Radionuclide Signatures Research Articles

Analysis of environmental radioxenon detections in the UK

Radioxenon activity concentrations are monitored globally using the International Monitoring System (IMS) of the Comprehensive Nuclear-Test-Ban Treaty Organisation, improving the monitoring community's ability to detect radionuclide signatures from an underground nuclear test (UNT). An IMS-like noble gas system is in operation at AWE (Aldermaston, UK) and can collect and measure radioxenon isotopes in environmental air samples. When operated in this mode, data produced is analysed at the UK National Data Centre (NDC) and significant detection events are flagged for further investigation. This work discusses a number of significant detection events analysed using the operational system deployed at the UK NDC, which includes atmospheric transport simulations and a real-time stack-monitoring data feed from the nearest medical isotope production facility in Belgium. A comparison of the expected radionuclide contributions with measured detections is presented, including a comparison of the isotopic ratios for the radioxenon isotopes of interest (133Xe, 131mXe, 133mXe, 135Xe).

Radiological Scouting, Monitoring and Inspection Using Drones.

Human populations and natural ecosystems are bound to be exposed to ionizing radiation from the deposition of artificial radionuclides resulting from nuclear accidents, nuclear devices or radiological dispersive devices (“dirty bombs”). On the other hand, Naturally Occurring Radioactive Material industries such as phosphate production or uranium mining, contribute to the on site storage of residuals with enhanced concentrations of natural radionuclides. Therefore, in the context of the European agreements concerning nuclear energy, namely the European Atomic Energy Community Treaty, monitoring is an essential feature of the environmental radiological surveillance. In this work, we obtain 3D maps from outdoor scenarios, and complete such maps with measured radiation levels and with its radionuclide signature. In such scenarios, we face challenges such as unknown and rough terrain, limited number of sampled locations and the need for different sensors and therefore different tasks. We propose a radiological solution for scouting, monitoring and inspecting an area of interest, using a fleet of drones and a controlling ground station. First, we scout an area with a Light Detection and Ranging sensor onboard a drone to accurately 3D-map the area. Then, we monitor that area with a Geiger–Müller Counter at a low-vertical distance from the ground to produce a radiological (heat)map that is overlaid on the 3D map of the scenario. Next, we identify the hotspots of radiation, and inspect them in detail using a drone by landing on them, to reveal its radionuclide signature using a Cadmium–Zinc–Telluride detector. We present the algorithms used to implement such tasks both at the ground station and on the drones. The three mission phases were validated using actual experiments in three different outdoor scenarios. We conclude that drones can not only perform the mission efficiently, but in general they are faster and as reliable as personnel on the ground.

Unveiling the provenance of sediments in the moraine complex of Aldegonda Glacier (Svalbard) after glacial retreat using radionuclides and elemental fingerprints

In the changing glacierized areas of the maritime Arctic region, fluxes of sediments are of high intensity during the Arctic melting season. On the Western Spitsbergen Island around Grønfjord, several glaciers have declined rapidly over the last century. The Aldegonda Glacier has retreated about 2 km since 1911 when the glacier tongue reached the seashore which lead to new exposed surfaces in the proglacial area supplying sediments to the fjord during the arctic summer. We explored if the geochemical signature of sediments can be used to discriminate sediment provenance in proglacial environments during different stages of the melting season. To this purpose a sampling campaign was undertaken in July 2015 in the Aldegonda Glacier area, to obtain 24 composite surface samples of moraine materials and sediments at the glacier surface and 12 sediment mixtures. Fingerprinting techniques were applied to determine the sediment provenance and tracers were selected using a novel conservative index and consensus ranking method. FingerPro model identified bottom moraines as predominant source in all cases (74%), recent moraines amounted to 15% and sediment on ice contributed 11%. Radionuclide signatures were of great value to identify sediment provenance, and 137Cs and 210Pbex were among the most selected tracers. Variations in source contributions depended on the location and type of the sediment mixtures. Differences in source contributions also varied temporarily suggesting different sediment mobilization processes during snow and ice melt. Snow and ice melt are the main drivers of sediment mobilization contributed from moraines during summer. Moreover, sediments accumulated on the glacier surface including cryoconite, deliver radionuclides and heavy metals associated to fine particles that have an impact on terrestrial and sea arctic ecosystems. Such deleterious impact could be one main effect of climate change on glacierized environments worldwide.

Expectation-propagation for weak radionuclide identification at radiation portal monitors

We propose a sparsity-promoting Bayesian algorithm capable of identifying radionuclide signatures from weak sources in the presence of a high radiation background. The proposed method is relevant to radiation identification for security applications. In such scenarios, the background typically consists of terrestrial, cosmic, and cosmogenic radiation that may cause false positive responses. We evaluate the new Bayesian approach using gamma-ray data and are able to identify weapons-grade plutonium, masked by naturally-occurring radioactive material (NORM), in a measurement time of a few seconds. We demonstrate this identification capability using organic scintillators (stilbene crystals and EJ-309 liquid scintillators), which do not provide direct, high-resolution, source spectroscopic information. Compared to the EJ-309 detector, the stilbene-based detector exhibits a lower identification error, on average, owing to its better energy resolution. Organic scintillators are used within radiation portal monitors to detect gamma rays emitted from conveyances crossing ports of entry. The described method is therefore applicable to radiation portal monitors deployed in the field and could improve their threat discrimination capability by minimizing “nuisance” alarms produced either by NORM-bearing materials found in shipped cargoes, such as ceramics and fertilizers, or radionuclides in recently treated nuclear medicine patients.

Pavement alters delivery of sediment and fallout radionuclides to urban streams

Sediment from urban impervious surfaces has the potential to be an important vector for contaminants, particularly where stormwater culverts and other buried channels draining large impervious areas exit from underground pipes into open channels. To better understand urban sediment sources and their relation to fallout radionuclides, we collected samples of rainfall, urban sediment (pavement sediment, topsoil), streambank sediment, and fluvial sediment (suspended sediment and bed sediment) for 7Be, 210Pbex, and 137Cs analysis. The results indicate that each rainfall event tags pavement sediment with elevated activities of 7Be and 210Pbex such that runoff from impervious surfaces in the buried channel part of the stream network contains the highest activities. Pavement sediment, because it is characteristically a thin veneer, has a small mass to rainwater ratio resulting in a greater tagging of 7Be and 210Pbex activity than does topsoil on a per gram basis. An unmixing model indicated that suspended-sediment samples collected at the culvert outlet from the buried-channel network are from pavement sediment sources (45 ± 25%) with a smaller component of topsoil (22 ± 19%), and a component from streambanks (32 ± 35%) that we infer to be older channel material and subsoil eroded from within the culvert system. Downstream from the culvert, suspended sediment collected from the open-channel parts of the stream had 7Be and 210Pbex activities that were substantially reduced by the contribution of sediment from streambanks (57 ± 15%), with pavement contributions decreasing to 15 (±9%) and topsoil contributing 28 (±7%). The results highlight the utility of 7Be, 210Pbex, and 137Cs as tracers of urban sediment sources, resulting in a unique radionuclide signature for urban watersheds compared to other sediment-source settings.

The detectability of the Wigwam underwater nuclear explosion by the radionuclide stations of the International Monitoring System

The Comprehensive Nuclear-Test-Ban Treaty (CTBT) bans all nuclear explosions, including those detonated from an underwater nuclear explosion. To improve the understanding of the radionuclide signatures of such an event, and whether it would be detectable under the verification regime of the CTBT, the 1955 Wigwam underwater nuclear explosive test has been modelled. Inventory calculations and atmospheric transport modelling has been performed to estimate the activity at the radionuclide stations (RN) of the International Monitoring System (IMS). This has utilized reported release values (0.92%) and meteorological data from the event. The research shows that there is a high probability that Wigwam would have been detectable at U.S. IMS stations at Wake Island (RN77) at 8.4 d, Upi, Guam (RN80) at 10.7 d and Sand Point, AK (RN71) at 13.7 d. At these locations, the majority of IMS relevant radionuclides were fission products, such that additional radionuclides from the seawater activation had largely decayed before reaching the stations.

Subsurface sources contribute substantially to fine‐grained suspended sediment transported in a tropical West African watershed in Burkina Faso

AbstractIncreasing watershed sediment yields is an important problem in Africa, but the sources of these sediment yields have only very rarely been investigated. This study therefore aims to discriminate subsurface and surface sources of fine‐grained sediments in a representative mesoscale (580 km2) West African savanna watershed. We used a sediment source fingerprinting approach for source apportionment including geochemical and radionuclide (137Cs, 210Pbex, and 7Be) composite signatures where 7Be was used as a tracer for the first time in the African environment. Two field campaigns were conducted collecting a total of 258 geochemical and 66 isotope samples. We found that subsurface source categories, dominantly river bank, contributed an unexpected high share of 43% (geochemistry) and 45% (radionuclides) to the sampled fine‐grained sediments. Pairwise comparison of the averaged frequency distributions for predicted source proportions using five geochemical signatures with the frequency distribution generated using the single radionuclide signature suggested that the two distributions are not statistically different. Extrapolating our measured contribution of subsurface erosion to areas with similar yields in comparable environmental settings, we can assume that subsurface sources are an important component of sediment loss across large areas of West Africa. Subsurface erosion, primarily associated with bank rather than gully erosion, is likely to increase in the future with projected rises in run‐off due to land use and climate change. Source tracing studies need to be undertaken more widely across Africa to help mitigation planning for sediment‐related and land degradation problems.

Xenon adsorption on geological media and implications for radionuclide signatures

The detection of radioactive noble gases is a primary technology for verifying compliance with the pending Comprehensive Nuclear-Test-Ban Treaty. A fundamental challenge in applying this technology for detecting underground nuclear explosions is estimating the timing and magnitude of the radionuclide signatures. While the primary mechanism for transport is advective transport, either through barometric pumping or thermally driven advection, diffusive transport in the surrounding matrix also plays a secondary role. From the study of primordial noble gas signatures, it is known that xenon has a strong physical adsorption affinity in shale formations. Given the unselective nature of physical adsorption, isotherm measurements reported here show that non-trivial amounts of xenon adsorb on a variety of media, in addition to shale. A dual-porosity model is then discussed demonstrating that sorption amplifies the diffusive uptake of an adsorbing matrix from a fracture. This effect may reduce the radioxenon signature down to approximately one-tenth, similar to primordial xenon isotopic signatures.

240+239Pu depositional signatures as a viable geochronological tool in the Amazon Basin

Abstract Anthropogenic radionuclide signatures associated with nuclear testing are increasingly utilized in environmental science to explore recent sedimentation. In this study, we assess the suitability of Pu radioisotope analysis in floodplain lake environments in the Amazon Basin to form geochronologies during the 20th century. The 240Pu + 239Pu (240+239Pu) signatures in six sediment cores indicate sediment accumulation rates in the floodplain lakes of the major rivers; Amazon (2.3 mm year-1), Tapajos (10.2 and 2.4 mm year-1) and Madeira (3.4, 4.2 and 6.2 mm year-1). The results from this study show that 240+239Pu fallout activities, and the well documented (240Pu/239Pu) atomic ratios of the above ground nuclear tests which began in the 1950’s, are sufficient and well preserved in Amazon floodplain lake sediments to infer chronologies. Lead-210 dating analyses in the same sediment cores produced comparable sediment accumulation rates at three of the six sites. The differences between dating methods may be attributed to the different time scale these dating methods represent and/or in the solubility between Pb and Pu along the sediment column. The geochronologies derived from the 240+239Pu and 210Pb dating methods outlined in this work are of interest to identify the effects of changing sediment accumulation rates during the previous century as a result of development, including deforestation, along the Amazon Basin which increased towards the middle of the 20th century. This study shows that Pu dating provides a viable alternative geochronology tool for recent sediment accumulation (previous ~60 years) along the Amazon Basin.

Evaluation of gamma-spectrometry equipment for on-site inspection

An On-site Inspection (OSI) is an important component of the verification regime of the Comprehensive Nuclear-Test-Ban Treaty (CTBT), with the objective of gathering evidence of a possible Treaty violation. This includes the use of gamma-spectrometry equipment to identify 17 particulate radionuclides that are indicative of a nuclear explosion. This research provides an evaluation of high- (germanium), medium- (cadmium zinc telluride) and low-resolution (sodium iodide and lanthanum bromide) detectors using modelled radionuclide signatures from a nuclear explosion and Monte Carlo simulations of a detector response. The complex radionuclide signatures are shown to only be distinguishable using a high-resolution system for 1 week and 1 year post-detonation cases.

Quantifying radionuclide signatures from a γ–γ coincidence system

A method for quantifying gamma coincidence signatures has been developed, and tested in conjunction with a high-efficiency multi-detector system to quickly identify trace amounts of radioactive material. The γ–γ system utilises fully digital electronics and list-mode acquisition to time–stamp each event, allowing coincidence matrices to be easily produced alongside typical ‘singles’ spectra. To quantify the coincidence signatures a software package has been developed to calculate efficiency and cascade summing corrected branching ratios. This utilises ENSDF records as an input, and can be fully automated, allowing the user to quickly and easily create/update a coincidence library that contains all possible γ and conversion electron cascades, associated cascade emission probabilities, and true-coincidence summing corrected γ cascade detection probabilities. It is also fully searchable by energy, nuclide, coincidence pair, γ multiplicity, cascade probability and half-life of the cascade. The probabilities calculated were tested using measurements performed on the γ–γ system, and found to provide accurate results for the nuclides investigated. Given the flexibility of the method, (it only relies on evaluated nuclear data, and accurate efficiency characterisations), the software can now be utilised for a variety of systems, quickly and easily calculating coincidence signature probabilities.

Plutonium release from Fukushima Daiichi fosters the need for more detailed investigations

The contamination of Japan after the Fukushima accident has been investigated mainly for volatile fission products, but only sparsely for actinides such as plutonium. Only small releases of actinides were estimated in Fukushima. Plutonium is still omnipresent in the environment from previous atmospheric nuclear weapons tests. We investigated soil and plants sampled at different hot spots in Japan, searching for reactor-borne plutonium using its isotopic ratio 240Pu/239Pu. By using accelerator mass spectrometry, we clearly demonstrated the release of Pu from the Fukushima Daiichi power plant: While most samples contained only the radionuclide signature of fallout plutonium, there is at least one vegetation sample whose isotope ratio (0.381 ± 0.046) evidences that the Pu originates from a nuclear reactor (239+240Pu activity concentration 0.49 Bq/kg). Plutonium content and isotope ratios differ considerably even for very close sampling locations, e.g. the soil and the plants growing on it. This strong localization indicates a particulate Pu release, which is of high radiological risk if incorporated.

Reinforced evidence of a low-yield nuclear test in North Korea on 11 May 2010

In May 2010 unique aerosol-bound and noble gas (xenon) radionuclide signatures were observed at four East Asian surveillance stations designed to detect evidence of nuclear testing. An article published in early 2012 provided an analysis that suggested the findings were due to a low-yield underground nuclear test in North Korea on 11 May 2010. As the aerosol and noble gas datings, however, only agreed on the fringes of their uncertainties an official North Korean telegram that on 12 May 2010 reported about a nuclear fusion experiment 1 month earlier inspired a solution. Assuming that included a low-yield nuclear explosion and that it had left xenon isotopes in the same cavity, the xenon dating could be “moved” to overlap with the aerosol dating. The article stirred a serious controversy where representatives of the U.S. government and the Comprehensive Nuclear-Test-Ban Treaty Organization (CTBTO) refused to comment on it. In this paper the xenon dating agrees with the aerosol one without resorting to a previous explosion. It shows instead that fractionation during lava cooling is the explanation and how that plays a paramount role in how xenon signatures from underground nuclear explosions should be interpreted. It also presents new observations that effectively imply that no nuclear reactor or any other nuclear installation could have caused the May 2010 signals. All in all these are the most interesting and rich ones ever encountered by the Organization and they truly demonstrate that the verification system can deliver much better sensitivity than it was originally designed for.

Pareto-Optimal Gamma Spectroscopic Radionuclide Identification Using Evolutionary Computing

Detection and identification of special nuclear materials (SNM) in measured gamma spectra is a challenge for nuclear security applications of spectroscopy. There are ongoing international efforts in industry, academia, and government to develop accurate, robust automated methods of gamma spectroscopic analysis to identify signature patterns characteristic of SNM. In this paper, we introduce a new approach for processing gamma-ray spectra measured by an NaI detector. The approach searches for radionuclide signature patterns in the measured spectrum by formulating a multiobjective optimization problem. Search in the multiobjective space is performed by an evolutionary algorithm, which identifies a solution in the context of Pareto Optimality Theory. The proposed approach is composed of two main steps: 1) signature selection, and 2) Pareto-optimal fitting. The output of the algorithm includes a list of all the identified radionuclides and their relative contributions to the gamma spectrum. The methodology is applied to a set of gamma spectra and compared to multiple linear regression fitting. Results demonstrate the superiority of the Pareto-optimal approach over multiple regression in the majority of the tested cases.

Radionuclide Evidence for Low-Yield Nuclear Testing in North Korea in April/May 2010

Between 13 and 23 May 2010, four atmospheric radionuclide surveillance stations, in South Korea, Japan, and the Russian Federation, detected xenon and xenon daughter radionuclides in concentrations up to 10 and 0.1 mBq/m3 respectively. All these measurements were made in air masses that had passed over North Korea a few days earlier. This article shows that these radionuclide observations are consistent with a North Korean low-yield nuclear test on 11 May 2010, even though no seismic signals from such a test have been detected. Appendix 1 presents a detailed analysis of the radioxenon data and Appendix 2 describes a hypothetical nuclear test scenario consistent with this analysis, including the possibility that the test used uranium-235 rather than plutonium-239. The analysis suggests that the technical and analytical basis to detect small nuclear tests using radionuclide signatures may be more developed than is generally assumed.

Assinatura da deposição atmosférica de testes nucleares em sedimentos da costa brasileira (240+239Pu e 137Cs)

The aim of this review is to take a look at Cold War era nuclear tests signatures found in Brazilian coastal sediments. Both 137Cs and 240+239Pu signatures have been documented in mangrove, coastal mudflats and continental shelf sediments, associated with above ground nuclear tests beginning in the 1950's. The dates associated to the anthropogenic radionuclide signatures 137Cs and 240+239Pu along sediment columns are confirmed by 210Pb geochronology in many of the studies highlighted in this review. The results outlined in this review characterize the extent to which nuclear fallout products reach the Brazilian coast in quantities sufficient for detection, allowing the use of these radioisotopes as geochronometers.

The use of7Be and210Pbxs to differentiate fine suspended sediment sources in South Slough, Oregon

Suspended sediment was collected in the South Slough, National, Estuarine Research Reserve, Oregon, over 8 tidal cycles during and following a single runoff event. The sediment was analyzed for its radionuclide signature to determine the relative contributions of different sources of sediment to the efflux from the estuary. Suspended sediment in the estuary is a mixture of sediment from three potential sources: the river system, Coos Bay, and the estuarine bed. Each source material has a distinctive7Be:210Pbxs ratio. The ratios of the source sediments decreased, in magnitude in the following order: riverine >bay>bed. The ratios, of the suspended sediment collected within a subsection of the South Slough estuary reflected the relative mixture of the source areas. The7Be:210Pbxs ratios provided a means of not only differentiating, between resuspended bed sediment and freshly delivered sediment from both the river system and Coos Bay, but also calculating the relative amount of resuspended bed sediment in the suspended sediment collected in the estuary. The sampled subsection of the South Slough estuary was a net sink of sediment during a 100-h sampling period associated with the runoff event, but the radionuclide analysis suggests that approximately 39% of the sediment efflux was resuspended bed sediment.

Suspended sediment sources and transport distances in the Yellowstone River basin

The activity of fallout radionuclides ( 7 Be, 1 3 7 Cs, and 2 1 0 Pb) was measured on upland and floodplain soils and on suspended sediments to quantify sources of fine sediment and to estimate sediment transport distances in stream channels in the Yellowstone River basin. Samples were collected seven times during snowmelt and runoff at nine locations from the headwaters of Soda Butte Creek to Billings, Montana, a 423-km-long reach of channel. The inventory of radionuclides in soil increases with precipitation and is highest in the headwaters. The activity of radionuclides in suspended sediment decreases downstream, and more activity is observed earlier than later in the flood hydrograph. The radionuclide activity of sediment derived from erosion of upland soils differs from that derived from bank erosion. Fine suspended sediment has an intermediate radionuclide signature that is quantified in terms of the relative contribution of these two sources of fine sediment. At sites high in the drainage, soils contribute 50% to the suspended load and this value decreases to 11%-26% downstream. Fine sediment transport distances were calculated from the exponential decrease in radionuclide concentration below a point source. Transport distances increase from a few kilometers in the headwaters to hundreds of kilometers downstream. These estimates are consistent with transport distances estimated from the settling velocity of the particles and from the distribution of mine tailings downstream from a dam failure. This study of a large watershed confirms earlier results from smaller basins and suggests that transport distances increase with basin size.

Sediment sources and transport pathways in a rural catchment, Herefordshire, UK

AbstractThe relative significance of primary and secondary suspended sediment sources has been identified in a small (15 km2) agricultural catchment through the application of a linear unmixing model using mineral magnetic, geochemical and radionuclide signatures of fine sediments. Roads appear to be important as a secondary source of suspended sediment and in the conveyance of topsoils to the river channel. Roads also alter the source signatures of sediment in transport, especially that derived from agricultural topsoils. Modelling suggests that c. 30% of the suspended sediment collected from suspended sediment traps in the River Leadon were derived from, or transported via, roads. Relative contributions from primary sources of c. 43% and c. 27% were estimated from a combined (subsoil and channel bank) subsurface source, and a combined (arable and grassland) topsoil source, respectively. Copyright © 2003 John Wiley & Sons, Ltd.

Sources of alluvium in a coastal plain stream based on radionuclide signatures from the 238U and 232Th decay series

Discerning alluvial sources and their change over time or distance is a fundamental question in hydrology and geology, often critical in identifying impacts of human and natural perturbations on fluvial systems. Surfaces of upland interfluves and subsoils, sources of alluvium in the lower Loco Bayou basin, Texas, were distinguished using the isotope ratios 226Ra/232Th, 226Ra/230Th, and 230Th/232Th. Channel alluvium indicates a transition from interfluve surface to subsoil sources during flood (subsoil ∼34% to ∼91%, over about 8 km) and bank‐full stages (subsoil ∼9% to ∼74%, over about 12 km), with distance downstream. These results indicate strong coupling between hillslope and channel processes, reflecting land use change from forested to agricultural, concentrated in lower Loco Bayou. This methodology shows that sediment sources can be differentiated based upon landscape placement where lithologic contrast is absent. The geochemistry, long half‐lives, and fractionation of 238U and 232Th decay series radionuclides during pedogenic and fluvial processes in humid climates suggest that these methods are applicable in a wide variety of fluvial systems.