SEARCH · Engineering Papers
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.
Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.
This report gives an introduction to nuclear forensics, high precision isotope ratio mass spectrometry techniques, and chemical separation procedures. The importance of isotope analysis is also discussed, and examples of measurement capabilities at C-NR are given.
We developed new detector technologies to identify the presence of radioactive materials for nuclear forensics applications. First, we investigated an optical radiation detection technique based on imaging nitrogen fluorescence excited by ionizing radiation. We demonstrated optical detection in air under indoor and outdoor conditions for alpha particles and gamma radiation at distances up to 75 meters. We also contributed to the development of next generation systems and concepts that could enable remote detection at distances greater than 1 km, and originated a concept that could enable daytime operation of the technique. A second area of research was the development of room-temperature graphene-based sensors for radiation detection and measurement. In this project, we observed tunable optical and charged particle detection, and developed improved devices. With further development, the advancements described in this report could enable new capabilities for nuclear forensics applications.
The existing photofission product yield data sets are often based on nuclear models, and limited experimental measurements of these fission product yields have been performed. These experiments resulted in measured cumulative fission product yields (CFPYs) for 238 U and 232 Th for the bremsstrahlung X-ray endpoint energies of 8, 14, and 20 MeV. The half-lives of the reported fission products range from 1.07–40.8 s. This work is motivated by a demonstrated need for novel isotope production methods for nuclear forensics and improved nuclear data to support the nonproliferation community. A high-purity germanium detector and a pneumatic transfer system were employed for measurements of short-lived fission products, collecting data between cycles of accelerator irradiation and measurement.
140 La is an important isotope in nuclear forensics. It is typically paired with 140 Ba as a chronometer for dating nuclear events. Here, in this work, we report the results of two measurements performed to fully characterize the decay scheme of 140 La. The experiments were performed using the Gammasphere array at Argonne National Laboratory and the CLARION2 array at Florida State University. Sources of 140 La were produced through neutron irradiation of natural lanthanum (99.9% 139 La) in the University of Massachusetts Lowell research reactor. We identify a total of 40 transitions, three of which were not previously reported. An angular correlation analysis was conducted confirming current literature 𝐽 assignments and mixing ratios. By considering all data available in the literature, we provide new recommended values for the intensities of the strongest transitions commonly used in applications.
Galaxy Serpent is a virtual, web-based international ongoing series of tabletop exercises designed to mature the concept of National Nuclear Forensics Libraries (NNFL) and illustrate their utility in answering investigative questions or providing investigative leads as part of an investigation involving nuclear or other radioactive material (R/N) out of regulatory control (MORC). Two prior versions of the exercise have been conducted; the first utilizing surrogate data for spent nuclear fuel as the material of interest, and the second using synthetic sealed radioactive source data. Teams participating in the recently concluded third version of the exercise were provided with synthetic uranium ore concentrate (UOC) data mimicking actual data characteristics (e.g. trace element concentrations), which was used to compile a model NNFL. Teams decided how to organize and interpret the data they were provided, dealt with real world features such as missing data, and assessed discriminating attributes. Next, a hypothetical scenario involving three UOC samples found out of regulatory control was provided, and each team had to assess the self-consistency of the individual sources in the unknown data, and employ their model NNFL as a comparative assessment instrument to determine whether the three UOC materials in question were consistent with any of the types of materials in their library. In conclusion, the design of the exercise, methodologies utilized by participating teams, and aggregate results of the exercise will be presented, along with challenges encountered and benefits realized.
X-ray fluorescence (XRF) is an attractive technique for nuclear forensics applications. We evaluated a handheld, portable XRF device by applying an external radiation field (10 mR/h to 17 R/h) using two types of radiography sources: a 60 Co radiography camera to observe effects from high-energy gamma emissions and an 192 Ir radiography camera to observe effects from several low-energy gamma (0.604, 0.468, and 0.317 MeV) and decay daughter x-ray emissions. External radiation tests proved that radiation, in general, has a significant effect on the dead time or background at dose rates over 1 R/hr for both the 192 Ir and 60 Co sources.
Nuclear forensics is the collection and analysis of nuclear or radiological material to support investigations into the diversion, trafficking, or illicit activities involving materials. The goal is to link nuclear or radioactive material to people, processes, events and/or locations.
Nuclear forensics is the collection and analysis of nuclear or radiological material to support investigations into the diversion, trafficking, or illicit activities involving materials. The goal is to link nuclear or radioactive material to people, processes, events and/or locations.
We report the production of surrogate nuclear explosive debris involves the dissolution of irradiated fissile material, elemental isolation, and recombination based on required fission product ratios. Gamma-ray spectrometry is used following each step to assess the radioactive fission product inventory. A high-purity germanium detector is used to measure each sample, and the detector efficiencies are determined prior to sample measurements. Through radiochemical techniques, elements are isolated and recombined into samples with specific fission product ratios. As a result, a matrix-based approach can account for imperfect chemical separations to calculate the proper mixture volumes to obtain intended volatile-to-refractory fission product ratios, or R-values.
Better characterization of uranium compounds related to the nuclear fuel cycle is a key goal of the nuclear forensics community. Understanding the chemical behavior of these compounds in various environmental conditions and the effect on observable properties is crucial to the identification of unknown materials. Uranyl fluoride, the hydrolysis product of uranium hexafluoride, is a material of particular interest. Previous studies have suggested that uranyl fluoride may degrade upon exposure to high humidity, but the chemical pathway of degradation was previously not well understood. Our work demonstrates that uranyl fluoride undergoes a chemical reaction with water vapor to form uranyl hydroxide and peroxide species. This understanding will help guide forensic analysis in the future.
Radiation detection is necessary for isotope identification and assay in nuclear forensic applications. The principles of operation of gas proportional counters, scintillation counters, germanium and silicon semiconductor counters will be presented. Methods for calibration and potential pitfalls in isotope quantification will be described.
Pu is separated from excess U and isotopically assayed using our novel microfluidic platform designed to miniaturize traditional laboratory techniques into a field-deployable system for rapid nuclear forensics in post-detonation nuclear scenarios.
Radiochemistry has been used to study fission since it’ discovery. Radiochemical methods are used to determine cumulative mass yields. These measurements have led to the two-mode fission hypothesis to model the neutron energy dependence of fission product yields. Fission product yields can be used for the nuclear forensics of nuclear explosions. The mass yield curve depends on both the fuel and the neutron spectrum of a device. Recent studies have shown that the nuclear structure of the compound nucleus can affect the mass yield distribution.
Provide hands-on laboratory training on gamma ray spectrometry-based techniques to support a nuclear forensic investigation.
Uranium ore is mined and milled to produce uranium ore concentrate (UOC), a regulated product of the nuclear fuel cycle. Additionally, diversion of UOC from the fuel cycle into possible weapons production is a key concern in global nonproliferation efforts. As such, the ability to trace the origin of seized nuclear materials is imperative to law enforcement efforts. Although isotopic signatures of UOCs have proven fruitful to pinpoint sample provenance, new isotopic signatures are needed because most existing isotopic signatures are not indicative of the original ore body from which the U is derived. In this work, we developed a new method to separate samarium (Sm) from a U-rich sample matrix and report the first Sm isotope compositions of 32 UOCs derived from a variety of worldwide uranium mines. Relative to terrestrial standards, approximately half the UOCs have resolved and anticorrelated 149 Sm- 150 Sm isotope compositions, consistent with the capture of thermal neutrons by 149 Sm in the ore body. The UOCs with anomalous Sm isotope compositions tend to derive from older (~>1.5Ga) and higher-grade ore bodies, although other factors, such as the presence of neutron moderators like water, also play a role. Nonetheless, the Sm isotope compositions of UOCs directly reflects the neutron fluence over the history of the original ore body and can be used to discern different geologic conditions associated with that ore body. Overall, this work demonstrates the potential use of Sm isotopes as a novel nuclear forensics signature for origin assessment of UOCs.
A slide deck intended for a presentation for university students to introduce them to the concepts of nuclear forensics.
This is a slide deck intended for use in an upcoming US-UK workshop on nuclear forensics.
If a terrorist were to obtain and possibly detonate a device that contained radiological material, radiological forensic analysis of the material and source capsule could provide law enforcement with valuable clues about the origin of the radiological material; this information could then provide further leads on where the material and sealed source was obtained, and the loss of control point. This information could potentially be utilized for attribution and prosecution. Analyses of nuclear forensic signatures for radiological materials are generally understood to include isotopic ratios, trace element concentrations, the time since irradiation or purification, and morphology. Radiological forensic signatures for sealed sources provide additional information that leverages information on the physical design and chemical composition of the source capsule and containers, physical markings indicative of an owner or manufacturer. Argonne National Laboratory (Argonne), in collaboration with Idaho National Laboratory (INL), has been working since 2003 to understand signatures that could be used to identify specific source manufacturers. These signatures include the materials from which the capsule is constructed, dimensions, weld details, elemental composition, and isotopic abundances of the radioactive material. These signatures have been compiled in a library known as the Argonne/INL Radiological Sealed Source Library. Data collected for the library has included open-source information from vendor catalogs and web pages; discussions with source manufacturers and touring of production facilities (both protected through non-disclosure agreements); technical publications; and government registries such as the U.S. Nuclear Regulatory Commission’s Sealed Source and Device Registry.