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At least 289 records · Page 16
All sourcesNASA NTRSDOE OSTI
DOE OSTI2015

Seaborg's plutonium? A case study in nuclear forensics

Passive X-ray and gamma-ray analysis was performed on a curious sample from UC Berkeley's Hazardous Material Facility inventory, and the object was found to contain 239 Pu. No other radioactive isotopes were observed. The mass of 239 Pu contained in this object was determined to be 2.0 ± 0.3 μg. Finally, these observations are consistent with the identification of this object as containing the 2.77-μg PuO 2 (2.44 μg 239 Pu) sample produced in 1942 and described by Seaborg and his collaborators as the first sample of 239 Pu that was large enough to be weighed.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2015

Design of the Laboratory-Scale Plutonium Oxide Processing Unit in the Radiochemical Processing Laboratory

This report describes a design for a laboratory-scale capability to produce plutonium oxide (PuO 2 ) for use in identifying and validating nuclear forensics signatures associated with plutonium production, as well as for use as exercise and reference materials. This capability will be located in the Radiochemical Processing Laboratory at the Pacific Northwest National Laboratory. The key unit operations are described, including PuO 2 dissolution, purification of the Pu by ion exchange, precipitation, and re-conversion to PuO 2 by calcination.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2018

Automated Clean Chemistry for Bulk Analysis of Environmental Swipe Samples – Final Report

Sample preparation methods for mass spectrometry are being automated using commercial-off-the-shelf (COTS) equipment to shorten lengthy and costly manual chemical purification procedures. This development addresses a serious need in the International Atomic Energy Agency’s (IAEA) Network of Analytical Laboratories (NWAL) to increase efficiency in the Bulk Analysis of Environmental Samples for Safeguards program with a method that allows unattended, overnight operation. In collaboration with Elemental Scientific Inc. (ESI), the prepFAST-MC2 was designed based on COTS equipment. It was modified for uranium/plutonium separations using renewable columns packed with Eichrom TEVA® and UTEVA® resins, with a chemical separation method based on the Oak Ridge National Laboratory (ORNL) NWAL chemical procedure. Initial verification of individual columns yielded small elution volumes with consistent elution profiles and good recovery. Combined column calibration demonstrated ample separation without crosscontamination of the eluent. Automated packing and unpacking of the built-in columns initially showed >15% deviation in resin loading by weight, which can lead to inconsistent separations. Optimization of the packing and unpacking methods led to a reduction in the variability of the packed resin to less than 5% daily. Based on the initial experience at ORNL with the prepFAST-MC2, a second-generation model, the prepFAST-SR, was built by ESI. The newly designed prepFAST-SR has several upgrades compared with the original prepFAST-MC2. The upgrades largely addressed issues with the reliability of unpacking the Eichrom columns and with ventilation to ensure adequate removal of acid vapors. Both systems are currently installed in the Ultra-Trace Forensics Science Center at ORNL. Separations of mixed uranium and plutonium samples containing certified reference materials were analyzed by multi-collector inductively coupled plasma mass spectrometry and yielded good results. Current efforts have demonstrated a wider applicability of the prepFAST system. Near-quantitative removal of metal interferences was achieved with the system in both uranium and plutonium separated fractions. Successful system validation was completed with several archived samples. Isotopic results from archived samples and certified reference materials were well within data quality limits for the IAEA NWAL. Additional COTS equipment has been evaluated for its potential to aid the prepFAST-SR system in reducing the time allotments and cleanroom infrastructure requirements for accurate separations. Overall, these efforts help ensure continued efficient and effective operation of the NWAL. Comparison of the amount of personnel time necessary for successful manual vs. automated chemical separations showed a significant decrease in hands-on time from 9.8 hours to 35 minutes for seven samples, respectively. This documented time savings and reduced labor translates to a significant cost savings per sample. Overall, the system will enable faster sample reporting times at reduced cost by limiting personnel hours dedicated to the chemical separation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Synthesis of Plutonium Oxide Specimens for a Statistically Designed Nuclear Forensics Study

This report describes the synthesis of plutonium oxide (PuO 2 ) samples at a bench-scale (10 g Pu) to support nuclear forensics research. The key unit operations that were performed included dissolving the PuO 2 feed material, purifying the Pu by ion exchange, precipitating as plutonium (III) oxalate, and reconverting to PuO 2 by calcination of the oxalate compound. Seventy-six PuO 2 synthetic runs were performed in execution of a statistically designed test matrix. The process parameters varied in these synthesis runs included temperature (30 or 50 °C), the Pu concentration in the feed solution (10, 30, or 50 g Pu/L), the HNO 3 concentration in the feed solution (1, 2, or 3 M), the direction of reagent addition (direct or reverse strike), the source of oxalic acid (solid or solution), and the reagent addition rate (as fast as possible, 20, or 40 minutes). This report describes the synthesis of the 76 PuO 2 specimens. The characterization of these specimens will be described in separate reports.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2019

Intercomparison of the Radio-Chronometric Ages of Plutonium-Certified Reference Materials with Distinct Isotopic Compositions

In this article, an intercomparison of the radio-chronometric ages of four distinct plutonium-certified reference materials varying in chemical form, isotopic composition, and period of production are presented. The cross-comparison of the different 234 U/ 238 Pu, 235 U/ 239 Pu, 236 U/ 240 Pu, and 241 Am/ 241 Pu model purification ages obtained at four independent analytical facilities covering a range of laboratory environments from bulk sample processing to clean facilities dedicated to nuclear forensic investigation of environmental samples enables a true assessment of the state-of-practice in “age dating capabilities” for nuclear materials. The analytical techniques evaluated used modern mass spectrometer instrumentation including thermal ionization mass spectrometers and inductively coupled plasma mass spectrometers for isotopic abundance measurements. Both multicollector and single collector instruments were utilized to generate the data presented here. Consensus values established in this study make it possible to use these isotopic standards as quality control standards for radio-chronometry applications. Results highlight the need for plutonium isotopic standards that are certified for 234 U/ 238 Pu, 235 U/ 239 Pu, 236 U/ 240 Pu, and 241 Am/ 241 Pu model purification ages as well as other multigenerational radio-chronometers such as 237 Np/ 241 Pu. Due to the capabilities of modern analytical instrumentation, analytical laboratories that focus on trace level analyses can obtain model ages with marginally larger uncertainties than laboratories that handle bulk samples. Lastly, when isotope ratio measurement techniques like thermal ionization mass spectrometry and inductively coupled plasma mass spectrometry with comparable precision are utilized, model purification ages with similar uncertainties are obtained.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Trace Actinide Signatures of a Bulk Neptunium Sample

In nuclear forensic analyses, measurements of actinide elements in a sample can assist with identifying interdicted or unknown materials. While these radiochemical signatures have been extensively investigated in uranium materials, less is known about bulk neptunium samples. This paper describes the measurement of trace actinide concentrations and isotopic profiles in a 237 Np oxide sample. Uranium, plutonium, americium, and curium concentrations and isotopic profiles in the sample were determined and deemed potentially useful for distinguishing different sources of 237 Np. Furthermore, several different potential radiochronometry systems were also investigated; discordant results indicate that the Np sample was never completely purified of other actinide elements, or that subsequent contamination of the sample occurred. Few prior studies of neptunium materials have been reported, and these data suggest that trace actinide constituents could provide unique signatures to identify material out of regulatory control.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
NASA NTRS2016

Characterizing GEO Titan Transtage Fragmentations using Ground-based Measurements

In a continued effort to better characterize the Geosynchronous Orbit (GEO) environment, NASA's Orbital Debris Program Office (ODPO) utilizes various ground-based optical assets to acquire photometric and spectral data of known debris associated with fragmentations in or near GEO. The Titan IIIC Transtage upper stage is known to have fragmented four times. Two of the four fragmentations were in GEO while a third Transtage fragmented in GEO transfer orbit. The forth fragmentation occurred in Low Earth Orbit. In order to better assess what may be causing these fragmentations, the NASA ODPO recently acquired a Titan Transtage test and display article that was previously in the custody of the 309th Aerospace Maintenance and Regeneration Group (AMARG) in Tucson, Arizona. After initial inspections at AMARG demonstrated that the test article was of sufficient fidelity to be of interest, the test article was brought to JSC to continue material analysis and historical documentation of the Titan Transtage. The Transtage will be a subject of forensic analysis using spectral measurements to compare with telescopic data; as well, a scale model will be created to use in the Optical Measurement Center for photometric analysis of an intact Transtage, including a BRDF. The following presentation will provide a review of the Titan Transtage, the current analysis that has been done to date, and the future work to be completed in support of characterizing the GEO and near GEO orbital debris environment.

Cowardin, H.↗
DOE OSTI2025

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)↗
DOE OSTI2012

Intrinsic dosimetry of glass containers: A potential interrogation tool for nuclear forensics and waste management

Intrinsic dosimetry is the method of measuring total absorbed dose received by the walls of a container holding radioactive material. By considering the total absorbed dose received by a container in tandem with the physical characteristics of the radioactive material housed within that container, this method has the potential to provide law enforcement officials or waste management personnel with enhanced pathway information regarding the history of the container and its radioactive contents. We report the latest in a series of experiments designed to validate and demonstrate this newly developed tool. Thermoluminescence (TL) dosimetry was used to measure dose effects on the raw stock material of borosilicate container glass with time up to 60 days after gamma ray, x-ray, beta particle or ultraviolet irradiations at doses from 0.15 to 20 Gy. Two peaks were identified in the TL glow curve when irradiated with 60Co, a relatively unstable peak around 120°C and a more stable peak around 225°C. Signal strength of both peaks decayed with time. The minimum measurable dose using this technique was measured to be 0.15 Gy, which is roughly equivalent to a 24 hr irradiation at 1 cm from a 50 ng source of 60Co. After fading, this dose would still be observable approximately 1 year post-irradiation. Similar doses with beta particles and x-rays produced TL glow curves of lower intensity. The TL glow curves were separated into five peaks centered at approximately 120, 160, 225, 300, and 340°C. Differences in TL glow curve shape and intensity were observed for the glasses from different geographical origins. These differences can be explained by changes in the intensities of the five peaks. EPR results showed production of BOHC and E’ silica centers.

Clark, Richard A.↗
DOE OSTI2023

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↗
NASA NTRS2001

Versatile Vials

Advanced Fuel Research, Inc. (AFR) developed a new sol-gel material coating for sample vials to be used in surface-enhanced Raman (SER) spectroscopy. In the fields of biomedical and forensic science, the coated vials are used to identify physiological chemicals present in blood and urine. The vials are used in the pharmaceutical industry in the area of drug development and discovery. In the drug enforcement field, using the vials helps with detection of trace amounts of drugs on surfaces. The SER vials will also help to identify contaminants in water sources, such as various inorganics and pesticides. The new vials have advantages over other SER materials. Former products required that samples be pre-mixed or dissolved into specific solvents or reagents. The SER vials do not have these limitations, and measurements can be performed using any solvent. Furthermore, the signal appears in less than one second. The sol-gel material will stay active for at least one year and the vials are compatible with any Raman spectrometer. Most importantly, the SER activity can be duplicated from vial-to-vial, allowing for reproducible results.

Source record↗
DOE OSTI2021

Progress in Uranium Chemistry: Driving Advances in Front-End Nuclear Fuel Cycle Forensics

The front-end of the nuclear fuel cycle encompasses several chemical and physical processes used to acquire and prepare uranium for use in a nuclear reactor. These same processes can also be used for weapons or nefarious purposes, necessitating the need for technical means to help detect, investigate, and prevent the nefarious use of nuclear material and nuclear fuel cycle technology. Over the past decade, a significant research effort has investigated uranium compounds associated with the front-end of the nuclear fuel cycle, including uranium ore concentrates (UOCs), UF 4 , UF 6 , and UO 2 F 2 . These efforts have furthered uranium chemistry with an aim to expand and improve the field of nuclear forensics. Focus has been given to the morphology of various uranium compounds, trace elemental and chemical impurities in process samples of uranium compounds, the degradation of uranium compounds, particularly under environmental conditions, and the development of improved or new techniques for analysis of uranium compounds. Overall, this research effort has identified relevant chemical and physical characteristics of uranium compounds that can be used to help discern the origin, process history, and postproduction history for a sample of uranium material. This effort has also identified analytical techniques that could be brought to bear for nuclear forensics purposes. Continued research into these uranium compounds should yield additional relevant chemical and physical characteristics and analytical approaches to further advance front-end nuclear fuel cycle forensics capabilities.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2017

Test and Analysis of Solid Rocket Motor Nozzle Ablative Materials

Asbestos free solid motor internal insulation samples were tested at the MSFC Hyperthermal Facility. Objectives of the test were to gather data for analog characterization of ablative and in-depth thermal performance of rubber materials subject to high enthalpy/pressure flow conditions. Tests were conducted over a range of convective heat fluxes for both inert and chemically reactive sub-sonic free stream gas flow. Instrumentation included use of total calorimeters, thermocouples, and a surface pyrometer for surface temperature measurement. Post-test sample forensics involved measurement of eroded depth, charred depth, total sample weight loss, and documentation of the general condition of the eroded profile. A complete Charring Material Ablator (CMA) style aero-thermal analysis was conducted for the test matrix and results compared to the measured data. In general, comparisons were possible for a number of the cases and the results show a limited predictive ability to model accurately both the ablative response and the in-depth temperature profiles. Lessons learned and modeling recommendations are made regarding future testing and modeling improvements that will increase understanding of the basic chemistry/physics associated with the complicated material ablation process of rubber materials.

Clayton, J. Louie↗
DOE OSTI2016

The Preparation of Non-radioactive Glassy Surrogate Nuclear Explosion Debris (SNED) Loaded with an Isotopically Altered Noble Gas

The measurement of the Kr and Xe isotope ratios in nuclear explosion debris is an important forensic tool as the method requires very little sample preparation. Fragments of debris are simply crushed or heated to release the trapped gases Kr and Xe arising from fission product decay. As suitable test materials are not readily available we have been investigating a method to incorporate isotopically enriched 129Xe in glassy materials that mimic nuclear explosion debris. The approach used to prepare these materials will be described along with some of the example results obtained.

Trinitite, Nuclear forensics, Fission Xe, Surrogat↗
DOE OSTI2015

Nuclear forensics: Soil content

Nuclear Forensics is a growing field that is concerned with all stages of the process of creating and detonating a nuclear weapon. The main goal is to prevent nuclear attack by locating and securing nuclear material before it can be used in an aggressive manner. This stage of the process is mostly paperwork; laws, regulations, treaties, and declarations made by individual countries or by the UN Security Council. There is some preliminary leg work done in the form of field testing detection equipment and tracking down orphan materials; however, none of these have yielded any spectacular or useful results. In the event of a nuclear attack, the first step is to analyze the post detonation debris to aid in the identification of the responsible party. This aspect of the nuclear forensics process, while reactive in nature, is more scientific. A rock sample taken from the detonation site can be dissolved into liquid form and analyzed to determine its chemical composition. The chemical analysis of spent nuclear material can provide valuable information if properly processed and analyzed. In order to accurately evaluate the results, scientists require information on the natural occurring elements in the detonation zone. From this information, scientists can determine what percentage of the element originated in the bomb itself rather than the environment. To this end, element concentrations in soils from sixty-nine different cities are given, along with activity concentrations for uranium, thorium, potassium, and radium in various building materials. These data are used in the analysis program Python.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Parametric optimization of the liquid sampling-atmospheric pressure glow discharge ionization source coupled to an Orbitrap mass spectrometer for neodymium isotope ratio determinations

Isotope ratio determinations are a valuable tool in several application areas. In nuclear forensics, the isotope ratios of uranium and plutonium are commonly used as a signature for the nuclear material's provenance and processing history. However, signatures from other coexisting elements, such as neodymium and samarium, can offer additional insights. Here, the liquid sampling-atmospheric pressure glow discharge (LS-APGD) ionization source coupled to an Orbitrap mass spectrometer (MS) has demonstrated its utility for actinide measurements. This instrumental platform can leverage the high resolution offered by the Orbitrap MS to overcome potential isobaric interferences, such as 144 Nd- 144 Sm, 148 Nd- 148 Sm, and 150 Nd- 150 Sm pairs. The work presented herein demonstrates the rapid, accurate, and precise determination of the isotope ratios for neodymium using the LS-APGD/Orbitrap MS. Both the LS-APGD and Orbitrap MS parameters were optimized systematically, with NdO + found to be the most abundant, most reduced species after applying the optimal collision-induced dissociation modalities. A limit of detection of 3 pg of 142 Nd was achieved when data was acquired and processed using the FTMS Booster, an external data acquisition and processing system offered by Spectroswiss. Excellent accuracy of better than 99 % and precision of <1 % RSD were achieved when a solution of the well-characterized neodymium standard (JNdi-1 standard) was analyzed under the optimized condition, indicating the LS-APGD/Orbitrap's great potential for isotope ratio analysis of Nd and other REEs for diverse applications.

47 OTHER INSTRUMENTATION↗