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Here, we investigate Mid- to Late-Holocene vegetation changes in low-lying coastal areas in Tonga and how changing sea levels and recurrent volcanic eruptions have influenced vegetation dynamics on four islands of the Tongan archipelago (South Pacific). To investigate past vegetation and environmental change at Ngofe Marsh (‘Uta Vava’u), we examined palynomorphs (pollen and spores), charcoal (fire), and sediment characteristics (volcanic activity) from a 6.7-m-long sediment core. Radiocarbon dating indicated the sediments were deposited over the last 7700 years. We integrated the Ngofe Marsh data with similar previously published data from Avai’o’vuna Swamp on Pangaimotu Island, Lotofoa Swamp on Foa Island, and Finemui Swamp on Ha’afeva Island. Plant taxa were categorized as littoral, mangrove, rainforest, successional/ disturbance, and wetland groups, and linear models were used to examine relationships between vegetation, relative sea level change, and volcanic eruptions (tephra). We found that relative sea level change has impacted vegetation on three of the four islands investigated. Volcanic eruptions were not identified as a driver of vegetation change. Rainforest decline does not appear to be driven by sea level changes or volcanic eruptions. From all sites analyzed, vegetation at Finemui Swamp was most sensitive to changes in relative sea level. While vegetation on low-lying Pacific islands is sensitive to changing sea levels, island characteristics, such as area and elevation, are also likely to be important factors that mediate specific island responses to drivers of change.

Hydroclimate on ‘Uvea (Wallis et Futuna) is controlled by rainfall associated with the South Pacific Convergence Zone (SPCZ), the southern hemisphere's largest precipitation feature. To extend the short observational precipitation record, the hydrogen isotopic composition of the algal lipid biomarker dinosterol (δ2Hdinosterol) was measured in sediment cores from two volcanic crater lakes on ‘Uvea. The modern lakes differ morphologically and chemically but both contain freshwater within the photic zone, support phytoplankton communities inclusive of dinosterol-producing dinoflagellates, and experience identical climate conditions. δ2Hdinosterol values track lake water isotope ratios, ultimately controlled in the tropics by precipitation amount and evaporative enrichment. However, in 88-m-deep Lac Lalolalo a steadily decreasing trend in sedimentary δ2Hdinosterol values from −227‰ around year 988 CE to modern values as low as −303‰, suggests this lake's evolution from an active volcanic setting to the present system strongly influenced δ2Hdinosterol values. Although current hydrology and water isotope systematics may now reflect precipitation and evaporation in this lake, the interaction between theseprocesses and large changes in basin morphology, geochemistry, and hydrology obstruct the recovery of a climate signal from Lac Lalolalo's sedimentary δ2Hdinosterol records. This work emphasizes the importance of site replication and the use of complementary climate reconstruction tools, especially when using molecular proxiesthat may be sensitive to more than one environmental parameter. Contrary to its neighbor, duplicate δ2Hdinosterol records from 23-m-deep Lac Lanutavake varied between −277‰ and −297‰ and indicate slightly drier conditions during the time-period known as the Medieval Climate Anomaly (MCA, 950–1250 CE). The δ2Hdinosterol signal in Lac Lanutavake was muted compared to published records from ‘Upolu (Samoa) and Efate (Vanuatu) indicating that ‘Uvea's location is not as sensitive to precipitation variability at sites farther from the SPCZ centralaxis. Lithogenic runoff proxies combined with δ2Hdinosterol support the interpretation of a relatively dry MCA on ‘Uvea, ‘Upolu, and Efate, potentially due to less intense precipitation, a contracted, or a more zonally oriented SPCZ.

Using diatoms, pollen, and geochemistry, we explore human habitation around Lina myr, Gotland, in relation to shore displacement. Archeological evidence has shown that Lina myr was an important area for its prehistoric human inhabitants. We investigate if and when Lina myr was connected to the sea and could therefore have been part of an inland water system useful for transport. A chronology was based on14C AMS dating of terrestrial macrofossils and bulk sediments with dates ranging between 9100 and 2360 cal. yr BP. The initiation of the Littorina transgression was dated to 8500 cal. yr BP. A twofold pattern for the maximum sub-phase of the Littorina Sea is suggested from 8100 to 7500 cal. yr BP and from 6500 to 6000 cal. yr BP. The onset of cultivation and grazing was indicated by the presence of Hordeum and Plantago lanceolata in the pollen record during the Late Neolithic, at about 4580 cal. yr BP. During this time sea level was relatively higher than today and the Lina myr basin was connected with the Littorina Sea, which it continued to be until isostatic uplift caused it to become isolated at about 3820 cal. yr BP. After about 3000 cal. yr BP, human-made landscape changes intensified, grasslands increased, and shrublands decreased.

The introduction and application of high resolution XRF core scanners has made an enormous contribution to palaeoclimate science over the last two decades. These core scanners have become essential analytical tools for the investigation of sedimentary and other natural cumulative records of environmental change. Their widespread adoption by the environmental and geoscience communities has had a significant impact on the ability to systematically record high resolution chemical profiles in marine and lake sediments and soils. The range of applications has broadened beyond sedimentology and palaeoclimatology and now extends into scanning samples of speleothems, corals, mumiyo mounds, rocks, sedimentary nodules, archaeological artefacts, tree sections and melt segregations. Other areas exploiting the capability of XRF core scanners are mineral exploration, geotechnical characterisation, soil remediation studies and carbon capture and storage research. As a consequence of their ability to efficiently determine detailed, non-destructive elemental records in sediments and soils, scientific papers published since the year 2000 now number more than 1000.

The Isle of Man, situated in the central Irish Sea, was a significant centre for Pb and Zn mineral extraction during the Industrial Revolution. Comminuted mining debris from the East Snaefell and North Laxey mining areas was transported, through hydrological action, from upland catchments to the coast. This study focuses on an eastern coastal sediment sink and a salt marsh sediment sequence from Port Cornaa. A sediment monolith was excavated, sub-sampled and geochemically investigated using Itrax scanning, WD-XRF analysis and radionuclide methods. Since the island is only 55 km from one of the world's major nuclear reprocessing sites (Sellafield), it was anticipated that a record of these radionuclide discharges (1951-present) would be identifiable and contribute clear chronological markers. The 137Cs profile shows a Sellafield discharge component and also a larger component that is attributed to the 1986 Chernobyl airborne plume. This contribution in the salt-marsh sediment would be derived from the erosion and transport of Chernobyl-labelled upland soils into the marsh. Sediment depth was converted to age using natural (210Pb) and anthropogenic radionuclides (137Cs and 239, 240Pu) and a compelling age vs depth relationship was obtained. The ability to reliably date the overall sediment section shows that sediment accumulation is uniform for the top 25 cm (5 mm/y) and from −25 to −70 cm (3.2 mm/y). The robust age-depth model allows features in the geochemical profiles for S, As, Pb, Zn and Cu to be dated and used to infer events at the East Snaefell and North Laxey mines. These include start-up of mining, introduction of more-efficient mining practises (i.e. water-wheel technology), change in the intensity of mining and final mine closure. The study provides a 200-year industrial archaeological record for the east coast of the Isle of Man. It demonstrates the benefits offered by a combined study involving non-destructive, high resolution Itrax scanning, conventional WDXRF and radionuclide dating.

The South Pacific Convergence Zone (SPCZ) is the largest precipitation feature in the Southern Hemisphere supplying freshwater to 11 million people. Despite its significance, little is known about the location and intensity of SPCZ precipitation prior to instrumental records, hindering attempts to predict precipitation changes in a warming world. Here we use sedimentary molecular fossils to establish a tool for extending the historical record of precipitation. Freshwater lake sediments and water samples were collected from 30 lakes that span a 4.6 mm d−1 range in precipitation rates from the Global Precipitation Climatology Project (GPCP). 2Hlakewater values from 29 lakes ranged from –29 to +23‰ and were inversely correlated (r= −0.51, R2=0.26, p

A numerical simulation method has been developed to describe the transfer of analytes between solid and aqueous phases and assessed for a commercially available extraction chromatography resin (UTEVA resin). The method employs an ordinary differential equation solver within the LabVIEW visual programming language. The method was initially developed to describe a closed batch system. The differential equations and kinetic rate constants determined under these conditions were then applied to the flow-through column geometry. This was achieved by modelling the resin bed as a series of discrete vertically stacked sections, thereby generating an array of solid and aqueous concentration values. Axial flow was simulated by the advancement of the aqueous phase values by one array position with the value advancing from the final array position representing the column output concentration. An investigation into the observed difference in breakthrough profiles obtained under repeated conditions revealed the relative tolerance of the numerical simulation method to errors in each input parameter. Additional physical processes such as backpressure and leaching of the extractant were considered as an explanation for observed inconsistencies between experimental and simulated datasets. An elution sequence featuring multiple eluents was also simulated, demonstrating that the prediction of analyte separation sequences is possible. The potential to develop the LabVIEW coding into user friendly software with an extendable kinetic database is also discussed. This software will be a useful tool to radiochemists particularly in the development of new analytical methods using automated separation systems.

From the early 1950s until the late 1970s, Augusta Bay (Sicily, Italy) served as a major European (petro) chemical hub. It thereafter began a progressive decline as several crude oil refining and industrial plants closed due to the transfer of production cycles to other sites around the globe. As a result of the rapid and relatively uncontrolled post-WWII development of the site, several environmental studies identified significant contamination in sediments around the southernmost sector of the bay. The pollution was mainly due to barium (Ba) and mercury (Hg), attributable to the former chlor-alkali plant (1958-2003), and polychlorobiphenyls (PCBs) and hexachlorobenzene (HCB). The present study focuses on understanding the broad legacy of pollution across the whole harbour by systematically analysing 10 sediment cores collected in 2008 for contaminant concentration profiles of Hg, Ba, PCBs, HCB and grain-size variations. Pre-industrial environmental geochemical background conditions were identified using data from the deeper parts of cores. The results show that contamination has affected the entire harbour area to varying degrees, and this has allowed identifying contamination transfer, based on decreasing concentrations and related depths in the sediment cores from the southernmost sector to the central and northern area. A recent finding by the current researchers is that the construction of the dam/breakwater in the early 1960s, that largely coincided with the start of industrial inputs, led to the trapping of fine terrestrial sediment inside the harbour, particularly in the central and northern area. This trapped sediment provides a granulometric time marker in those cores. The presence of highly contaminated sediments inside the harbour represents a significant future liability unless remedial action is applied to remove the worst of the polluted sediment.

The environmental occurrence, fate and ecotoxicity of emerging contaminants (ECs) has been the subject of increasing research, policy and public concern over the past two decades. While a wide range of publications have examined the environmental persistence and sediment/soil interactions of ECs following their discharge into aquatic environments, the extent to which ECs are sequestered in estuarine sediments, and the impact of this on their environmental persistence and supply to the ocean, in comparison remains unclear. This Article examines the environmental concentrations of seven, relatively water-soluble and environmentally mobile, ECs (including pharmaceuticals, perfluoroalkyl compounds, and plasticisers) in dated intertidal saltmarsh cores from two contrasting estuarine sites in the southern U.K. (one heavily urbanised/industrial, the other non-urbanised). Mean sediment EC concentrations are similar in both estuarine systems (in the range 0.1 (acetaminophen) to 17 (4-hydroxyacetophenone) ng/g dry weight). Despite their variable reported Log Kow values (from ca. 0.5 to > 7), the ECs are all apparently mobile in the marsh systems studied, and where subsurface concentration maxima are present these most likely relate to local flushing or diffusive processes and cannot be clearly linked to likely input trends or changes in sediment geochemistry (including sedimentary organic carbon content). The “estuarine filter” here, at least with respect to intertidal saltmarsh sediments, shows reduced potential to sequester the seven ECs examined and mediate their supply to coastal and shelf environments.

In the Carrazeda de Ansiães region, northern Portugal, a mesozonal granitic suite intruded Precambrian to Ordovician metasedimentary rocks during the late kinematic stages of the Variscan orogeny. In this multiphase granitic complex, consisting of ten granite types, the youngest group of two-mica granites (G7–G10) was emplaced between 318 ± 1 Ma and 316.2 ± 0.7 Ma, as determined by ID-TIMS U–Pb on zircon and monazite. Granite types G7–G9 were affected by the third phase of deformation (D 3) before they were completely crystallized, as indicated by their internal NW–SE magmatic foliation concordant with the regional structures. The granite type G10 shows some distinctive textural features, showing a strong brittle deformation, probably due to its preferential emplacement in late NNE-SSW fault zones. Granites G7–G9 have equal or higher amounts of muscovite than biotite and contain surmicaceous enclaves, xenoliths, “schlieren”, and, more rarely, microgranular enclaves. The muscovite-dominant granite G10 does not contain enclaves. These Variscan granites are peraluminous, with ASI ranging between 1.22 and 1.39 and normative corundum of 2.79–4.39%, having the characteristics of S-type granites. In fact, the enrichment in LREE relatively to HREE, the negative Eu anomalies, and similar mean values of ( 87Sr/ 86Sr) i, εNd t and δ 18O for G7 (0.7156 ± 0.0005; − 8.5; 11.49 ‰) and G8 (0.7155 ± 0.0007; − 8.4; 11.39 ‰) show that these two granite types resulted from sequential partial melting of the same metasedimentary material, where granite G8 would have derived from a higher degree of partial melting than G7. Granites G8–G10 and their minerals show a fractionation trend that is confirmed by modeling of major and trace elements. The subparallel REE patterns and the decreasing REE contents within the differentiation series, the Rb–Sr isochron for G8, G9 and G10 (315.5 ± 5.4 Ma; MSWD = 1.3) and the relatively uniform εNd t and δ 18O data suggest that fractional crystallization was the main mechanism, which would have lasted less than 1 Ma. The tin-bearing granites G7 and G10 have ≥ 20 ppm Sn, but the main quartz veins containing cassiterite and wolframite cut granite G10, which contains 31 ppm Sn. Fractional crystallization was responsible for the increase in Sn content in granites from the G8–G10 series and their micas.

Industrial and commercial port activities are widely recognized worldwide as an important source of pollution to proximal estuaries. In this study, we analysed geochemical and sedimentological parameters including major and trace elements, organic matter and sediment texture in surface sediments from the estuarine environment of Southampton Water, U.K. Using these data, and multivariate statistical tools [correlation, factor and cluster analysis and pollution indices such as Enrichment Factor (EF), Pollution Load Index (PLI) and the Adverse Effect Index (AEI)], we examine sedimentary trace metal and metalloid contamination, contamination sources, and potential biological impacts of the contamination present. The geochemical data, multivariate statistical analysis and pollution indices indicate that the spatial distribution of trace metals and metalloids is influenced by both sediment composition (and mixing) and anthropogenic activities. Most trace metal and metalloid concentrations are close to local geological background levels, except for Cu, Zn and Pb. The spatial distribution of these elements indicates that the Exxon oil refinery, Southampton port, local marinas and runoff from domestic and industrial activities act effectively as point sources of these elements. Pollution indices calculations highlight a degraded environment as a result of these pollutants, and further work is needed to assess the current impact of trace metals and metalloids on local ecology.

Many lakes undergo anthropogenically driven eutrophication and pollution leading to decreased water and sediment quality. These effects can enhance seasonally changing lake redox conditions that may concentrate potentially toxic elements. Here we report the results of a multi-method geochemical and sediment microfabric analysis applied to reconstruct the history of cultural eutrophication and pollution of the North and South Basins of Windermere, UK. Eutrophication developed from the mid-19th to the earliest 20th centuries. Enhanced lake productivity is indicated by increased sedimentary δ13C, and increased pollution by a higher concentration of metals (Pb, Hg, and As) in the sediment, likely enhanced by incorporation and adsorption to settling diatom aggregates, preserved as sedimentary laminae. In the South Basin, increasing sediment δ15N values occur in step with Zn, Hg, and Cu, linking metal enrichment to isotopically heavy nitrate (N) from anthropogenic sources. From around 1930, decreases in Mn and Fe-rich laminae indicate reduced deep-water ventilation, whereas periods of sediment anoxia increased, being most severe in the deeper North Basin. Strongly reducing sediment conditions promoted Fe and Mn reduction and Pb-bearing barite formation, hitherto only described from toxic mine wastes and contaminated soils. From 1980 there was an increase in indicators of bottom water oxygenation, although not to before 1930. But in the South Basin, the continued impacts of sewage are indicated by elevated sediment δ15N. Imaging and X-ray microanalysis using scanning electron microscopy has shown seasonal-scale redox mineralisation of Mn, Fe, and Ba related to intermittent sediment anoxia. Elevated concentrations of these metals and As also occur in the surficial sediment and provide evidence for dynamic redox mobilisation of potentially toxic elements to the lake water. Concentrations of As (up to 80 ppm), exceed international Sediment Quality Standards. This process may become more prevalent in the future with climate change driving lengthened summer stratification.

Significance We combine indicators from lake sediments with archaeological records that identify an earlier and incremental arrival of humans in East Polynesia than indicated by current models. We use lake sediments to reconstruct a quantitative, multiproxy hydroclimate sequences from Vanuatu, Samoa, and the Southern Cook Islands and combine these with published data to show that the timing of human migration into East Polynesia coincided with a prolonged drought. We postulate this regional drought was a significant contributory factor in eastward exploration and subsequent colonization of the Southern Cook Islands and beyond. The return of wetter conditions in East Polynesia after c. AD 1150 supported subsequent colonization of other central islands and, eventually, migration into far eastern and South Polynesia., The timing of human colonization of East Polynesia, a vast area lying between Hawai‘i, Rapa Nui, and New Zealand, is much debated and the underlying causes of this great migration have been enigmatic. Our study generates evidence for human dispersal into eastern Polynesia from islands to the west from around AD 900 and contemporaneous paleoclimate data from the likely source region. Lake cores from Atiu, Southern Cook Islands (SCIs) register evidence of pig and/or human occupation on a virgin landscape at this time, followed by changes in lake carbon around AD 1000 and significant anthropogenic disturbance from c. AD 1100. The broader paleoclimate context of these early voyages of exploration are derived from the Atiu lake core and complemented by additional lake cores from Samoa (directly west) and Vanuatu (southwest) and published hydroclimate proxies from the Society Islands (northeast) and Kiribati (north). Algal lipid and leaf wax biomarkers allow for comparisons of changing hydroclimate conditions across the region before, during, and after human arrival in the SCIs. The evidence indicates a prolonged drought in the likely western source region for these colonists, lasting c. 200 to 400 y, contemporaneous with the phasing of human dispersal into the Pacific. We propose that drying climate, coupled with documented social pressures and societal developments, instigated initial eastward exploration, resulting in SCI landfall(s) and return voyaging, with colonization a century or two later. This incremental settlement process likely involved the accumulation of critical maritime knowledge over several generations.

Many lakes in industrialised areas have undergone anthropogenically driven eutrophication and increases in pollution leading to decreased water and sediment quality. In some cases, these effects are enhanced by seasonally changing lake redox conditions that may act to concentrate potentially toxic elements sufficiently to exceed internationally recognised Sediment Quality Standards, impacting key species and jeopardizing water supply. A combined, geochemical and sediment microfabric analysis is applied to reconstruct the history of cultural eutrophication and pollution in the North and South Basins of Windermere, England’s largest natural lake. We also document a record of seismicity and link increased sedimentation rates and sediment instability. The onset and development of eutrophication in Windermere occurred from the mid-19th to the early 20th centuries. Raised lake productivity is indicated by an increase in sedimentary δ13C, and increased pollution by elevated sedimentary trace metals (Pb, Zn, Cu, Hg, and As), likely enhanced by incorporation and adsorption to settling diatom aggregates, preserved as sedimentary laminae. In the South Basin of the lake, contemporaneous increasing sediment δ15N values also occur in step with increasing Zn, Hg, Cu from this time, linking metal enrichment to the input of isotopically heavy nitrate (N) from anthropogenic sources including sewage. From around 1930, a decrease in Mn and Fe-rich laminae indicate reduced deep water ventilation, and increased incidence of sediment anoxia, being most intense in the deeper North Basin where benthic activity intermittently ceased. Strongly reducing conditions in the sediment promoted Fe and Mn reduction and the formation of unusual Pb-bearing barite, hitherto only described from toxic mine wastes and contaminated soils. In the North Basin cores a clay rich laminae dated 1979-1980 is shown to be a mass transport deposit linked to large scale slope failure likely caused by the 4.7 ML 1979 Carlisle earthquake. Slope failure was exacerbated by preconditioning principally by increased sedimentation as a result of anthropogenic activities. From 1980 there was a partial recovery in oxygenation with Mn and Fe rich laminae returning in some parts. But in the South Basin, the continued impacts of sewage discharge is indicated by elevated δ15N of organic matter. Imaging and X-ray microanalysis using scanning electron microscopy has enabled the identification of seasonal-scale redox mineralisation of Mn, Fe and Ba related to intermittent sediment anoxia. Elevated concentrations of Mn, Fe, Ba, and As also occur in the surficial sediment and provide evidence for dynamic redox mobilisation of potentially toxic elements that may be released to the lake waters. Concentrations of As, in particular, exceed international Sediment Quality Standards. These surface enrichments in As and other toxic elements may become more prevalent in the future with climate change driving lengthened summer stratification in the lake.

The El Niño-Southern Oscillation (ENSO) is a driver of global atmosphere-ocean dynamics, but projections of frequency and magnitude in different climate states remain uncertain. Palaeoclimate records offer the potential to improve our understanding of ENSO behaviour but most are fragmentary, suffer low resolution, and/or typically do not cover periods warmer than present day. The Last Interglacial (129-116 kyr BP) was the most recent period during which global temperatures were close to 21st century projections, and potentially provides insights into operation of climate modes of variability in the future. Here we report a continuous, inter-annually resolved record of hydroclimate spanning 220-80 ka from Lynch’s Crater in tropical northeast Australia, a region highly sensitive to ENSO. Our reconstruction is based on a micro-X-ray fluorescence (XRF)-generated elemental profile at 200 µm resolution, combined with loss-on-ignition, magnetic susceptibility, and pollen analysis. We find that during globally warmer periods (including super-interglacial Stage 5e, and 5c), there are significantly larger amplitudes in high-frequency ENSO spectral range (3-8 years), which are absent from the record during the glacial stages MIS6 and MIS4. Our results imply an ENSO dependence on mean climate, with enhanced ENSO variance during interglacials globally warmer than present. These results are consistent with climate model projections for a future slowdown of the Walker circulation and more extreme El Niño events under greenhouse warming.

Eutrophication and sedimentation are affecting global Marine Protected Area (MPA) ecosystems, such as estuaries, as catchments are developed and sea levels rise. Managers are often faced with short term datasets and modelling evidence with which to undertake management of these complex open systems. Longer term datasets which monitor environmental change can be used to improve understanding of estuary biogeochemistry and the resulting ecological response. In this paper we use the case study of Holes Bay, Poole Harbour to explore how palaeoenvironmental archives can be used to extend the evidence base for sediment, nutrient and ecological management within a coastal MPA.

A compact dual zone, two work-tube, vertical tube furnace system (Raddec Pyrolyser-Mini) has been designed for the determination of H-3 and C-14 in decommissioning wastes. An optimised methodology was developed following improvements to sample holder and bubbler trap design, sample loading and loading temperature, as well as length and style of heating programmes. A significant efficiency enhancement was obtained through 'hot-loading' of the sample into the furnace at 600 °C before finally ramping to 900 °C. Direct trapping of H-3 and C-14 in a scintillation vial located in a special anti-suck-back bubbler further improved operations, leading to a reduction in analysis time and measurement sensitivity. Co-trapping of the analytes and dual-label liquid scintillation counting also proved effective. Overall, the developed methodology led to a reduced analyte extraction/trapping time of 150 min whilst achieving limits of detection of

Quantitative extraction of tritium from a sample matrix is critical to efficient measurement of the low-energy pure beta emitter. Oxidative pyrolysis using a tube furnace (Pyrolyser) has been adopted as an industry standard approach for the liberation of tritium (Warwick et al. in Anal Chim Acta 676:93–102, 2010) however pyrolysis of organic-rich materials can be problematic. Practically, the mass of organic rich sample combusted is typically limited to

Estuarine sediments provide an important sink for contaminants discharged into fluvial, estuarine, and nearshore settings, and numerous authors have utilized this trapping function to assess historical contaminant loadings and contaminant breakdown/transformation processes. This Article examines the retention of elemental and isotopic sedimentary signatures in an industrialized estuarine system subject to a strongly upward sea-level trend, over a 20 year period. Two contrasting saltmarsh sites (at Hythe and Hamble, part of the wider Southampton Water estuarine system, UK) were examined, which had been previously cored and analyzed in the early 1990s. Much of the geochemical record of recent anthropogenic activity has been eroded and lost at the Hamble site. In contrast, radiometric, isotopic and elemental records of anthropogenic activity have been retained in the Hythe marsh, with 137Cs and Cu depth profiles showing retention of input maxima related to fallout and local industrial discharges, respectively. Stable Pb isotope data show a broad degree of correspondence in cores analyzed in 1994 and 2014 when plotted against sediment (radiometric) age, indicating the usefulness of isotopic data in retaining information on Pb sources and in disentangling Pb input histories. New ultrahigh precision, double-spike mass spectrometry stable Pb isotope data allow clearer discrimination of historical Pb input phases, and highlight within-estuary mixing and supply of reworked, secondary contamination from erosion of anthropogenically labeled sediments elsewhere in the estuary.

Liquid scintillation spectrometry is widely used for the analysis of alpha and beta emitting radionuclides. Robust calibration of liquid scintillation (LS) spectrometers is fundamental to accurate LS measurement but at the same time is time consuming and costly, particularly if a wide range of radionuclides are analysed by the laboratory. The frequency of the calibration varies in different laboratories and is based on many practical and operational factors. This work summarizes the observations regarding variations in 1220 Quantulus spectrometers efficiency calibrations performed annually using various radionuclides: 3H 63Ni, 55Fe, 36Cl, 45Ca, 147Pm, 241Pu, 99Tc for a period of 9 years and discusses the implication to calibration frequency.

Tritium is ubiquitous in and around nuclear plants, being formed via neutron capture by 2H, 6Li, 10B and 14N and via ternary fission. The highly mobile nature of 3H species results in widespread distribution of the radionuclide. Predictive modeling of 3H activity concentrations is challenging and direct measurement of 3H activities in materials is the preferred approach to underpin waste and environmental assessments. For well over a decade, the UK nuclear industry has engaged in a significant program of site decommissioning of its first generation reactors. This has resulted in a high demand for the rapid characterization of 3H in a diverse range of matrices, including concretes, metals, plastics, sludges, resins, soils and biota. To support such assessments, it has been necessary to develop dedicated instrumentation in parallel with robust radioanalytical methodologies; namely a multi-tube furnace and a high-capacity, closed (pressurized) oxygen combustion system. Data are presented on the development and validation of these instruments, designed specifically to enable the quantitative extraction of 3H (and other volatile radionuclides) from diverse sample types. Furthermore the furnace system has been employed as a tool to gain insights into the 3H association in decommissioning and environmental matrices exposed to 3H arising from nuclear power plant operations through tritium evolution with temperature profiling. The impact of the chemical speciation of 3H on analytical strategy is discussed. A major benefit of the multi-sample furnace is its ease of use and applicability to 3H determination in virtually any sample type. The complementary HBO2 oxygen combustion system has been developed for the quantitative oxidation of organic-rich samples (e.g. wood, plastic, oil, biota) and analytical data prove its effectiveness.

The ability to efficiently identify potential radiological threats or actual radioactive assaults on society and the environment demands a sophisticated and dedicated infrastructure comprising specialised personnel, mobile and fixed laboratories and advanced analytical instrumentation. Most developed countries have such systems but ensuring a long-term and resilient capability is recognised as a perennial challenge. National government laboratories specialising in nuclear forensics play a key role in maintaining capability but these organisations continue to benefit significantly from interdisciplinary and innovative contributions derived from universities and other research institutions. This review provides an insight into the range of technologies used and also provides a broad overview of applied techniques and instrumentation that contribute to rapid screening and analysis in the context of nuclear forensics and radiological emergencies.

Concern is growing that climate change may amplify global flood risk but short hydrological data series hamper hazard assessment. Lake sediment reconstructions are capturing a fuller picture of rare, high-magnitude events but the UK has produced few lake palaeoflood records. We report the longest lake-derived flood reconstruction for the UK to date, a 1500-year record from Brotherswater, northwest England. Its catchment is well-suited physiographically to palaeoflood research, but its homogeneous, dark brown sediment matrix precludes visual identification of flood layers. Instead, an outlier detection routine applied to high-resolution particle size measurements showed a >90% match, in stratigraphic sequence, to measured high river flows. Our late-Holocene palaeoflood reconstruction reveals nine multi-decadal periods of more frequent flooding (510–630 CE, 890–960, 990–1080, 1470–1560, 1590–1620, 1650–1710, 1740–1770, 1830–1890 and 1920–2012), and these show a significant association with negative winter North Atlantic Oscillation (wNAO) phasing and some synchrony with solar minima. These flood-rich episodes also overlap with local and regional land-use intensification, which we propose has amplified the flood signal by creating a more efficient catchment sediment conveyor and more rapid hillslope-channel hydrological connectivity. Disentangling anthropogenic and climatic drivers is a challenge but anthropogenic landscape transformation should evidently not be underestimated in palaeoflood reconstructions. Our paper also demonstrates that flood histories can be extracted from the numerous lakes worldwide containing organic-rich, visually homogeneous sediments. This transformative evidence base should lead to more reliable assessments of flood frequency and risks to ecosystems and infrastructure.

We present the first quantitative reconstruction of palaeofloods using lake sediments for the UK and show that for a large catchment in NW England the cluster of devastating floods from 1990 to present is without precedent in this 558‐year palaeo‐record. Our approach augments conventional flood magnitude and frequency (FMF) analyses with continuous lake sedimentary data to provide a longer‐term perspective on flood magnitude recurrence probabilities. The 2009 flood, the largest in >558 years, had a recurrence interval larger (1:2,200 year) than revealed by conventional flood estimation using shorter duration gauged single station records (1:1,700 year). Flood‐rich periods are non‐stationary in their correlation with climate indices, but the 1990‐2018 cluster is associated with warmer Northern Hemisphere Temperatures and positive Atlantic Multidecadal Oscillation. Monitored records rarely capture the largest floods and our palaeoflood series shows, for this catchment, such omissions undermine evaluations of future risk. Our approach provides an exemplar of how to derive centennial palaeoflood reconstructions from lakes coupled well with their catchments around the world.

Decommissioning and monitoring around nuclear sites presents challenges with regards to the range of sample matrices and radionuclides that must be accurately characterised. Over the last few decades, inductively coupled plasma mass spectrometry (ICP-MS) has been increasingly used in the nuclear sector as a rapid alternative to decay counting techniques for long-lived radionuclides, as well as an expanding range of shorter-lived radionuclides. The presence of various interferences still presents a major challenge in achieving accurate measurements, often necessitating extensive chemical clean-up prior to measurement. This study evaluates the potential application of tandem ICP-MS/MS for the measurement of a range of radionuclides of interest to nuclear decommissioning and waste management. The flexibility of the instrumental setup is shown in achieving improved interference removal compared to alternative instrument designs, improving sample throughput by reducing reliance on offline separation, and increasing the potential application of ICP-MS/MS for routine measurement of difficult-to-measure radionuclides.

Managed realignment (MR) schemes are being implemented to compensate for the loss of intertidal saltmarsh habitats by breaching flood defences and inundating the formerly defended coastal hinterland. However, studies have shown that MR sites have lower biodiversity than anticipated, which has been linked with anoxia and poor drainage resulting from compaction and the collapse of sediment pore space caused by the site's former terrestrial land use. Despite this proposed link between biodiversity and soil structure, the evolution of the sediment sub-surface following site inundation has rarely been examined, particularly over the early stages of the terrestrial to marine or estuarine transition. This paper presents a novel combination of broad- and intensive-scale analysis of the sub-surface evolution of the Medmerry Managed Realignment Site (West Sussex, UK) in the three years following site inundation. Repeated broad-scale sediment physiochemical datasets are analysed to assess the early changes in the sediment subsurface and the preservation of the former terrestrial surface, comparing four locations of different former land uses. Additionally, for two of these locations, high-intensity 3D-computed X-ray microtomography and Itrax micro-X-ray fluorescence spectrometry analyses are presented. Results provide new data on differences in sediment properties and structure related to the former land use, indicating that increased agricultural activity leads to increased compaction and reduced porosity. The presence of anoxic conditions, indicative of poor hydrological connectivity between the terrestrial and post-inundation intertidal sediment facies, was only detected at one site. This site has experienced the highest rate of accretion over the terrestrial surface (ca. 7 cm over 36 months), suggesting that poor drainage is caused by the interaction (or lack of) between sediment facies rather than the former land use. This has significant implications for the design of future MR sites in terms of preparing sites, their anticipated evolution, and the delivery of ecosystem services.

Conventional pollution monitoring strategies for heavy metals are often costly and unpractical. Innovative sampling and analytical approaches are therefore needed to efficiently monitor large areas. This study presents a novel, simple, fast, and inexpensive method to monitor heavy metal pollution that uses cation-exchange resin sachets and the micro-XRF core-scanning technique (XRF-CS). The resin passive samplers act as concentrators of cationic species and can be readily deployed spatially and temporally to record pollution signals. The large number of analytical tasks are then overcome by the fast and non-destructive XRF-CS to precisely assess elemental concentrations. Quantifying element loading involves direct comparison with a set of identically prepared and scanned resin reference standards containing Ca, Ti, Cr, Mn, Ni, Cu, Zn, Pb. The results show that within the test range (from 0–1000 s mg kg −1 ), the calibration lines have excellent regressions (R 2 ≥ 0.97), even at the shortest exposure time (1 s). A pilot field survey of a suspected polluted area in central Taiwan, where 30 resin sachets had been deployed, identified a pollution hot spot in a rapid and economical manner. Therefore, this approach has the potential to become a valuable tool in environmental monitoring and forensics.

XRF core scanning has evolved to become a standard analytical technique for the rapid assessment of elemental, density and textural variations in a wide range of sediments and other materials, with applications ranging from palaeoceanography, paleoclimatology, geology, and environmental forensics to environmental protection. In general, scanning provides rapid, non-destructive acquisition of elemental and textural variations at sub-millimetre resolution for a wide range of materials. Numerous procedural adaptations have been developed for the growing number of applications, such as analyses of unconsolidated, water-rich sediments, powdered soil samples, or resin bags. Here, practical expertise and guidance from the Itrax community, gained over 15 years, is presented that should provide insights for new and experienced users.

Electrokinetic remediation, EKR, is technology that circumvents the traditional challenges faced by many existing remediation technologies in low permeability substrates. Cheap, non-toxic additives such as KCl may further help EKR remediation efficiency by increasing electrolyte strength; their use has been reported in concretes, but not soils. Here, we investigate the efficiency of low-energy EKR (with and without electrolyte additives) in the mobilisation of radiostable Cs and Sr in a clayey, organic-rich soil. Soil maturation time and voltage are key factors in determining success of EKR. Although Cs and Sr are effectively mobilised (up to 317 and 330%, respectively) in the electric field in our soils (determined by XRF), maturation time (7 or 45 days) and voltage (15 or 20 V) are key to successful remediation using EKR. We more broadly show that understanding speciation and the local ionic environment of relevant radionuclides within entrained matrices is vital to effective application of this technology.

The application of Principal Components Analysis (PCA) to U and Th series gamma spectrometry data provides a discriminatory tool to help determine the provenance of illicitly recovered uranium ore concentrates (UOCs). The PCA is applied to a database of radiometric signatures from 19 historic UOCs from Australia, Canada, and the USA representing many uranium geological deposits. In this study a key process to obtain accurate radiometric data (gamma and alpha) is to digest the U-ores and UOCs using a lithium tetraborate fusion. Six UOCs from the same sample set were analysed ‘blind’ and compared against the database to identify their geolocation. These UOCs were all accurately linked to their correct geolocations which can aid the forensic laboratory in determining which further analytical techniques should be used to improve the confidence of the particular location.

Published version. Source at http://doi.org/10.1111/nph.14199. License CC BY 4.0. Sedimentary DNA (sedDNA) has recently emerged as a new proxy for reconstructing past vegetation, but its taphonomy, source area and representation biases need better assessment. We investigated how sedDNA in recent sediments of two small Scottish lakes reflects a major vegetation change, using well-documented 20th Century plantations of exotic conifers as an experimental system. We used next-generation sequencing to barcode sedDNA retrieved from subrecent lake sediments. For comparison, pollen was analysed from the same samples. The sedDNA record contains 73 taxa (mainly genus or species), all but one of which are present in the study area. Pollen and sedDNA shared 35% of taxa, which partly reflects a difference in source area. More aquatic taxa were recorded in sedDNA, whereas taxa assumed to be of regional rather than local origin were recorded only as pollen. The chronology of the sediments and planting records are well aligned, and sedDNA of exotic conifers appears in high quantities with the establishment of plantations around the lakes. SedDNA recorded other changes in local vegetation that accompanied afforestation. There were no signs of DNA leaching in the sediments or DNA originating from pollen.

A study of heavy metals in estuarine sediments and foraminiferal tests along with foraminiferal distributions from Southampton Water indicates that:a) heavy metals have a marked effect upon foraminiferid distribution. Some species are able to tolerate pollution and their relative abundance increases at discharge points, whereas other species develop test deformities. Investigation of cores show that no deformed specimens exist within sediments prior to the introduction of pollution.b) deformed specimens contain higher levels of elements such as Cu and Zn than non-deformed specimens. This indicates that heavy metals may be responsible for the abnormalities within foraminiferid tests. Culture experiments support this hypothesis. Specimens of Ammonia beccarii (Linné) developed abnormal chambers over a period of 12 weeks within a culture medium containing 10–20ppb of Cu.

The expression of storm events in the geological record is poorly understood; therefore, stratigraphic investigations of known events are needed. The 1953 North Sea storm surge was the largest natural disaster for countries bordering the southern North Sea during the twentieth century. We characterize the spatial distribution of a sand deposit from the 1953 storm surge in a salt marsh at Holkham, Norfolk (UK). Radionuclide measurements, core scanning X-ray fluorescence (Itrax), and particle size analyses, were used to date and characterise the deposit. The deposit occurs at the onset of detectable 137Cs - coeval with the first testing of nuclear weapons in the early 1950s. The sand layer is derived from material eroded from beach and dunes on the seaward side of the salt marsh. After the depositional event, accumulation of finer-grained silt and clay materials resumed. This work has important implications for understanding the responses of salt marshes to powerful storms and provides a near-modern analogue of storm surge events for calibration of extreme wave events in the geological record.

Sediment cores are used to reconstruct the chronological evolution of contamination in impacted areas while deep core levels may be considered as reference conditions for the assessment of environmental status. For this purpose, the collection of undisturbed cores is essential. Vibro and gravity corers are the most used devices for environmental research. In this study, chemical (Ba, Hg and PCBs) and grain size data obtained by means of gravity (SW-104) and vibro (Rossfelder®) corer from 3 stations of the heavily contaminated Augusta harbor (Sicily, Italy) were considered. Their vertical profiles were compared considering the different technical characteristics of corers, in order to highlight differences in data acquisition. Results showed that, for areas characterized by high sedimentation rates, the vibrocorer is the best choice for the higher penetration capacity. No significant differences were recognized for sediment compaction and potential downward drag of the contaminants.

Lake sediments commonly contain detrital layers that record events such as floods or earthquakes, but these may be disturbed or partially destroyed by bioturbation. Here we use a novel combination of techniques to relate microscopic sediment fabric features to processes at the lake basin scale. X-radiography and micro-X-ray fluorescence analysis of cores are complemented by back-scattered electron imagery and energy-dispersive X-ray microanalysis of resin-embedded sediment. Together, the microfabric and geochemical methods enable the identification of clay layer mass transport deposits despite bioturbational mixing of the original end-members. Two cores with robust radionuclide chronologies contain correlative clay layers dated to 1979 (1974–1982) and 1979–1980 (1973–1986), respectively. These clay layers probably represent the distal turbidite generated by a major mass flow deposit identified from multi-beam swath bathymetry and sediment grab sampling. A probable trigger for the mass flow and associated turbidity current is the 4.7 ML 1979 Carlisle earthquake. The lake basin slope was probably preconditioned for failure by increased sedimentary biogenic gas production and sediment in-wash as a result of anthropogenic activities, coupled with sediment disruption and dredging. This study highlights the effectiveness of microstratigraphic techniques in the recognition and characterization of event layers in sediments where bioturbative disruption has occurred.

Microplastics are an increasingly important contaminant in the marine environment. Depending on their composition and degree of biofouling, many common microplastics are less dense than seawater and so tend to float at or near the ocean surface. As such, they may exhibit high concentrations in the sea surface microlayer (SML – the upper 1–1000 μm of the ocean) relative to deeper water. This paper examines the accumulation of microplastics, in particular microfibres, in the SML in two contrasting estuarine systems – the Hamble estuary and the Beaulieu estuary, southern U.K., via a novel and rapid SML-selective sampling method using a dipped glass plate. Microplastic concentrations (for identified fibres, of 0.05 to 4.5 mm length) were highest in the SML-selective samples (with a mean concentration of 43 ± 36 fibres/L), compared to

The Gulf of Mexico is considered one of the world's major marine ecosystems, supporting important fisheries and habitats such as barrier islands, mangrove forests, seagrass beds, coral reefs etc. It also hosts a range of complex offshore petroleum exploration, extraction, and refining industries, which may have chronic or acute impacts on ecosystem functioning. Previous work on the marine effects of this activity is geographically incomplete, and has tended to focus on direct hydrocarbon impacts, while impacts from other related contaminants (e.g. heavy metals, salt-rich drilling muds) which may be discharged from oil facilities have not been widely assessed. Here, we examine historical trace element accumulation in marine sediments collected from four sites in the Tamaulipas shelf, Gulf of Mexico, in the area of the Arenque oil field. Dated sediment cores were used to examine the sources, and historical and contemporary inputs, of trace metals (including those typically present in oil industry discharges) and their potential biological impact in the Tamaulipas aquatic environment over the last 100 years. CaO (i.e. biogenic component) normalized data showed increasing V, Cr, Zn, Cu, Pb, Zr and Ba towards the sediment surface in three of the four cores, with Ba and V (based on an adverse effect index) possibly associated with adverse effects on organisms. Dated Ba/CaO profiles show an increase of 30–137% after opening of oil installations in the study area, and can be broadly correlated with increasing oil industry activities across the wider Gulf of Mexico. Data do not record however a clear enhancement of Ba concentration in sediment cores collected near to oil platforms over more distal cores, indicating that any Ba released from drilling platforms is incorporated quickly into the sediments around the drilling sites, and once this element has been deposited its rate of resuspension and mobility is low. Capsule abstract Sediment core data from the Tamaulipas shelf show the influence of oil industry activities on selected trace element concentrations, with Ba/CaO broadly correlating with increasing oil industry activities across the wider Gulf of Mexico.

International audience; Organically bound tritium (OBT) has become of increasing interest within the last decade, with a focus on its behaviour and also its analysis, which are both important to assess tritium distribution in the environment and dose consequences. After the first OBT International Workshop which was held in France in May 2012, an international working group was created. The expected benefits are the following remove or reduce uncertainty in OBT analysis results, provide better OBT model validation data and better public dose results, increase the number of potential measuring OBT laboratories, validate all of the stages of the procedures based on a larger population and more statistically significant results, and investigate the feasibility of CRM's and RM's production. In this framework, three OBT exercises were organised; the 1st one on potatoes was conducted in 2013 by the Canadian National Laboratories (former AECL) with about 20 participating labs from around the world, the 2nd one on a sediment was organised in 2014 by GAU Radioanalytical (University of Southampton) on a sediment with again about 20 participating labs and the third one on wheat was organised in 2015 by the Commissariat à l’énergie atomique (CEA) with about 25 participating labs. © 2017

Radionuclides of caesium are environmentally important since they are formed as significant high yield fission products ((135)Cs and (137)Cs) and activation products ((134)Cs and (136)Cs) during nuclear fission. They originate from a range of nuclear activities such as weapons testing, nuclear reprocessing and nuclear fuel cycle discharges and nuclear accidents. Whilst (137)Cs, (134)Cs and (136)Cs are routinely measurable at high sensitivity by gamma spectrometry, routine detection of long-lived (135)Cs by radiometric methods is challenging. This measurement is, however, important given its significance in long-term nuclear waste storage and disposal. Furthermore, the (135)Cs/(137)Cs ratio varies with reactor, weapon and fuel type, and accurate measurement of this ratio can therefore be used as a forensic tool in identifying the source(s) of nuclear contamination. The shorter-lived activation products (134)Cs and (136)Cs have a limited application but provide useful early information on fuel irradiation history and have importance in health physics. Detection of (135)Cs (and (137)Cs) is achievable by mass spectrometric techniques; most commonly inductively coupled plasma mass spectrometry (ICP-MS), as well as thermal ionisation (TIMS), accelerator (AMS) and resonance ionisation (RIMS) techniques. The critical issues affecting the accuracy and detection limits achievable by this technique are effective removal of barium to eliminate isobaric interferences arising from (135)Ba and (137)Ba, and elimination of peak tailing of stable (133)Cs on (135)Cs. Isobaric interferences can be removed by chemical separation, most commonly ion exchange chromatography, and/or instrumental separation using an ICP-MS equipped with a reaction cell. The removal of the peak tailing interference is dependent on the instrument used for final measurement. This review summarizes and compares the analytical procedures developed for determination of (135)Cs/(137)Cs, with particular focus on ICP-MS detection and the methods applied to interference separation.

The determination of background concentration values (BGVs) in areas, characterised by the presence of natural geochemical anomalies and anthropogenic impact, appears essential for a correct pollution assessment. For this purpose, it is necessary to establish a reliable method for determination of local BGVs. The case of the Orbetello lagoon, a geologically complex area characterized by Tertiary volcanism, is illustrated. The vertical concentration profiles of As, Cd, Cr, Cu, Hg, Ni, Pb and Zn were studied in four sediment cores. Local BGVs were determined considering exclusively samples not affected by anthropogenic influence, recognized by means of multivariate statistics and radiochronological dating ((137)Cs and (210)Pb). Results showed BGVs well-comparable with mean crustal or shale values for most of the considered elements except for Hg (0.87 mg/kg d.w.) and As (16.87 mg/kg d.w.), due to mineralization present in the catchment basin draining into the lagoon.

Many methods allow analysing the various forms of tritium in environmental samples; however, there are no published standard methods for measuring organically bound tritium (OBT). Furthermore, there are no certified reference materials of OBT for environmental samples. In environmental samples (plants and animals), the measurement of the various tritium fractions requires extraction of the free water, often through freeze drying processes. Combustion of the dry sample is then carried out to recover organically bound tritium in the combustion water. By measuring these water fractions, the tissue-free water tritium (TFWT) and the OBT concentration can be assessed. However, these techniques are tricky and sometimes not available in all monitoring labs. Indeed, most of them measure only the TFWT fraction in food samples, such as wine or milk. Researches to promote the use of validated procedures are on-going in several countries. However, for almost all comparison exercise organisers it is difficult on a yearly basis to provide the samples and to realise the statistical treatment of the results. Therefore, to improve OBT analytical skills, an international task group devoted to the improvement of OBT analytical procedures was created to overcome these limitations. For the first exercise about 20 labs from 8 countries were registered. The samples, specially-prepared potatoes, were provided in March 2013 to each participant. Technical information and results from this first exercise are discussed here for all the labs which have realised the five replicates necessary to allow a reliable statistical treatment. From this work an optimised procedure can start to be developed to deal with OBT analysis and will guide subsequent planned OBT trials by the international group.

Analytical precision for Pb isotope measurement by thermal and plasma source mass spectrometry has improved by an order of magnitude in the last 20 years. Much of this improvement relates to a shift away from the external method of correcting instrumental mass fractionation – where samples are assumed to fractionate to the same extent as an average value of a working measurement standard. Implementation of a variety of techniques, including thallium spiking, sample–standard bracketing and double/triple spiking has provided more robust methods of fractionation correction. Isotope laboratories use one or more of these procedures, but an assessment of the measurement precision and relative merits of each system is needed to determine which is the most appropriate for the purpose. This study reviews each of these methods and provides a comparison based on an extensive analytical record covering 18 years, and using a variety of mass spectrometers. As two or three of the methods have been applied to most measurements, direct and robust comparisons can be made between correction protocols. In particular the effects of sample purity and variable sample matrices on measurement precision and accuracy have been examined. Data acquired from the measurement of rock, soil and metal are used to provide a statistical comparison of the analytical uncertainty of each technique, guiding the choice of the most appropriate method. Isotope standard data acquired over this period is also compared with other high-precision laboratories to generate a set of concordant working ratios for the NIST SRM 981 Pb standard: 206Pb/204Pb = 16.9412; 207Pb/204Pb = 15.4988; 208Pb/204Pb = 36.7233.

This paper describes an early-stage evaluation of a purpose-designed extraction / detection system that can be deployed by non-specialists either on-site or as part of a mobile laboratory. The system comprises three main components; (1) an optimised compact extraction system for recovery of radionuclides from the waste form; (2) an extraction test strip designed to recover the radionuclides from the waste digest; (3) a scintillation-based detection system capable of quantification of alpha, low energy beta and high energy beta emitting radionuclides. Data are presented on the preliminary assessment of the extraction / detection system for the measurement of 90Sr and 99Tc in aqueous wastes.

There is an increasing demand for rapid and effective analytical tools to support nuclear forensic investigations of seized or suspect materials. Some methods are simply adapted from other scientific disciplines and can effectively be used to rapidly prepare complex materials for subsequent analysis. A novel sample fusion method is developed, tested, and validated to produce homogeneous, flux-free glass beads of geochemical reference materials (GRMs), uranium ores, and uranium ore concentrates (UOC) prior to the analysis of 14 rare earth elements (REE) via laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS). The novelty of the procedure is the production of glass beads using 9 parts high purity synthetic enstatite (MgSiO3) as the glass former with 1 part of sample (sample mass ∼1.5 mg). The beads are rapidly prepared (∼10 min overall time) by fusing the blended mixture on an iridium strip resistance heater in an argon-purged chamber. Many elements can be measured in the glass bead, but the rare earth group in particular is a valuable series in nuclear forensic studies and is well-determined using LA-ICP-MS. The REE data obtained from the GRMs, presented as chondrite normalized patterns, are in very good agreement with consensus patterns. The UOCs have comparable patterns to solution ICP-MS methods and published data. The attractions of the current development are its conservation of sample, speed of preparation, and suitability for microbeam analysis, all of which are favorable for nuclear forensics practitioners and geochemists requiring REE patterns from scarce or valuable samples.

The efficient characterization of nuclear waste materials represents a significant challenge during nuclear site decommissioning, with a range of radionuclides requiring measurement in varied and often complex sample matrices. Of the available measurement techniques, inductively coupled plasma mass spectrometry (ICP-MS) has traditionally been applied to long-lived radionuclides, particularly in the actinide series. With recent advances in the technique, both the sensitivities achievable and number of radionuclides potentially measurable has expanded, with the reduced procedural time offering significant economic benefits to nuclear site waste characterization compared with traditional radiometric (typically alpha and beta spectrometry) techniques. This review provides a broad assessment of recent developments, improvements in capability and describes the advantages and drawbacks of ICP-MS with regards to sample introduction and instrument design. The review will be of interest to international agencies concerned with nuclear decommissioning as well as nuclear site laboratories, project managers and sites involved in environmental monitoring and nuclear forensics.

Advances in the sensitivities achievable by sector field inductively coupled plasma mass spectrometry (ICP-SFMS) offer the prospect of low-level measurement of shorter and longer lived radionuclides, thus expanding options for environmental and radioactively contaminated land assessment. In ICP-SFMS, the critical requirement for accurate detection is the effective chemical separation of isobaric and polyatomic interferences prior to sample introduction. As instrumental detection limit capability improves, accurate radionuclide determination requires highly effective separation materials that combine high analyte selectivity with subsequent quantitative analyte recovery compatible with ICP-SFMS detection. Two radioactive isotopes measurable by ICP-SFMS are the high yield fission products 135Cs and 137Cs that have entered the environment as a result of anthropogenic nuclear activities. ICP-SFMS enables reliable measurement of 135Cs/137Cs ratios, which can be used as a forensic tool in determining the source...