Source of radium in a well-water-augmented Florida lake

A study of the lake waters of Saddleback Lake, Florida was undertaken with the goal of determining the source of elevated radium activities in the lake. Four radium isotopes, (226)Ra, (228)Ra, (223)Ra and (224)Ra, were measured and activities of all the four radium isotopes were substantially greater in the well water used to augment the lake as compared to the lake waters. In the surface water, radium activities were highest close to the well used for augmentation in the initial sampling. Activities initially decreased with time after augmentation from the well ceased. The (223)Ra/(226)Ra activity ratio decreased during the first month of sampling and closely followed an exponential decay curve based on the (223)Ra decay constant. Trends in the activities and the (223)Ra/(226)Ra activity ratios support the conclusion that the well used to augment the lake was the dominant source of (223)Ra and (226)Ra to Saddleback Lake during this study. The (224)Ra/(226)Ra activity ratio did not follow the expected trend of exponential decay based on the (224)Ra decay constant. While the augmentation well supplied some (224)Ra, these results suggest that there must be an additional source of (224)Ra to the lake. The most likely additional source of (224)Ra appears to be the ingrowth of (224)Ra on the sediment within the lake from (228)Ra (via (228)Th).     

Measuring the radium quartet (Ra, Ra, Ra, Ra) in seawater samples using gamma spectrometry

Radium isotopes are widely used in marine studies (eg. to trace water masses, to quantify mixing processes or to study submarine groundwater discharge). While ²²⁸Ra and ²²⁶Ra are usually measured using gamma spectrometry, short-lived Ra isotopes (²²⁴Ra and ²²³Ra) are usually measured using a Radium Delayed Coincidence Counter (RaDeCC). Here we show that the four radium isotopes can be analyzed using gamma spectrometry. We report ²²⁶Ra, ²²⁸Ra, ²²⁴Ra, ²²³Ra activities measured using low-background gamma spectrometry in standard samples, in water samples collected in the vicinity of our laboratory (La Palme and Vaccarès lagoons, France) but also in seawater samples collected in the plume of the Amazon river, off French Guyana (AMANDES project). The ²²³Ra and ²²⁴Ra activities determined in these samples using gamma spectrometry were compared to the activities determined using RaDeCC. Activities determined using the two techniques are in good agreement. Uncertainties associated with the ²²⁴Ra activities are similar for the two techniques. RaDeCC is more sensitive for the detection of low ²²³Ra activities. Gamma spectrometry thus constitutes an alternate method for the determination of short-lived Ra isotopes.     

Distribution of uranium and radium isotopes in an aquifer of a semi-arid region (Manouba-Essijoumi, Northern Tunisia)

Groundwaters from the Sebkhet Essijoumi drainage basin, situated in northern Tunisia, West of the city of Tunis, were sampled and analyzed for uranium and radium isotopes. Low (234)U/(238)U activity ratios coupled with relatively high (228)Ra and (238)U concentrations were found in the Manouba plain phreatic aquifer, at the northern part of the basin, where remote sensing has indicated that this plain corresponds to the main humid zone of the area. Low (234)U/(238)U ratios probably reflected short residence time for waters in the Manouba plain, and high ratios longer residence time in the south, where water reaching the phreatic aquifer seems to have previously circulated in rocks constituting the southern hills. Assuming that, in the Manouba plain aquifer, the groundwater flows downstream from the Oued Lill pass area to the South-West of the Sebkha, the difference in the (228)Ra/(226)Ra activity ratio suggests that the residence time of water has been 2.8 years longer near the Sebkha than upstream.     

Isotope tracing of submarine groundwater discharge offshore Ubatuba, Brazil: results of the IAEA-UNESCO SGD project

Results of groundwater and seawater analyses for radioactive ((3)H, (222)Rn, (223)Ra, (224)Ra, (226)Ra, and (228)Ra) and stable (D and (18)O) isotopes are presented together with in situ spatial mapping and time series (222)Rn measurements in seawater, direct seepage measurements using manual and automated seepage meters, pore water investigations using different tracers and piezometric techniques, and geoelectric surveys probing the coast. This study represents first time that such a new complex arsenal of radioactive and non-radioactive tracer techniques and geophysical methods have been used for simultaneous submarine groundwater discharge (SGD) investigations. Large fluctuations of SGD fluxes were observed at sites situated only a few meters apart (from 0cmd(-1) to 360cmd(-1); the unit represents cm(3)/cm(2)/day), as well as during a few hours (from 0cmd(-1) to 110cmd(-1)), strongly depending on the tidal fluctuations. The average SGD flux estimated from continuous (222)Rn measurements is 17+/-10cmd(-1). Integrated coastal SGD flux estimated for the Ubatuba coast using radium isotopes is about 7x10(3)m(3)d(-1) per km of the coast. The isotopic composition (deltaD and delta(18)O) of submarine waters was characterised by significant variability and heavy isotope enrichment, indicating that the contribution of groundwater in submarine waters varied from a small percentage to 20%. However, this contribution with increasing offshore distance became negligible. Automated seepage meters and time series measurements of (222)Rn activity concentration showed a negative correlation between the SGD rates and tidal stage. This is likely caused by sea level changes as tidal effects induce variations of hydraulic gradients. The geoelectric probing and piezometric measurements contributed to better understanding of the spatial distribution of different water masses present along the coast. The radium isotope data showed scattered distributions with offshore distance, which imply that seawater in a complex coast with many small bays and islands was influenced by local currents and groundwater/seawater mixing. This has also been confirmed by a relatively short residence time of 1-2 weeks for water within 25km offshore, as obtained by short-lived radium isotopes. The irregular distribution of SGD seen at Ubatuba is a characteristic of fractured rock aquifers, fed by coastal groundwater and recirculated seawater with small admixtures of groundwater, which is of potential environmental concern and has implications on the management of freshwater resources in the region.     

Determination of 228Ra, 226Ra and 224Ra in natural water via adsorption on MnO2-coated discs

A fast procedure based on sorption of Ra on MnO2 coated polyamide discs is presented for determination of radium isotopes (i.e. 228Ra, 226Ra, 224Ra) in aqueous samples. The sample discs can be used directly for low-level alpha-spectrometry without the need for further separation and preparation methods to produce planar sample sources. While the activity of alpha-emitting 224Ra and 226Ra can be determined during a first measurement, beta-emitting 228Ra is obtained via ingrowth of the progeny 228Th on the same sample disc after a standing time of about six months. Calculations are presented for optimizing the analytical accuracy as well as for predicting the sorption yield or chemical recovery of radium on the sample disc as a function of exposure time because the sorption uptake proceeds with first-order kinetics. The analyses can be carried out on small samples of 0.5-11 and, for long counting times of one week and use of high-purity silicon surface barrier detectors, a detection limit of 0.15 mBq l-1 is obtained for 226Ra. Since the half-life of 224Ra is only 3.7 d and since 228Th (as a measure for 228Ra) is built up only partially on the sample disc, a slightly higher detection limit of 0.24 mBq l-1 results for the latter isotopes. The procedure is therefore sufficiently sensitive to allow the investigation of Ra isotope relationships in aquifers at typical environmental levels.     

Estimating the dynamics of groundwater input into the coastal zone via continuous radon-222 measurements

Submarine groundwater discharge (SGD) into the coastal zone has received increased attention in the last few years as it is now recognized that this process represents an important pathway for material transport. Assessing these material fluxes is difficult, as there is no simple means to gauge the water flux. To meet this challenge, we have explored the use of a continuous radon monitor to measure radon concentrations in coastal zone waters over time periods from hours to days. Changes in the radon inventories over time can be converted to fluxes after one makes allowances for tidal effects, losses to the atmosphere, and mixing with offshore waters. If one assumes that advective flow of radon-enriched groundwater (pore waters) represent the main input of 222Rn in the coastal zone, the calculated radon fluxes may be converted to water fluxes by dividing by the estimated or measured 222Rn pore water activity. We have also used short-lived radium isotopes (223Ra and 224Ra) to assess mixing between near-shore and offshore waters in the manner pioneered by. During an experiment in the coastal Gulf of Mexico, we showed that the mixing loss derived from the 223Ra gradient agreed very favorably to the estimated range based on the calculated radon fluxes. This allowed an independent constraint on the mixing loss of radon-an important parameter in the mass balance approach. Groundwater discharge was also estimated independently by the radium isotopic approach and was within a factor of two of that determined by the continuous radon measurements and an automated seepage meter deployed at the same site.     

Surface water mixing estimated from 228Ra and 226Ra in the northwestern North Pacific

We investigated the horizontal distributions of (228)Ra and (226)Ra in surface waters of the northwestern North Pacific Ocean and Okhotsk Sea. Ratios of (228)Ra/(226)Ra were relatively large in the Tsugaru Current (0.6-0.8) and Okhotsk Sea (0.4-0.5), and small in the Western Subarctic Gyre (<0.2) and the Oyashio (0.25-0.3). (228)Ra/(226)Ra ratios in western Subarctic Water (SAW) rose slightly upon mixing with Okhotsk Water (OKW), before becoming the Oyashio Water (OYW). Also, ratios in the OYW increased during mixing with Tsugaru Current Water (TCW). Estimating from (228)Ra/(226)Ra ratios and (226)Ra activities with a simple two-end members-mixing model, we assumed that approximately 23% of the OYW originated from the OKW and the coastal region off northern Honshu (Japan) was strongly influenced by the TCW. From a diagram of (228)Ra activities against salinity, we could roughly divide surface seawater in the study area into the five water masses, which were SAW, OYW, OKW, TCW, and Subtropical Water (STW).     

228Ra/226Ra/224Ra and 87Sr/86Sr isotope relationships for determining interactions between ground and river water in the upper Rhine valley

Ground and river waters of the upper Rhine valley (Alsace, France) were investigated for chemical composition of the major elements, Sr isotopes and radionuclides from the U and Th series. In particular, the isotope ratios and concentrations of Ra and Sr were used as geochemical tracers to distinguish between different types of water and their interactions. The bulk chemical analyses suggest that the surface waters in the Rhine valley can be described as mixtures between Ca-Na-HCO3-rich ground water and less mineralized slightly acidic river waters which have migrated through crystalline (mainly granitic) basement rocks of the Vosges mountains. Mixing of these waters yields positive correlation between bulk Sr, U, Ca and HCO3, indicating that carbonate-rich sediments are the main source of U and (non-radiogenic) Sr in the Rhine valley aquifers. The combination of the Ra and Sr isotope systems (228Ra/226Ra, 87Sr/86Sr) shows, however, that probably three sources contribute to the surface river waters in the upper Rhine valley, i.e. (i) a highly radiogenic crystalline component, (ii) a ground water source and, (iii) a third component from infiltrating Rhine water along the flow path of the parallel running river Ill in the northerly direction. The Sr and Ra isotope systems were also used to calculate small-scale mixing fractions of tributaries along the flow path of the Ill. Mixing ratios of non-pure end-member waters were determined using three isotope diagrams (i.e. 224Ra/226Ra vs. 228Ra/226Ra) and the results obtained with the Ra isotope system were found to be consistent with the data using Sr isotope relationships (i.e. 87Sr/86Sr vs. 1/Sr).     

Radionuclide and chemical concentrations in mineral waters at Saratoga Springs, New York

A project to characterize the radionuclide and chemical components in natural spring waters in the vicinity of Saratoga Springs, New York (USA) has been completed. As a result of the measured radionuclide and chemical content, eight springs were labeled as mineral waters, whereas three springs contained very low concentrations of these components. The mineral waters were highly enriched in alkaline and alkaline-earth elements, as well as chloride ions. Three isotopes of radium ((224)Ra, (226)Ra, (228)Ra) were detected in the mineral waters and reached concentrations of 1, 20, and 2 Bq/L, respectively. Overall, the (226)Ra isotope constituted about 80% of the total radioactivity measured in the water samples. Dissolved uranium concentrations in the mineral waters were very low (mean approximately 50 mBq/L).     

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.     

226Ra and 228Ra activities associated with agricultural drainage ponds and wetland ponds in the Kankakee Watershed, Illinois-Indiana, USA

Background radioactivity is elevated in many agricultural drainage ponds and also constructed wetland ponds in the Kankakee watershed. During 1995-1999, gross-alpha and -beta activities were measured up to 455 and 1650 mBq L-1, respectively. 226Ra and 228Ra averaged 139 and 192 mBq L-1 in controlled drainage ponds compared to 53 and 58 mBq L-1 for 226Ra and 228Ra, respectively, in native wetland ponds. Analyses of applied ammonium phosphate fertilizers near both native and controlled ponds indicate comparable 226Ra/228Ra and 228Ra/232Th activity ratios with only the surface waters in the controlled ponds. For example, 226Ra/228Ra activity ratios in controlled ponds ranged from 0.791 to 0.91 and group with a local fertilizer batch containing FL phosphate compounds with 226Ra/228Ra activity ratios of 0.831-1.04. Local soils of the Kankakee watershed have 226Ra/228Ra activity ratios of 0.541-0.70. Calculated Ra fluxes of waters, in drainage ditches associated with these controlled ponds, for 226Ra ranged from 0.77 to 9.00 mBq cm-2 d-1 and for 228Ra ranged from 1.22 to 8.43 mBq cm-2 d-1. Ra activity gradients were measured beneath these controlled ponds both in agricultural landscapes and in constructed wetlands, all being associated with drainage ditches. Ra had infiltrated to the local water table but was below regulatory maximum contaminant limits. Still, measurable Ra activity was measured downgradient of even the constructed wetlands in the Kankakee watershed, suggesting that the attenuation of Ra was low. However, no Ra excess was observed in the riparian zone or the Kankakee River downgradient of the native wetland ponds.     

Seasonal variation of 228Ra/226Ra 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.     

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.     

Radiological impacts of natural radioactivity in Abu-Tartor phosphate deposits, Egypt.

Phosphate and environmental samples were collected from Abu Tartor phosphate mine and the surrounding region. The activity concentration of 226Ra (238U) series, 232Th series and 40K were measured using a gamma-ray spectrometer. The activities of uranium isotopes (238U, 235U and 234U) and 210Pb were measured using an alpha spectrometer and a low-background proportional gas counting system, respectively, after radiochemical separation. The results are discussed and compared with the levels in phosphate rocks from different countries. It seems that the Abu Tartor phosphate deposit has the lowest radioactivity level of exploited phosphate of sedimentary origin. 226Ra/238U, 210Pb/226Ra, 234U/238U and 226Ra/228Ra activity ratios were calculated and are discussed. The radioactivity levels in the surrounding region and the calculated exposure dose (nGy/h) will be considered as a pre-operational baseline to estimate the possible radiological impacts due to mining, processing and future phosphate industrial activities. To minimize these impacts, the processing wastes should be recycled to the greatest possible extent.     

Determination and comparison of uranium and radium isotopes activities and activity ratios in samples from some natural water sources in Morocco.

Radiochemical results (238U, 226Ra and 228Ra activities; 234U/238U, 228Ra/226Ra and 226Ra/238U activity ratios) are reported for 42 natural water samples collected from wells, hot mineral springs, rivers, tap water, lakes and irrigation water in 15 Moroccan locations. Results show that 238U activity varies between 4.5 and about 309 mBq l(-1) in wells, 0.6 and 8.5 mBq l(-1) in hot springs, 9.7 and 28 mBq l(-1) in rivers, 2.5 and 16 mBq l(-1) in tap waters and between 6 and 24 mBq l(-1) in lakes. The 234U/238U activity ratio varies in the range 0.87-3.35 in all analyzed water samples except for hot springs where it reaches values higher than 7. Unlike well water, mineral water samples present low 238U activities and high 234U/238U activity ratios and 226Ra activities. The highest activity of radium in mineral water is 150 times higher than the highest activity of 226 Ra found in well water. 226Ra/238U activity ratios are in the ranges 0.07-1.14 in wells, 0.04-0.38 in rivers, 0.04-2.48 in lakes, and 1.79-2115 in springs. The calculated equivalent doses to all the measured activities are inferior to the maximum contaminant levels recommended by the International Commission of Radioprotection and they do not present any risk for public health in Morocco.     

Isotope tracing of submarine groundwater discharge offshore Ubatuba, Brazil: results of the IAEA–UNESCO SGD project

Results of groundwater and seawater analyses for radioactive (³H, ²²²Rn, ²²³Ra, ²²⁴Ra, ²²⁶Ra, and ²²⁸Ra) and stable (D and ¹⁸O) isotopes are presented together with in situ spatial mapping and time series ²²²Rn measurements in seawater, direct seepage measurements using manual and automated seepage meters, pore water investigations using different tracers and piezometric techniques, and geoelectric surveys probing the coast. This study represents first time that such a new complex arsenal of radioactive and non-radioactive tracer techniques and geophysical methods have been used for simultaneous submarine groundwater discharge (SGD) investigations. Large fluctuations of SGD fluxes were observed at sites situated only a few meters apart (from 0 cm d⁻¹ to 360 cm d⁻¹; the unit represents cm³/cm²/day), as well as during a few hours (from 0 cm d⁻¹ to 110 cm d⁻¹), strongly depending on the tidal fluctuations. The average SGD flux estimated from continuous ²²²Rn measurements is 17 ± 10 cm d⁻¹. Integrated coastal SGD flux estimated for the Ubatuba coast using radium isotopes is about 7 × 10³ m³ d⁻¹ per km of the coast. The isotopic composition (δD and δ¹⁸O) of submarine waters was characterised by significant variability and heavy isotope enrichment, indicating that the contribution of groundwater in submarine waters varied from a small percentage to 20%. However, this contribution with increasing offshore distance became negligible. Automated seepage meters and time series measurements of ²²²Rn activity concentration showed a negative correlation between the SGD rates and tidal stage. This is likely caused by sea level changes as tidal effects induce variations of hydraulic gradients. The geoelectric probing and piezometric measurements contributed to better understanding of the spatial distribution of different water masses present along the coast. The radium isotope data showed scattered distributions with offshore distance, which imply that seawater in a complex coast with many small bays and islands was influenced by local currents and groundwater/seawater mixing. This has also been confirmed by a relatively short residence time of 1–2 weeks for water within 25 km offshore, as obtained by short-lived radium isotopes. The irregular distribution of SGD seen at Ubatuba is a characteristic of fractured rock aquifers, fed by coastal groundwater and recirculated seawater with small admixtures of groundwater, which is of potential environmental concern and has implications on the management of freshwater resources in the region.     

Environmental characterization and radio-ecological impacts of non-nuclear industries on the Red Sea coast

The Red Sea is a deep semi-enclosed and narrow basin connected to the Indian Ocean by a narrow sill in the south and to the Suez Canal in the north. Oil industries in the Gulf of Suez, phosphate ore mining activities in Safaga-Quseir region and intensified navigation activities are non-nuclear pollution sources that could have serious radiological impacts on the marine environment and the coastal ecosystems of the Red Sea. It is essential to establish the radiological base-line data, which does not exist yet, and to investigate the present radio-ecological impact of the non-nuclear industries to preserve and protect the coastal environment of the Red Sea. Some natural and man-made radionuclides have been measured in shore sediment samples collected from the Egyptian coast of the Red Sea. The specific activities of 226Ra and 210Pb (238U) series, 232Th series, 40K and 137Cs (Bq/kg dry weight) were measured using gamma ray spectrometers based on hyper-pure germanium detectors. The specific activities of 210Po (210Pb) and uranium isotopes (238U, 235U and 234U) (Bq/kg dry weight) were measured using alpha spectrometers based on surface barrier (PIPS) detectors after radiochemical separation. The absorbed radiation dose rates in air (nGy/h) due to natural radionuclides in shore sediment and radium equivalent activity index (Bq/kg) were calculated. The specific activity ratios of 228Ra/226Ra, 210Pb/226Ra, 226Ra/238U and 234U/238U were calculated for evaluation of the geo-chemical behaviour of these radionuclides. The average specific activity of 226Ra (238U) series, 232Th series, 40K and 210Pb were 24.7, 31.4, 427.5 and 25.6 Bq/kg, respectively. The concentration of 137Cs in the sediment samples was less than the lower limit of detection. The Red Sea coast is an arid region with very low rainfall and the sediment is mainly composed of sand. The specific activity of 238U, 235U and 234U were 25.3, 2.9 and 25.0 Bq/kg. The average specific activity ratios of 226Ra/228Ra, 210Pb/226Ra and 234U/238U were 1.67, 1.22 and 1.0, respectively. The relationship between 226Ra/228Ra activity ratio and sample locations along the coastal shoreline indicates the increase of this ratio in the direction of the Shuqeir in the north and Safaga in the south where the oil exploration and phosphate mining activities are located. These activities may contribute a high flux of 226Ra. The concentration and distribution pattern of 226Ra in sediment can be used to trace the radiological impact of the non-nuclear industries on the Red Sea coast.     

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.     

Use of multitracers for the study of water mixing in the Paraíba do Sul River estuary

Multitracers were used to study water mixing in the Paraíba do Sul River estuary region in August 2007 (dry season) and March 2008 (rainy season) and to evaluate the reach of the river plume in the direction of the open ocean. Two sampling campaigns were carried out, each in a different season. Based on these results, it was possible to conclude that the multitracers used in this study (salinity, Si, Ba and U, as well as the radium isotopes ²²³Ra, ²²⁴Ra, ²²⁶Ra and ²²⁸Ra) presented satisfactory results toward defining the plume reach and determining the residence time and water-mixing processes in the estuary. A strong correlation was observed between tracers and the distance to the coast. During the low river water discharge period, the riverine water took about 10 days to reach open ocean waters (salinity ∼ 35). During the rainy period this value decreased to 6 days. Based on the radium results, it was possible to calculate diffusion coefficients (K_h) of 23 km² d⁻¹ and 38 km² d⁻¹ for ²²⁴Ra and ²²³Ra, respectively, during the dry season (winter). Values of 65 km² d⁻¹ and 68 km² d⁻¹ for ²²³Ra and ²²⁴Ra, respectively, were found for the rainy period (summer).     

An efficient and simple method for measuring (226)Ra using the scintillation cell in a delayed coincidence counting system (RaDeCC)

A delayed coincidence counter (RaDeCC), developed to determine ultra-low levels of (223)Ra (half life = 11.1 days) and (224)Ra (half life = 3.6 days) in seawater, was adapted to measure (226)Ra (half life = 1622 years). After pre-concentration of Ra from seawater onto MnO(2)-coated fiber we show in this study that the (226)Ra activity can be determined using the RaDeCC's ability to record alpha decay of its daughters as total counts. For sufficient ingrowth of (222)Rn, the Mn-fiber is hermetically sealed in a column for a few days. Then, the ingrown (222)Rn is circulated through the RaDeCC air-loop system followed by shutting down of the pump and closure of the scintillation cell for equilibration. Counting may be completed within a few hours for seawater samples. Sample measurements with this method agreed well with data obtained using gamma-ray spectrometry. This proves that a set of Ra isotopes ((223)Ra, (224)Ra, and (226)Ra), commonly used for geophysical studies such as mixing rates of different water masses and submarine groundwater discharge, can be efficiently and rapidly measured using the RaDeCC.