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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 199 records · Page 11
All sourcesNASA NTRSDOE OSTI
DOE OSTI2015

Qualification and initial characterization of a high-purity 233 U spike for use in uranium analyses

Several high-purity 233 U items potentially useful as isotope dilution mass spectrometry standards for safeguards, non-proliferation, and nuclear forensics measurements are identified and rescued from downblending. By preserving the supply of 233 U materials of different pedigree for use as source materials for certified reference materials (CRMs), it is ensured that the safeguards community has high quality uranium isotopic standards required for calibration of the analytical instruments. One of the items identified as a source material for a high-purity CRM is characterized for the uranium isotope-amount ratios using thermal ionization mass spectrometry (TIMS). Additional verification measurements on this material using quadrupole inductively coupled plasma mass spectrometry (ICPMS) are also performed. As a result, the comparison of the ICPMS uranium isotope-amount ratios with the TIMS data, with much smaller uncertainties, validated the ICPMS measurement practices. ICPMS is proposed for the initial screening of the purity of items in the rescue campaign.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2016

Surrogate Post-Detonation Urban Debris (SPUD): Standard Reference Materials 4600 and 4601

If a terrorist nuclear explosion were to occur in the United States, high-quality (accurate and precise) legally defensible nuclear forensics measurements will be required to assure the certainty and confidence needed, for conclusions drawn from these data will be coupled with law enforcement and intelligence information for the purposes of attribution and retribution. Standard Reference Materials (SRMs)/Certified Reference Materials (CRMs) establish the traceability, accuracy, and precision of nuclear forensic measurements and provide the ability to benchmark measurement methods essential to meeting the requirements of legal scrutiny. Currently there is a critical shortage of key SRMs/CRMs required for accurate and precise measurements that are fundamental to nuclear measurements supporting pre- and post-detonation nuclear forensics. Supplies either do not exist, are not good enough, are in short supply, and/or are very expensive. The radionuclide measurement techniques and data quality objectives for pre- and post-detonation nuclear forensics are quite different than the applications for which the current suite of available SRMs/CRMs was developed. Specifically, 1) modern mass spectrometry methods have largely replaced traditional activity-based measurement methods for quantifying small quantities of long-lived radionuclides and most trace radionuclide SRMs/CRMs are certified for activity and are thus not adequate for current applications, 2) modern instrumental methods are capable of higher precision than historic measurement techniques, and in some cases exceed the precision of the available SRMs/CRMs, and 3) the quality assurance requirements for pre- and post-detonation nuclear forensics are such that the existing cadre of SRMs/CRMs does not adequately support the needs for method validation. There are numerous governmental stakeholders both within the US (DOE, DoD) and internationally (IAEA, JRC-ITU) whose missions are either directly involved with nuclear forensics measurements or rely on the forensic data obtained to make the exacting policy decisions (DOJ (FBI), DHS, CIA, DIA, DoD) associated with disrupting the production of illicit nuclear materials, interdicted nuclear materials or a nuclear/radiological detonation event. Starting in 2008 the DHS NTNFC, in collaboration with NBL and NIST, took on the production of suitable SRMs/CRMs for the pre-detonation nuclear forensics community. Two CRMs have been released since the start of this effort and two more are slated for completion in 2016. More recently, NIST, as a part of its mission as the US National Metrology Institute (NMI) to deliver standards (providing traceability) and foster homeland security, has launched the first certification campaign of a measurement traceable post nuclear detonation SRM. NIST, in cooperation with partner labs (AFIT (DoD), FBI (DOJ), and NPL) and with support from the FBI, has developed two Surrogate Post-Detonation Urban Debris (SPUD) Standard Reference Materials (SRMs) - SRM 4600 and 4601. These SRMs have been developed to simulate the expected debris mixture from the detonation of an Improvised Nuclear Device (IND) in an urban environment, which is capable of producing fresh fission as well as activation products. The elemental composition of the vitrified debris materials is a composite of minerals and metals characteristic of the concrete and steel, the building materials that would be exposed to a nuclear detonation and whose resulting activation products would be found in rubble samples collected for forensics evidence and attribution. Additionally, because post-detonation samples would also contain short-lived fission products, the debris materials have been doped with Uranium (U). To create the nuclear fission products, samples of the SPUD materials can be placed in a well-characterized nuclear reactor and exposed to a set neutron flux and energy, causing the encased U atoms to split and yield short-lived fission products. Because a known amount of U is added to the SPUD materials it is feasible to determine the concentration of the resulting fission products. The subsequent irradiated SPUD glass would be chemically similar to samples that would be generated in an actual detonation, and thus can serve as a standardized reference material for nuclear forensic post detonation measurements. (authors)

61 RADIATION PROTECTION AND DOSIMETRY↗
DOE OSTI2025

Internal-Gelation Production of Uranium Oxide Sol-Gel Particles for Forensic Applications

The purpose of this project was to develop and demonstrate a novel method for the production of uranium oxide microsphere particles with tunable chemical compositions via a sol-gel process using a 3D-printer setup. These particles can serve several purposes in research and development as a forensic training tool or as standard reference materials. A key component of the project was to demonstrate the ability to control physical and chemical parameters of the particles created. First, we demonstrated the ability to employ an internal gelation sol-gel process to create individual uranium oxide particles. The particles were successfully dispensed using a unique 3D-printing setup onto a substrate to react and then were collected and thermally processed. A series of temperatures for the annealing process was tested on individual samples to investigate the effect on the sol-gel chemical composition and physical integrity. Next, we demonstrated the ability to control matrix composition of the particles by separately incorporating fission product isotopes as well as Np-237 into the sol-gel solution. It was shown by gamma-ray spectroscopy that these matrix elements were successfully retained during the gelation process. We studied the retention of the elements across a series of annealing temperatures. Additionally, we demonstrated the ability to quantitatively control the isotopic composition of the particles by altering the U-237/U-238 ratio to a controlled value. Finally, X-ray diffraction analysis (XRD) was used to investigate the oxidation state of the sol-gel after annealing at different temperatures.

37 - INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL C↗
DOE OSTI2014

Final Scientific/Technical Report

JHU/APL conducted solid propellant fire characterization tests in warm, humid, ambient conditions near sea level. Yttria and ceria surrogate materials were placed in the fires. The substrates simulating ground surfaces were concrete from a Kennedy Space Center launch pad, and steel covered with a protective ablative material representing a launch platform. In-situ instrumentation consisted of witness materials, thermocouples, air handlers, filters, and cascade impactors; remote instrumentation consisted of optical cameras and spectrometers. Test and analysis team members included the Naval Air Warfare Center Aircraft Division, Sandia National Laboratories (SNL), Alliant Techsystems, and the Johns Hopkins University. Test data were analyzed, reported, and delivered, including plume rise and transport captured on video. Derivation of the alumina particle size distributions formed the basis for condensing vapor and agglomeration estimates. Assessment of alumina mass in the plume, along with the surrogate fraction from filter forensics, provided an estimate of airborne surrogate mass. Technical interchange meetings were held with SNL and the Jet Propulsion Laboratory. Specifications for the fire environment were developed and delivered. A thermochemistry model that simultaneously provides the maximum temperature and heat flux was developed and delivered. An SPIE paper on 3D pyrometry of the fire was written and presented.

36 MATERIALS SCIENCE↗
DOE OSTI2023

A data analysis method to rapidly characterize gallium concentration in plutonium matrices using LIBS

The processing of actinide samples is a complex and costly endeavor that requires compositional analysis at various stages. Laser-induced breakdown spectroscopy (LIBS) has been used to analyze actinide-containing samples in many nuclear applications including waste management, fuel processing and forensics. The LIBS spectrum obtained from actinide materials are generally extremely complex, exhibiting many thousands of strong emission lines. This makes it difficult to identify other elements within the sample of interest, given the rich and dominant actinide spectrum. Here, in this article, we describe a recent effort to identify and quantify impurities and alloying constituents in plutonium matrices using a hand-held LIBS instrument that is used to rapidly and efficiently measure an emission spectrum from a material sample. We tabulate the emission line positions and intensities of plutonium. We report the development of machine-learning software that can identify gallium and quantify its concentration in plutonium matrices. This work has the potential to provide a rapid and nearly non-destructive technique that allows more confidence in characterizing the composition of materials that are present within complex actinide associated targets. We describe how our LIBS measurements and data analysis methods have successfully quantified the gallium concentration in a variety of samples.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

DHS-Postdoc Mid- and year-end report for FY13

The focus of my effort during the second half of FY13 was planning and performing experiments that enable the high precision isotopic measurement of the heavy rare earth elements (HREEs) gadolinium (Gd) and dysprosium (Dy). The isotopic compositions of these elements will be used as forensic signatures in a variety of nuclear materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Results from the fifth galaxy serpent exercise

Galaxy Serpent is an ongoing series of virtual, web-based international tabletop exercises designed to advance the application of National Nuclear Forensics Libraries (NNFLs) in investigations involving nuclear and other radioactive material found out of regulatory control. Here, this iteration emphasized interactions between scientific teams and mock investigative entities. Participants utilized their provided NNFLs to assess material consistency with a provided database of holdings, assign confidence levels, and identify key characteristics relevant to investigative queries. The exercise highlighted both challenges encountered and lessons learned, and advanced best practices for integrating a NNFL into nuclear forensics as part of an investigation.

Database↗
DOE OSTI2015

Oxidation and Hydration of U 3 O 8 Materials Following Controlled Exposure to Temperature and Humidity

Chemical signatures correlated with uranium oxide processing are of interest to forensic science for inferring sample provenance. Identification of temporal changes in chemical structures of process uranium materials as a function of controlled temperatures and relative humidities may provide additional information regarding sample history. In our study, a high-purity α-U 3 O 8 sample and three other uranium oxide samples synthesized from reaction routes used in nuclear conversion processes were stored under controlled conditions over 2–3.5 years, and powder X-ray diffraction analysis and X-ray absorption spectroscopy were employed to characterize chemical speciation. We measured signatures from the α-U 3 O 8 sample indicated that the material oxidized and hydrated after storage under high humidity conditions over time. Impurities, such as uranyl fluoride or schoepites, were initially detectable in the other uranium oxide samples. After storage under controlled conditions, the analyses of the samples revealed oxidation over time, although the signature of the uranyl fluoride impurity diminished. The presence of schoepite phases in older uranium oxide material is likely indicative of storage under high humidity and should be taken into account for assessing sample history. Finally, the absence of a signature from a chemical impurity, such as uranyl fluoride hydrate, in an older material may not preclude its presence at the initial time of production.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Laser ablation spectrometry for studies of uranium plasmas, reactor monitoring, and spent fuel safety

Nuclear security is one of the defining challenges of our time. Nuclear threats range from deliberate dispersal of radioactive material to contaminate the vital infrastructure to diversion and smuggling of special nuclear material for clandestine nuclear programs and nuclear terrorism, respectively. There is an associated need to develop and sustain the nuclear forensics capabilities, which requires the understanding of complex processes that occur in plasmas of nuclear materials. The area of nuclear safety has seen a resurgence of public interest, and there is a concomitant need to safely store used nuclear fuel and detect structural material failure in nuclear power systems, especially in innovative reactor designs envisioned for future adoption. Laser-produced plasmas are complicated extreme environments that can generate intense and rich, highly specific signatures of nuclear and radiological materials, which can then be explored in a wide range of applications. They include interdiction and rapid detection of nuclear materials, including their isotopic composition, detection over long distances, laboratory simulation of weapons effects, monitoring the condition of structural materials in dry cask storage containers, and novel instrumentation for nuclear power systems. We present a compilation of recent representative examples of the application of laser spectroscopy, and laser-induced breakdown spectroscopy in particular, to nuclear safety and security problems. A case is made that spectroscopic techniques based on laser-produced plasmas offer complementary, and sometimes unique, capabilities that motivate the continued exploration of their efficient production and understanding of the signatures they produce

(020.3260) Isotope shifts, (140.3440) Laser-induce↗
DOE OSTI2026

Forensic characterization of surrogate nuclear explosion debris: radiochemical and spectroscopic strategies for method validation

Surrogate nuclear explosion debris (SNED) has emerged as a critical platform for advancing post-detonation nuclear forensic analysis in the absence of readily accessible historic materials. SNED enables controlled investigation and validation of analytical methodologies used to interrogate the chemical, isotopic, radiological, and microstructural signatures preserved in nuclear explosion debris. This review presents an integrated assessment of destructive and non-destructive analytical techniques commonly employed within decision-driven nuclear forensic workflows. Each technique is discussed individually while highlighting how it contributes to different stages of post-detonation analysis. Core methods – including gamma and alpha spectrometry, ICP-MS, TIMS, SIMS, SEM-EDS, XRF, LIBS, vibrational spectroscopy, and X-ray absorption spectroscopy – are critically evaluated with respect to forensic maturity, information content, and matrix limitations. Emphasis is placed on the role of SNED in benchmarking multi-modal workflows and identifying gaps in reproducing heterogeneity, fractionation, and radiation-driven evolution relevant to forensic attribution.

X-ray spectroscopic methods↗
DOE OSTI2015

Nuclear forensic analysis of uranium oxide powders interdicted in Victoria, Australia

Nuclear forensic analysis was conducted on two uranium samples confiscated during a police investigation in Victoria, Australia. The first sample, designated NSR-F-270409-1, was a depleted uranium powder of moderate purity (~1000 μg/g total elemental impurities). The chemical form of the uranium was a compound similar to K 2 (UO 2 ) 3 O 4 ·4H 2 O. While aliquoting NSR-F-270409-1 for analysis, the body and head of a Tineid moth was discovered in the sample. The second sample, designated NSR-F-270409-2, was also a depleted uranium powder. It was of reasonably high purity (~380 μg/g total elemental impurities). The chemical form of the uranium was primarily UO 3 ·2H 2 O, with minor phases of U 3 O 8 and UO 2 . While aliquoting NSR-F-270409-2 for analysis, a metal staple of unknown origin was discovered in the sample. The presence of 236 U and 232 U in both samples indicates that the uranium feed stocks for these samples experienced a neutron flux at some point in their history. The reactor burn-up calculated from the isotopic composition of the uranium is consistent with that of spent fuel from natural uranium (NU) fueled Pu production. These nuclear forensic conclusions allow us to categorically exclude Australia as the origin of the material and greatly reduce the number of candidate sources.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2013

Design and Application of TIMS-Based Thorium Measurement Methods in the Actinide Analytical Chemistry Group at Los Alamos National Laboratory

Quantitation of inter-related actinides in nuclear materials, whether they be intercepted (e.g. stolen fuel pellets) or purposefully collected (e.g. cotton swipe samples), is essential in modern nuclear forensics and safeguards. Well-designed procedures may provide insight into a material’s “age” (i.e. time since last purification), suggest processing/preparation routes, and point to involved parties. In the present work, we detail the design and preliminary application of a thermal ionization mass spectrometry (TIMS) based approach to the analysis of thorium-230 within uranium-bearing materials. These efforts are in-line with a chronometric-type analysis strategy and focused on identification of appropriate preparation procedures, development of required spiking materials (i.e. 229 Th), and evaluation of uranium certified reference materials (CRMs). The presence of thorium in these materials is expected to be largely due to a combination of the decay of parent uranium (e.g. 234 U) to daughter nuclides (e.g. 230 Th), and thorium persistence following last purification.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Model ages of three uranium metal CRMs and implications for radiochronometry data interpretation

In this study, we report 230 Th/ 234 U and 231 Pa/ 235 U model ages in three uranium metal certified reference materials with distinct production histories and isotopic compositions ranging from depleted to highly enriched (CRMs 112-A, 115, and 116-A). Here, our results provide the first model age values for these materials using multiple radiochronometers, which can be used as reference values for quality control of radiochronometry measurements performed during nuclear forensic investigations. Furthermore, we evaluate the model ages in the context of available production records for the materials, which provides insight into the processes that may impact radiochronometry systems during uranium metal production.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2024

Separation of gold from irradiated actinide material utilizing a 2- thenoyltrifluoroacetone extraction resin

Post-detonation nuclear forensics capabilities depend on the ability to rapidly isolate radionuclides to improve measurement quality. In this work an extraction chromatography resin was developed utilizing the extractants thenoyltrifluoroacetone and 1-octanol supported on Eichrom prefilter resin. Here the resin was tested in nitric and hydrochloric acid matrices. In nitric acid matrices the resin is able to extract zirconium, while in hydrochloric acid matrices it is possible to extract iron and gallium. In all acid conditions tested gold is retained but can be removed from the column with a 10% thiourea rinse.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2018

Lessons from Past Nuclear Disarmament: What Worked What Did Not

This report studies the efforts of the international community and the United States to verif)/ the denuclearization of various countries: Ukraine, South Africa, Iraq, Taiwan, and Libya. In doing so, it considers the verification of nuclear warhead destruction and the accounting of nuclear materials. Each case study contributes to the understanding we have of which verification procedures worked and which did not and what factors contributed to that success and which did not. The most important factor contributing to successful verification is the cooperation of the subject country. If a country has made the strategic decision to cooperate, then it is possible that verification can be successful. If the country chooses not to cooperate, verification might rest on random and unpredictable events. This unpredictability of verification is politically unacceptable. Even if verification is judged to be successful by the implementing agencies, outsiders can cast doubts on it by pointing out small and potentially unavoidable errors in material amounts verified. It is vitally important to systematically preserve forensic evidence, especially shipping and receiving records to avoid just such issues. Historically, such records are the most important evidence in verifying denuclearization. Technology is far less important than forensic analysis of records. It does play a supporting role in verifying some declarations but there can be an enormous delay in drawing conclusions caused by the necessity to analyze statistically large samples of materials. The confidence one gets from such analysis can be delayed well past the time it is politically significant. The most important advance in technology would be to accelerate that sample analysis process.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗
DOE OSTI2025

Utilization of the LS-APGD microplasma/orbitrap-FTMS booster system for detection and isotopic analysis of neodymium nanoparticles

Detection and isotopic analysis of particle populations has seen rapid growth across several application areas, including environmental analysis, nuclear forensics, and food safety. The ability to characterize the particles' unique elemental and isotopic fingerprints could provide information related to formation, processing history, and transport. Regarding nuclear forensics, isotopic analysis of particles derived from diverse materials is often used as a tool to trace the origin and processing history. Mass spectrometric-based techniques currently used for particle population analysis often suffer from limited mass resolution, particularly when dealing with real-world samples that are affected by isobaric and polyatomic interferences from the matrix. To address these analytical challenges, we propose a novel method utilizing the liquid sampling-atmospheric pressure glow discharge (LS-APGD) microplasma ionization source coupled to an ultrahigh resolution Orbitrap mass spectrometer, further enhanced with the FTMS X2T Booster data acquisition and processing unit. The FTMS Booster enables acquisition of extended transient times of up to 3 s, significantly improving mass resolution, thereby reducing or even eliminating the need for prior separation of isobaric or polyatomic interferences. Additionally, the detection of low-abundance isotopes was improved by increasing the signal-to-noise (S/N) ratio. As proof of concept, this study demonstrates the feasibility of the LS-APGD/Orbitrap-FTMS X2T Booster platform for direct analysis using a suspension of well-characterized ∼120 nm neodymium particles. The quality of the isotope ratios values obtained from a few hundred particles were in good agreement with those obtained from homogeneous ionic solutions. These results highlight the potential of the LS-APGD/Orbitrap platform for rapid, accurate, and interference-resilient isotope ratio analysis of particle populations without the need for dissolution and subsequent chemical separations, offering significant advantages for nuclear forensics, safeguards, and environmental applications. The effort here also points to further paths forward, hopefully towards single particle (SP) analysis using microplasma ionization and the ultrahigh resolving power of the Orbitrap mass analyzer.

FTMS X2T booster↗
DOE OSTI2023

Machine learning in analytical spectroscopy for nuclear diagnostics [Invited]

Analytical spectroscopy methods have shown many possible uses for nuclear material diagnostics and measurements in recent studies. In particular, the application potential for various atomic spectroscopy techniques is uniquely diverse and generates interest across a wide range of nuclear science areas. Over the last decade, techniques such as laser-induced breakdown spectroscopy, Raman spectroscopy, and x-ray fluorescence spectroscopy have yielded considerable improvements in the diagnostic analysis of nuclear materials, especially with machine learning implementations. These techniques have been applied for analytical solutions to problems concerning nuclear forensics, nuclear fuel manufacturing, nuclear fuel quality control, and general diagnostic analysis of nuclear materials. The data yielded from atomic spectroscopy methods provide innovative solutions to problems surrounding the characterization of nuclear materials, particularly for compounds with complex chemistry. Implementing these optical spectroscopy techniques can provide comprehensive new insights into the chemical analysis of nuclear materials. In particular, recent advances coupling machine learning methods to the processing of atomic emission spectra have yielded novel, robust solutions for nuclear material characterization. This review paper will provide a summation of several of these recent advances and will discuss key experimental studies that have advanced the use of analytical atomic spectroscopy techniques as active tools for nuclear diagnostic measurements.

Rao, Ashwin P. (ORCID:0000000319312568)↗
DOE OSTI2021

Application of HRGS for forensic characterization of uranium oxides, pure uranium metals and uranium alloys

A nondestructive iterative method for uranium-bearing material characterization with HRGS developed earlier in (J. appl. Rad. Isotopes, 166 (2020) 109433) is applied to determine matrix densities and uranium isotope masses of a variety of uranium materials, namely uranium ore, UO 2 and U 3 O 8 powders, fuel elements in the form of UO2 microspheres, uranium metal and uranium alloys. It is shown that U 3 O 8 powders with uranium mass fraction of about 84% can be distinguished from the powders of UO 2 with uranium mass fraction of about 87%; uranium products in the form of liquid or loose powder with matrix density of 0.5-2.0 g/cm 3 can be distinguished from uranium products in the form of compacted fuel elements with matrix density of 6.0-10.0 g/cm 3 and from pure metal uranium and uranium alloys with matrix density of 14.0- 19.0 g/cm 3 . In fuel microspheres based on UO2 the uranium mass fraction 88.02% measured by HRGS is consistent, within the measurement uncertainties, with the results of isotope dilution mass spectrometry 87.76±0.64 % and also is confirmed by X-ray diffraction technique. The uranium mass fraction of the uranium ore estimated as 0.08% by HRGS is consistent, within the measurement uncertainties, with the value 0.09±0.01% determined with WDXRF. Densities of two different uranium metal samples, estimated as 18.42 g/cm 3 and 19.33 g/cm 3 by HRGS are consistent with values 18.24±0.55 g/cm 3 and 18.86±0.59 g/cm 3 , respectively, obtained by the gas pycnometry technique.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗