technology, along with roadmaps to push each particular option forward. Variations in turnkey line processes can and do result in finished solar device performance. Together with variations in starting material quality, the result is a distribution of efficiencies. Forensic analysis and characterization of each crystalline Si based technology will determine the most promising approach with respect to cost, efficiency and reliability. Forensic analysis will also shed light on the causes of binning variations. Si solar cells were forensically analyzed from each turn key supplier using a host of techniques

14 SOLAR ENERGY↗