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This is a poster about a current LDRD project, it is intended for the FY2020 NHSS&T Strategic Advisory Committee review meeting.
Fission products from photon-induced fission are routinely used at Idaho National Laboratory as part of nuclear forensics activities. Typically, the focus is on fission products with relatively large fission yields (Ba-140, Mo-99, etc.). The nuclear data associated with the well-known isotopes have small uncertainties, and many have well-known angular correlations between emitted gamma-rays, if applicable. However, for isotopes with smaller fission yields or less intense gamma-ray emission intensities, the nuclear decay schemes and gamma-ray emission intensities may be less well-known. The Germanium Rotational Measurements for Angular Correlation (GeRMAC) system was designed to use two high-purity germanium (HPGe) detectors in a coincidence counting set-up but allows one of the HPGe detectors to rotate at a constant distance from a radioactive source, changing the relative angle between the two HPGe detectors. Angular correlations can then be determined from the relative photopeak areas between two gamma-rays emitted as part of the same nuclear decay. By recording the HPGe spectra in list mode, the angular correlations of gamma-rays emitted from complex sources, consisting of multiple isotopes, can be measured simultaneously and the individual isotope emissions can be isolated. Using the GeRMAC system, a multi-isotope fission product source, produced with photon-induced fission of U-238, was measured using a single rotational arc (180 degrees) to obtain the angular correlation between gamma-rays emitted by the large number of fission products contained in the solution with an angular accuracy of 1 degree. In particular, La-140 (38 gamma rays) and Nd-147 (26 gamma rays) are of interest to the nuclear forensics community.
Biobanks containing formalin-fixed, paraffin-embedded (FFPE) tissues from animals and human atomic-bomb survivors exposed to radioactive particulates remain a vital resource for understanding the molecular effects of radiation exposure. These samples are often decades old and prepared using harsh fixation processes which limit sample imaging options. Optical imaging of hematoxylin and eosin (H&E) stained tissues may be the only feasible processing option, however, H&E images provide no information about radioactive microparticles or radioactive history. Synchrotron X-ray fluorescence microscopy (XFM) is a robust, non-destructive, semi-quantitative technique for elemental mapping and identifying candidate chemical element biomarkers in FFPE tissues. Still, XFM has never been used to uncover distribution of formerly radioactive micro-particulates in FFPE canine specimens collected more than 30 years ago. In this work, we demonstrate the first use of low-, medium-, and high-resolution XFM to generate 2D elemental maps of ~ 35-year-old, canine FFPE lung and lymph node specimens stored in the Northwestern University Radiobiology Archive documenting distribution of formerly radioactive micro-particulates. Additionally, we use XFM to identify individual microparticles and detect daughter products of radioactive decay. The results of this proof-of-principle study support the use of XFM to map chemical element composition in historic FFPE specimens and conduct radioactive micro-particulate forensics.
For applications related to nuclear security, safeguards, and nonproliferation, it is often critical to know the molecular compositions of lanthanide- and actinide-containing samples. Spectroscopy is a widely used tool that looks at the interaction between light and matter: Different species absorb or emit light at unique wavelengths which act as signatures. However, there is a limited number of tools that can achieve high-sensitivity, accurate measurements of lanthanide and actinide molecular compositions. Candidate methods include mass spectrometry, which usually destroys at least part of the sample and requires complicated stoichiometry to guess the original sample’s molecular compositions; optical spectroscopies, which have great atomic but limited molecular sensitivities or other drawbacks which make sensing molecules difficult like limited light sources or strong absorption in the atmosphere; and nuclear spectroscopies (gamma, neutron) which also have limited sources and long (>minute) collection times. As such, the purpose of our research is to develop a new tool to better distinguish between subtle differences in molecules containing lanthanides and actinides. Soft x-ray spectroscopy is sensitive to molecular form and is minimally intrusive/nondestructive to the sample. However, soft x-ray light with sufficient brightness for spectroscopy is typically limited to user-facilities like synchrotrons or free electron lasers, where beamtimes are competitive, and work with radiological materials may be difficult or entirely prohibited. To overcome this issue, our Team has developed a custom tabletop laser-driven, soft x-ray light source which employs high harmonic generation (HHG). Soft x-ray spectroscopy can distinguish between subtly different molecules, in the spectral range which we need to study these heavy elements. A tabletop system provides an effective and affordable tool to find both the elemental and chemical specificity of lanthanide and samples. Creating a light source in the soft x-ray spectrum is difficult because these wavelengths in the range 5-20 nm (20-350 eV photon energies) only penetrate several 100s of nm in most solid materials and only reflect well in shallow, grazing incident angles. The results are applicable to nuclear forensics, because molecular fingerprinting of lanthanide and actinide samples can be used to back out the origin and processing method of nuclear materials (Skrodzki, et al.).
The commercialization of DNA tagging is a growing trend that demonstrates the increasing practicality of this novel approach. This interdisciplinary technology is based on the distinctive characteristics of DNA as a molecule that can remain stable in varying environmental conditions and store data following appropriate preparation. Moreover, newly developed technologies could simplify DNA synthesis and the encoding of data within DNA. The implementation of DNA tagging presents distinctive benefits in comparison to conventional labelling techniques, including universal product code (UPC) barcoding, radio-frequency identification (RFID), quick response (QR) codes, and Bluetooth technologies, by surmounting the limitations encountered by these systems. The discourse pertains to extant DNA-tagging mechanisms along with prospective implementations in a wide range of domains, including but not limited to art, the metaverse, forensics, wildlife monitoring, and the military. The potential of DNA labelling in various contexts underscores the importance of continued research and development in this rapidly evolving field.
The ATONA technology has the potential to impact measurement capabilities in the broad field nuclear forensics, and not just for uranium. We remain cautiously optimistic that we can develop ATONA based environmental measurement techniques that will be of use to some of our partners.
Characterizing neutron activation of stainless steel is a critical task for many applications, and yet little activation data is available for this alloy. To address the need, a series of neutron activation experiments have been performed using the Flattop critical assembly at the National Criticality Experiments Research Center. Several experimental conditions were probed for complete understanding of the neutron environment, including foil composition and position within the assembly. The experimental results reported here will aid in the production of stainless steel benchmarks for a range of nuclear data applications including those used in nuclear forensics analysis.
The Z Machine at Sandia National Laboratories is a pulsed power facility for high-energy density physics experiments that can shock materials to extreme temperatures and pressures through a focused energy release of up to ~ 25 MJ in < 100 nanoseconds. It has been in operation for more than two decades and conducts up to ~ 100 experiments, or “shots,” per year. Based on a set of 74 known shot times from 2018, we determined that Z Machine shots produce detectable ~ 3–17 Hz ground motion 12 km away at the Albuquerque Seismological Laboratory, New Mexico (ANMO), borehole seismograph, with peak signal at ~ 7 Hz. The known shot waveforms were used to create a three-component template, leading to the detection of 2339 Z Machine shots since 1998 through single-station cross-correlation. Local seismic magnitude estimates range from local magnitude (M L ) —2 to —1.3 and indicate that only a small fraction of the shot energy is transmitted by seismic phases observable at 12 km distance. The most recent major facility renovation, which was intended to decrease mechanical dissipation, is associated with an abrupt decrease in observed seismic amplitudes at ANMO despite stable maximum shot energy. The highly repetitive impulsive sources are well suited to coda-wave interferometry to investigate time-dependent velocity structures. Relative velocity variations (dv/v) show an annual cycle with amplitude of ~ 0.2%. Local minima are observed in the late spring, and dv/v increases through the summer monsoon rainfall, possibly reflecting patchy saturation as rainfall infiltrates near the eastern edge of the Albuquerque basin. Importantly, the cumulative results demonstrate that forensic seismology can provide insight into long-term operation of facilities such as pulsed-power laboratories, and that their recurring signals may be valuable for studies of time-dependent structure
Retinex Imaging Processing, winner of NASA's 1999 Space Act Award, is commercially available through TruView Imaging Company. With this technology, amateur photographers use their personal computers to improve the brightness, scene contrast, detail, and overall sharpness of images with increased ease. The process was originally developed for remote sensing of the Earth by researchers at Langley Research Center and Science and Technology Corporation (STC). It automatically enhances a digital image in terms of dynamic range compression, color independence from the spectral distribution of the scene illuminant, and color/lightness rendition. As a result, the enhanced digital image is much closer to the scene perceived by the human visual system, under all kinds and levels of lighting variations. TruView believes there are other applications for the software in medical imaging, forensics, security, recognizance, mining, assembly, and other industrial areas.
Several days following the Columbia accident a team formed and began planning for the reconstruction of Columbia. A hangar at the Kennedy Space Center was selected for this effort due to it's size, available technical workforce and materials science laboratories and access to the vehicle ground processing infrastructure. The Reconstruction team established processes for receiving, handling, decontamination, tracking, identifying, cleaning and assessment of the debris. Initially, a 2-dimensional reconstruction of the Orbiter outer mold line was developed. As the investigation progressed fixtures which allowed a 3-dimensional reconstruction of the forward portions of the left wing's leading edge was developed. To support the reconstructions and forensic analyses a Materials and Processes (M&P) 'team was formed. This M&P team established processes for recording factual observations, debris cleaning, and engineering analysis. Fracture surfaces and thermal effects of selected airframe debris were assessed, and process flows for both nondestructive and destructive sampling and evaluation of debris were developed. The Team also assessed left hand airframe components that were believed to be associated with a structural breach of Columbia. A major portion of this analysis was evaluation of metallic deposits were prevalent on left wing leading edge components. Extensive evaluation of the visual, metallurgical and chemical nature of the deposits provided conclusions that were consistent with the visual assessments and interpretations of the NASA lead teams and the findings of the Columbia Accident Investigation Board. Analytical data collected by the M&P Team showed that a significant thermal event occurred at the left wing leading edge in the proximity of LH RCC Panels 8-9, and a correlation was formed between the deposits and overheating in these areas to the wing leading edge components. The analysis of deposits also showed exposure to temperatures in excess of 1649 C (3200 F), which would severely degrade support structure, tiles, and RCC panel materials. The integrated failure analysis of wing leading edge debris and deposits strongly supported the hypothesis that a breach occurred at LH RCC Panel 8.
The naturally occurring rare isotopes are versions of common elements, such as hydrogen, carbon and oxygen, that contain a larger than usual number of neutrons in their atomic nuclei and therefore are higher in mass than the common atoms of that element. Isotopes exist for most elements and are found in most natural and synthetic materials, but are uneven in their distribution because chemical and physical processes are isotope-selective (e.g., a chemical reaction may proceed more rapidly for one isotope than for another). For this reason, abundances of isotopes in a material of interest can provide a record, or ‘signature’ of various features of that material’s origin and history. These signatures have been used in the geo, life, chemical and physical sciences in a wide variety of ways over close to 8 decades. However, many such applications struggle to reach unique interpretations of isotopic data because multiple factors combine to control a given sample’s overall isotopic content. That is, the factors controlling isotopic content are too numerous and complex to fully constrain from a simple measurement of a material’s isotope abundances. However, the distribution of isotopes within materials, at molecular scales potentially provides a vastly larger number and diversity of constraints on the chemical and physical processes that comprise a material’s history. The rare isotopes may be concentrated into one atomic position in a molecule relative to another, some proportion of molecules in a sample may contain two or more rare isotopes, and those multiply-isotope-substituted forms of molecules may also have uneven distributions of those isotopes across individual atomic sites. For these reasons, even small, seemingly simple molecules, such as sugars, amino acids or drug compounds, actually exist in a vast number of isotopically unique forms (often millions or more), and each one of those forms is in some sense an independent ‘vote’ on that sample’s history. This project has focused on opening this rich archive of information by enabling the creation of routinely and widely applicable ways of measuring and interpreting isotopic structures of molecules. This work has included the development of core technologies and analytical methods, advancing fundamental understanding of the physical and chemical properties of isotopic versions of molecules, and conducting proof of concept studies of illustrative geochemical, cosmochemical and forensic problems in order to show how these technologies, methods and principles come together to solve problems in new ways. A key to the success of this project was the adaptation of ‘Fourier transform mass spectrometry’ (FTMS) to the task of precisely measuring proportions of the rare, naturally occurring isotopic forms of molecules. FTMS is a highly specialized form of mass spectrometry that traps ions within magnetic or electrostatic cavities and, effectively, ‘listens’ (through registering of subtle electrical signals) to the harmonic signals they make while rapidly orbiting within those cavities. These signals have periods that are a function of their mass and strength (or ‘loudness’) that is proportional to their abundances. Thus, these signals constrain relative amounts of molecules that differ in their mass due to various isotopic substitutions. This technology has been essential to the identification of organic molecules in the life, chemical and environmental sciences for over 4 decades, but generally has lacked the control, stability and precision to meaningfully measure rare isotope forms of molecules. This project’s most fundamental contribution has been to modify FTMS, both in terms of hardware and methods, to enable such measurements. The raw data of molecular isotopic structure is tremendously voluminous and complex, so another important activity of this project has been developing the theoretical and data-science tools needed to interpret the data generated by this new form of isotopic measurement. A particularly challenging part of this task has been predicting molecular isotopic structure, as only through the comparison of measurements with predictions can we make progress on hypothesis driven research questions. We have attacked this this prediction task through a combination of first-principles chemical-physics models of the effects of isotope substitution on molecule properties and data-science models that permit us to generalize that chemical physics to cases that have not yet been studied by detailed chemical physics theory. The proof of concept applications we have pursued over the course of this study include biological reactions of amino acids and other biomolecules, non-biological synthesis of organic molecules in extra-terrestrial settings such as meteorites, petroleum geoscience questions concerning the origin and evolution of natural gas, oil and kerogen compounds, and forensic questions such as the sourcing of chemical weapons. The successes of these applications have laid the groundwork for the next phase of this field’s development, which will include larger scale and more ambitious studies of molecular isotopic structure as a means of diagnosing human diseases, such as cancer, and reconstructing detailed interpretations of the origin and evolution of organic molecules in modern and geological environments.
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.
Publicly accessible weather radar data have significant capabilities for meteorological measurements and predictions and, further, have the potential to measure nonmeteorological events that include smoke, ash, and debris plumes as well as explosions. The ability to identify and track nonmeteorological events can be of assistance in emergency response, hazard mitigation, and related activities in locations where radar coverage both exists and is recorded and accessible to the user. Here, in this study, events from multiple locations in the United States that are reported in news outlets are assessed using a manual inspection process of Level 2 weather radar data to identify anthropogenic and nonbiological returns. Explosive events are also identified, and a large high-altitude debris cloud from the intentional destruction of the SpaceX Starship is tracked across a wide area. Finally, future efforts using a machine learning model are discussed as a means of automating the process and potentially enabling near-real-time nonmeteorological event identification in the same areas where the data are accessible. Using weather radar data can be a valuable new tool for Department of Defense systems to aid in military awareness, and for interagency emergency response and forensic mission experts to consider national weather service data in their mission profiles. Radar data can be effective in detecting several common types of emergencies and inform and aid response personnel.
Analysis of byproducts from thermal degradation of polymer materials provides a wealth of information about a materials’ composition, thermal stability, degradation mechanisms, and kinetics. However, regardless of the instrumentation used, only limited information is obtainable from a single experiment. Microfurnace technology, when interfaced to a gas chromatography-mass spectrometry (GC-MS), can be used to obtain both thermal and chemical information via evolved gas analysis-MS (EGA-MS) and GC-MS analysis modes. While both EGA-MS and Py-GC-MS are valuable when characterizing polymer materials, at least two experiments on distinct samples are required, which can be a liability for clear interpretation of results from inhomogeneous samples. Here, we seek to overcome this limitation by combining EGA-MS and Py-GC-MS modes in a single experimental setup. Further, this was done by developing new gas line modifications to allow for tandem Pyrolysis Evolved Gas-Gas Chromatography-Mass Spectrometry (Py/EG-GC-MS) analysis. Verification of Py/EG-GC-MS analysis was performed using a polystyrene standard. Results demonstrate successful Py/EG-GC-MS analysis for the first-time showing the potential of these modifications for application in areas where sample is limited or direct correlation of products to the thermal profile is desirable such as in forensics or product-specific kinetics.
Three important upgrades provide unsurpassed TIMS measurement capabilities 1. HI-VAC (installed 5 of 7 instruments) 2. ATONA Faraday amplification (2 of 7 instrument) 3. Multiple ion-counting system for ultra-low level detection (installed 4 of 7 instruments).
Forensic analysis of man-made, non-nuclear events (such as industrial accidents, explosion experiments and mine collapses) has become more frequent and detailed owing to advancements in geophysical monitoring. Here, in this Technical Review, we demonstrate how geophysical forensic monitoring using seismic, infrasound and hydroacoustic recordings provides insights on events in the solid earth, atmosphere and underwater. Advanced techniques, including machine-learning-based models, have been developed to detect, identify and investigate these events, providing information on location, subevents, sources and explosive yield. The increase in data availability, application of advanced methods and computation and the growth of multitechnology approaches have increased the accuracy of forensic event analysis and enabled more realistic characterization of uncertainties. For example, the 2020 Beirut explosion in Lebanon demonstrated that various seismic, acoustic and other methods could be used to estimate explosive yield (and yield uncertainties) of about 1 ktonne, providing confidence in the application of these methods to smaller events where data are available. However, forensic investigations remain largely limited to known events with identified sources. Increased access to data, sophisticated analysis methods and high-resolution earth models will improve forensic event analysis further, enabling civil and scientific applications, such as localization in the search for the lost ARA San Juan submarine.
Nuclear forensics is a key part of the nuclear security strategy for the United States and the international community. The NACS Division is central to the leadership role that LLNL has had in nuclear forensics over the past 25 years. Our current nuclear forensic program includes conducting R&D on provenance and attribution signatures, collaborating with international partners, training the next generation of nuclear forensic experts, developing test materials for verification and validation exercises, and providing expert advice to national and international policy makers. Key to our success in these areas has been the strong and continuing involvement in nuclear forensic casework obtained through law enforcement and intelligence channels as well as our outstanding analytical capabilities. NACS must continue to conduct forward-thinking R&D in nuclear forensics that supports operational programs and addresses intelligence gaps. To maintain leadership in nuclear forensics, we must attract, develop, and retain the best talent. The NNSA has a central leadership role in developing educational initiatives for nuclear forensics. In concert with the Glenn T. Seaborg Institute, the NACS Division will continue to participate in all nuclear forensic educational initiatives (undergraduate, graduate, postdoctoral) and incorporate LLNL’s D&I vision into its student and postdoc recruitment efforts. We will continue to build formal relationships with key academic partners and institutions with active and emerging nuclear forensic research interests. We will also strengthen relationships with NNSA DNN and SSAA funded university consortia (e.g. NSSC, ACE, CNEC, CVT, ETI, MTV), helping them conduct research of interest and relevance to nuclear forensics, while at the same time evaluating and recruiting promising talent from these programs.
The topics include: 1) Spectral Profiler Probe for In Situ Snow Grain Size and Composition Stratigraphy; 2) Portable Fourier Transform Spectroscopy for Analysis of Surface Contamination and Quality Control; 3) In Situ Geochemical Analysis and Age Dating of Rocks Using Laser Ablation-Miniature Mass Spectrometer; 4) Physics Mining of Multi-Source Data Sets; 5) Photogrammetry Tool for Forensic Analysis; 6) Connect Global Positioning System RF Module; 7) Simple Cell Balance Circuit; 8) Miniature EVA Software Defined Radio; 9) Remotely Accessible Testbed for Software Defined Radio Development; 10) System-of-Systems Technology-Portfolio-Analysis Tool; 11) VESGEN Software for Mapping and Quantification of Vascular Regulators; 12) Constructing a Database From Multiple 2D Images for Camera Pose Estimation and Robot Localization; 13) Adaption of G-TAG Software for Validating Touch and Go Asteroid Sample Return Design Methodology; 14) 3D Visualization for Phoenix Mars Lander Science Operations; 15) RxGen General Optical Model Prescription Generator; 16) Carbon Nanotube Bonding Strength Enhancement Using Metal Wicking Process; 17) Multi-Layer Far-Infrared Component Technology; 18) Germanium Lift-Off Masks for Thin Metal Film Patterning; 19) Sealing Materials for Use in Vacuum at High Temperatures; 20) Radiation Shielding System Using a Composite of Carbon Nanotubes Loaded With Electropolymers; 21) Nano Sponges for Drug Delivery and Medicinal Applications; 22) Molecular Technique to Understand Deep Microbial Diversity; 23) Methods and Compositions Based on Culturing Microorganisms in Low Sedimental Fluid Shear Conditions; 24) Secure Peer-to-Peer Networks for Scientific Information Sharing; 25) Multiplexer/Demultiplexer Loading Tool (MDMLT); 26) High-Rate Data-Capture for an Airborne Lidar System; 27) Wavefront Sensing Analysis of Grazing Incidence Optical Systems; 28) Foam-on-Tile Damage Model; 29) Instrument Package Manipulation Through the Generation and Use of an Attenuated-Fluent Gas Fold; 30) Multicolor Detectors for Ultrasensitive Long-Wave Imaging Cameras; 31) Lunar Reconnaissance Orbiter (LRO) Command and Data Handling Flight Electronics Subsystem; and 32) Electro-Optic Segment-Segment Sensors for Radio and Optical Telescopes.