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At least 19 records

Development of spectroscopic tools for nuclear forensics signatures development

The Savannah River National Laboratory (SRNL) has been developing advanced spectroscopic tools for the characterization of plutonium-bearing compounds with the intent to develop material and process signatures for nuclear forensics. Plutonium in a production, refining, or finishing facility will exist in many forms including oxide precursors (PuF4, PuF3, Pu oxalate, etc.), oxide, and metal. The ability to identify plutonium in each of these chemical forms and determine their processing history is crucial for the development of spectroscopic signatures. This presentation will focus on our work to develop and apply spectroscopic tools at SRNL using doubled-walled cells (DWC) to characterize the thermal decomposition of oxalates, calcination chemistry, alpha-decay-induced chemistry, age dating since last calcination, and other signatures related to plutonium processing.

Villa-Aleman, Eliel↗

Exploring the use of thorium isotope compositions and concentrations as nuclear forensic signatures for uranium ore concentrates

This interlaboratory study measured thorium concentrations and isotope compositions in uranium ore concentrates from different geographical locations to examine whether thorium impurities may be useful forensic signatures for uranium ore concentrates found out of regulatory control. Measured 230 Th/ 232 Th in fifteen uranium ore concentrates record over three orders of magnitude of compositional variation. Results demonstrate that 230 Th/ 232 Th used in combination with U/Th ratios resulted in a unique signature for individual uranium ore concentrates from different processing locations. Data presented here suggest potential for 230 Th/ 232 Th and U/Th to be used as comparative signatures to investigate the provenance of seized uranium ore concentrates.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Samarium isotope compositions of uranium ore concentrates: A novel nuclear forensic signature

Uranium ore is mined and milled to produce uranium ore concentrate (UOC), a regulated product of the nuclear fuel cycle. Additionally, diversion of UOC from the fuel cycle into possible weapons production is a key concern in global nonproliferation efforts. As such, the ability to trace the origin of seized nuclear materials is imperative to law enforcement efforts. Although isotopic signatures of UOCs have proven fruitful to pinpoint sample provenance, new isotopic signatures are needed because most existing isotopic signatures are not indicative of the original ore body from which the U is derived. In this work, we developed a new method to separate samarium (Sm) from a U-rich sample matrix and report the first Sm isotope compositions of 32 UOCs derived from a variety of worldwide uranium mines. Relative to terrestrial standards, approximately half the UOCs have resolved and anticorrelated 149 Sm- 150 Sm isotope compositions, consistent with the capture of thermal neutrons by 149 Sm in the ore body. The UOCs with anomalous Sm isotope compositions tend to derive from older (~>1.5Ga) and higher-grade ore bodies, although other factors, such as the presence of neutron moderators like water, also play a role. Nonetheless, the Sm isotope compositions of UOCs directly reflects the neutron fluence over the history of the original ore body and can be used to discern different geologic conditions associated with that ore body. Overall, this work demonstrates the potential use of Sm isotopes as a novel nuclear forensics signature for origin assessment of UOCs.

58 GEOSCIENCES↗

CADIS and FW-CADIS Variance Reduction in Gamma Transport for Predicting Prompt Forensics Signatures

The goal of prompt nuclear forensics is to determine the characteristics of a nuclear detonation based on the signatures available almost immediately after the explosion. An important characteristic is the reaction time history (RTH), a measure of the device’s rate of neutron multiplication. The RTH can be estimated by observation of the gamma radiation emitted from the detonation, which can be detected directly or observed indirectly as Teller light. Gamma transport simulations used to predict these radiation fields are often modeled stochastically using the Monte Carlo N-Particle (MCNP) code, which can be a computationally demanding task due to the number of particle histories needed to achieve statistical convergence. In an attempt to improve the efficiency of these calculations, we evaluate two variance reduction techniques: Consistent Adjoint-Driven Importance Sampling (CADIS) and Forward-Weighted Consistent Adjoint-Driven Importance Sampling (FW-CADIS). These methods use a deterministically calculated adjoint flux to create weight windows and source biasing that guide MCNP sampling. We study the utility of CADIS and FW-CADIS for their use in MCNP gamma transport for nuclear forensics prediction simulations. Furthermore, the results demonstrate that both CADIS and FW-CADIS improve the accuracy for forensics-focused simulations, with CADIS being most beneficial in direct detection and FW-CADIS being ideal for computing a global Teller light source.

CADIS↗

Evaluating Nuclear Forensic Signatures for Advanced Reactor Deployment: A Research Priority Assessment

The development and deployment of a new generation of nuclear reactors necessitates a thorough evaluation of techniques used to characterize nuclear materials for nuclear forensic applications. Advanced fuels proposed for use in these reactors present both challenges and opportunities for the nuclear forensic field. Many efforts in pre-detonation nuclear forensics are currently focused on the analysis of uranium oxides, uranium ore concentrates, and fuel pellets since these materials have historically been found outside of regulatory control. The increasing use of TRISO particles, metal fuels, molten fuel salts, and novel ceramic fuels will require an expansion of the current nuclear forensic suite of signatures to accommodate the different physical dimensions, chemical compositions, and material properties of these advanced fuel forms. In this work, a semi-quantitative priority scoring system is introduced to identify the order in which the nuclear forensics community should pursue research and development on material signatures for advanced reactor designs. This scoring system was applied to propose the following priority ranking of six major advanced reactor categories: (1) molten salt reactor (MSR), (2) liquid metal-cooled reactor (LMR), (3) very-high-temperature reactor (VHTR), (4) fluoride-salt-cooled high-temperature reactor (FHR), (5) gas-cooled fast reactor (GFR), and (6) supercritical water-cooled reactor (SWCR).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Trace Impurities Identified as Forensic Signatures in CMX-5 Fuel Pellets Using X-ray Spectroscopic Techniques

We report that small-particle analysis is a highly promising emerging forensic tool for analysis of interdicted special nuclear materials. Integration of microstructural, morphological, compositional, and molecular impurity signatures could provide significant advancements in forensic capabilities. We have applied rapid, high-sensitivity, hard X-ray synchrotron chemical imaging to analyze impurity signatures in two differently fabricated fuel pellets from the 5th Collaborative Materials Exercise (CMX5) of the IAEA Nuclear Forensics International Working Group. The spatial distributions, chemical compositions, and morphological and molecular characteristics of impurities were evaluated using X-ray absorption near-edge structure (XANES) and X-ray fluorescence chemical imaging to discover principal impurities, their granularity, particle sizes, modes of occurrence (distinct grains vs incorporation in the UO 2 lattice), and sources and mechanisms of incorporation. Differences in UO 2+x stoichiometry were detected at the microscale in nominally identical UO 2 ceramics (CMX5-A and CMX5-B), implying the presence of multiple UO 2 host phases with characteristic microstructures and feedstock compositions. Al, Fe, Ni, W, and Zr impurities and integrated impurity signature analysis identified distinctly different pellet synthesis and processing methods. For example, two different Al, W, and Zr populations in the CMX5-B sample indicated a more complex processing history than the CMX5-A sample. K-edge XANES measurements reveal both metallic and oxide forms of Fe and Ni but with different proportions between each sample. Altogether, these observations suggest multiple sources of impurities, including fabrication (e.g., force-sieving) and feedstock (mineral oxides). This study demonstrates the potential of synchrotron techniques to integrate different signatures across length scales (angstrom to micrometer) to detect and differentiate between contrasting UO 2 fuel fabrication techniques.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Development of Spectroscopic Tools for Nuclear Forensics Signatures Development

Diversion of nuclear materialsfrom legitimate commercial processes for use by nefarious actors is a frightening and surreptitious problem. Smuggled nuclear material can be used to manufacture a simple radiological dispersion device (RDD) and potentially incorporated into the development of a nuclear weapon. With some frequency, smuggled nuclear material is interdicted in foreign countries as actors cross border checkpoints. Nuclear material interdicted in this way can be analyzed using a variety of tools. Plutonium-239 is commonly used as the fissile material in nuclear weapon production as an alternative to uranium-235. Plutonium in a production, refining, or finishing facility will exist in many forms including oxide precursors (PuF4, PuF3, Pu oxalate, etc.), oxide, and metal. The ability to identify plutonium in each of these forms and determine properties, characteristics, or history of these materials is crucial for determining if the processes occurring in a nuclear facility are legitimate or not. This presentation will focus on the development and application ofspectroscopic tools developed at SRNL using doubled-walled cells (DWC) to characterize Pu-bearing compounds. Advances in the use of vibrational spectroscopy techniques (Raman and IR), UV-VIS-SWIR diffuse reflectance spectroscopy, gamma emission spectroscopy, luminescence spectroscopy, laser-induced breakdown spectroscopy in conjunction with XRD and SEM in the characterization of Pu-bearing compounds will be presented with emphasis in material processing history.

Villa-Aleman, Eliel↗

Physics-Based Machine Learning Methods for U-235 Forensics Signatures

Signatures of low-intensity U-235 sources have been recently studied by utilizing a variety of machine learning (ML) classifiers using features derived from gamma spectral measurements collectedunder structured campaigns. Several ML classifiers, such as ensemble of tress and classification trees, revealed misleadingly-optimistic training error due to over-fitting, and furthermore,their performance is not directly relatable to the physical properties due to their data-driven, opaque designs. We present a regression-based ML method that first estimates the inverse distanceto the source and then utilizes a threshold to infer its presence, by representing the background as a source located at an infinite distance. For the inverse distance estimation, we study the ensembleof trees and Gaussian process regression methods, and a hyper parameter auto-tuning and selection method that employs five regression estimators. These methods avoid the over-fittingobserved in several ML classifiers, while providing the classification error nearly comparable to them based on independent test data. Their error is directly related to estimates of the inversephysical distance to source, and the precision of error determines the seperability property that determines the false alarm and missed detection rates. The property of monotonic decrease of thesource strength with increasing detector distance combined with Poisson distribution of measurements is utilized to analytically validate these methods by deriving the generalization equations ofunderlying regression methods.

Rao, Nageswara↗

Physics-Based Machine Learning Methods for U-235 Forensics Signatures

Signatures of low-intensity U-235 sources have been recently studied by utilizing a variety of machine learning (ML) classifiers using features derived from gamma spectral measurements collected under structured campaigns. Several ML classifiers, such as ensemble of tress and classification trees, revealed misleadingly-optimistic training error due to over-fitting, and furthermore, their performance is not directly relatable to the physical properties due to their data-driven, opaque designs. We present a regression-based ML method that first estimates the inverse distance to the source and then utilizes a threshold to infer its presence, by representing the background as a source located at an infinite distance. For the inverse distance estimation, we study the ensemble of trees and Gaussian process regression methods, and a hyper parameter auto-tuning and selection method that employs five regression estimators. These methods avoid the over-fitting observed in several ML classifiers, while providing the classification error nearly comparable to them based on independent test data. Their error is directly related to estimates of the inverse physical distance to source, and the precision of error determines the seperability property that determines the false alarm and missed detection rates. The property of monotonic decrease of the source strength with increasing detector distance combined with Poisson distribution of measurements is utilized to analytically validate these methods by deriving the generalization equations of underlying regression methods.

Rao, Nageswara↗

Sample screening of uranium ore concentrates using portable spectrophotometers: investigating the correlation between visible colors and chemical signatures

A research collaboration between the Japan Atomic Energy Agency and the Department of Energy’s National Nuclear Security Administration examined nuclear forensic signatures and analytical methods for tracing the origins of uranium ore concentrates (UOCs). Here, this study focuses on utilizing portable spectrophotometers capable of reflectance measurements in the visible light spectrum as a potential rapid screening tool for nuclear forensics analysis. Unlike laboratory-based near-infrared spectroscopy or digital image analysis, this research investigated the potential to correlate visible color measurements with key nuclear forensics signatures using seven types of UOC samples with known origins and three UOC certified reference materials. Results demonstrated that distinct color groups, quantified using CIELAB values, correlated with major uranium compounds. Furthermore, the findings indicated that trace elements can influence the UOC colors, providing additional insights into material characteristics. Although this approach requires further validation across a broader range of UOC species, this study demonstrated that simple colorimetric analysis using visible spectrophotometry, which does not require complex sample preparation or data processing, can serve as a practical and novel rapid tool for preliminary screening and attribution in nuclear forensics investigations.

and nuclear chemistry↗

Results from a controlled depleted uranium metal casting experiment designed to investigate nuclear Forensic Radiochronometry Signatures

The accurate interpretation of uranium metal 230 Th/ 234 U and 231 Pa/ 235 U radiochronometry model ages requires an understanding of how uranium parent nuclides and decay progeny ( 230 Th and 231 Pa) behave during uranium metal casting. In order to directly measure the spatial distribution of 230 Th and 231 Pa in uranium metal before and after vacuum induction melting (VIM), Los Alamos National Laboratory identified uranium metal feedstock, characterized the metal feedstock, conducted a controlled casting experiment of an approximately 120 kg uranium metal rod, and characterized the cast metal. Herein this study presents radiochronometry results and quantified 230 Th and 231 Pa VIM separation factors from bulk uranium.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Oxygen stable isotopes in the nuclear fuel cycle: Assessment of the potential for determining the fabrication and provenance history of anhydrous and hydrous uranium oxides

Determining the origin and history of interdicted nuclear materials is a central challenge in nuclear forensics. The oxygen stable isotope composition of uranium oxide compounds has emerged as a promising forensic signature, attracting increasing attention since the early 2000s. This review examines analytical techniques for measuring oxygen isotope compositions in uranium oxides and evaluates how the nuclear fuel production cycle introduces or modifies these isotopic signatures. The potential for forensic geolocation is explored through workflows that calibrate the relationship between environmental water oxygen isotopes and those found in uranium oxides. Key strengths and limitations of this approach are assessed, including gaps in knowledge related to isotope fractionation during specific stages of the fuel cycle, and processing facility water inputs. The importance of proper sample handling and storage under inert atmospheres, as well as a deeper understanding of both intra-sample oxygen isotope heterogeneity, and hydrous uranium oxide phase formation, is highlighted for improving the reliability of forensic interpretations. In conclusion, the development of uranium oxide standards with well-characterized δ 18 O values and international collaboration toward consensus on their use are identified as essential steps for advancing the field.

Attribution↗

CWMD Nuclear Forensics Quarterly Report

Analysis and evaluation of nuclear debris is a key component to identify forensic signatures in a post-detonation environment. Currently, methods exist and are practiced in obtaining signatures from post-detonation debris. However, efforts to reduce the timeline in obtaining signatures is continuous within nuclear forensics research and will be forwarded by this research. This education and research project will explore combined material chemistry and separations of radionuclides to provide actionable signatures in less time than standard methods. The research will use the phase distribution of radionuclides in debris to develop targeted and rapid dissolution methods. These dissolution methods will be coupled with microfluidics to achieve samples suitable for analysis within reduced timelines.

and nuclear chemistry↗

Characterizing microscale signatures in uranium ore concentrates using electron probe microanalyzer

Impurities in uranium ore concentrates (UOCs) serve as forensic signatures of processing history and origin. Here, this study utilizes Electron Probe Microanalyzer (EPMA) to characterize microscale compositional and textural features in individual UOC particles from both commercial and bench-scale production. At the particle scale, multiple internal phases with distinct morphologies, chemical signatures, and stoichiometries are documented. Our data shows that chemical impurities are heterogeneously distributed within single particles and among particles within a sample. These microscale heterogeneities correlate with known processing histories, indicating that microscale signatures of early fuel cycle materials can provide valuable information for nuclear forensic material analysis.

organic↗

Nuclear fuel irradiation testbed for nuclear security applications

The nuclear security community has long been interested in the identification and quantification of nuclear material signatures to understand a material’s provenance, use, and ultimate application. New forensics signatures and methods intended for non-traditional or advanced nuclear fuel applications require fuel irradiation experiments to demonstrate viability and validity. Integral fuel irradiations have historically required significant costs and long timelines to design, irradiate, and characterize. This paper describes how a recently developed nuclear fuel irradiation testbed can be used to provide a low cost, rapid turnaround, modular test environment for irradiation and evaluation of nuclear fuel specimens for nuclear security applications. The irradiation testbed houses six small ‘MiniFuel’ samples within hermetically sealed capsules inside targets that can be removed in between each ∼25-day operating cycle of the High Flux Isotope Reactor (HFIR). As many as nine targets can be irradiated using a single irradiation position (reflector region) in HFIR, allowing for varying irradiation temperatures and burnups. A suite of hot cell capabilities have been established to perform post-irradiation examination for measuring performance (e.g., fuel swelling, fission gas release) and facilitating experiment disassembly for subsequent property measurements, microstructural analysis, or chemical assay. This new testbed allows fuel irradiations to be conducted on an accelerated timeframe to enable rapid proof of concept testing and to provide reference material for nuclear fuel security applications. Recent applications using this testbed include the testing of isotopic taggants in UO 2 fuel (intentional forensics), testing of U-10Mo fuel for down-conversion of highly enriched uranium–fueled reactors, and the production of irradiated UO 2 fuel material for signature analysis of its isotopic composition (plutonium, fission gases, etc.).

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

A Review of Nuclear Forensics: 2016-2020

The study of nuclear forensics harkens back to the Manhattan Project-era, when scientists first started to analyze the debris from the 1945 Trinity test. Political turmoil stemming from the Cold War and the rehabilitation of Germany following WWII has led to new challenges in international security involving nuclear proliferation. Nuclear materials have, on occasion, been lost, misplaced, or stolen from former Soviet countries, and illicit materials have been interdicted all over the world. The National Technical Nuclear Forensics Center (NTNFC) was established in 2006, and has been at the forefront of drive to advance nuclear forensic capabilities in the United States. The ultimate goal of nuclear forensics is to examine nuclear and other radioactive materials using analytical techniques to determine origin and history of the material, particularly in the context of law enforcement investigations. Nuclear forensics can be divided into two parts: predetonation and post-detonation. Pre-detonation forensics, as the name implies, is the investigation of a nuclear material or weapon that has not been detonated or involved in an explosion, whereas postdetonation forensics is the study of activation or fission products in debris or the environment following the use of a nuclear or radiological dispersal device (RDD). Both parts require a number of analytical chemical and radiochemical techniques to determine identification of the material. Many advancements in analytical techniques, including rapidity, sample size, and forensic signatures have been made in recent years. The analytical methods that can be used in a nuclear forensic investigation, such as mass spectrometry and gamma spectroscopy, have been described in detail in previous reviews, including Straub et.al, and will not be explained here. This review will discuss recent publications (from 2016 to present) describing advancements of techniques such as radiochronometry, morphology, development of novel reference materials, and inter-laboratory collaborations for both pre- and post-detonation nuclear forensics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗