Transport of the environmental radionuclides in an alpine watershed

The radionuclides¹³⁷Cs,²¹⁰Pb and⁷Be have been examined in the alpine Rhoˆne watershed (Switzerland) during a period of two years in order to evaluate their usefulness as tracers of the removal and transport rate of top-soil particles and particle-reactive contaminants of atmospheric origin. The specific activities of the radionuclides in fluvial suspension show a distinct seasonal pattern which depends on the hydrologic regime of the stream and the sources of the suspended matter. Input-output budgets based on the atmospheric deposition and fluvial removal of three radionuclides in the alpine Rhoˆne watershed are used to estimate their erosional residence times. The simplest one box model yields mean residence times of about 800 and 1400 years for¹³⁷Cs and²¹⁰Pb, respectively. The removal rate of short-lived⁷Be suggests that a part of the watershed (0.6–2.3% of the total surface) is exposed to a rapid erosion, in which the mean residence time of the radionuclides is in the range of 1–220 days. This has little influence on the calculated residence time of¹³⁷Cs but increases the estimated residence time of²¹⁰Pb in soil to over 1800 years. The use of²¹⁰Pb-⁷Be pair in fluvial output may be very helpful in the assessment of the impact of atmospheric pollutants on the water quality in rivers and lakes.     

Natural radionuclide analysis in chattarpur area of southeastern coastal area of Odisha, India

The energy released in a spontaneous decay process of natural radionuclides is the main source of the total radiation dose to human beings. Natural radionuclides are widely distributed in soil, rocks, air, and groundwater. In present investigation, the analysis of terrestrial radionuclides such as ²²⁶Ra, ²³²Th, and ⁴⁰K in soil and sand of Chattarpur area of southeastern coast of Odisha has been carried out using NaI(Tl) gamma ray detector. The higher activity concentrations of naturally occurring radionuclides have been reported from the study area. The gamma radiationdose originating from the terrestrial radionuclides was found to vary from 95 to 1813 nGy/h with an average of 700 nGy/h. This study is important to generate a baseline data of radiation exposure in the area. Health hazard effects due to natural radiation exposure are discussed in details.     

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.     

Implication and hazard of radiation level in the building materials

The natural radioactivity due to radium, thorium, and potassium in building material samples contribute to the radiation dose received by human beings significantly. It is essential to evaluate the activity levels of these nuclides for the assessment of natural radiation dose. Activity concentrations of the gamma emitting primordial radionuclides ²³²Th, ²²⁶Ra, and ⁴⁰K were measured using high resolution gamma spectrometry technique with high purity germanium (HPGe) detector in building materials: sand, brick, granite, cement and rock, collected from various areas of Gulbarga and Koppal districts. The standard ASTM procedure was followed for the sample preparation. The distribution of radionuclides and variation in activity concentration depend upon the rock formation and the geological properties of the region. The activity of the three radionuclides, ²³²Th, ²²⁶Ra, and ⁴⁰K, were found to be in the range of 3.1–227.1, 1.6–111, and 23.2–1505 Bq/kg, respectively. The dose related radiological parameters were also calculated for all the samples and the observations show that the activity concentrations of the radionuclides are well within the UNSCEAR limits.     

Quantitative assessment of dissolved radiotracers in the English Channel: Sources, average impact of la Hague reprocessing plant and conservative behaviour (1983, 1986, 1988, 1994)

Knowledge of long-term movements of water-masses in the English Channel has been substantially improved using hydrodynamic modelling coupled with radio-tracers studies; nevertheless, the precision of results so obtained is still largely dependent on measurement precision. New tools are now available to make more accurate determinations of radio-tracer distribution: (1) Repositioning of station locations at the same tide reference-time, giving a homogeneous spatial data set, coupled with the possibility of interpolating and quantifying the amounts of dissolved radioactivity flowing through the English Channel; (2) the first measurements of tritium (³H) in seawater on a large scale in the English Channel demonstrate that this fully conservative radionuclide is a clearly identifiable marker of industrial releases; (3) recent campaigns carried out during the FLUXMANCHE II CCE (1994) programme show the general distribution of dissolved radionuclides ¹³⁷Cs, ¹³⁴Cs, ⁶⁰Co, ¹²⁵Sb, ¹⁰⁶Ru and ³H in the English Channel and the Irish Sea; and (4) the re-utilisation of data from previous campaigns (1983, 1986, 1988) provides indications, at any given location in the English Channel, about the average dilution and distribution of releases derived from the La Hague reprocessing plant. Excesses and losses of radionuclides are now quantified with respect to known source terms; estimates of losses are provided for non-conservative radionuclides, while an excess of ¹³⁷Cs was observed in the English Channel during the period 1983–1994. This excess, which has the same order of magnitude as the quantities released from La Hague plant in the English Channel, could be explained by about 1% of the Sellafield reprocessing plant releases entering the Channel. These results confirm and give a more detailed picture of the previously known distribution of water masses in the English Channel. They lead to clear information about transit times and dilution at this scale, and provide directly comparable data for the validation of hydrodynamic models.     

Rating Water Quality in Sevastopol Bay by the Fluxes of Pollutant Deposition in Bottom Sediments

Sevastopol Bay is used as an example for the development of criteria for rating anthropogenic impact by elimination fluxes from the water area of post-Chernobyl (⁹⁰Sr, ¹³⁷Cs, ^239,240Pu) and natural (²¹⁰Pо) radionuclides, as well as mercury and organochlorine compounds. The differentiation of the bay water area into zones with different biogeochemical conditions and the balance approach to interpreting field observation data were used to assess the conditioning capacity of Sevastopol Bay ecosystem for conservative radioactive and chemical substances by elimination fluxes of pollutants into aqueous depot, which is the open part of the Black Sea and into the geological depot, i.e., its bottom sediment stratum.     

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.     

Disequilibria betweenRa, Pb and Po in the Arctic Ocean and the implications for chemical modification of the Pacific water inflow

Measurements have been made of²²⁶Ra and both dissolved and particulate forms of²¹⁰Pb and²¹⁰Po in a vertical profile at 85°50′N, 108°50′W in the Arctic Ocean.In the upper water column²²⁶Ra shows a concentration maximum that is coincident with one in the nutrients, silicate, phosphate, and nitrate, while at the same depth, dissolved and particulate²¹⁰Pb and²¹⁰Po all show minimum concentrations. It is suggested that the concentration maxima are partly due to sources of the respective elements in the continental shelf sediments, the shelf waters being subsequently advected into the Arctic Ocean basins. The²¹⁰Pb and²¹⁰Po minima have similarly been explained by interaction between the shelf sediments and overlying waters. An estimate is made of the possible contributions of shelf sediments to the layer of silica-rich water which covers the Canada Basin at a depth of 100–150 m.Residence times have been calculated for dissolved²¹⁰Pb and²¹⁰Po at various depths in the water column. Surface water residence times of dissolved and particulate forms of these radionuclides are longer than in surface Atlantic waters, probably due to lower biological activity in the surface waters of the Canada Basin. An estimatee has been made of the average sinking velocity of particulate material.     

Natural radionuclides in the water of Narragansett Bay

The concentrations of radionuclides of the U-Th series (²³⁸U,²³⁴Th,²³⁴U,²³⁰Th,²²⁶Ra,²¹⁰Pb,²¹⁰Po, and²³²Th,²²⁸Ra,²²⁸Th) in the water of Narragansett Bay are reported. Analysis of the total, particulate, dissolved and colloidal forms of Th isotopes reveal a consistent removal behavior which is controlled mainly by the particulate matter concentration and the sediment resuspension rate. Half-removal times of Th from solution onto particles range from 1.5 to 15 days, and settling velocities of Th containing particles range generally between 1 and 11 m/day.²¹⁰Pb and²¹⁰Po concentrations are seasonally dependent, with higher concentrations and slower removal during the early summer (half-removal times from solution onto particles of 1–5 days in winter and up to 2 months in early summer).     

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.     

Floodplain sedimentation rates in an alpine watershed determined by radionuclide techniques

Vertical profiles of the activities of ¹³⁷Cs and ²¹⁰Pb were measured on floodplain sediment cores and upland soil cores along the Soda Butte Creek and the Yellowstone River to determine floodplain sedimentation rates. The position of mine tailings from a 1950 impoundment failure was used as a stratigraphic marker to estimate the sedimentation rates and to make comparisons with rates provided by radionuclide‐based methods. Mass accumulation (sedimentation) rates calculated from the position of the mine tailings ranged from 0·00 to 0·17 g cm^?2 yr^?1 and were in good agreement with sedimentation rates calculated from the inventories of ¹³⁷Cs and ²¹⁰Pb. Sedimentation rates calculated from the position of the ¹³⁷Cs peak generally overestimated the sedimentation rates, probably because of increased downward migration of ¹³⁷Cs caused by the low pH of water moving through the mine tailings or the high permeability of floodplain sediments relative to upland reference soils. This study demonstrates that the ¹³⁷Cs and ²¹⁰Pb inventory methods for determining sedimentation rates can be applied to an alpine floodplain where sedimentation events are episodic and where orographic effects on precipitation generate strong downstream gradients in the delivery of atmospheric radionuclides. Copyright © 2007 John Wiley & Sons, Ltd.     

Sedimentary processes in the inner New York Bight: Evidence from excess210Pb and239,240Pu

Particle-reactive radionuclides were determined in sediments from the inner New York Bight to trace transport and storage of fine-grained sediments and associated reactive materials. Seven sediment ? cores 20–50 cm in length were analyzed for water content, loss on ignition (LOI) and excess²¹⁰Pb; three of these were also analyzed for^239,240Pu. Excepting some depth horizons in a core from a dredge-spoil dumpsite, every sample analyzed contained excess²¹⁰Pb. Variations in the concentration of excess²¹⁰Pb with depth in the sediment at all stations correlated strongly with LOI, which apparently traces that fraction of the sediment which is active in removing reactive elements from the water column. In the cores analyzed for^239,240Pu, every sample contained finite Pu, and Pu concentrations correlated strongly with excess²¹⁰Pb.The radionuclide distributions may be simply viewed as products of steady-state sediment accumulation or of mixing. Geochemically reasonable accumulation rates are very high (0.5–2.6 g/cm² y) and could probably only be sustained by offshore transport of dumped materials. At the other extreme the relationships between excess²¹⁰Pb and LOI are compatible with rapid mixing of a²¹⁰Pb carrier phase (traced by LOI) into the pre-existing substrate with little or no actual accumulation. Other non-steady-state processes, such as sediment gravity flow, could also explain the observed distributions.Measured sediment inventories (dpm/cm²) of excess²¹⁰Pb and Pu at these stations are greatly in excess of those supportable by direct atmospheric deposition: lateral supply is required. Incorporation of sedimentary fines into the sand substrate could make the inner New York Bight an important repository of reactive materials.     

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.     

Surface Water Contamination by Uranium Mining/Milling Activities in Northern Guangdong Province,China

The northern region of Guangdong Province, China, has suffered from the extensive mining/milling of uranium for several decades. In this study, surface waters in the region were analyzed by inductively coupled plasma optical emission spectrometry (ICP‐OES) for the concentrations of uranium (U), thorium (Th), and non‐radioactive metals (Fe, Mn, Mg, Li, Co, Cu, Ni, and Zn). Results showed highly elevated concentrations of the studied radionuclides and metals in the discharged effluents and the tailing seepage of the U mining/milling sites. Radionuclide and heavy metal concentrations were also observed to be overall enhanced in the recipient stream that collected the discharged effluents from the industrial site, compared to the control streams, and rivers with no impacts from the U mining/milling sites. They displayed significant spatial variations and a general decrease downstream away from upper point‐source discharges of the industrial site. In addition, obvious positive correlations were found between U and Th, Fe, Zn, Li, and Co (R² > 0.93, n = 28) in the studied water samples, which suggest for an identical source and transport pathway of these elements. In combination with present surface water chemistry and chemical compositions of uraniferous minerals, the elevation of the analyzed elements in the recipient stream most likely arose from the liquid effluents, processing water, and acid drainage from the U mining/milling facilities. The dispersion of radionuclides and hazardous metals is actually limited to a small area at present, but some potential risk should not be negligible for local ecosystem. The results indicate that environmental remediation work is required to implement and future cleaner production technology should be oriented to avoid wide dispersion of radioactivity and non‐radioactive hazards in U mining/milling sites.     

Radionuclide ratios in wet and dry deposition samples from June 1976 through December 1977

²³⁸Pu,²³⁹Pu and¹³⁷Cs in rain and dry fallout and⁹⁰Sr in rain samples were measured at Woods Hole, Massachusetts, from June 1976 through December 1977. The dry fallout was estimated to be about 7.8% of the total deposition of²³⁹Pu and¹³⁷Cs.²³⁹Pu/¹³⁷Cs ratios, almost constant at about 0.011 in rain or dry fallout, February through December 1977, suggested that fractionation between the refractory and volatile radionuclides is insignificant in stratospheric fallout. This supports the idea of regional homogeneity of radionuclide ratios in fallout.     

Isotopic Characterization of Radioiodine and Radioxenon in Releases from Underground Nuclear Explosions with Various Degrees of Fractionation

Both radioxenon and radioiodine are possible indicators for a nuclear explosion. Therefore, they will be, together with other relevant radionuclides, globally monitored by the International Monitoring System in order to verify compliance with the Comprehensive Nuclear-Test-Ban Treaty once the treaty has entered into force. This paper studies the temporal development of radioxenon and radioiodine activities with two different assumptions on fractionation during the release from an underground test. In the first case, only the noble gases are released, in the second case, radioiodine is released as well while the precursors remain underground. For the second case, the simulated curves of activity ratios are compared to prompt and delayed atmospheric radioactivity releases from underground nuclear tests at Nevada as a function of the time of atmospheric air sampling for concentration measurements of ¹³⁵I, ¹³³I and ¹³¹I. In addition, the effect of both fractionation cases on the isotopic activity ratios is shown in the four-isotope-plot (with ¹³⁵Xe, ^133mXe, ¹³³Xe and ^131mXe) that can be utilized for distinguishing nuclear explosion sources from civilian releases.     

Geothermal springs of the West Florida continental shelf: Evidence for dolomitization and radionuclide enrichment

On the sea bed of the West Florida continental shelf about 45 km SSW of Ft. Myers, Florida, an 85-km² area has been discovered in which six thermal springs discharge warm, chemically altered seawater from vents and seepage zones. The spring water apparently originates in the subsurface ocean around the Florida Platform and penetrates the highly porous strata of the platform about 500–1000 meters below sea level. It percolates toward the interior of the platform and is geothermally heated to about 40°C en route. Then it rises along more vertical flow channels and is discharged in warm submarine springs.Beneath the platform, several chemical processes alter the percolating seawater. One process seems to be a secondary dolomitization of the limestone of the platform because, in the discharging seawater, magnesium is lower by 2.7 mmole/kg and calcium higher by 3.6 mmole/kg than in normal seawater with the same chlorinity. Other reactions within the sediments of the platform enrich the spring effluents 1000-fold in²²⁶Ra, 10,000-fold in²²²Rn, and 90-fold in²²⁸Ra compared to the seawater surrounding the platform. Thus, the springs may be important sources of radionuclides for the Gulf of Mexico. The percolating seawater also loses all of its oxygen and nitrate to reduction processes, loses most of its phosphate and 40% of its²³⁸U, and roughly quadruples its silica content.Coastal carbonate platforms are fairly common geological features. Thus, processes like those beneath the West Florida Shelf may function on a world-wide basis to play an important role in the diagenesis of carbonate sediments.     

Role of in situ cosmogenic nuclides 10be and 26al in the study of diverse geomorphic processes

The central premises of applications of the in situ cosmogenic dating method for studying specific problems in geomorphology are outlined for simple and complex exposure settings. In the light of these general models, we discuss the information that can be derived about geomorphic processes, utilizing concentrations of in situ produced cosmogenic radionuclides ¹⁰Be (half-life=1·5 ma) and ²⁶A1 (half-life=0·7 ma) in a variety of geomorphic contexts: glacial polish and tills; meteorite impact craters; alluvial fans; paleo-beach ridges; marine terraces; sand dunes; and bedrock slopes. We also compare ¹⁰Be-²⁶Al data with results obtained by other dating methods. We conclude that the technique of measuring in situ cosmic ray produced nuclides holds promise for quantitative studies of processes and time-scales in a wide range of geomorphological problems.     

Comparison of 14C and 210Pb - 137Cs - 241Am dating methods of a recent bat guano deposit (Lot,SW France)

Bat guano deposits are increasingly used as records of past environmental changes, an approach that requires a precise chronology of the guano layers. This paper presents a comparison between the well-established ¹⁴C dating method and methods based on natural ²¹⁰Pb excesses, (²¹⁰Pb)_ex, and artificial radionuclides ¹³⁷Cs and ²⁴¹Am. The studied example is a bat guano deposit from a cave in SW France (the Brantites III cave), which is currently investigated for paleo-environmental reconstructions using stable isotopes. ¹⁴C data show that the upper part of the guano deposit accumulated during the last 150 years with a marked increase in accumulation rates after around 1960 AD. While the incorporation of atmospheric ¹⁴C in guano is a well-understood process, the origin of ²¹⁰Pb excesses is more complex. Based on consideration of ¹³⁷Cs and (²¹⁰Pb)_ex inventories recorded in undisturbed soils in France, and the measured inventories in the guano deposit, we suggest that most of the ²¹⁰Pb excess is produced by ²²²Rn decay in the cave air and then adsorbed onto the guano. As Radon concentrations in caves can vary significantly on both short and long-term timescales, one needs to be cautious before applying the often-used CRS (constant rate of supply of ²¹⁰Pb excess) model to guano dating. Our (²¹⁰Pb)_ex data are best interpreted by two successive periods of roughly constant, but widely different accumulation rates (0.3 cm/y and 2.6 cm/y before and after 1960, respectively) and (²¹⁰Pb)_ex fluxes. We suggest that these relatively abrupt variations result from a change in cave ventilation leading to a more favourable shelter for bats after 1960. The upper 40 cm of the deposit shows evidence of ²¹⁰Pb mobility, adding a further complexity to the interpretation of (²¹⁰Pb)_ex profiles in guano deposits. However, the existence of well-defined ¹³⁷Cs and ²⁴¹Am peaks allows a precise identification of the year of maximum atmospheric fallouts (∼1963–1964). When the ages provided by artificial radionuclides are combined with the ²¹⁰Pb-derived accumulation rates, an age model can be built, which is in good agreement with the ¹⁴C age model. This example shows that the (²¹⁰Pb)_ex method, when associated with ¹³⁷Cs (²⁴¹Am) data, can be used to date recent guano deposit, although its application is not as straightforward as the ¹⁴C method.     

Influence of melt‐freeze‐cycles on the radionuclide transport in homogeneous laboratory snowpack

Radionuclides released to the environment and deposited with or onto snow can be stored over long time periods if ambient temperature stays low, particularly in glaciated areas or high alpine sites. The radionuclides will be accumulated in the snowpack during the winter unless meltwater runoff at the snow base occurs. They will be released to surface waters within short time during snowmelt in spring. In two experiments under controlled melting conditions of snow in the laboratory, radionuclide migration and runoff during melt‐freeze‐cycles were examined. The distribution of Cs‐134 and Sr‐85 tracers in homogeneous snow columns and their fractionation and potential preferential elution in the first meltwater portions were determined. Transport was associated with the percolation of meltwater at ambient temperatures above 0 °C after the snowpack became ripe. Mean migration velocities in the pack were examined for both nuclides to about 0.5 cm hr^?1 after one diurnal melt‐freeze‐cycle at ambient temperatures of ?2 to 4 °C. Meltwater fluxes were calculated with a median of 1.68 cm hr^?1. Highly contaminated portions of meltwater with concentration factors between 5 and 10 against initial bulk concentrations in the snowpack were released as ionic pulse with the first meltwater. Neither for caesium nor strontium preferential elution was observed. After recurrent simulated day‐night‐cycles (?2 to 4 °C), 80% of both radionuclides was released with the first 20% of snowmelt within 4 days. 50% of Cs‐134 and Sr‐85 were already set free after 24 hr. Snowmelt contained highest specific activities when the melt rate was lowest during the freeze‐cycles due to concentration processes in remaining liquids, enhanced by the melt‐freeze‐cycling. This implies for natural snowpack after significant radionuclide releases, that long‐time accumulation of radionuclides in the snow during frost periods, followed by an onset of steady meltwater runoff at low melt rates, will cause the most pronounced removal of the contaminants from the snow cover. This scenario represents the worst case of impact on water quality and radiation exposure in aquatic environments.