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There has been a considerable reduction in anthropogenic lead (Pb) emission in the atmosphere in recent decades. However, the reduction in Pb inputs in many lakes does not match this as the Pb stored in catchment upper soil layers, derived from previous deposition, has become an important source although it is difficult to assess quantitatively. This work uses atmospherically deposited 210 Pb as a tracer to track Pb movement, and so for the first time, we were able to calculate the relative Pb inputs from direct atmospheric deposition and catchment sources to lakes in the U.K. directly. Within individual lake sites, ratios of 210 Pb/Pb in the catchment terrestrial mosses were normally an order of magnitude higher than those in the catchment surface soils, trapped lake sediments, and the surface sediments in the lake bottom. Results suggest that the Pb isotope signatures in the mosses are close to or dominated by atmospheric depositions, and it is reasonable to use the ratios of 210 Pb/Pb in terrestrial mosses collected from the lake sites with a high annual rainfall over 2000 mm to represent those in atmospheric depositions. It reveals that after the reduction in Pb emissions, catchment Pb inputs now typically account for more than 95% of the total Pb entering the lakes.

Peat cores were collected from five bogs in the vicinity of open pit mines and upgraders of the Athabasca Bituminous Sands, the largest reservoir of bitumen in the world. Frozen cores were sectioned into 1 cm slices, and trace metals determined in the ultraclean SWAMP lab using ICP-QMS. The uppermost sections of the cores were age-dated with 210 Pb using ultralow background gamma spectrometry, and selected plant macrofossils dated using 14 C. At each site, trace metal concentrations as well as enrichment factors (calculated relative to the corresponding element/Th ratio of the Upper Continental Crust) reveal maximum values 10 to 40 cm below the surface which shows that the zenith of atmospheric contamination occurred in the past. The age-depth relationships show that atmospheric contamination by trace metals (Ag, Cd, Sb, Tl, but also V, Ni, and Mo which are enriched in bitumen) has been declining in northern Alberta for decades. In fact, the greatest contemporary enrichments of Ag, Cd, Sb, and Tl (in the top layers of the peat cores) are found at the control site (Utikuma) which is 264 km SW, suggesting that long-range atmospheric transport from other sources must be duly considered in any source assessment.

Floating islands mysteriously moving around on lakes were described by several Latin authors almost two millennia ago. These fascinating ecosystems, known as free-floating mires, have been extensively investigated from ecological, hydrological and management points of view, but there have been no detailed studies of their rates of accumulation of organic matter (OM), organic carbon (OC) and total nitrogen (TN). We have collected a peat core 4 m long from the free-floating island of Posta Fibreno, a relic mire in Central Italy. This is the thickest accumulation of peat ever found in a free-floating mire, yet it has formed during the past seven centuries and represents the greatest accumulation rates, at both decadal and centennial timescale, of OM (0.63 vs. 0.37 kg/m 2 /yr), OC (0.28 vs. 0.18 kg/m 2 /yr) and TN (3.7 vs. 6.1 g/m 2 /yr) ever reported for coeval peatlands. The anomalously high accretion rates, obtained using 14 C age dating, were confirmed using 210 Pb and 137 Cs: these show that the top 2 m of Sphagnum-peat has accumulated in only ~100 years. As an environmental archive, Posta Fibreno offers a temporal resolution which is 10x greater than any terrestrial peat bog, and promises to provide new insight into environmental changes occurring during the Anthropocene.

The residence time of (210)Pb created in the atmosphere by the decay of gaseous (222)Rn is a key parameter controlling its distribution and fallout onto the landscape. These in turn are key parameters governing the use of this natural radionuclide for dating and interpreting environmental records stored in natural archives such as lake sediments. One of the principal methods for estimating the atmospheric residence time is through measurements of the activities of the daughter radionuclides (210)Bi and (210)Po, and in particular the (210)Bi/(210)Pb and (210)Po/(210)Pb activity ratios. Calculations used in early empirical studies assumed that these were governed by a simple series of equilibrium equations. This approach does however have two failings; it takes no account of the effect of global circulation on spatial variations in the activity ratios, and no allowance is made for the impact of transport processes across the tropopause. This paper presents a simple model for calculating the distributions of (210)Pb, (210)Bi and (210)Po at northern mid-latitudes (30°-65°N), a region containing almost all the available empirical data. By comparing modelled (210)Bi/(210)Pb activity ratios with empirical data a best estimate for the tropospheric residence time of around 10 days is obtained. This is significantly longer than earlier estimates of between 4 and 7 days. The process whereby (210)Pb is transported into the stratosphere when tropospheric concentrations are high and returned from it when they are low, significantly increases the effective residence time in the atmosphere as a whole. The effect of this is to significantly enhance the long range transport of (210)Pb from its source locations. The impact is illustrated by calculations showing the distribution of (210)Pb fallout versus longitude at northern mid-latitudes., (Copyright © 2016 Elsevier Ltd. All rights reserved.)

Lead (Pb) released from anthropogenic sources and stored in environmental repositories can be a potential source for secondary pollution. Here we develop a novel approach for tracking Pb from atmospheric deposition and other sources in the environment using fallout (210)Pb as a tracer, and apply the method to samples collected from Richmond Park, London, the UK. The mean ratio of (210)Pb to total Pb in atmospheric depositions collected from a site adjacent to the park during August-October 2012 was 96 Bq mg(-1), while the ratio in surface soils from the park was typically an order of magnitude lower. The difference between these values made it possible to trace the source of Pb in the plants. The (210)Pb/Pb ratios in plants varied from 0 to 34 Bq mg(-1) indicating different levels of Pb absorption from the atmosphere. The ratio in mosses had an average value of 22 Bq mg(-1). This suggests that only around 20% of the Pb they contain was from direct atmospheric deposition, revealing possible limitations in the use of terrestrial mosses for monitoring atmospheric pollution. As well as tracking sources, variations in the (210)Pb/Pb ratio can also reveal ways in which Pb is transferred within plants.

Cadmium zinc telluride (CdZnTe or CZT) is the leading semiconductor detector for gamma spectroscopy at room temperature. In the present study, a coplanar-grid CZT detector was used for gamma-ray measurements of environmental radioactivity on a contaminated saltmarsh sediment core in comparison with results from a coaxial high-purity germanium detector to assess their comparative performance. The findings reveal that the CZT performs well for both (241)Am and (137)Cs measurements over a broad range of activities, despite limited detector efficiency, and can be used to good effect in the study of environmental radioactivity in contaminated estuarine settings.

The present study focuses on the detection of Sellafield-derived (137)Cs and (241)Am in contaminated saltmarshes from North-West England, UK, with a view to assessing the radiological impacts from radioactivity stored within the sediment record. The surface activities from these radionuclides were found in the range between 73 and 851 Bq kg(-1) whereas peak activities ranging from 383 to 12690 Bq kg(-1) were found below the surface of the upper marsh at a depth of approximately 5-20 cm. Potential radioactive exposure to humans from these highly active radionuclides comes mainly from direct exposure and resuspended dust inhalation for different saltmarsh users, which may be exacerbated by the remobilisation of radionuclides resulting from saltmarsh erosion. The total annual minimum, maximum and 'best estimate' doses ranging from 11 to 972 μSv y(-1), fall below the ICRP-recommended annual dose limit, but the highest estimated total effective dose (972 μSv y(-1)) for a marsh user falls within 97% of the recommended dose limit and the highest 'best estimate' total annual doses of 110 and 307 μSv y(-1) for Dee estuary and Biggar marshes, respectively, are almost 3 and 4 times higher than the estimated doses that are based on existing surface activities., (Copyright © 2011 Elsevier Ltd. All rights reserved.)

(210)Pb-dated sediment cores taken from lakes on the Falkland Islands, the South Orkney Islands, and the Larsemann Hills in Antarctica were analyzed for fly ash particles to assess the temporal record of contamination from high temperature fossil-fuel combustion sources. Very low, but detectable, levels were observed in the Antarctic lakes. In the Falkland Island lakes, the record of fly ash extended back to the late-19th century and the scale of contamination was considerably higher. These data, in combination with meteorological, modeling, and fossil-fuel consumption data, indicate most likely sources are in South America, probably Chile and Brazil. Other southern hemisphere sources, notably from Australia, contribute to a background contamination and were more important historically. Comparing southern polar data with the equivalent from the northern hemisphere emphasizes the difference in contamination of the two circumpolar regions, with the Falkland Island sites only having a level of contamination similar to that of northern Svalbard.

Seasonal snowpack, lichens, and lake sediment cores were collected from fourteen lake catchments in eight western U.S. National Parks and analyzed for sixteen polycyclic aromatic hydrocarbons (PAHs) to determine their current and historical deposition, as well as to identify their potential sources. Seasonal snowpack was measured to determine the current wintertime atmospheric PAH deposition; lichens were measured to determine the long-term, year around deposition; and the temporal PAH deposition trends were reconstructed using lake sediment cores dated using (210)Pb and (137)Cs. The fourteen remote lake catchments ranged from low-latitude catchments (36.6 degrees N) at high elevation (2900 masl) in Sequoia National Park, CA to high-latitude catchments (68.4 degrees N) at low elevation (427 masl) in the Alaskan Arctic. Over 75% of the catchments demonstrated statistically significant temporal trends in SigmaPAH sediment flux, depending on catchment proximity to source regions and topographic barriers. The SigmaPAH concentrations and fluxes in seasonal snowpack, lichens, and surficial sediment were 3.6 to 60,000 times greater in the Snyder Lake catchment of Glacier National Park than the other 13 lake catchments. The PAH ratios measured in snow, lichen, and sediment were used to identify a local aluminum smelter as a major source of PAHs to the Snyder Lake catchment. These results suggest that topographic barriers influence the atmospheric transport and deposition of PAHs in high-elevation ecosystems and that PAH sources to these national park ecosystems range from local point sources to diffuse regional and global sources.

An analytical method was developed for the trace analysis of 98 semivolatile organic compounds (SOCs) in remote, high-elevation lake sediment. Sediment cores from Lone Pine Lake (west of the Continental Divide) and Mills Lake (east of the Continental Divide) in Rocky Mountain National Park, CO, were dated using 210Pb and 137Cs and analyzed for polybrominated diphenyl ethers (PBDEs), organochlorine pesticides, phosphorothioate pesticides, thiocarbamate pesticides, amide herbicides, triazine herbicides, polychlorinated biphenyls (PCBs), and polycyclic aromatic hydrocarbons (PAHs) using this method. SOC deposition profiles were reconstructed, and deposition half-lives and doubling times were calculated, for U.S. historic-use pesticides (HUPs) and current-use pesticides (CUPs) as well as PBDEs, PCBs, and PAHs. Sediment records indicate that the deposition of CUPs has increased in recent years, while the deposition of HUPs has decreased since U.S. restriction, but has not been eliminated. This is likely due to the revolatilization of HUPs from regional soils, atmospheric transport, and deposition. Differences in the magnitude of SOC sediment fluxes, flux profiles, time trends within those profiles, and isomeric ratios suggest that SOC deposition in high-elevation ecosystems is dependent on regional upslope wind directions and site location with respect to regional sources and topographic barriers.

The Taunton River is a partially mixed tidal estuary in southeastern Massachusetts (USA) which has received significant contaminant inputs, yet little information exists on the history of discharge and the subsequent fate of these contaminants. Three sediment cores taken along a transect were analyzed, reconstructing the spatial and temporal trends of pollution in the estuary. A combination of radiometric dating, contaminant markers, and storm layers from major hurricanes were used to establish age models and sedimentation rates. Age estimates obtained from the different dating methods compared well, establishing an accurate history of contaminant release to the estuary. Polycyclic aromatic hydrocarbons (PAHs) were present in one core at depths corresponding to the early 1860s, earlier than previously established dates of introduction. Temporal and spatial trends of Cr, Cu, Hg and Pb indicated multiple sources of varying input to the river. Polychlorinated biphenyls (PCBs) were present in each of the cores from the 1930s onward, with elevated levels still present in surficial sediments at several sites. A unique organic compound, Topanol, which was produced locally was used as a tracer to track contaminant transport in the river. Tracer data indicates that contaminants are still being transported and deposited to surficial sediments at high concentrations well after their discharge. This reconstruction demonstrates the utility of using multiple dating proxies where often the sole use of radiometric dating techniques is not an option and provides insights into the fate of contaminants discharged decades ago but continue to represent environmental risks.

Tributyltin (TBT) is an organotin compound used since the early 1960s as a biocide in boat antifouling paints. Its use has been linked to a host of negative effects in marine ecosystems including malformations and imposex in Mollusca and acute toxicity in many other aquatic animals. Yet, the consequences of TBT use in freshwaters are largely unknown. Here, for the first time we reveal that TBT may have caused hitherto unsuspected damage to freshwater ecosystems. Through an analysis of dated sediment cores collected from a system of recreationally boated, shallow lakes, we show that first evidence of TBT is associated with a dramatic loss of submerged vegetation and associated diverse animal communities. Cause and effect are difficult to unravel in our study. However, we hypothesize that TBT, through reducing populations of grazing organisms in lakes already affected by eutrophication, promoted the replacement of macrophytes by phytoplankton, ultimately leading to a regime shift in the ecosystem. Our findings may have parallels in freshwater ecosystems all over the world.

The (239+240)Pu activity profile is determined for a sediment core collected from 170-m depth at Loch Ness, Scotland. These measurements use magnetic sector inductively coupled plasma mass spectrometry for rapid determination of Pu activities and (240)Pu/(239)Pu atom ratios. A (239+240)Pu detection limit of 0.1 Bq/kg is obtained for 2 g of acid-leached sediment; (242)Pu is used as a spike isotope. The Pu activity profile exhibits a maximum of 42.7+/-0.3 Bq/kg (239+240)Pu in the 9-10-cm depth interval. The position of this maximum coincides with peaks in the (241)Am and (137)Cs activity profiles. These peak activities are ascribed to the 1963/1964 peak fallout from atmospheric testing of nuclear weapons. The (240)Pu/(239)Pu atom ratios are in the range 0.15-0.20, in agreement with the expected range of 0.166-0.194 for Northern Hemisphere fallout, and do not suggest the presence of other contributing sources. This study demonstrates that ICPMS has considerable potential for rapid determination of the chronology of post-1950 sediments, and also for validating (210)Pb dates where chronologies over longer time-scales are needed.

A peat core collected at Etang de la Gruère, an ombrotrophic bog in the Jura Mountains of Switzerland, was analyzed for organolead species (DEL, TEL, DML, and TML) using GC-MIP AES, Pb isotopes using TIMS, and total Pb using XRF and age-dated using 210Pb. The earliest occurrence of quantifiable alkyllead is found at a depth of 24 cm, which is dated at AD 1946 +/- 3; this finding is consistent with the introduction of leaded gasoline in Switzerland in 1947. The maximum concentration of alkyllead (2.89 ng/g) is found at 5 cm, which is dated at AD 1988 +/- 2. This same sample yielded 206Pb/207Pb = 1.1254, which is the least radiogenic value in the entire 2K core and comparable to the isotopic composition of Pb in leaded gasoline. The highest concentrations of DML (906 ng/g) and DEL (1906 ng/g) also were found in this sample. Total alkyllead never accounts for more than 0.02% of total Pb in any given sample. The spatial and temporal variations in organolead species is matched by the changes in the isotopic composition of Pb over the same interval. Despite this, the decline in anthropogenic Pb pre-dates the maximum in total alkyllead and minimum 206Pb/207Pb, indicating that atmospheric Pb emissions had already begun their decline prior to the introduction of unleaded gasoline. In fact the decline in anthropogenic Pb was probably in response to the introduction of legislation, first in Germany and later in the European Union, establishing a maximum allowable concentration of Pb in gasoline.

The temporal evolution of atmospheric lead deposition and its possible sources were assessed in eastern Canada and in western Scotland, using blanket peat bogs as geochemical archives. Short cores were taken from two remote sites located close to the sea. Significant lead enrichments in the upper layers at both sites reflect the increasing emission of lead into the atmosphere due to anthropogenic activities during the last century. At the Scottish site, a region under aeolian influence from Europe, anthropogenic derived lead could be recognized by the distinctive unradiogenic composition (206Pb/207Pb ratios down to approximately 1.115), being clearly different from the pre-industrial values (206Pb/207Pb approximately 1.166). In contrast, the lead pollution in eastern Canada (influenced by North American sources) is identified by a more radiogenic lead isotope composition (206Pb/207Pb ratios up to approximately 1.199) compared to preindustrial values (206Pb/207Pb approximately 1.161). Emission inventories and isotope characteristics suggest that industrial (coal burning, mining) and traffic (leaded gasoline) outputs are the most likely sources during the first and the second half of the 20th century, respectively, in both, western Scotland and eastern Canada alike. The Scottish record is in line with previous studies of past atmospheric lead deposition. However, the Canadian deposit suggests that the wind derived, pre-industrial lead, is less radiogenic as previously implied using sediment archives. These results are thus the first to report pre-industrial lead isotope ratios and concentrations of atmospheric derived aerosols in North America.

The objective of this paper is to report on the results of a study of 238Pu, 239 + 240Pu and 241Am inventories onto Blelham Tarn in Cumbria (UK). The atmospheric fallout inventory was obtained by analysing soil cores and the results are in good agreement with the literature: 101 Bq m(-2) for 239 + 240Pu; 4.5 Bq m(-2) for 238Pu and 37 Bq m(-2) for 241Am. The sediment core inventory for the whole lake is compared to the atmospheric fallout inventory. The sediment activity is 60-80% higher than the estimated fallout activity, showing a catchment area contribution and in particular the stream input.

The study of fish concentrations and sediment inventories in 19 European high mountain lakes (40-67 degrees N) shows that a fraction of organochlorine compounds (OCs), the less volatile compounds (LVC; subcooled liquid vapor pressure < or = 10(-2.5) Pa), are trapped in the higher locations. This general trend is not significantly influenced by possible local sources. Compound distribution is related to average air temperatures. The phase-change pseudoenthalpies calculated from the sediment inventories closely match the summed theoretical volatilization and dissolution enthalpies. This fractionation effect is responsible for the accumulation of high concentrations of the LVC, the more persistent and toxic according to literature data, in organisms inhabiting sites far from the locations of synthesis or use.

The Arctic is recognized as an important focus for long-range transport of contaminants, such as mercury (Hg), from industrial regions at lower latitudes. In addition to large geographic gaps, there are few long-term retrospective time trends in arctic research, besides the Greenland ice record, to assess the onset of atmospheric pollution as well as to establish the rates of change in the terrestrial environment. In a study of sediments from 21 lakes along a 150 km transect from the coast to the ice sheet margin in the Søndre Strømfjord (Kangerlussuaq) region, we present stratigraphic evidence for elevated Hg inputs to this ice-free region on Greenland's west coast. Nineteen study lakes showed Hg concentration enrichments (HgEFconc) in surface compared to deeper sediments, with a mean HgEFconc of 3. Higher HgEFconc are found in lakes closest to the ice margin. The existence of this Hg gradient is supported by pollution Hg inventories in three 210Pb-dated cores. While 210Pb inventories and Pb pollution are higher at the coast, pollution Hg inventories are nearly 3-fold higher at the ice margin (570 micrograms m-2) than at the coast (210 micrograms m-2). These dated cores also indicate an onset of Hg pollution in the region beginning at least by the late 19th century but possibly as early as the 17th century.

A continuous record of atmospheric lead since 12,370 carbon-14 years before the present (14C yr BP) is preserved in a Swiss peat bog. Enhanced fluxes caused by climate changes reached their maxima 10, 590 (14)C yr BP (Younger Dryas) and 8230 (14)C yr BP. Soil erosion caused by forest clearing and agricultural tillage increased lead deposition after 5320 (14)C yr BP. Increasing lead/scandium and decreasing lead-206/lead-207 beginning 3000 (14)C yr BP indicate the beginning of lead pollution from mining and smelting, and anthropogenic sources have dominated lead emissions ever since. The greatest lead flux (15.7 milligrams per square meter per year in A.D. 1979) was 1570 times the natural, background value (0.01 milligram per square meter per year from 8030 to 5320 (14)C yr BP).

As part of the UK Ministry of Agriculture Fisheries and Food Directorate of Fisheries Research (MAFF/DFR) post-Chernobyl monitoring program, a detailed study was carried out of the change over time in dissolved-phase 137Cs concentrations in a number of lakes in Cumbria, UK. These measurements have been combined with published data on 137Cs in Cumbrian and other European lakes in order to develop and test a "double exponential" model for changes in lakewater concentrations: A exp(-k1t) + B exp(-k2t) where the exponential terms correspond, respectively, to the initial fast flush of activity through the system followed by longer-term transfers (timescale, years) from the catchment. Parameter values have been determined for this model by curve-fitting to the set of measurements of post-Chernobyl 137Cs activities in lakes. Values of fitted parameters are shown to be related, in a simple manner, to the physical characteristics of the system, in particular water residence time and mean lake depth. These parameters are generalized to give a simple empirical model for the full set of study lakes. The model is shown to give estimates of 137Cs activity to within a factor of 5 of field data for a period of several years after the fallout. Initial fractional losses of activity from catchment to lake were determined to be within the range 0.44-8.7% per year, declining exponentially with a mean rate constant 0.98 x 10(-3) d(-1).

Inventories of weapons-test and Chernobyl derived (137)Cs within the upper Wye and upper Severn catchments have been estimated using a variety of techniques. Transport rates of radiocaesium from the catchments have been determined from measurements of radionuclide activities on suspended and bedload sediments. Radiocaesium transport coefficients calculated from the results of 0.46-5.42 x 10(-3) y(-1) for freshly deposited Chernobyl (137)Cs contrast with that for older weapons-test fallout (137)Cs deposits (0.035-0.36 x 10(-3) y(-1)). These results show that freshly deposited Chernobyl (137)Cs is presently being lost at a significantly higher rate than weapons-test derived (137)Cs. For (137)Cs from both sources, residence times in the undisturbed upper Wye catchment are significantly higher than in the afforested upper Severn catchments.