Uranium isotopic composition can provide valuable information about the history and provenance of a nuclear material; therefore, uranium isotopic analyses are frequently made in the nuclear ...forensics, safeguards, and environmental monitoring communities. These measurements have always presented challenges due to the extreme variability in the relative abundance between the major (235U, 238U) and minor (233U, 234U, 236U) isotopes of uranium. The recently developed ATONA (Atto- to Nano-Amp) amplification system paired with Faraday cup detectors has a large dynamic range and low noise floor making it ideal for measuring uranium isotopic ratios in materials of both natural and anthropogenic origin. A wide variety of certified reference materials were analyzed to investigate the utility of the ATONA amplification system for determining uranium isotopic composition in samples ranging from depleted to highly enriched. The ATONA amplifiers provide nearly an order of magnitude improvement in external reproducibility over 1011 Ω amplifiers when measuring the minor 234U/238U ratio in isotopically natural and depleted samples and when paired with a secondary electron multiplier can measure very low relative abundance uranium isotopes (i.e., 236U).
The Washington State University TRIGA reactor was modeled in the SCALE system’s KENO neutron transport code. The model includes 119 fuel rods, a central boral control rod, 4 control blades, 5 ...irradiation ports, and 20 graphite reflector blocks within a rectangular aluminum grid box. The model accurately simulated the irradiation of depleted uranium and highly enriched uranium foils and predicted reaction rate ratios for
238
U(n,2n)
237
U /
238
U(n,
γ
)
239
U and
99
Mo / fission, which compared favorably to empirical values previously measured at Los Alamos. Finally, a sensitivity/uncertainty analysis was performed using the continuous-energy TSUNAMI-3D module of SCALE.
In the course of the Fukushima nuclear accident, radionuclides were released in various forms, including so-called radiocesium-bearing microparticles (CsMP). So far, four types of CsMP were ...described: Type A is smaller in size (< 10 μm), Types B, C, and D are larger (> 100 μm). In this work, we present a novel type of CsMP (proclaimed Type E). Three particles of Type E were extracted from a contaminated blade of grass that was sampled 1.5 km from the Fukushima Daiichi nuclear power plant in late 2011. They were located using autoradiography, isolated using an optical microscope and micromanipulator, and characterized using scanning electron microscopy, energy dispersive x-ray spectroscopy, and low-level gamma-ray spectrometry. Type E CsMPs are 10–20 μm in size and exhibit an unusually low and barely detectable
137
Cs activity of only ≤ 10 mBq per particle. Their brittle and fragile character may indicate a high surface tension.
We report results of precise and sensitive mass spectrometric measurements of uranium, plutonium, neptunium, and americium concentrations and isotope ratios in a variety of environmental reference ...materials. Most of our work has been done on NIST SRM 4350b, River Sediment, but we also present results for NIST SRM 4354, Lake Sediment; NIST SRMs 4355 and 4355a, Peruvian Soil; NIST SRM 4357, Ocean Sediment; NIST SRM 1648a, Urban Particulate Material; NIST SRM 1649b, Urban Dust; IAEA CRM 385, Ocean Sediment; USGS BCR-2, Columbia River Basalt; and USGS BHVO-2, Hawaiian Volcanic Observatory Basalt. These materials reflect a wide range in long-lived actinide concentrations (e.g. 1E4 to 1E10 atoms 239Pu/g) and isotope ratios. Measurements were performed in a clean laboratory by isotope dilution, multi-collector thermal ionization and multi-collector inductively coupled plasma mass spectrometry. In general, our results are in agreement with, but lower the uncertainty of, literature or certificate values for these reference materials. Our uranium results for the basalts also confirm previously reported high-precision mass spectrometric results from our laboratory. In many cases our measurements of U-Pu-Np-Am nuclides appear to be novel.
Extensive results for NIST SRM 4350b, River Sediment, indicate that this material is heterogeneous for Pu-Np-Am concentrations and isotope ratios at a sample size of 5 g or lower. Pu–Np isotope ratios and a241Pu-241Am model age of 1954 reflect a mix of plutonium production operations at the nearby Hanford, Washington site, and global atmospheric fallout from nuclear weapons testing. Results for the oceanic sediment materials (NIST SRM 4357 and IAEA 385) collected near Sellafield, U.K. vary but are also indicative of local anthropogenic sources of varying Pu isotopic composition and a mean 241Pu-241Am model age of 1964. Large environmental fractionation between Pu and Np is observed for the ocean, river, and lake sediment reference materials. Novel measurements for the two air particulate SRMs indicate high U, Pu and Np concentrations for these collections in 1976–1977 with an anomalous regional fallout Pu isotopic signature. Results for BHVO-2 and other Hawaiian basalts indicate that those which erupted before or during the period of abundant atmospheric nuclear weapons testing (1950–1970) contain significant levels of Pu (on the order of 1E7 atoms 239Pu/g) with a global fallout Pu isotopic composition, compared to more recent eruptions which incorporated less Pu. Hence, Hawaiian basalts may provide an integrated temporal record of anthropogenic actinide fallout deposition from the atmosphere since eruption.
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•Improved and novel data for long-lived U-Pu-Np-Am nuclides are presented.•Data uncertainties are greatly reduced for many reference materials.•Isotopic fingerprinting and Pu–Am model ages of actinide sources are provided.•Large Pu–Np environmental fractionation is observed for many materials.•Hawaiian basalts may provide a temporal record of actinide fallout deposition.
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 237Np 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 237Np. 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.
Particulate isotopic analysis in nuclear forensics has developed rapidly during the past two decades due to technical advances in determining the isotopic composition of individual particles. This ...paper introduces basic statistical concepts that can be applied by analysts to understand the importance of statistical adequacy when interpretating particle data. While these basic statistical methods provide a useful point-of-entry to particle data analysis, more sophisticated statistical and modeling approaches are needed to extract maximal information from such datasets in the future.
The accurate interpretation of uranium metal
230
Th/
234
U and
231
Pa/
235
U radiochronometry model ages requires an understanding of how uranium parent nuclides and decay progeny (
230
Th and
231
...Pa) behave during uranium metal casting. In order to directly measure the spatial distribution of
230
Th and
231
Pa in uranium metal before and after vacuum induction melting (VIM), Los Alamos National Laboratory identified uranium metal feedstock, characterized the metal feedstock, conducted a controlled casting experiment of an approximately 120 kg uranium metal rod, and characterized the cast metal. This study presents radiochronometry results and quantified
230
Th and
231
Pa VIM separation factors from bulk uranium.
Foraging behaviour of marine top predators is increasingly being used to identify areas of ecological importance. This is largely enabled by the ability of many such species to forage extensively in ...search of prey that is often concentrated in oceanographically productive areas. To identify important habitat in the Southern Indian Ocean within and around South Africa's Prince Edward Islands' Marine Protected Area (MPA), satellite transmitters were deployed on 12 lactating Subantarctic fur seals Arctocephalus tropicalis at Prince Edward Island (PEI) itself. Switching state space models were employed to correct ARGOS tracks and estimate behavioural states for locations along predicted tracks, namely travelling or area restricted search (ARS). A random forest model showed that distance from the study colony, longitude and distance from the Subantarctic Front were the most important predictors of suitable foraging habitat (inferred from ARS). Model-predicted suitable habitat occurred within the MPA in relatively close access to the colony during summer and autumn, but shifted northwards concurrently with frontal movements in winter and spring. The association of ARS with the MPA during summer-autumn was highly significant, highlighting the effectiveness of the recently declared reserve's design for capturing suitable foraging habitat for this and probably other marine top predator species.
The NansClim project (2010–2013) represented a regional collaboration to assess the effects of climate on Benguela dynamics. Based on in situ (since the 1960s in Namibia and South Africa and 1985 in ...Angola) and satellite (since the 1980s) observations, the project focussed on four subsystems, namely the Angola subtropical, northern Benguela upwelling, southern Benguela upwelling and Agulhas Bank. This contribution summarizes the findings for selected key questions, ranging from changes in the physico‐chemical habitats, plankton, pelagic and demersal fish communities, to cross‐cutting evaluation at subsystem and regional scales. The results underline the overriding importance to of considering the combined effects of climate and fishing as drivers of the dynamics of the ecosystem components. Each subsystem currently continues to function largely as a separate entity as described in earlier reviews. However, some changes have been observed across several subsystems, e.g., a coherent shift from one relatively stable period to another occurred in the northern and southern Benguela in the mid‐1990s. Future climate change could weaken the boundaries between the four subystems. The findings underline the need for continued regional research collaboration and regional surveys focussed at ecosystem, rather than resource, assessment. Our conclusions include implications for ecosystem‐based fisheries management, and recommendations for future regional research.
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