Atmospheric residence time of (210)Pb determined from the activity ratios with its daughter radionuclides (210)Bi and (210)Po.

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.

Potential health risks from radioactive contamination of saltmarshes in NW England.

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.

Assessing CZT detector performance for environmental radioactivity investigations.

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.

New peat bog record of atmospheric lead pollution in Switzerland: Pb concentrations, enrichment factors, isotopic composition, and organolead species.

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.

Plutonium and americium inventories in atmospheric fallout and sediment cores from Blelham Tarn, Cumbria (UK).

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.

Selective trapping of organochlorine compounds in mountain lakes of temperate areas.

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.

Mercury accumulation rates and spatial patterns in lake sediments from west Greenland: a coast to ice margin transect.

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.

Towards a generalized model for the primary and secondary contamination of lakes by Chernobyl-derived radiocesium.

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).

Rates of removal of sediment associated radiocaesium from the plynlimon experimental catchments, Powys, UK.

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.