Age determination of plutonium material in nuclear forensics by thermal ionisation mass spectrometry

Age is a key parameter when deducing the history of plutonium material, i.e. the plutonium produced in the nuclear reactors. This is of vital importance, when a smuggled plutonium sample has been seized and the origin has to be determined. A methodology is described which allows accurately to determine the age of plutonium material by thermal ionisation mass spectrometry using independent parent/daughter relations. This has been demonstrated for Reference Materials of known ages as well as for real samples. The already established method using gamma spectrometry is compared to this.     

Age determination of plutonium material in nuclear forensics by thermal ionisation mass spectrometry

Age is a key parameter when deducing the history of plutonium material, i.e. the plutonium produced in the nuclear reactors. This is of vital importance, when a smuggled plutonium sample has been seized and the origin has to be determined. A methodology is described which allows accurately to determine the age of plutonium material by thermal ionisation mass spectrometry using independent parent/daughter relations. This has been demonstrated for Reference Materials of known ages as well as for real samples. The already established method using gamma spectrometry is compared to this.     

Characterization of californium sources by gamma spectrometry: relevance for nuclear forensics

As part of an experimental validation of a nuclear forensics methodology for Pu source reactor-type discrimination, destructive analysis has been performed on two irradiated UO₂ pellets with different irradiation histories. Analysis has focused on measuring key Sm fission product isotope ratios used in a previously published maximum likelihood methodology to determine the most likely irradiation history of the pellets. A total of 21 Sm isotope ratios were measured within the irradiated pellets, and generally agreed within 20% of the irradiations as simulated using the Monte Carlo Radiation Transport and material depletion code, MCNP6. Results indicate the chosen approach can accurately measure the isotope ratios within 5% experimental error.

     

Development of a data-mining methodology for spent nuclear fuel forensics

The purpose of this study is to categorize the type of spent nuclear fuels using simulation data-based classification methods. Considering the practical conditions making the full analysis of radioactive nuclides difficult, the classification methods were designed to be robust to noise and missing information. The strength and weakness of three classifiers, linear discriminant analysis, quadratic discriminant analysis and support vector classification were compared, which is developed by the history information such as burnup, enrichment, and cooling type generated from ORIGEN-ARP upon fuel assembly types. Auto-Associative Kernel Regression improved outlier management as a pre-processing technique.     

Development of a data-driven classification algorithm for fresh nuclear fuel forensics

Journal of Radioanalytical and Nuclear Chemistry - According to the Incident and Trafficking Database of the International Atomic Energy Agency, incidents involving illegal transactions or...     

Monte Carlo analysis of thermochromatography as a fast separation method for nuclear forensics

Nuclear forensic science has become increasingly important for global nuclear security, and enhancing the timeliness of forensic analysis has been established as an important objective in the field. New, faster techniques must be developed to meet this objective. Current approaches for the analysis of minor actinides, fission products, and fuel-specific materials require time-consuming chemical separation coupled with measurement through either nuclear counting or mass spectrometry. These very sensitive measurement techniques can be hindered by impurities or incomplete separation in even the most painstaking chemical separations. High-temperature gas-phase separation or thermochromatography has been used in the past for the rapid separations in the study of newly created elements and as a basis for chemical classification of that element. This work examines the potential for rapid separation of gaseous species to be applied in nuclear forensic investigations. Monte Carlo modeling has been used to evaluate the potential utility of the thermochromatographic separation method, albeit this assessment is necessarily limited due to the lack of available experimental data for validation.     

Identification of uranium signatures relevant for nuclear safeguards and forensics

The paper describes the applicability of different characteristics (signatures) in nuclear safeguards and forensics for assessment of uranium material provenance in terms of production process. The study follows a uranium ore concentrate production from an ore to a U₃O₈ product. It turned out that rare-earth elemental pattern, radiochronometry (age of ore body and material production date), sulphur and organic impurities are useful to find out the origin or history of the material, while certain trace-elements and isotopics of Pb or Sr were found to be inconclusive. The results will be important to understand the signatures in nuclear safeguards and forensics.     

A highly-enriched 244Pu reference material for nuclear safeguards and nuclear forensics measurements

Journal of Radioanalytical and Nuclear Chemistry - A highly-enriched 244Pu isotope dilution reference material has been prepared and characterized for metrologically traceable measurements of very...     

Environmental monitoring as an important tool for safeguards of nuclear material and nuclear forensics

Summary The use of environmental monitoring as a technique to identify activities related to the nuclear fuel cycle has been proposed by international safeguards organizations. The elements specific for each kind of nuclear activity, or “nuclear signatures”, inserted in the ecosystem can be intercepted by different live organisms. This work demonstrates the technical viability of using pine needles as bioindicators of nuclear signatures associated with uranium enrichment activities. Additionally, it proposes the use of HR-ICP-MS to identify the signature corresponding to that kind of activities in the ecosystem. Nitric acid solutions, used to wash pine needles sampled near nuclear facilities and containing only 0.1 mg ^. kg^-1 of uranium, exhibit a n(²³⁵U)/n(²³⁸U) isotopic abundance ratio of 0.0092±0.0002, while solutions originated from samples collected at places located more than 200 km far from activities related to the nuclear fuel cycle exhibit a value of 0.0074±0.0002. Similar results were obtained for sample solutions prepared using the acid leaching process. The different values of n(²³⁵U)/n(²³⁸U) isotopic abundance ratio obtained permit to confirm the presence of anthropogenic uranium and demonstrate the viability of using the methodology proposed in this work.     

Evaluating uranium radiochronometry by single-collector mass spectrometry for nuclear forensics: a multi-instrument investigation

Radiochronometric data, a key signature in evaluating the provenance and process history of nuclear material out of regulatory control, are conventionally acquired via multi-collector mass spectrometry. Here we explore the potential of age-dating by single-collector mass spectrometry. To evaluate model age accuracy/precision across different instrument designs, we performed ²³⁰Th–²³⁴U and ²³¹Pa–²³⁵U radiochronometry of CRM 125-A using two single-collector and one multi-collector plasma source mass spectrometers. Single-collector instruments produce accurate model ages for this uranium standard and thus hold promise for nuclear forensics radiochronometry. Increased acquisition of age information via multiple instrument designs will bolster the global response to nuclear interdictions.

     

Nuclear forensics: searching for nuclear device debris in trinitite-hosted inclusions

This study documents the 3D morphology of trinitite-hosted metallic inclusions and the first observations of alloys consisting primarily of Pb, Ta, Ga, and W. Scanning electron and backscatter electron imaging, as well as energy dispersive X-ray spectra chemical composition data are reported for heavy metal inclusions in 14 different samples of trinitite. Inclusions consisting of Fe?CTi?CSi are the most abundant and presumably derived predominantly from the explosion tower. Grains of Cu, Pb, Ta?+?Ga?+?W were also observed and are likely derivatives of the trinitite device wiring, tamper, and tamper and core, respectively. Additionally, a Ba-rich grain and multiple zircons (ZrSiO₄) were observed in a large majority of samples. The spherical morphology and the ubiquitous positioning of the heavy metal inclusions on the crater walls of the glassy trinitite surfaces indicate a two-step formation. Stage one involves formation of the glassy trinitite, while the second stage involved the precipitation of the inclusions that were incorporated onto the surface of the trinitite. Furthermore, the precarious positioning of these inclusions further emphasizes the need for analysis using non-destructive techniques prior to methods employing a bulk sample digestion approach.     

Activation analysis of Se in biological samples through75Se and77mSe

A method is described to separate trace amounts of selenium in biological samples without using a carrier. This method is based on the adsorption on active carbon of the complex ion formed with APDC /ammonium salt of l-pyrrolidine carbodithioic acid/ at pH 1. The efficiency of the radiochemical separation described is measured by using carrier-free⁷⁵Se labelled solutions of sodium selenite at selenium concentrations from 3.5×10^–8 to 3.5×10^–11 g ml^–1. The results were between 95% and 98% with statistical variations from 2% to 10%. The determination of selenium can be made following this separation either through⁷⁵Se in the traditional way, or through^77mSe if the separation is performed prior to irradiation. The detection limits on the available conditions were 0.01 ppm for⁷⁵Se and 0.1 ppm for^77mSe. When the analysis is performed through⁷⁵Se /t=120 d/, the statistical error is notably smaller because the counting time may be considerable, whereas through^77mSe/t=17.5 s/it is higher than 20%, depending on the concentration and the available neutron flux. However, the advantages of gaining time and the fact of performing the trace separation from a non radioactive material, make both procedures competitive as useful tools for the research on the function of Se in vertebrates.     

Determination of Q 0 and k 0 factors for 75Se

Since the initial determination of the Q ₀ and k ₀ factors for ⁷⁵Se systematic errors in Se determination in various matrices have been noticed by several users of the k ₀ method. A number of publications have been made on this subject, resulting in different k ₀ and Q ₀ values for this radio-isotope. This work consists of a re-determination of Q ₀ and k ₀ values for ⁷⁵Se using the bare and Cd-ratio methods making use of three different irradiation channels from the BR1 reactor. For this re-determination three different kinds of standards were used: a pure Se powder standard, an ICP standard solution and pure Se shots. Results were compared with previously published literary data. Differences in k ₀ with the official published data ranging from 3.5 to 12 % were observed and potential reasons for this discrepancy are discussed. A good consistency with recent work was found. The impact on recent certification and intercomparison exercises demonstrates the effectiveness of the newly proposed values.     

A rapid dissolution procedure to aid initial nuclear forensics investigations of chemically refractory compounds and particles prior to gamma spectrometry

A rapid and effective preparative procedure has been evaluated for the accurate determination of low-energy (40–200 keV) gamma-emitting radionuclides (²¹⁰Pb, ²³⁴Th, ²²⁶Ra, ²³⁵U) in uranium ores and uranium ore concentrates (UOCs) using high-resolution gamma ray spectrometry. The measurement of low-energy gamma photons is complicated in heterogeneous samples containing high-density mineral phases and in such situations activity concentrations will be underestimated. This is because attenuation corrections, calculated based on sample mean density, do not properly correct where dense grains are dispersed within a less dense matrix (analogous to a nugget effect). The current method overcomes these problems using a lithium tetraborate fusion that readily dissolves all components including high-density, self-attenuating minerals/compounds. This is the ideal method for dissolving complex, non-volatile components in soils, rocks, mineral concentrates, and other materials where density reduction is required. Lithium borate fusion avoids the need for theoretical efficiency corrections or measurement of matrix matched calibration standards. The resulting homogeneous quenched glass produced can be quickly dissolved in nitric acid producing low-density solutions that can be counted by gamma spectrometry. The effectiveness of the technique is demonstrated using uranium-bearing Certified Reference Materials and provides accurate activity concentration determinations compared to the underestimated activity concentrations derived from direct measurements of a bulk sample. The procedure offers an effective solution for initial nuclear forensic studies where complex refractory minerals or matrices exist. It is also significantly faster, safer and simpler than alternative approaches.     

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 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 raw stock borosilicate container glass up to 70 days after gamma ray, X-ray, beta particle or ultraviolet irradiations at doses from 0.15 to 20 Gy. Two main 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 is 0.15 Gy, which is roughly equivalent to a 24 h irradiation at 1 cm from a 50 ng ⁶⁰Co source. As a result of fading, this dose would be detectable for approximately 1 year post-irradiation. In a more detailed analysis, the TL glow curves were separated into five peaks centered near 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. This suggests that mechanisms controlling radiation induced defect formation from gamma, beta, X-ray, and UV sources may be similar.     

Radioanalytical chemistry for nuclear forensics in China: Progress and future perspective

A relatively new branch of science-nuclear forensics, aiming at providing the nature, origin, history and possible trafficking route of seized nuclear materials/devices, has been established and rapidly developed over decades to screen illicit nuclear activities. This highly interdisciplinary science is built upon a foundation of analytical chemistry, radiochemistry, nuclear physics, material sciences, geology, and other scientific disciplines, within which radiochemical methodologies and radioa...     

Study of a neutron radiography system using Cf neutron source

This paper presents a study about moderation and collimation of a neutron radiography system using ²⁵²Cf. A Monte Carlo Code, MCNP4B, has been used to obtain a maximum and more homogeneous thermal neutron flux in the collimator outlet next to the image plane. Among the various moderator materials investigated, high density polyethylene proved to be the most efficient, with a thermalization factor of 56 cm². Using a collimator design assembly it was possible to obtain a normalized thermal neutron flux, at the image plane of 6×10⁻⁶ n cm⁻² s⁻¹ at an effective collimator ratio of 7.5, or 3.2×10⁻⁷ n cm⁻² s⁻¹ at an effective collimator ratio of 50.     

Determination of the optical purity of L-selenomethionine-75Se

The method developed for the determination of the optical purity of L-selenomethionine-⁷⁵Se is based on the conversion of the mixture of L-and D-amino acids into the diastereoisomeric derivatives by reaction with (−)-camphorsulphonyl chloride. The diastereoisomeric derivatives are separated by means of thin layer chromatography. From the ratio of the radioactivities of the two spots on the chromatogram, the optical purity is calculated, and given in % D. For a sample of L-methionine-¹⁴C the following value was found: 0.53±0.05 (S.D. of mean, n=7). For a sample of DL-methionine-¹⁴C the percentage of D found, was: 48.5±0.5 (S. D. of mean, n=7). Of 30 different samples of L-selenomethionine-⁷⁵Se the percentages of D-isomer were determined in duplicate. From the 30 differences between duplicates the S. D. of a single measurement is calculated to be 0.2.