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At least 37 records · Page 2

Chemical speciation correlated with microstructural heterogeneity of interdicted uranium materials

Two uranium powders seized by law enforcement in Victoria, Australia, have been characterized by established nuclear forensic methods in a previously published study. Here, in this work, the results of further characterization by a scanning transmission x-ray microscope (STXM) operating in the soft x-ray regime are reported. STXM images are used to estimate the elemental distribution in micrometer-scale particles of each powder, and oxygen K-edge absorption spectra are used to determine the chemical state of uranium. The results of the current study are consistent with the previous analysis; the first powder is found to be a potassium-uranium hydrate, while the second powder is determined to be a mixture of uranium oxides primarily consisting of UO 3 .

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

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↗

Advances in Autoradiography Systems for Nuclear Forensic Analysis

Nuclear forensic analysis techniques work to determine the contents of radiological samples with nondestructive and destructive analysis methods. Autoradiography is a nondestructive analysis method that creates an image of the distribution of radioactivity within the sample. These images allow the location of the radiological content within a sample to be ascertained, which can be used for further analysis. Autoradiography has been used since the discovery of radiation and has been continuously developed to better suit the needs of the medical, nuclear security, nuclear safeguards, and nuclear forensic communities. Recent developments in autoradiography have led to a higher spatial resolution down to a level of tens of microns, real-time capabilities that minimize the risk of overexposure, and the ability to discriminate particles. All of these developments in autoradiography would assist the nuclear forensics community in understanding the placement of radiological content within a sample and in understanding the locations of beta-particle interactions versus those for alpha-particle interactions. This article aims to discuss the history of autoradiography as well as multiple different autoradiographic technologies while focusing on imaging plates, the BeaQuant system, and the ionizing-radiation Quantum Imaging Detector system. This article reviews three autoradiographic techniques and detectors, discusses how they relate to nuclear forensics, and addresses the drawbacks and benefits of each detector.

Autoradiography↗

Mixed Element Microparticle Characterization by Electron Probe Microanalysis

Abstract Microparticle compositional characterization for nuclear forensics has traditionally been achieved by “gold-standard” destructive analytical techniques such as large geometry-secondary ion mass spectrometry and fission track-thermal ionization mass spectrometry, but long processing times and total sample consumption eliminate the option of subsequent analysis by other methods. Electron probe microanalysis has long been widely employed for rapid, nondestructive, micrometer-scale compositional measurements and imaging in fields such as material science and geology and may therefore need to be reevaluated as an alternative tool for microparticle analysis for the nuclear forensics community. This study presents the use of electron probe microanalysis for imaging and quantitative characterization of homogeneous microparticles utilizing a calibration curve based on high-precision quadrupole-inductively coupled plasma-mass spectrometry analyses. Samples of opportunity synthesized at Savannah River National Laboratory, nickel-doped cerium oxide microparticles, were selected as analogs for plutonium-doped uranium oxide microparticles. Positive detection and accurate quantification of variable amounts of nickel dopant down to trace levels (10s of parts per million) suggest applicability of this technique to other mixed element systems (e.g., actinides). Quantitative single-particle characterization via electron probe microanalyzer may thus provide a high fidelity, nondestructive complement to techniques currently in use.

Riche, Alexis T. (ORCID:0009000121978126)↗

Expanding Accurate Person Recognition to New Altitudes and Ranges: The BRIAR Dataset

Face recognition technology has advanced significantly in recent years due largely to the availability of large and increasingly complex training datasets for use in deep learning models. These datasets, however, typically comprise images scraped from news sites or social media plat-forms and, therefore, have limited utility in more advanced security, forensics, and military applications. These applications require lower resolution, longer ranges, and ele-vated viewpoints. To meet these critical needs, we collected and curated the first and second subsets of a large multi-modal biometric dataset designed for use in the research and development (R&D) of biometric recognition technolo-gies under extremely challenging conditions. Thus far, the dataset includes more than 350,000 still images and over 1,300 hours of video footage of approximately 1,000 sub-jects. To collect this data, we used Nikon DSLR cameras, a variety of commercial surveillance cameras, specialized long-rage R&D cameras, and Group 1 and Group 2 UAV platforms. The goal is to support the development of algorithms capable of accurately recognizing people at ranges up to 1,000 m and from high angles of elevation. These ad-vances will include improvements to the state of the art in face recognition and will support new research in the area of whole-body recognition using methods based on gait and anthropometry. This paper describes methods used to col-lect and curate the dataset, and the dataset's characteristics at the current stage.

Brogan, Joel↗

High-Energy X-ray Diffraction Microscopy for Nuclear Forensics FY2022 Project Report

Morphological information on nuclear material has been identified using visible light and scanning electron microscopy. These identify qualitative differences in particle morphology. Three-dimensional imaging of materials through alternating scanning electron microscopy imaging and focused ion beam milling has also been used. Unfortunately, these techniques are time- and labor-intensive, with significant sample preparation required and lengthy analysis times. Further, the resulting 3D images are qualitative, require manual identification, and do not capture statistically-representative populations. High energy X-ray 3D imaging using a direct-beam or diffracted-beam (High-Energy Diffraction Microscopy) have been developed at the Advanced Photon Source and can produce quantitative information on grains (phase, location, etc.) and pores (size distribution, sphericity) in a material. These techniques require only minutes to characterize a sample volume and are non-destructive, thus suitable for a wide range of existing samples and for confirmatory analyses to be carried out using conventional microscopy techniques. In this first year of the project, all uranium oxide samples were synthesized and characterized using conventional analyses by the analytical chemistry laboratory. Conventional analysis methods included powder x-ray diffraction, scanning electron microscopy, impurity analysis via inductively coupled plasma mass spectrometry, and infrared spectroscopy. Impurity analysis shows a drop in boron content from UO 3 to the lowest U 3 O 8 calcination temperature, but otherwise no appreciable difference in any sample. Analysis of diffraction data shows a flip of peaks from UO 3 dominated for the 600 °C calcined sample to U 3 O 8 dominated at 700 °C and 800 °C. Analysis of scanning electron microscopy images shows that with increased calcination temperature the size distribution of particles seems to increase and broaden. Both of these last findings are in line with previously published data, though this work used significantly fewer particles to simply show similar trends instead of getting truly quantitative particle analysis. Infrared analysis similarly shows ingrowth of U 3 O 8 as calcination temperature is increased, along with depression of peaks associated with UO 3 and water. Samples were prepared for analysis at the Advanced Photon Source at beamline 1-ID. It is anticipated that analysis will occur in November of 2022. AI/ML techniques to de-noise data coming out of 1-ID during the analyses was also developed during this time using previously gathered data. Preliminary results using a self-supervision technique called Noise2Selfshow good de-noising of data. Once the uranium oxide samples are analyzed, real data will be used to test the de-noising and other AI/ML techniques that may be developed in the second year of the project.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

High-Energy X-ray Diffraction Microscopy for Nuclear Forensics (FY23 Project Report)

Morphological information on nuclear material has been identified using visible light and scanning electron microscopy. These identify qualitative differences in particle morphology. Three-dimensional imaging of materials through alternating scanning electron microscopy imaging and focused ion beam milling has also been used. Unfortunately, these techniques are time- and labor-intensive, with significant sample preparation required and lengthy analysis times. Further, the resulting 3D images are qualitative, require manual identification, and do not capture statistically-representative populations. High energy X-ray 3D imaging using a direct-beam or diffracted-beam (High-Energy Diffraction Microscopy) have been developed at the Advanced Photon Source and can produce quantitative information on grains (phase, location, etc.) and pores (size distribution, sphericity) in a material. These techniques require only minutes to characterize a sample volume and are non-destructive, thus suitable for a wide range of existing samples and for confirmatory analyses to be carried out using conventional microscopy techniques.

36 MATERIALS SCIENCE↗

Review of multi-faceted morphologic signatures of actinide process materials for nuclear forensic science

Particle morphology is an emerging signature that has the potential to identify the processing history of unknown nuclear materials. Using readily available scanning electron microscopes (SEM), the morphology of nearly any solid material can be measured within hours. Coupled with robust image analysis and classification methods, the morphological features can be quantified and support identification of the processing history of unknown nuclear materials. The viability of this signature depends on developing databases of morphological features, coupled with a rapid data analysis and accurate classification process. With developed reference methods, datasets, and throughputs, morphological analysis can be applied within days to (i) interdicted bulk nuclear materials (gram to kilogram quantities), and (ii) trace amounts of nuclear materials detected on swipes or environmental samples. In conclusion, this review aims to develop validated and verified analytical strategies for morphological analysis relevant to nuclear forensics.

36 MATERIALS SCIENCE↗

Improving robustness for model discerning synthesis process of uranium oxide with unsupervised domain adaptation

The quantitative characterization of surface structures captured in scanning electron microscopy (SEM) images has proven to be effective for discerning provenance of an unknown nuclear material. Recently, many works have taken advantage of the powerful performance of convolutional neural networks (CNNs) to provide faster and more consistent characterization of surface structures. However, one inherent limitation of CNNs is their degradation in performance when encountering discrepancy between training and test datasets, which limits their use widely. The common discrepancy in an SEM image dataset occurs at low-level image information due to user-bias in selecting acquisition parameters and microscopes from different manufacturers. Therefore, in this study, we present a domain adaptation framework to improve robustness of CNNs against the discrepancy in low-level image information. Furthermore, our proposed approach makes use of only unlabeled test samples to adapt a pretrained model, which is more suitable for nuclear forensics application for which obtaining both training and test datasets simultaneously is a challenge due to data sensitivity. Through extensive experiments, we demonstrate that our proposed approach effectively improves the performance of a model by at least 18% when encountering domain discrepancy, and can be deployed in many CNN architectures.

scanning electron microscopy↗

A case study in contrastive learning information combination: Application to technical forensics of additive manufacturing filament source identification

Combination of information from disparate data sources into a single decision is a core challenge in many fields, including the field of technical forensics. Technical forensics (TF) utilizes technical characterization of questioned samples to determine properties of that sample; these properties are then used to infer information of forensic interest, such as provenance, age, or attribution. TF is utilized in traditional forensic applications, such as the attribution of material fragments from an explosive, and in nuclear forensic applications, such as the attribution of actinides which have been interdicted out of regulatory control. The challenge of combining information from disparate sources, described alternately by many terms including “Data Fusion” and “Data Integration”, is exacerbated in the technical forensics domain due to at least two factors: the challenge of interpreting each information source singularly, and the relatively small data set sizes available. Extensive literature exists attempting to combine technical forensics information sources, both in manual and automated processes. These attempts are often bespoke to the specific information sources (such as the bi-, tri-, or quad-isotope chart (Moody, Grant, and Hutcheon 2005)), with some emerging examples of simple early- and late- fusion (, respectively). Simultaneous to the information combination efforts described in the previous paragraph, the field of natural language processing attempted (and largely succeeded) in combining information from multiple non-technical information sources. The ecosystem of “multi-modal” language models, which can take text and images as input, and generate text and images as output, became large and diverse by 2025 (Khan et al. 2025). In a generalized sense, many of these methods are trained by learning neural networks which can convert raw text or images into a vector of numbers describing the text or image, hereafter called “embeddings” and the neural networks performing the conversion are called “embedders”. By using a separate embedder for text and images, finding coincident text and images (such as images with their captions), and optimizing the parameters of the embedders such that the embeddings for the text and the image are similar, the field has found a bridge between text and images (Girdhar et al. 2023). It is the contention of the authors of this report that this insight is not limited to text and images but instead can be extended to any modality which can be found coincidently. The subject of the rest of this report is the application of this method to example multi-modal technical forensic data. Some details about the data used in this report are not appropriate for this report, and are included in a companion report (PNNL-38669).

36 MATERIALS SCIENCE↗

Analytical workflow dependence of experimental observables for uranium chemistries

In this work, we investigated how the sequencing of laboratory analytical methods used for chemical and morphological characterization influences analytical findings for particulate materials relevant to the nuclear fuel cycle, including UO2, U3O8, studtite (UO2O2·4H2O), and β-UO3, in the context of nuclear forensic analysis. Particles of each chemistry obtained from consistent production batches were exposed to Raman spectroscopy and scanning electron microscopy in varying orders to elucidate how the order in which the techniques are applied influences morphological and chemical observations as a function of particle size. The results indicate that particles from all four chemistries exposed to high-resolution electron imaging before Raman spectral analysis demonstrate optical vibrational spectral changes that reduce accurate interpretation of the underlying chemistry via Raman spectral analysis. We hypothesize that these changes are due to the thermal load of the electron beam imparted to the sample being unable to be dissipated by materials with poor thermal conduction properties. Results from this study will aid in determining best practices for forensic analysis procedures to reduce uncertainty in chemical determination of unknown particulate samples.

Manns, Rebecca [University of Nevada, Las Vegas]↗

Ion Mobility – Mass Spectrometry Rapid Imaging of Special Nuclear Materials

Robot Nose will use new fast data throughput methods and experience with laser microfocus to dramatically improve the speed and spatial resolution of an established instrument, making it a useful tool for imaging special nuclear materials (SNM). Mass spectrometry imaging instruments have traditionally been too slow and mass alone is generally an insufficient measurement for organic analyses. This situation was markedly improved by Ionwerks Inc., who pioneered the combination of ion mobility with mass spectrometry imaging. In 2D mobility-mass plots, clearly identifiable trend lines can be selected and reduced to 1D mass spectra without isobaric interferences. This is a major advantage over other imaging mass spectrometers that generally cannot distinguish isobars without custom-built lasers or high voltage accelerators. Special nuclear material (SNM) contains substantial fissile isotopes, particularly 233U, 235U, and 239Pu. A complete forensic analysis of SNM therefore requires quantitative isotopic measurement – often through some form of mass spectrometry. SNM contaminated with inclusions such as pollen grains can help identify its prior locations. The project team is presently working on an approach to allow rapid screening of 1-3 cm diameter thin samples of such material.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Automated nuclear cloud feature extraction from film

Chemical, biological, radiological, nuclear, and explosives incidents require rapid detection and characterization for appropriate response. For a nuclear detonation, visible-light cameras may be used to locate the cloud and characterize fallout deposition when coupled with numerical models. Films from the United States’ nuclear testing era compose the only sizeable collection of imagery depicting high-yield detonations. These films offer unique insights into characteristics of flows involving scales that are difficult to replicate experimentally, and they are a valuable source of data for the validation of models for nuclear fallout transport, either as part of emergency response or forensic activities. In this work, we implement modern computer vision and machine learning techniques to identify and track the cloud automatically and subsequently determine the time dependence of some of its features. We trained a ResNet-18 image classifier on hundreds of images to categorize nuclear cloud morphology. Each category or cloud regime is determined by early cloud evolution and is associated to constitutive properties of the flow, such as distribution of vorticity. Next, we identified keypoint features using the KAZE algorithm and tracked these keypoints in the images, allowing us to determine the dimensions and velocities of the cloud across film frames. These measurements converted to real-world units provide valuable experimental data that can be used in the development and validation of nuclear cloud models. We compared the results of this method against manual cloud rise measurements from two different films. In one, our automated method accelerated the feature extraction process without sacrificing measurement accuracy.

Khristy, Joel [ORNL] (ORCID:0000000209963060)↗

Uranium Oxide Synthetic Pathway Discernment through Unsupervised Morphological Analysis

We present a novel unsupervised machine learning method for quantitative representation of scanning electron micrographs and its applications and performance for nuclear forensic analysis of uranium ore concentrates. The method uses a vector quantizing variational autoencoder followed by a histogram operation to encode a micrograph into a single dimensional representation, called the latent vector. The method requires no extant labeling of the data and can be applied over large datasets of micrographs with minimal human interaction. The representations generated are broadly descriptive of each micrograph and the microstructure of the material imaged. In the case of uranium ore concentrate analysis, the representations were amenable to processing reagent and ore concentrate species classification with accuracy of 81:8%, which is competitive with state-of-the-art supervised networks. The representations were also used to classify previously unseen processing routes, were able to classify imaging parameters such as magnification (to 76:0% accuracy), were able to classify fine grained process parameters such as calcining temperature (to 74:4% accuracy), and their informatic properties indicate that they are generally descriptive of the image represented. This method can be applied across microstructure analysis fields to perform quantitative analysis without the need for labor intensive and possibly biased human analysis.

Scanning Electron Microscopy, Vector Quantizing Va↗

Forensic Analysis of SOHO Router Binaries

Small Office/Home Office (SOHO) routers are used by millions of consumers across the United States, and are commensurately vulnerable. Forensic analysis of SOHO router firmware helps to understand and mitigate those vulnerabilities. This poster focused particularly on analysis of BusyBox executables, a software suite that provides several Unix utilities in a single file. Three main tools were used to analyze the binaries. BinWalk was used to extract the files, but also to build entropy graphs, extract Linux kernel images, and identify CPU architectures; WiiBin processed the binaries to find endianness, architecture, the percent compressed/encrypted, and compiler data; and @DisCo, a machine learning tool used to determine function similarity in disassembled binaries, analyzed similarities and determined versions of extracted BusyBox files from each router. These tools found that venders from all five routers utilized the same version of the BusyBox software across different firmware updates, demonstrating the importance of constant firmware scrutiny to protect against security vulnerabilities.

24 POWER TRANSMISSION AND DISTRIBUTION↗

Nanotomography for Quantitative 3D Particle Reconstruction

Particulates are ubiquitous across fuel cycle operations and carry critical information about particle formation, processing, and potential proliferation-related activities. Traditional analytical techniques, including micro-Raman spectroscopy and standard electron microscopy, are often limited in spatial resolution or dimensionality, particularly when used to examine metallic or submicron-scale features. Understanding particle morphology, phase distribution, and internal porosity is essential for constraining formation conditions, thermodynamic environments, and material transport behavior. In this report, we demonstrate the application of plasma focused ion beam nanotomography to reconstruct micron-scale particulates at nanoscale resolution. Using high-resolution backscattered electron imaging and Avizo software, we obtained 3D reconstructions that enabled quantitative analysis of particle morphology, phase composition, and internal voids. Representative examples include a Ta particle with a large central void and a composite particle with embedded tetrahedral crystalline structures. These reconstructions reveal structural and compositional details that are inaccessible through conventional 2D imaging. The results demonstrate that nanotomography provides both qualitative and quantitative insights into particle formation and behavior. Using nanotomography, porosity and phase distributions can be quantified to inform models of particle density, transport, and solidification conditions. Beyond technical insights, the workflow developed here establishes a transferable capability for analyzing heterogeneous particles and has potential applications in bulk materials studies via x-ray computed tomography or other volumetric imaging modalities. Ongoing efforts are focused on optimizing the workflow to process multiple particles simultaneously, increasing throughput and statistical robustness. Overall, this work illustrates the power of nanotomography as a tool for connecting particulate morphology to formation mechanisms, composition, and transport, thereby strengthening analytical capabilities for nuclear forensics, fuel cycle analysis, and related scientific investigations.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗