Plutonium,radiocesium and radiocobalt in sediments of the Hudson River estuary

Anthropogenic radionuclides have reached the Hudson estuary as global fallout from nuclear weapons testing and through local releases from commercial nuclear reactors. Significant activities of²³⁸Pu and^239,240Pu (fallout-derived),¹³⁴Cs and⁶⁰Co (reactor-released), and¹³⁷Cs (derived from both sources), have accumulated in the sediments throughout the estuary, with the primary zone of accumulation near the downstream end of the system in New York harbor. The estuary appears to have trapped nearly all of the^239,240Pu delivered as fallout, and consequently, ocean dumping of dredged harbor sediment is currently the primary means for the net transport of these nuclides to coastal waters. In contrast, only 10–30% of the¹³⁷Cs,¹³⁴Cs and⁶⁰Co delivered to the estuary have been retained on the fine particles which accumulate at a rapid rate in the harbor.The primary factors which have governed the distribution of anthropogenic radionuclides in Hudson sediments are: (1) spread of fine particles labeled with both fallout and reactor nuclides throughout the axis of the estuary, (2) differences in timing of the peak fallout years (1962–1964) and years of maximum reactor releases (1971–1972), (3) large variations in sediment accumulation rates, ranging from a few millimeters per year or less to many tens of centimeters per year, (4) appreciable desorption of¹³⁷Cs and¹³⁴Cs from particles at higher salinities, and (5) possible enhanced desorption of⁶⁰Co at higher salinities (relative to¹³⁴Cs and¹³⁷Cs) which may be associated with the release of reduced manganese from the harbor sediments.     

Fallout radionuclides in the Pacific Ocean: Vertical and horizontal distributions,largely from GEOSECS stations

From GEOSECS stations, largely, the 1974 distributions of Pu and of¹³⁷Cs are described in the Pacific Ocean north of about 20°S latitude. Changes in some of these distributions are described from 1978 cruises by the authors.The Pacific exhibited, everywhere, a shallow subsurface layer of Pu-rich water with its concentration maximum at about 465 m in 1974; over a large portion of the central North Pacific a second layer of Pu-labelled water, less concentrated than the shallow layer, lay just above the bottom. Similar features were not observed in the case of¹³⁷Cs.The inventories of both Pu and¹³⁷Cs in the water column at most 1974 stations are substantially greater than those to be expected from world-wide fallout alone; these inventory excesses appear to be attributable to close-in fallout, but only if the ratio Pu/¹³⁷Cs in this source was much higher than in world-wide fallout. The North Pacific mean ratio of the inventories is 2.2 times that observed in world-wide fallout.Resolubilization of Pu both from sinking particles and from sediments explains peculiarities of its depth distributions.There is little evidence for tracer movement by sliding downward along density surfaces;¹³⁷Cs appears to have moved to depth by downmixing at the edge of the Kuroshio, and then moved horizontally and upward alongσ_t contours. The shallow Pu-rich layer shows no coordination with density, salinity or O₂ isopleths. The deep Pu-rich layer is restricted to a narrow range of O₂ concentrations that confirm its origin in the Aleutian Trench and rapid spread southward and laterally. Near-bottom circulation processes have been much more active than here-to-fore described.     

Fallout240Pu and239Pu in Atlantic marine samples

Mass spectrometric analyses of low levels of global fallout plutonium separated from Atlantic marine samples have differentiated fallout²³⁹Pu and²⁴⁰Pu in aquatic samples for the first time. The results show no single characteristic²⁴⁰Pu/²³⁹Pu ratio in marine samples; the observed range is from 0.11 to 0.24 on an atom basis. There are indications that differences exist in the chemical or physical form of plutonium from atmospheric fallout in Atlantic surface water and that selective concentration in surface organisms is occurring. No single²⁴⁰Pu/²³⁹Pu value is found in pelagic sediments collected from different depths and locations. Discounting sources other than fallout, our results show that the plutonium deposited at any given time since atmospheric testing began may have carried a unique²⁴⁰Pu/²³⁹Pu tag. This label may be extremely useful to trace fallout plutonium through biogeochemical cycles.     

Concentrations of 137Cs, 90Sr, 108m Ag, 239+240 Pu and atom ratio of 240Pu/239Pu in tanner crabs, Chionoecetes japonicus and Chionoecetes opilio collected around Japan

The anthropogenic radionuclides, ¹³⁷Cs, ⁹⁰Sr, ^108mAg, ^239+240Pu, were measured in two Chionoecetes species, red queen crab (Chionoecetes japonicus) and snow crab (Chionoecetes opilio) collected around Japan during 1996–2007. There was no increase in the concentrations of these radionuclides and no large variation of the atom ratio of ²⁴⁰Pu/²³⁹Pu during this research period. These results indicated that the source of the radionuclides was not the radioactive wastes dumped by the former USSR and Russia and originated from past nuclear weapon tests. The higher atom ratio in the crab species than that from global fallout would be contributed by the Pacific Proving Grounds close-in fallout. The variability of the concentration of radionuclides in the crab species would result from the variability of the composition and quantity in the diet. However, the decrease in the concentration of radionuclides with sampling depth would depend on the concentration in the seawater and diet.     

Depositional history of artificial radionuclides in the Ross Ice Shelf,Antarctica

The annual fluxes of artificial radionuclides (²³⁸Pu,^239+240Pu,²⁴¹Am,¹³⁷Cs,⁹⁰Sr and³H) from the atmosphere to the Ross Ice Shelf in Antarctica were determined from measurements in strata dated by²¹⁰Pb. Recognizable sources include the U.S. tests (Mike-Ivy and Castle Hill) in the early 1950s, the U.S.S.R. tests of the early 1960s, the SNAP-9A burnup of 1964 and the French and Chinese tests in the late 1960s and 1970s. There are several problems still awaiting resolution: the differences in atmospheric chemistries of fission products and of transuranics produced in weapons tests and the anomalous fluxes of²³⁸Pu to the ice shelf which do not appear to reflect a one-year stratospheric residence. There is no evidence for a smearing of the fallout record as a consequence of diffusion of these radionuclides in the glacial column.     

Pu and137Cs in coastal sediments

Analyses are presented of¹³⁷Cs,²³⁸Pu, and^239,240Pu, in relation to depth in sediment, in 21 gravity cores. These cores span the ranges of times 1964–1975, and of water depths 12–2000 m; they come from three distinct sedimentation areas off the northeast coast of the United States. Although the ranges of total sediment inventories of^239,240Pu and of¹³⁷Cs from the various areas hardly overlap, the range of ratios of the inventories of these two nuclides is probably the same in all the areas. In the shallow-water cores the^239,240Pu/¹³⁷Cs ratio regularly diminishes with depth in the core, and a tendency is seen for curves of this function to have similar slopes in each area; ratios of²³⁸Pu/^239,240Pu show no change with depth in these shallow-water cores. In the deeper-water cores, the^239,240Pu/¹³⁷Cs ratio shows no systematic change with depth, but sometimes the²³⁸Pu/^239,240Pu ratio shows a minimum at the sediment surface, and is much higher deeper in the cores. We believe that these phenomena can be explained in terms of a complicated bioturbational process moving the nuclides, together, down into the sediments, of chemical resolubilization, at depth, of plutonium only, and of its subsequent upward translocation in the interstitial solution. Some re-immobilization of plutonium near the sediment surface is implied, and a mechanism is suggested for this, based on displacement of plutonium from organic complexes by the increasing concentrations, in upper layers of the sediment, of re-oxidized dissolved iron.     

The application of caesium‐137 measurements to investigate floodplain deposition in a large semi‐arid catchment in Queensland,Australia: a low‐fallout environment

Floodplains comprise geomorphologically important sources and sinks for sediments and associated pollutants, yet the sedimentology of large dryland floodplains is not well understood. Processes occurring on such floodplains are often difficult to observe, and techniques used to investigate smaller perennial floodplains are often not practical in these environments. This study assesses the utility of ¹³⁷Cs inventory and depth‐profile techniques for determining relative amounts of floodplain sedimentation in the Fitzroy River, northeastern Australia; a 143 000 km² semi‐arid river system. Caesium‐137 inventories were calculated for floodplain and reference location bulk soil cores collected from four sites. Depth profiles of ¹³⁷Cs concentration from each floodplain site and a reference location were recorded. The areal density of ¹³⁷Cs at reference locations ranged from 13 to 978 Bq m^–2 (0–1367 Bq m^–2 at the 95% confidence interval), and the mean value ± 2 (standard error of the mean) was 436 ± 264 Bq m^–2, similar to published data from other Southern Hemisphere locations. Floodplain inventories ranged from 68 to 1142 Bq m^–2 (0–1692 Bq m^–2 at the 95% confidence interval), essentially falling within the range of reference inventory values, thus preventing calculation of erosion or deposition. Depth‐profiles of ¹³⁷Cs concentration indicate erosion at one site and over 66 cm of deposition at another since 1954. Analysis of ^239+240Pu concentrations in a depositional core substantiated the interpretation made from ¹³⁷Cs data, and depict a more tightly constrained peak in concentration. Average annual deposition rates range from 0 to 15 mm. The similarity between floodplain and reference bulk inventories does not necessarily indicate a lack of erosion or deposition, due to low ¹³⁷Cs fallout in the region and associated high measurement uncertainties, and a likely influence of gully and bank eroded sediments with no or limited adsorbed ¹³⁷Cs. In this low‐fallout environment, detailed depth‐profile data are necessary for investigating sedimentation using ¹³⁷Cs. Copyright © 2009 John Wiley & Sons, Ltd.     

Distribution and content of different artifical radio nuclides in the water of the North Sea during the years 1977 to 1981 (complemented with some results from 1982 to 1984)

Summary The measured concentrations of¹³⁷Cs in the water of the North Sea gained during the years 1977 to 1982 largely confirm the results found in the preceding years (Fig. 1). After a distinct maximum in 1978 — brought about by a particularly strong influx during 1977 — the total quantity of¹³⁷Cs present in the North Sea has reced, to around half of these peak values by the year 1982 (Table 1).On the way from the Sellafield Works near the Irish Sea as far as into the North Sea, a strong shift of the¹³⁷Cs:⁹⁰Sr ratio in favour of the⁹⁰Sr can be observed.By following the temporal course of that ratio at different measurement points, a transport time can be deduced of around 3 years between the Sellafield Works and the Pentland Firth; a further year would be needed to reach into the southeastern North Sea.The ratio Cs:Sr furthermore permits, in the southeastern North Sea, a good distinction between the watermasses comming from the north into the North Sea with respect to those that come through the Channel from the South. These masses practically flow side by side until about the entrance to the Skagerrak.The vertical distribution of the¹³⁷Cs shows, as is to be expected, seasonally conditioned differences. However, effects also occur, which — on the basis of the data available to date — do not yet permit a clear explanation.The⁹⁰Sr, as well as the^239+240Pu, present in the North Sea show an analogous distribution scheme compared with that of the¹³⁷Cs. Their concentrations lie far below that of the¹³⁷Cs (⁹⁰Sr 17.5%;^239+240Pu 0.03%).Tritium, on the other hand — with essentially higher concentrations — shows a completely different distribution, because it is principly introduced via the freshwater flowing in from the land.

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Verteilung und Gehalt verschiedener künstlicher Radionuklide im Wasser der Nordsee in den Jahren 1977 bis 1981 (ergänzt durch einige Ergebnisse von 1982 bis 1984)

Zusammenfassung Die in den Jahren 1977 bis 1982 gewonnenen Meßdaten der Aktivitätskonzentrationen von¹³⁷Cs im Wasser der Nordsee bestätigen weitgehend die in den vorhergehenden Jahren gefundenen Ergebnisse (Fig. 1) Nach einem deutlichen Maximum im Jahre 1978 — hervorgerufen durch eine besonders starke Zufuhr im Jahre 1977 —ist die in der Nordsee insgesamt vorhandene Menge an¹³⁷Cs bis zum Jahre 1982 wieder auf rund die Hälfte zurückgegangen (Tab. 1).Auf dem Weg von den Sellafield Works an der Irischen See bis in die Nordsee ist eine starke Verschiebung des¹³⁷Cs:⁹⁰Sr Verhältnisses zugunsten des⁹⁰Sr zu beobachten.Aus dem zeitlichen Verlauf dieses Verhältnisses an verschiedenen Meßpunkten ergeben sich Transportzeiten zwischen den Sellafield Works und dem Pentland Firth von rund 3 Jahren; bis in die südöstliche Nordsee wird ein weiteres Jahr benötigt.Das Verhältnis Cs:Sr erlaubt außerdem in der südöstlichen Nordsee eine gute Unterscheidung der aus der Nordsee bzw. durch den Kanal von Süden kommenden Wassermassen, die praktisch nebeneinander her bis etwa zum Beginn des Skagerraks fließen.Die Vertikalverteilung des¹³⁷Cs zeigt, wie zu erwarten ist, jahreszeitlich bedingte Unterschiede. Es treten aber auch Effekte auf, die sich anhand der bisher vorliegenden Daten noch nicht eindeutig erklären lassen.Das in der Nordsee vorhandene⁹⁰Sr sowie das^239+240Pu zeigen ein analoges Verteilungsschema verglichen mit dem des¹³⁷Cs. Ihre Konzentrationen liegen weit unter der des¹³⁷Cs (⁹⁰Sr 17,5%,^239+240Pu 0,03%).Das Tritium zeigt bei wesentlich höheren Konzentrationen dagegen eine völlig andere Verteilung, da seine Hauptzufuhr im wesentlichen über das von Land her zufließende Süßwasser erfolgt.

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Distribution et teneur de differents radionucleides artificiels, dans les eaux de la Mer du Nord entre les années 1977 et 1981 (completes par quelques résultats de 1982 à 1984)

Résumé Les mesures de concentration du Césium 137 dans les eaux de la Mer du Nord, acquises entre les années 1977 et 1982, confirment largement les résultats obtenus au cours des années précédentes. Après un net maximum en 1978 — occassionné par un apport particulièrement fort en 1977 — la quantité totale de Césium 137 présent en Mer du Nord a régressé,jusqu'en 1982, aux alentours de la moitié de ces valeurs maximales.Il a pu être observé une modification importante du rapport Césium 137/Strontium 90, en faveur du Strontium 90, sur le trajet de Sellafield Works prés de la Mer d'Irlande jusqu'à la Mer du Nord.En suivant l'évolution temporelle de la valuer de ce rapport en différents points de mesure, on peut en déduire une durée de transport d'environ 3 ans entre Sellafield Works et Pentland Firth; une année supplémentaire est ensuite nécessaire pour pénétrer en Mer du Nord Sud-orientale.En Mer du Nord Sud-orientale, le rapport Césium/Strontium permet en outre d'effectuer une nette distinction entre les masses d'eau pénétrant respectivement par le Nord dans la Mer du Nord et celles pénétrant par le Sud et venant de la Manche. Ces masses d'eau s'écoulent pratiquement côte à côte jusqu'à l'entrée du Skagerrak.Comme l'on pouvait s'y attendre, la distribution verticale du Césium est différente suivant les saisons. Cependant il apparaît également des effects qui, sur la base des données disponibles à ce jour, ne s'expliquent pas encore clairement.Le Strontium 90 aussi bien que le Plutonium 239+240 présent dans la Mer du Nord, montrent une distribution comparable, analogue à celle du Césium 137. Leurs concentrations sont bien inférieures à celle du Césium 137 (Strontium 90 17,5%; Plutonium 239+240 0,03%).Le tritium d'autre part, — avec des concentrations significativement plus fortes —montre une distribution complètement différente, due principalement au fait qu'il est introduit par l'intermédiaire de l'écoulement d'eau douce provenant de la terre.

     

The state of Lake Ladoga pollution by global 90Sr, 137Cs, and 239,240Pu

The state of radioactive pollution of Lake Ladoga has been studied. The purification half-life of lake water from ⁹⁰Sr was found to be 21.7 year. The ratio of ⁹⁰Sr storage in lake water volume to its storage in silts (0?C10 cm layer) was 2: 1. Lake water purification from global ¹³⁷Cs was slower than that from ¹³⁷Cs originating from Chernobyl emergency emission because of the chronic supplement of global ¹³⁷Cs reserve by atmospheric fallouts. The behavior of ⁹⁰Sr, ¹³⁷Cs, and ^239,240Pu in bed soils was in agreement with the geochemical nature of the elements. By the distribution of ^{239, 240}Pu in bed soils, the sedimentation of substances of non-radiation nature was estimated at 0.3 and 0.5 mm/year at denting and flat relief, respectively.     

239+240Pu and 137Cs concentrations for zooplankton and nekton in the Northwest Pacific and Antarctic Oceans (1993-1996)

The concentrations of 239+240Pu and 137Cs in zooplankton and nekton in the Northwest Pacific and Southern Oceans were measured during the period 1993-1996. The object of the sampling was to assess the potential impacts of existing submerged anthropogenic-radioactive materials in the western North Pacific as well as the East China Sea. Samples from the Bransfield Strait of the Antarctic Ocean provided a control source impacted by only atmospheric bomb fallout. No particularly elevated levels of 239+240Pu were found in zooplankton samples from the Northwest Pacific, although significantly lower levels of 239+240Pu were found in three mixed zooplankton samples from the Bransfield Strait. The body burden of 239+240Pu in zooplankton appears to reflect concentrations in ambient seawater with some variation. Some additional measurements of 137Cs in fish are also reported here to complement existing databases and for future reference in the regional marine environmental radioactivity monitoring effort.     

Transport and deposition of plutonium in the ocean: evidence from Gulf of Mexico sediments

A study of sediments in the Gulf of Mexico shows dramatic gradients in Pu content and isotope ratios from the continental shelf to the Sigsbee Abyssal Plain. In terms of predicted direct fallout inventory of Pu, one shelf core contains 745% of the predicted inventory, while abyssal plain sediments contain only 15–20% of the predicted value. Absolute Pu concentrations of shelf sediments are also conspicuously high, up to 110 dpm/kg, compared to 13.5 dpm/kg in Mississippi River suspended sediment. There is no evidence of Pu remobilization in Gulf of Mexico shelf sediments, based on comparison of Pu profiles with Mn/Al and Fe/Al profiles. Horizontal transport of fallout nuclides from the open ocean to removal sites in ocean margin sediments is concluded to be the source of both the high concentrations and high inventories of Pu reported here.The shelf sediments show²⁴⁰Pu/²³⁹Pu ratios close to 0.179, the average stratospheric fallout value, but the ratios decrease progressively across the Gulf to low values of 0.06 in abyssal plain sediments. The source of low-ratio Pu in deep-water sediments may be debris from low yield tests transported in the troposphere. Alternatively, it may represent a fraction of the Pu from global stratospheric fallout which has been separated in the water column from the remainder of the Pu in the ocean. In either case, the low-ratio material must have been removed rapidly to the sea floor where it composes a major fraction of the Pu in abyssal plain sediments. Pu delivered by global atmospheric fallout from the stratosphere has apparently remained for the most part in the water or has been transported horizontally and removed into shallow-water sediments.     

Spatial variability in sedimentation rates and artificial radionuclide storage in alluvial banks of the lower Rh?ne River

This paper analyzes the relationship between bank sediment storage and radionuclide content in six alluvial sites located in different geomorphic contexts along the lower Rh?ne River. The ¹³⁷Cs, ²³⁸Pu, ^239+240Pu, ²⁴¹Am and ²¹⁰Pb profiles show different patterns, which indicates a differential storage of contaminated sediment in the banks. Three sites record historical nuclear releases in the river and give evidence for long-term retention of particle-reactive long-lived radionuclides. Two sites record only atmospheric global fallout. Only one site, connected to the river groundwater, provides some evidence for desorption of particle-bound contaminants, with a low and constant ¹³⁷Cs activity profile. The history of the releases from the Marcoule spent-fuel reprocessing plant—the main source of artificial radioactivity—provides a reliable chronology of the last 50?years. Sediment grain size and bank topography are important factors in determining where artificial radionuclides are stored, but these two parameters cannot be used alone to determine variations in high concentrations of radionuclides. The chronology of fluvial geomorphic “metamorphosis” during the twentieth Century, especially after 1960, is also a critical factor affecting the spatial variability in sedimentation rates and artificial radionuclide storage; the timing of channel deepening and bank sedimentary accretion interfere with the chronology of major floods and the short period of low discharge during the height of contamination from nuclear liquid effluents. The reach-scale adjustment described in this paper can contribute to determining what the local history may have been. This result has important implications for river management decisions.     

137Cs湖泊沉积年代学方法应用的局限——以Crawford湖为例

＾１３７Ｃｓ湖泊沉积年代学方法是测定现代湖泊沉积物沉积年代和沉积速率的重要同位素年代学方法之一。对加拿大Ｃｒａｗｆｏｒｄ湖采集的沉积孔柱内＾１３７Ｃｓ垂直分布的研究发现,该方法给出时的标有明显偏差。比较＾２１０Ｐｂ和纹层等年代方法的结果,其１９６３年时标蓄积峰值所在位置明显移向表层,而作为１９５４年时标的该核素出现蓄积的层位则远早于该年沉积物蓄积层位。研究还表明,孔柱中较高的间隙水含量、缺少足以吸     

The240Pu239Pu ratio,a potential geochronometer

The Arctic and Antarctic ice sheets maintain records of the atmospheric fallout in their datable strata. The ²⁴⁰Pu²³⁹Pu ratios in these polar reservoirs uniquely distinguish particulate fallout from the pre-moratorium nuclear atmospheric weapons tests, dominated by the U.S., and the post-moratorium atmospheric weapons tests, dominated by the U.S.S.R. Thus, they offer the possibility of use as a geochronological tool for some marine, glacial, lacustrine and soil systems.     

Geochronological reconstruction of Cs transport from the Coruh river to the SE Black Sea: comparative assessment of radionuclide retention in the mountainous catchment area

The deposition record of ¹³⁷Cs was traced in the SE Black Sea sediments adjacent to the Coruh river mouth in comparison with the earlier studied chronology of ¹³⁷Cs deposition in front of the Danube delta (NW Black Sea). In both cases, the ¹³⁷Cs profiles showed two subsurface peaks attributable to maximum fallout of ‘bomb’ and Chernobyl radionuclides. The Coruh profile revealed a larger contribution of ‘bomb’ ¹³⁷Cs in comparison with the Chernobyl input, suggesting different coverage of NW and SE Black Sea regions with the Chernobyl fallout. The ¹³⁷Cs-derived dating showed that maximum deposition of particulate bound ¹³⁷Cs in sediments adjacent to the Coruh river mouth was delayed for 14 yr relative to date of Chernobyl accident, reflecting a buffer effect of the watershed soils. This transit time is 3 times longer than in the Danube catchment area, indicating a difference in retention processes in these mountainous (Coruh) and lowland (Danube) river basins. The ¹³⁷Cs profile in Coruh sediments showed penetration of ¹³⁷Cs to much greater depth than would be expected from ¹³⁷Cs fallout chronology, suggesting the sediment mixing rate of 1.3 cm² yr⁻¹. This value was used to evaluate deposition chronology of ¹³⁷Cs, applying the model developed for pulse fallout case. Comparing the measured and modelled data has allowed differentiation of the flood-induced discharge of the ¹³⁷Cs-containing suspended matter and the slower transit of eroded soil particles from the contaminated catchment areas. The obtained results may be used for the prediction of period when the pollutants, deposited over the river basins, can reach the Black Sea.     

241Pu/239+240Pu ratios in polar glaciers

The analyses of plutonium isotopes in dated strata of polar ice sheets indicate that the²⁴¹Pu/^239+240Pu activity ratio produced in the U.S.-dominated nuclear tests during the 1950s was about 26, while that in the U.S.S.R.-dominated weapons tests in the early 1960s was between 12 and 14. This difference provides time horizons for sedimentary deposits. Further, the²³⁹Pu/²⁴⁰Pu ratio may show a similar difference in fallout values from these two periods of weapons testing and may provide an additional, and perhaps more sensitive, chronology for sediments.     

Investigations of gram quantities of Atlantic and Pacific surface particulates

Particulates amounting to 0.1–2.0 g efficiently collected from large volumes of Atlantic and Pacific surface waters have been analyzed for carbonate, opal, quartz and several natural and man-made radioisotopes.The concentrations of particles range between 10 and 600 μg/kg. In the equatorial regions particle concentrations are low and similar in both the oceans. At higher latitudes (>30°N or S), the Atlantic waters, however, have higher concentrations of particles compared to those in the Pacific. The latitudinal distribution exhibits a north-south symmetry with higher concentrations in the 30°–60° belt. Based on the particulate abundance for CaCO₃ and opal and their sedimentation, we have estimated their production and in-situ integrated dissolution rates for a few regions.Radioisotopes having different source functions, namely¹⁴C and²³⁹Pu injected due to nuclear weapon tests,²³⁴Th,²³⁰Th and²²⁸Th produced in-situ in seawater,²³²Th which derives primarily from land,²¹⁰Pb introduced via wet precipitations and²²⁶Ra introduced through diffusion from deep-sea sediments have been measured in the particulates. The relative enrichment factors for these nuclides in particles vary as Th ? Pu > Pb > Ra. The atmospheric bomb fallout pattern is discernible in the surface particulates; the²³⁹Pu concentration increases with latitude in both the hemispheres; however, the values are about a factor of two lower in the southern hemisphere.The distribution pattern of radioisotopes is found to be complex, even for²³⁴Th whose source function in the oceans is uniform. In view of the differences in the source functions it becomes possible to delineate the principal geochemical/geophysical processes which determine the concentrations of these nuclides in surface waters.     

Natural and anthropogenic radionuclide distributions in the northwest Atlantic Ocean

We have used in-situ pumps which filter large volumes of sea water through a 1 μm cartridge prefilter and two MnO₂-coated cartridges to obtain information on dissolved and particulate radionuclide distributions in the oceans. Two sites in the northwest Atlantic show subsurface maxima of the fallout radionuclides¹³⁷Cs,^239,240Pu and²⁴¹Am. Although the processes of scavenging onto sinking particles and release at depth may contribute to the tracer distributions, comparison of predicted and measured water column inventories suggests that at least 35–50% of the Pu and²⁴¹Am are supplied to the deep water by advection.The depth distributions of the naturally occurring radionuclides²³²Th,²²⁸Th and²³⁰Th reflect their sources to the oceans.²³²Th shows high dissolved concentrations in surface waters, presumably as a result of atmospheric or riverine supply. Activities of²³²Th decrease with depth to values 0.01 dpm/1000 l.²²⁸Th shows high activities in near surface and near bottom water, due to the distribution of its parent,²²⁸Ra. Dissolved²³⁰Th, produced throughout the water column from²³⁴U decay, increases with depth to 3000 m. Values in the deep water (> 3000 m) are nearly constant ( 0.6–0.7 dpm/1000 l), and the distribution of this tracer (and perhaps other long-lived particle-reactive tracers as well) may be affected by the advection inferred from Pu and²⁴¹Am data.The ratio of particulate to dissolved activity for both²³⁰Th and²²⁸Th is 0.15–0.20. This similarity precludes the calculation of sorption rate constants using a simple model of reversible sorption equilibrium. Moreover, in mid-depths²²⁸Th tends to have a higher particulate/dissolved ratio than²³⁰Th, suggesting uptake and release of²³⁰Th and²²⁸Th by different processes. This could occur if²²⁸Th, produced in surface water, were incorporated into biogenic particles formed there and released as those particles dissolved or decomposed during sinking.²³⁰Th, produced throughout the water column, may more closely approach a sorption equilibrium at all depths.²³⁰Th,²⁴¹Am and^239,240Pu are partitioned onto particles in the sequence Th > Am > Pu with 15% of the²³⁰Th on particles compared with 7% for Am and 1% for Pu. Distribution coefficients (K_d) are 1.3–1.6 × 10⁷ for Th, 5–6 × 10⁶ for Am and 7–10 × 10⁵ for Pu. The lower reactivity for Pu is consistent with analyses of Pu oxidation states which show 85% oxidized (V + VI) Pu. However, theK_d value for Pu may be an upper limit because Pu, like²²⁸Th, may be incorporated into particles in surface waters and released at depth only by destruction of the carrier phase.     

The use of 137Cs as a tracer in an erosion study in south limburg (the Netherlands) and the influence of chernobyl fallout

The ¹³⁷Cs radioactivity of soils was used as a tracer of soil erosion in a catchment in the Netherlands: 143 samples were analysed to map the ¹³⁷Cs redistribution using geostatistical interpolation methods. Caesium-137 activities on grassland are significantly higher than on arable land. Also, ¹³⁷Cs activities on waning slopes are higher and activities on steep slopes are lower. The soil erosion estimates, derived from the ¹³⁷Cs data, are used to validate the USLE erosion model. The recent Chernobyl nuclear accident also contributed to the ¹³⁷Cs activity. However, the Chernobyl input of ¹³⁷Cs, with a constant ratio of 1.765:1 to ¹³⁴Cs, cannot be used as a tracer of soil erosion. Because of the rapid decay of ¹³⁴Cs, we will not be possible to separate the sources of ¹³⁷Cs in the near future in areas significantly influenced by Chernobyl fallout and in these areas ¹³⁷Cs can no longer be used as a soil erosion tracer.     

Landscape‐scale controls on the spatial distribution of caesium 137: A study based on an airborne geophysical survey across Northern Ireland

The spatial distribution of ¹³⁷Cs across the landscape and the processes controlling its redistribution are of interest because (i) ¹³⁷Cs has been widely used to quantify the movement of soil and sediments and (ii) substantial fallout of ¹³⁷Cs after the Chernobyl accident has led to contamination of foodstuffs in some places. A high‐resolution airborne geophysical radiometric survey of Northern Ireland has provided an opportunity to study the distribution and possible redistribution of ¹³⁷Cs. The ¹³⁷Cs activity (recorded at 1·2 million points) is distributed in a series of bands oriented approximately 160° and 115° clockwise from north. Geostatistical analysis of the data shows a strong, short‐range structure (correlation ranges between 0·6 and 8 km) in ¹³⁷Cs activity across the vast majority of the region; the spatial distribution shows association with a published, coarse‐scale depositional pattern of ¹³⁷Cs from Chernobyl. Two indices of land form derived from a digital elevation model, namely compound topographic index and the length–slope factor of the Revised Universal Soil Loss Equation, account for only 3% of the variance in ¹³⁷Cs activity. In contrast, soil type and land cover in combination (including their interaction) account for 20% of the variance. In areas that received moderate fallout from Chernobyl, soil type alone accounts for a substantial proportion of the spatially correlated ¹³⁷Cs activity. We attribute this to each soil type having a fairly uniform radiocaesium interception potential that differs from those of other soil types and that this potential controls the vertical migration of ¹³⁷Cs. Over the granitic Mourne Mountains there is a strong spatial cross‐correlation between ¹³⁷Cs activity and airborne estimates of soil potassium, suggesting that the latter provides a measure of the soil's radiocaesium interception potential; this is probably dominated by the quantity of the mineral illite. Copyright © 2010 John Wiley & Sons, Ltd. and British Geological Survey