226Ra and 228Ra in scale and sludge samples and their correlation with the chemical composition

In order to contribute to a future waste management policy related to the presence of technologically enhanced natural occurring radioactive material (TENORM) in the Brazilian petroleum industry, the present work presents the chemical composition and the (226)Ra and (228)Ra content of sludge and scales generated during the offshore E and P petroleum activities in the Campos Basin, the primary offshore oil production region in Brazil. The (226)Ra and (228)Ra content on 36 sludge and scales samples were determined by gamma-spectrometry. Based on X-ray diffractometry results, a chemical analysis schema for these samples was developed. The results have shown that scales are 75% barium and strontium sulfates, with a mean (226)Ra and (228)Ra content of 106 kBq kg(-1) and 78 kBq kg(-1), respectively. On the other hand, sludge samples have a much more complex chemical composition than the scales. The (226)Ra and (228)Ra content in sludge also varies much more than the content observed in the scales samples and ranged from 0.36 to 367 kBq kg(-1) and 0.25 to 343 kBq kg(-1), respectively.     

Seasonal variation of Ra/Ra ratio in seaweed: implications for water circulation patterns in coastal areas of the Noto Peninsula, Japan

To examine water circulation patterns of coastal water, 72 seaweed (Sargasso) samples and 27 coastal water samples were collected from coastal areas of the Noto Peninsula, Japan, during the period from December 1998 to June 2002. The (228)Ra and (226)Ra activities of those samples were measured by low-background gamma-ray spectrometry. There was a wide range of activities of (228)Ra (0.5-2Bq/kg-fresh) and (226)Ra (0.5-1.2Bq/kg-fresh) in the Sargasso samples. The (228)Ra/(226)Ra activity ratio of Sargasso samples exhibited seasonal variation with minimum values in June ((228)Ra/(226)Ra= approximately 1) and maximum values in December (1.5-2.5), which was mainly governed by changes in (228)Ra activity. It is also notable that the seasonal variation of the (228)Ra/(226)Ra ratio of Sargasso is in approximate agreement with that of the ambient coastal water. Sargasso samples appear to have retained the (228)Ra/(226)Ra ratio of the ambient coastal waters, and the temporal variations in that ratio provide insight into seasonal changes in water circulation in the Noto Peninsula coastal area.     

Time-series sampling of Ra and Ra at the inlet to Great South Bay (New York): a strategy for characterizing the dominant terms in the Ra budget of the bay

Ra isotopes are a powerful tool for quantifying the flux of submarine groundwater discharge (SGD) into the sea. Previous studies of ²²³Ra and ²²⁴Ra mass balances in coastal embayments have shown that the Ra balance is dominated by supply via SGD, exchange with the open ocean and radioactive decay. The current study shows that a single time series over a tidal cycle at the principal inlet to Great South Bay (NY, US) is sufficient to determine the net flux of Ra across the inlet, and also can be used to estimate the decay of short-lived Ra in the bay. Estimates of the net Ra flux obtained from a single tidal time-series by using three different approaches agree with those determined from a more time-consuming survey of Ra within the bay, and may represent a first step of estimating SGD in bays and coastal lagoons.     

Environmental fate of Ra in cation-exchange regeneration brine waste disposed to septic tanks, New Jersey Coastal Plain, USA: migration to the water table

Fate of radium (Ra) in liquid regeneration brine wastes from water softeners disposed to septic tanks in the New Jersey Coastal Plain was studied. Before treatment, combined Ra (²²⁶Ra plus ²²⁸Ra) concentrations (maximum, 1.54 Bq L⁻¹) exceeded the 0.185 Bq L⁻¹ Maximum Contaminant Level in 4 of 10 studied domestic-well waters (median pH, 4.90). At the water table downgradient from leachfields, combined Ra concentrations were low (commonly ≤0.019 Bq L⁻¹) when pH was >5.3, indicating sequestration; when pH was ≤5.3 (acidic), concentrations were elevated (maximum, 0.985 Bq L⁻¹ - greater than concentrations in corresponding discharged septic-tank effluents (maximum, 0.243 Bq L⁻¹)), indicating Ra mobilization from leachfield sediments. Confidence in quantification of Ra mass balance was reduced by study design limitations, including synoptic sampling of effluents and ground waters, and large uncertainties associated with analytical methods. The trend of Ra mobilization in acidic environments does match observations from regional water-quality assessments.     

Bioaccumulation and lack of oxidative stress response in the ragworm H. diversicolor following exposure to Ra in sediment

The main effluent from oil and gas production, produced water, from some platforms in the North Sea contains elevated concentrations of ²²⁶Ra. The aim of this study was to investigate whether ²²⁶Ra in sediment would accumulate in and affect sediment-dwelling organisms. In addition, we wanted to determine if the bioavailability would be modulated by the presence of a scale inhibitor which is used during oil and gas production. Hediste diversicolor was therefore exposed to different levels of ²²⁶Ra (30–6600 Bq kg⁻¹) in combination with scale inhibitor in the sediments in a flow through system. The levels of radioactivity in the exposures were close to levels that can be measured in proximity to oil/gas production facilities. ²²⁶Ra spiked to natural sediment partitioned into pore water and accumulated in the sediment-dwelling polychaete following a four-week exposure period. The results suggest that ²²⁶Ra did not bind strongly to sediment (low sediment:water partitioning coefficient), but it was not shown to bioaccumulate in any great extent (bioaccumulation factors of 0.019–0.022). Exposure of H. diversicolor in sediments with up to 6600 Bq kg⁻¹²²⁶Ra had no measurable effect on the total oxyradical scavenging capacity of the organisms compared to control. So although they accumulated the alpha-emitter, the treatments did not appear to cause oxidative stress in polychaete tissues.     

Bioaccumulation of Ra by plants growing in fresh water ecosystem around the uranium industry at Jaduguda, India

A field study has been conducted to evaluate the ²²⁶Ra bioaccumulation among aquatic plants growing in the stream/river adjoining the uranium mining and ore-processing complex at Jaduguda, India. Two types of plant group have been investigated namely free floating algal species submerged into water and plants rooted in stream & riverbed. The highest ²²⁶Ra activity concentration (9850 Bq kg⁻¹) was found in filamentous algae growing in the residual water of tailings pond. The concentration ratios of ²²⁶Ra in filamentous algae (activity concentration of ²²⁶Ra in plant Bq kg⁻¹ fresh weight/activity concentration of ²²⁶Ra in water Bq l⁻¹) widely varied i.e. from 1.1 × 10³ to 8.6 × 10⁴. Other aquatic plants were also showing wide variability in the ²²⁶Ra activity concentration. The ln-transformed filamentous algae ²²⁶Ra activity concentration was significantly correlated with that of ln-transformed water concentration (r = 0.89, p < 0.001). There was no correlation between the activity concentrations of ²²⁶Ra in stream/riverbed rooted plants and the substrate. For this group, correlation between ²²⁶Ra activity concentration and Mn, Fe, Cu concentration in plants were statistically significant.     

Origin and transport of U and Ra in riverine,estuarine and marine sediments of the Krka River,Croatia

Spatial distribution of ²³⁸U and ²²⁶Ra activities in sediment columns along the Krka River and estuary, were studied using gamma spectrometry. Markedly different ²³⁸U and ²²⁶Ra activities between riverine, estuarine and marine sediments were observed. Distribution of these radionuclides, as well as their anthropogenic and natural origin, was evaluated by activity measurements, taking into account sedimentation rates estimated by ¹³⁷Cs distribution in sediment columns.     

Suitable gamma energy for gamma-spectrometric determination of U in surface soil samples of a high rainfall area in India

The paper presents a systematic study on suitability of various gamma lines for monitoring of ²³⁸U activity in soil samples around a uranium mineralized zone of Kylleng Pyndengsohiong Mawthabah (Domiasiat), Meghalaya in India. The area lies in a plateau region which recieves the highest average annual rainfall (12,000 mm) in the world. The geochemical behaviour of the uranium and its daughter products at such wet climatic conditions imposes restrictions to assess ²³⁸U through gamma lines of radon decay products. Soil samples were collected from nine locations around the uranium mineralization zone for analysis. The ratio of the concentration of uranium obtained from gamma energies of radium daughter products to the 63.29 keV of ²³⁴Th was found to vary from 1.01 to 2.07, which indicates a pronounced disequilibrium between uranium and radium daughters. The results obtained from various gamma energies were validated from the data generated by Instrumental Neutron Activation Analysis (INAA) technique. The ²³⁸U activities from the two analytical methods show a well fitted regression line with correlation coefficient 0.99 which validates the reliability of 63.29 keV energy for estimation of uranium in such conditions.     

Ra–Po–Pb isotope systematics in waters of Sambhar Salt Lake,Rajasthan (India): geochemical characterization and particulate reactivity

The Sambhar Salt Lake hydrological system, including river waters, groundwaters, evaporating pans and sub-surface brines, has been analyzed for the salt content (TDS) and naturally occurring radionuclides (²¹⁰Po, ²¹⁰Pb and ^226,228Ra). The abundance of these radionuclides and their activity ratios show a wide variation in different hydrological regimes, which helps to geochemically characterize the lake system. A significantly lower Ra to total dissolved solids (TDS) ratio in the brines (by two to three orders of magnitude), when compared to the groundwaters and river waters, suggests removal of dissolved Ra by co-precipitation with Ca–Mg minerals at an early stage of the brine evolution. The concentration of Ra in evaporating lake/pan waters saturates at a value of about 35 Bq L⁻¹ over the salinity range of 100–370 g L⁻¹; attributable to its equilibration with the clay minerals. The two distinct regimes, saline lake system (lake water, evaporating pans and sub-surface brines) and groundwaters have been identified based on their differences in the distribution of ^226,228Ra isotopes. This observation points to the conclusion that the groundwaters and the lake brines are not intimately coupled in terms of their origin and evolution. The abundances of ²¹⁰Po and ²¹⁰Pb along with their activity ratios (²¹⁰Po/²¹⁰Pb) are markedly different among the surface lake waters/evaporating pans, sub-surface lake brines and groundwaters. These differences are explained in terms of different geochemical behaviour of these nuclides in presence of algae and organic matter present in these water regimes.     

External gamma-ray dose rate and radon concentration in indoor environments covered with Brazilian granites

Health hazard from natural radioactivity in Brazilian granites, covering the walls and floor in a typical dwelling room, was assessed by indirect methods to predict external gamma-ray dose rates and radon concentrations. The gamma-ray dose rate was estimated by a Monte Carlo simulation method and validated by in-situ measurements with a NaI spectrometer. Activity concentrations of ²³²Th, ²²⁶Ra, and ⁴⁰K in an extensive selection of Brazilian commercial granite samples measured by using gamma-ray spectrometry were found to be 4.5-450 Bq kg⁻¹, 4.9-160 Bq kg⁻¹ and 190-2029 Bq kg⁻¹, respectively. The maximum external gamma-ray dose rate from floor and walls covered with the Brazilian granites in the typical dwelling room (5.0 m × 4.0 m area, 2.8 m height) was found to be 120 nGy h⁻¹, which is comparable with the average worldwide exposure to external terrestrial radiation of 80 nGy h⁻¹ due to natural sources, proposed by United Nations Scientific Committee on the Effects of Atomic Radiation. Radon concentrations in the room were also estimated by a simple mass balance equation and exhalation rates calculated from the measured values of ²²⁶Ra concentrations and the material properties. The results showed that the radon concentration in the room ventilated adequately (0.5 h⁻¹) will be lower than 100 Bq m⁻³, value recommended as a reference level by the World Health Organization.     

137Cs in marine samples from the Brazilian southeastern coastal region

The present work presents the results of ¹³⁷Cs concentration in seawater, fish and sediments samples collect in 11 sampling points, crossing the Brazilian Southeastern coastal region, from Vitória (ES) to Santos (SP), on a routine basis from 1997 to 2002. This monitoring program was carried out by the Instituto de Radioproteção e Dosimetria (IRD/CNEN/MCT), in cooperation with the Instituto de Estudos do Mar Almirante Paulo Moreira (IEAPM/Brazilian Navy), aiming at determining artificial radionuclides in marine samples. Additionally to the ¹³⁷Cs results, ⁹⁰Sr concentrations in fish samples from 1998 to 2002 are also reported.The ¹³⁷Cs in seawater follows a lognormal distribution, with a geometric mean of 1.8 Bq m^-3 and a geometric standard deviation of 1.4 (n=54), decay corrected to June/2002. For ¹³⁷Cs levels in fish samples a geometric mean of 0.19 Bq kg⁻¹ and a geometric standard deviation of 2.9 (n=39), decay corrected to June/2002, with a range of 0.03 to 1.7 Bq kg⁻¹, were obtained. Based on the ¹³⁷Cs mean concentration in fish as well as in seawater, a transfer factor of 1 × 10² was calculated, which is quite in agreement with the recommended value found in the Safety Report Serie 19.     

Concentrations of U,U, U,Th, Th,Th, Ra,Ra, Ra,Po, Pb and Pb in drinking water in Italy: reconciling safety standards based on measurements of gross α and β

Some important naturally occurring α- and β-radionuclides in drinking water samples collected in Italy were determined and the radiological quality evaluated. The mean activity concentrations (mBq L⁻¹) of the radionuclides in the water samples were almost in the order: 26 ± 36 (²³⁴U) > 21 ± 30 (²³⁸U) > 8.9 ± 15 (²²⁶Ra) > 4.8 ± 6.3 (²²⁸Ra) > 4.0 ± 4.1 (²¹⁰Pb) > 3.2 ± 3.7 (²¹⁰Po) > 2.7 ± 1.2 (²¹²Pb) > 1.4 ± 1.8 (²²⁴Ra) > 1.1 ± 1.3 (²³⁵U) > 0.26 ± 0.39 (²²⁸Th) > 0.0023 ± 0.0009 (²³⁰Th) > 0.0013 ± 0.0006 (²³²Th). The mean estimated dose (μSv yr⁻¹) to an adult from the water intake was in this order: 2.8 ± 3.3 (²¹⁰Po) > 2.4 ± 3.2 (²²⁸Ra) > 2.1 ± 2.1 (²¹⁰Pb) > 1.8 ± 3.1 (²²⁶Ra) > 0.94 ± 1.30 (²³⁴U) > 0.70 ± 0.98 (²³⁸U) > 0.069 ± 0.087 (²²⁴Ra) > 0.036 ± 0.044 (²³⁵U) > 0.014 ± 0.021 (²²⁸Th) > 0.012 ± 0.005 (²¹²Pb) > 0.00035 ± 0.00029 (²³⁰Th) > 0.00022 ± 0.00009 (²³²Th). It is obvious that ²¹⁰Po, ²²⁸Ra, ²¹⁰Pb and ²²⁶Ra are the most important dose contributors in the drinking water intake. As far as the seventeen brands of analysed drinking water were concerned, the committed effective doses were in the range of 2.81–38.5 μSv yr⁻¹, all well below the reference level of the committed effective dose (100 μSv yr⁻¹) recommended by the WHO. These data throw some light on the scale of the radiological impact on the public from some naturally occurring radionuclides in drinking water, and can also serve as a comparison for the dose contribution from artificial radionuclides released to the environment as a result of human practices. Based on the radionuclide composition in the analysed waters, comment was made on the new screening level for gross α activity in guidelines for drinking-water quality recommended by the WHO, 2004.     

Radium and radium-daughter nuclides in carbonates: a brief overview of strategies for determining chronologies

Radium isotopes have been used extensively to trace the movement of groundwater as well as oceanic water masses, but these radionuclides (and their daughters) are also useful chronometers for the determination of the time scales of other Earth and environmental processes. The purpose of this overview is to present the application of Ra and Ra daughters in the dating of carbonates. We show that the choice of dating method (decay of excess radionuclide or ingrowth of daughter) depends strongly on the parent/daughter activity ratios in the water in which the carbonate was precipitated. Thus freshly precipitated carbonates uniformly show excesses of ²²⁶Ra relative to its parent ²³⁰Th, and ²²⁶Ra decay can provide ages of carbonates over Holocene time scales. In contrast, carbonates are precipitated in waters of greatly varying ²¹⁰Pb/²²⁶Ra. Corals, deep-sea hydrothermal vent clams and the shelled cephalopod Nautilus live in waters with significant dissolved ²¹⁰Pb and all show excesses of ²¹⁰Pb in their carbonate. Bivalve molluscs from nearshore and coastal waters, and carbonates deposited from groundwater environments (e.g. travertines) in which ²¹⁰Pb is efficiently scavenged from solution, show deficiencies of ²¹⁰Pb relative to ²²⁶Ra. In contrast, fish otoliths strongly discriminate against ²¹⁰Pb regardless of the environment in which the fish lives. Deficiencies of ²²⁸Th relative to ²²⁸Ra are common in all carbonates. Useful time ranges for the ²¹⁰Pb/²²⁶Ra and ²²⁸Th/²²⁸Ra chronometers are ∼100 y and ∼10 y, respectively.     

Radioactivity measurements in moss (Hypnum cupressiforme) and lichen (Cladonia rangiformis) samples collected from Marmara region of Turkey

The present study was conducted to compare the ¹³⁷Cs, ⁴⁰K, ²³²Th, and ²³⁸U activity concentrations in epigeic moss (Hypnum cupressiforme) and lichen (Cladonia rangiformis). The activity levels in 37 moss and 38 lichen samples collected from the Marmara region of Turkey were measured using a gamma spectrometer equipped with a high purity germanium (HPGe) detector. The activity concentrations of ¹³⁷Cs, ⁴⁰K, ²³²Th, and ²³⁸U in the moss samples were found to be in the range of 0.36-8.13, 17.1-181.1, 1.51-6.17, and 0.87-6.70 Bq kg⁻¹ respectively, while these values were below detection limit (BDL)-4.32, 16.6-240.0, 1.32-6.47, and BDL-3.57 Bq kg⁻¹ respectively in lichen. The average moss/lichen activity ratios of ¹³⁷Cs, ⁴⁰K, ²³²Th, and ²³⁸U were found to be 1.32 ± 0.57, 2.79 ± 1.67, 2.11 ± 0.82, and 2.19 ± 1.02, respectively. Very low ¹³⁷Cs concentrations were observed in moss and lichen samples compared to soil samples collected from the same locations in a previous study. Seasonal variations of the measured radionuclide activities were also examined in the three sampling stations.     

Artificial radionuclides in the atmosphere over Lithuania

Measurements of airborne radioactive aerosol concentration were carried out on the basis of 1-3 days samples after the Chernobyl disaster and during the period of 1992-2003. Transport of "hot" particles of different composition resulted in the high activity concentrations of (137)Cs, (238)Pu, (239,240)Pu and (241)Am in the atmosphere in Vilnius at the end of April 1986. The (240)Pu/(239)Pu atom ratio showed clear evidence of non-global plutonium originating from the Chernobyl accident in the atmosphere over Lithuania. The (240)Pu/(239)Pu atom ratio ranged from 0.14 to 0.40 in monthly samples in Vilnius in 1995-2003. An increase in activity concentration of (137)Cs by a factor of 100 (up to 300 microBq/m(3)) was found following forest fires in the Ukraine and Belarus. However, no transport of the Chernobyl plutonium was observed and the (240)Pu/(239)Pu atom ratio in samples collected during the forest fires was found to be 0.229 and 0.185, respectively. The exponential decrease in the (240)Pu/(239)Pu atom ratio from 0.30 to 0.19 (mean values) was observed in 1995-2003.     

Geochronology of anthropogenic radionuclides in Ribeira Bay sediments, Rio de Janeiro, Brazil

Ribeira Bay is located approximately 130 km south of the city of Rio de Janeiro and receives discharges of liquid effluent from the Angra dos Reis nuclear power plant (NPP) site, where two pressurized water reactors are located. To test whether the presence of anthropogenic radionuclides in sediments in Ribeira Bay could be correlated to the NPP operations, we sampled seven sediment cores and determined accumulation rates and chronologies. Only one sediment core did not exhibit a superficial mixing layer; this sample was used for dating purposes. Cesium-137 and ²⁰⁷Bi were observed in this sediment profile, but their presence was associated with atmospheric fall-out rather than the nearby NPP. The exponential decay of ²¹⁰Pb concentration with sediment layer depth was verified below a superficial mixing layer for all other sediment cores. Calculated accumulation rates ranged from 1.2 mm y⁻¹ in the inner bay to 6.2 mm y⁻¹ close to its entrance.     

210Po in the marine environment with emphasis on its behaviour within the biosphere

The distribution and behaviour of the natural-series alpha-emitter polonium-210 in the marine environment has been under study for many years primarily due to its enhanced bioaccumulation, its strong affinity for binding with certain internal tissues, and its importance as a contributor to the natural radiation dose received by marine biota as well as humans consuming seafoods. Results from studies spanning nearly 5 decades show that ²¹⁰Po concentrations in organisms vary widely among the different phylogenic groups as well as between the different tissues of a given species. Such variation results in ²¹⁰Po concentration factors ranging from approximately 10³ to over 10⁶ depending upon the organism or tissue considered. ²¹⁰Po/²¹⁰Pb ratios in marine species are generally greater than unity and tend to increase up the food chain indicating that ²¹⁰Po is preferentially taken up by organisms compared to its progenitor ²¹⁰Pb. The effective transfer of ²¹⁰Po up the food chain is primarily due to the high degree of assimilation of the radionuclide from ingested food and its subsequent strong retention in the organisms. In some cases this mechanism may lead to an apparent biomagnification of ²¹⁰Po at the higher trophic level. Various pelagic species release ²¹⁰Po and ²¹⁰Pb packaged in organic biodetrital particles that sink and remove these radionuclides from the upper water column, a biogeochemical process which, coupled with scavenging rates of this radionuclide pair, is being examined as a possible proxy for estimating downward organic carbon fluxes in the sea. Data related to preferential bioaccumulation in various organisms, their tissues, resultant radiation doses to these species, and the processes by which ²¹⁰Po is transferred and recycled through the food web are discussed. In addition, the main gaps in our present knowledge and proposed areas for future studies on the biogeochemical behaviour of ²¹⁰Po and its use as a tracer of oceanographic processes are highlighted in this review.     

Cs, Pu concentrations and the Pu/Pu atom ratio in a sediment core from the sub-aqueous delta of Yangtze River estuary

A sediment core collected from the sub-aqueous delta of the Yangtze River estuary was subjected to analyses of ¹³⁷Cs and plutonium (Pu) isotopes. The ¹³⁷Cs was measured using γ-spectrometry at the laboratories at the Nanjing University and Pu isotopes were determined with Accelerator Mass Spectrometry (AMS), measurements made at the Australian National University. The results show considerable structure in the depth concentration profiles of the ¹³⁷Cs and ^239+240Pu. The shape of the vertical ¹³⁷Cs distribution in the sediment core was similar to that of the Pu. The maximum ¹³⁷Cs and ^239+240Pu concentrations were 16.21 ± 0.95 mBq/g and 0.716 ± 0.030 mBq/g, respectively, and appear at same depth. The average ²⁴⁰Pu/²³⁹Pu atom ratio was 0.238 ± 0.007 in the sediment core, slightly higher than the average global fallout value. The changes in the ²⁴⁰Pu/²³⁹Pu atom ratios in the sediment core indicate the presence of at least two different Pu sources, i.e., global fallout and another source, most likely close-in fallout from the Pacific Proving Grounds (PPG) in the Marshall Islands, and suggest the possibility that Pu isotopes are useful as a geochronological tool for coastal sediment studies. The ¹³⁷Cs and ^239+240Pu inventories were estimated to be 7100 ± 1200 Bq/m² and 407 ± 27 Bq/m², respectively. Approximately 40% of the ^239+240Pu inventory originated from the PPG close-in fallout and about 50% has derived from land-origin global fallout transported to the estuary by the river. This study confirms that AMS is a useful tool to measure ²⁴⁰Pu/²³⁹Pu atom ratio and can provide valuable information on sedimentary processes in the coastal environment.     

Medical radioisotopes in the environment – following the pathway from patient to river sediment

Motivated by the detection of ¹³¹I in river sediment in routine long-term surveillance samples, a systematic short-term study of the wastewater treatment chain was planned and conducted. Inflow, effluent and primary sludge were collected on a daily basis during two weeks at a regional wastewater treatment plant. Samples were investigated by gamma spectroscopy. Four medically used isotopes could be identified (¹³¹I and ^99mTc regularly, ¹⁵³Sm and ¹²³I sporadically). The concentration levels coincide well with literature data for ¹³¹I, and with our own long-term data for ¹³¹I and ^99mTc for the same plant. Cosmogenic ⁷Be activity in primary sludge correlated well with rainfall intensity. Surface sediment was sampled at low tide at both shores of the river, up- and downstream of the plant. ¹³¹I was identified in all samples, with a sharp maximum (about 100 Bq kg⁻¹ d.m.) at the discharge point of the plant and lower levels elsewhere, decreasing monotonically in downstream direction. ⁷Be and ¹³⁷Cs showed the same behaviour, but no peak at the discharge point. Predictions from simple equilibrium models for the transport and sedimentation of ¹³¹I show good agreement with the experimental data and suggest that the wastewater treatment plant is the main source for this isotope.     

Plutonium as a chronomarker in Australian and New Zealand sediments: a comparison with Cs

The construction of high resolution chronologies of sediment profiles corresponding to the last 50-100 years usually entails the measurement of fallout radionuclides ²¹⁰Pb and ¹³⁷Cs. The anthropogenic radionuclide, ¹³⁷Cs, originating from atmospheric nuclear weapons testing can provide an important “first appearance” horizon of known age (1954-1955), providing much-needed validation for the sometimes uncertain interpretations associated with ²¹⁰Pb geochronology. However, while ¹³⁷Cs usually provides a strong signal in sediment in the northern hemisphere, total fallout of ¹³⁷Cs in the southern hemisphere was only 25% that of the north and the low activities of ¹³⁷Cs seen in Australian and New Zealand sediments can make its horizon of first appearance somewhat arguable. Low ¹³⁷Cs fallout also limited the size of the 1963-1964 fallout peak, a peak that is usually seen in northern hemisphere sediment profiles but is often difficult to discern south of the equator.This paper shows examples of the use of nuclear weapons fallout Pu as a chronomarker in sediment cores from Australia (3 sites) and New Zealand (1 site). The Pu profiles of five cores are examined and compared with the corresponding ¹³⁷Cs profiles and ²¹⁰Pb geochronologies. We find that Pu has significant advantages over ¹³⁷Cs, including greater measurement sensitivity using alpha spectrometry and mass spectrometric techniques compared to ¹³⁷Cs measurements by gamma spectrometry. Moreover, Pu provides additional chronomarkers associated with changes in the Pu isotopic composition of fallout during the 1950s and 1960s. In particular, the ²³⁸Pu/^239+240Pu activity ratio shows distinct shifts in the early 1950s and the mid to late 1960s, providing important known-age horizons in southern hemisphere sediments. For estuarine and near-shore sediments Pu sometimes has another significant advantage over ¹³⁷Cs due to its enrichment in bottom sediment relative to ¹³⁷Cs resulting from the more efficient scavenging of dissolved Pu in seawater by sediment particles.