An assessment of the reported leakage of anthropogenic radionuclides from the underground nuclear test sites at Amchitka Island, Alaska, USA to the surface environment

Three underground nuclear tests representing approximately 15-16% of the total effective energy released during the United States underground nuclear testing program from 1951 to 1992 were conducted at Amchitka Island, Alaska. In 1996, Greenpeace reported that leakage of radionuclides, 241Am and 239+240Pu, from these underground tests to the terrestrial and freshwater environments had been detected. In response to this report, a federal, state, tribal and non-governmental team conducted a terrestrial and freshwater radiological sampling program in 1997. Additional radiological sampling was conducted in 1998. An assessment of the reported leakage to the freshwater environment was evaluated by assessing 3H values in surface waters and 240Pu/239Pu ratios in various sample media. Tritium values ranged from 0.41 Bq/l +/- 0.11 two sigma to 0.74 Bq/1 +/- 0.126 two sigma at the surface water sites sampled, including the reported leakage sites. Only at the Long Shot test site, where leakage of radioactive gases to the near-surface occurred in 1965. were higher 3H levels of 5.8 Bq/1 +/- 0.19 two sigma still observed in 1997, in mud pit #3. The mean 240Pu/239Pu for all of the Amchitka samples was 0.1991 +/- 0.0149 one standard deviation, with values ranging from 0.1824 +/- 1.43% one sigma to 0.2431 +/- 6.56% one sigma. The measured 3H levels and 240Pu/239Pu ratios in freshwater moss and sediments at Amchitka provide no evidence of leakage occurring at the sites reported by Buske and Miller (1998 Nuclear-Weapons-Free America and Alaska Community Action on Toxics, Anchorage, Ak, p.38) and Miller and Buske (1996 Nuclear Flashback: The Return to Anchitka, p.35). It was noted that the marine sample; 240Pu/239Pu ratios are statistically different than the global fallout ratios presented by Krey et al. (1976) and Kelley, Bond, and Beasley (1999). The additional non-fallout component 240Pu/239Pu ratio, assuming a single unique source, necessary to modify the global fallout 240Pu/239Pu ratio to that measured in the marine samples is on the order of 0.65 (Hameedi, Efurd, Harmon, Valette-Silver, & Robertson, 1999; Kelley et al., 1999). While this potentially suggests another plutonium source, such as high burn-up nuclear reactor fuel, rather than underground nuclear tests, the uncertainties in analyses and environmental processes need to be fully assessed before any conclusion can be reached. Further work is needed to evaluate these findings and to support any radiological assessment of the marine environment surrounding Amchitka. Based on geohydrological testing and modeling, leakage from the Amchitka Underground Nuclear Tests is projected to occur to the marine environment (Claassen, 1978; Fenske, 1972; Wheatcraft, 1995).     

Characterisation of prompt and delayed atmospheric radioactivity releases from underground nuclear tests at Nevada as a function of release time

A database with information on about 500 cases of atmospheric radioactivity releases from underground nuclear tests is analysed. The data are statistically evaluated and systematically aggregated in order to characterise prompt uncontrolled as well as delayed operational releases of radioactivity into the atmosphere. The focus is put on the latter. The reported data compare well with theoretically derived xenon activities for reasonable nuclear test scenarios. Conclusions are drawn on the main features of releases that can be expected from underground nuclear tests as a function of release time. These findings are relevant for developing and validating methods to be applied in global monitoring of atmospheric radioactivity with respect to indications of an underground nuclear explosion.     

A toxicity assessment of soils sampled from the Balapan site of the Semipalatinsk nuclear test site

Toxicity of soils sampled from the area of the “Chagan” explosion (the Balapan site of the Semipalatinsk nuclear test site, Kazakhstan) were assayed with the use of biological tests and physicochemical analysis. Soils from the most part (2.56 km² out of 4 km²) of the area studied were found to be toxic. Soil aqueous extracts toxicity substantially resulted from ¹³⁷Cs and ⁹⁰Sr effects. The soil toxicity assessment with the use of biological test—an increase Chlorella vulgaris Beijer. biomass production after 24 exposure of soil aqueous extracts in 63% cases are in agree with conclusions on the degree of radioactive contamination based on Basic Sanitary Rules of Radiation Safety (BSRRS-99). The IAEA safety norms were found to be quite stricter than the results of the biological test.     

Assessing field-scale migration of radionuclides at the Nevada Test Site: "mobile" species

Many long-lived radionuclides are present in groundwater at the Nevada Test Site (NTS) as a result of 828 underground nuclear weapons tests conducted between 1951 and 1992. In conjunction with a comprehensive geochemical review of radionuclides ((3)H, (14)C, (36)Cl, (99)Tc and (129)I) that are presumably mobile in the subsurface, we synthesized a body of radionuclide activity data measured from groundwater samples collected at 18 monitoring wells, to qualitatively assess their migration at the NTS over distances of hundreds of meters and over timescales of decades. Tritium and (36)Cl showed little evidence of retardation, while the transport of (14)C may have been retarded by its isotopic exchange with carbonate minerals in the aquifer. Observed local reducing conditions (either natural or test-induced) will impact the mobility of certain redox-sensitive radionuclides (especially (99)Tc) that were otherwise soluble and readily transported under oxidizing conditions. Conversely, strongly oxidizing conditions may impact the mobility of (129)I which is mobile under reducing conditions. The effect of iodine speciation on its transport deserves further attention. Indication of delayed transport of some "mobile" radionuclides (especially (99)Tc) in the groundwater at the NTS suggested the importance of redox conditions of the natural system in controlling the fate and transport of radionuclides, which has implications in the enhanced performance of the potential Yucca Mountain repository, located adjacent to the NTS, to store high-level nuclear wastes as well as management of radionuclide contamination in legacy nuclear operations facilities.     

The effective and environmental half-life of 137Cs at Coral Islands at the former US nuclear test site

The United States (US) conducted nuclear weapons testing from 1946 to 1958 at Bikini and Enewetak Atolls in the northern Marshall Islands. Based on previous detailed dose assessments for Bikini, Enewetak, Rongelap, and Utirik Atolls over a period of 28 years, cesium-137 (137Cs) at Bikini Atoll contributes about 85-89% of the total estimated dose through the terrestrial food chain as a result of uptake of 137Cs by food crops. The estimated integral 30, 50, and 70-year doses were based on the radiological decay of 137Cs (30-year half-life) and other radionuclides. However, there is a continuing inventory of 137Cs and 90Sr in the fresh water portion of the groundwater at all contaminated atolls even though the turnover rate of the fresh groundwater is about 5 years. This is evidence that a portion of the soluble fraction of 137Cs and 90Sr inventory in the soil is lost by transport to groundwater when rainfall is heavy enough to cause recharge of the lens, resulting in loss of 137Cs from the soil column and root zone of the plants. This loss is in addition to that caused by radioactive decay. The effective rate of loss was determined by two methods: (1) indirectly, from time-dependent studies of the 137Cs concentration in leaves of Pisonia grandis, Guettarda specosia, Tournefortia argentea (also called Messerschmidia), Scaevola taccada, and fruit from Pandanus and coconut trees (Cocos nucifera L.), and (2) more directly, by evaluating the 137Cs/90Sr ratios at Bikini Atoll. The mean (and its lower and upper 95% confidence limits) for effective half-life and for environmental-loss half-life (ELH) based on all the trees studied on Rongelap, Bikini, and Enewetak Atolls are 8.5 years (8.0 years, 9.8 years), and 12 years (11 years, 15 years), respectively. The ELH based on the 137Cs/90Sr ratios in soil in 1987 relative to the 137Cs/90Sr ratios at the time of deposition in 1954 is less than 17 years. The magnitude of the decrease below 17 years depends on the ELH for 90Sr that is currently unknown, but some loss of 90Sr does occur along with 137Cs. If the 15-year upper 95% confidence limit on ELH (corresponding to an effective half-life of 9.8 years) is incorporated into dose calculations projected over periods of 30, 50, or 70 years, then corresponding integral doses are 58, 46 and 41%, respectively, of those previously calculated based solely on radiological decay of 137Cs.     

Estimation of internal radiation dose to the adult Asian population from the dietary intakes of two long-lived radionuclides

Daily dietary intakes of two naturally occurring long-lived radionuclides, 232Th and 238U, were estimated for the adult population living in a number of Asian countries, using highly sensitive analytical methods such as instrumental and radiochemical neutron activation analysis (INAA and RNAA), and inductively coupled plasma mass spectrometry (ICP-MS). The Asian countries that participated in the study were Bangladesh (BGD), China (CPR), India (IND), Japan (JPN), Pakistan (PAK), Philippines (PHI), Republic of Korea (ROK) and Vietnam (VIE). Altogether, these countries represent more than 50% of the world population. The median daily intakes of 232Th ranged between 0.6 and 14.4 mBq, the lowest being for Philippines and the highest for Bangladesh, and daily intakes of 238U ranged between 6.7 and 62.5 mBq, lowest and the highest being for India and China, respectively. The Asian median intakes were obtained as 4.2 mBq for 232Th and 12.7 mBq for 238U. Although the Asian intakes were lower than intakes of 12.3 mBq (3.0 ug) 232Th and 23.6 mBq (1.9 ug) 238U proposed by the International Commission on Radiological Protection (ICRP) for the ICRP Reference Man, they were comparable to the global intake values of 4.6 mBq 232Th and 15.6 mBq 238U proposed by the United Nation Scientific Commission on Effects of Radiation (UNSCEAR). The annual committed effective doses to Asian population from the dietary intake of 232Th and 238U were calculated to be 0.34 and 0.20 microSv, respectively, which are three orders of magnitude lower than the global average annual radiation dose of 2400 microSv to man from the natural radiation sources as proposed by UNSCEAR.     

Assessing field-scale migration of radionuclides at the Nevada Test Site: “mobile” species

Many long-lived radionuclides are present in groundwater at the Nevada Test Site (NTS) as a result of 828 underground nuclear weapons tests conducted between 1951 and 1992. In conjunction with a comprehensive geochemical review of radionuclides (³H, ¹⁴C, ³⁶Cl, ⁹⁹Tc and ¹²⁹I) that are presumably mobile in the subsurface, we synthesized a body of radionuclide activity data measured from groundwater samples collected at 18 monitoring wells, to qualitatively assess their migration at the NTS over distances of hundreds of meters and over timescales of decades. Tritium and ³⁶Cl showed little evidence of retardation, while the transport of ¹⁴C may have been retarded by its isotopic exchange with carbonate minerals in the aquifer. Observed local reducing conditions (either natural or test-induced) will impact the mobility of certain redox-sensitive radionuclides (especially ⁹⁹Tc) that were otherwise soluble and readily transported under oxidizing conditions. Conversely, strongly oxidizing conditions may impact the mobility of ¹²⁹I which is mobile under reducing conditions. The effect of iodine speciation on its transport deserves further attention. Indication of delayed transport of some “mobile” radionuclides (especially ⁹⁹Tc) in the groundwater at the NTS suggested the importance of redox conditions of the natural system in controlling the fate and transport of radionuclides, which has implications in the enhanced performance of the potential Yucca Mountain repository, located adjacent to the NTS, to store high-level nuclear wastes as well as management of radionuclide contamination in legacy nuclear operations facilities.     

Genotoxicity and cytotoxicity assay of water sampled from the underground nuclear explosion site in the north of the Perm region (Russia)

The results of our study revealed a local biologically relevant surface water contamination in the radionuclide anomaly in the north of Russia (Perm region) by means of Allium schoenoprasum L. anaphase-telophase chromosome aberration assay. This radionuclide anomaly was formed in 1971 as a result of an underground nuclear explosion with soil excavation. Specific activities of main dose-forming radionuclides in all examined reservoirs are below intervention levels officially adopted in Russia for drinking water. We found that (90)Sr significantly contributes to induction of cytogenetic disturbances. Our previous data and the data described here suggest that metal and radionuclide combined exposure (with the dose below permissible exposure limits for human) may cause substantial biological effects. These effects are in part due to synergic response. The findings described here indicated that development of a new concept of radiation protection for humans and biota should be based on the clear understanding of biological effects of low doses of radiation in chronic exposure to multi-pollutant mixtures.     

Radiostrontium hot spot in the Russian Arctic: ground surface contamination by (90)Sr at the "Kraton-3" underground nuclear explosion site

Strontium-90 activity concentrations in surface soils and areal deposition densities have been studied at a site contaminated by an accidental release to atmosphere from the underground nuclear explosion "Kraton-3" conducted near the Polar Circle (65.9 degrees N, 112.3 degrees E) within the territory of the former USSR in 1978. In 2001-2002, the ground surface contamination at 14 plots studied ranged from 20 to 15 000 kBq m(-2), which significantly exceeds the value of 0.44 kBq m(-2) deduced for three background plots. The zone with substantial radiostrontium contamination extends, at least, 2.5 km in a north-easterly direction from the borehole. The average (137)Cs/(90)Sr ratio in the ground contamination originated from the "Kraton-3" fallout was estimated to be 0.55, which is significantly different from the ratio of 2.05 evaluated for background plots contaminated mostly from global fallout. Although vertical migration of (90)Sr in all undisturbed soil profiles studied is more rapid than that for (137)Cs, the depth of percolation of both radionuclides into the ground is mostly limited to the top 10-20 cm, which may be explained, primarily, by permafrost conditions. The horizontal migration rate of radiostrontium in the aqueous phase exceeds the radiocaesium migration rate by many times. This phenomenon seems to be a reason for the significant enrichment of the soil surface layers by radiostrontium at some sites, with variations occurring in accordance with small-scale irregularities of landscape.     

137Cs and 90Sr in live and dead reindeer lichens (genera Cladonia) from the "Kraton-3" underground nuclear explosion site

The contents of 137Cs and 90Sr have been determined in 29 samples of live and dead reindeer lichens (genera Cladonia) collected at the "Kraton-3" underground nuclear explosion site (65.9 degrees N 112.3 degrees E, event year--1978) in Yakutia, Russia in 2002. The area contamination was within the range of 0.36-700 and 0.13-770 kBq m(-2) for 137Cs and 90Sr, respectively. The dead organisms were on average much more contaminated than the live ones. Vertical fractionation of the live lichen carpet demonstrated maximal activity concentrations of both radionuclides in the lower older section of the plants, while for the dead lichens the maximal activity concentrations of 137Cs were detected in the upper part. The vertical distribution of 90Sr was more or less homogeneous in the cushions of dead lichens. Elevated levels of 137Cs and 90Sr activity concentrations were also detected in the re-establishing young lichens growing over the residua of some dead lichens.     

Tritium concentrations in the atmospheric environment at Rokkasho, Japan before the final testing of the spent nuclear fuel reprocessing plant

This study aimed at obtaining background tritium concentrations in precipitation and air at Rokkasho where the first commercial spent nuclear fuel reprocessing plant in Japan has been under construction. Tritium concentration in monthly precipitation during fiscal years 2001-2005 had a seasonal variation pattern which was high in spring and low in summer. The tritium concentration was higher than that observed at Chiba City as a whole. The seasonal peak concentration at Rokkasho was generally higher than that at Chiba City, while the baseline concentrations of both were similar. The reason for the difference may be the effect of air mass from the Asian continent which is considered to have high tritium concentration. Atmospheric tritium was operationally separated into HTO, HT and hydrocarbon (CH₃T) fractions, and the samples collected every 3 d-14 d during fiscal year 2005 were analyzed for these fractions. The HTO concentration as radioactivity in water correlated well with that in the precipitation samples. The HT concentration was the highest among the chemical forms analyzed, followed by the HTO and CH₃T concentrations. The HT and CH₃T concentrations did not have clear seasonal variation patterns. The HT concentration followed the decline previously reported by Mason and Östlund with an apparent half-life of 4.8 y. The apparent and environmental half-lives of CH₃T were estimated as 9.2 y and 36.5 y, respectively, by combining the present data with literature data. The Intergovernmental Panel on Climate Change used the atmospheric lifetime of 12 y for CH₄ to estimate global warming in its 2007 report. The longer environmental half-life of CH₃T suggested its supply from other sources than past nuclear weapon testing in the atmosphere.     

The geographic distribution of radionuclide deposition across the continental US from atmospheric nuclear testing

For the first time, calculations for the more than 3000 counties of the US have been completed that estimate the average deposition density (Bq m(-2)) of more than 40 radionuclides in fallout from atmospheric nuclear weapons tests conducted in the US (1951-1962) and 19 radionuclides from tests conducted elsewhere in the world (1952-1963). The geographic pattern of deposition across the US, as well as the amount of fallout deposited, varied significantly depending on whether the tests were conducted within or outside of the US. Fallout deposited from the Nevada Test Site (NTS) varied geographically as a result of dispersion and dilution in the atmosphere, the wind patterns following each test, and the occurrence of localized rainfall events. In general, states immediately east of the NTS received the highest deposition from tests conducted there. In contrast, the variation in deposition across the country from global fallout was less than for NTS fallout primarily reflecting variations in annual precipitation across larger regions. Hence, in the eastern and mid-western US, where rainfall is above the national average, higher levels of global fallout were deposited than in the more arid southwestern states. This paper presents a summary of the methods used and findings of our studies on fallout from NTS and global fallout, with emphasis on two of the most important radionuclides, (131)I and (137)Cs.     

Residual radioactive contamination at the peaceful underground nuclear explosion sites "Craton-3" and "Crystal" in the Republic of Sakha (Yakutia)

In this paper, results are reported on the concentrations and activity ratios of 137Cs, 239+240Pu and 238Pu in soils, lichen and bottom sediments collected at the peaceful underground nuclear explosion sites "Craton-3" and "Crystal" (Republic of Sakha (Yakutia), North-East Siberia). At the "Craton-3" site, 239- 240Pu concentrations in the range 6.2 mBq/g to 5.9 Bq/g in surface soils (0-5 cm) and 239+240Pu concentrations up to 7.4 Bq/g in lichen were observed. The 137Cs concentration in measured soils range from 0.52 to 216 Bq/g for the near-plume and from 1.65 to 21.5 Bq/g for the far-plume. In lichen, 137Cs concentration varied from a global background level up to 251 Bq/g. Radioactive contamination at "Crystal" demonstrates an extremely irregular distribution of 239,240Pu and 137Cs in environmental samples taken at locations within 150 m radius of the site. Further work on compiling detailed maps of radioactive contamination of the territory around "Craton-3" and "Crystal" is discussed.     

Surface ground contamination and soil vertical distribution of 137Cs around two underground nuclear explosion sites in the Asian Arctic, Russia

Vertical distributions of 137Cs have been determined in vegetation-soil cores obtained from 30 different locations around two underground nuclear explosion sites--"Crystal" (event year - 1974) and "Kraton-3" (event year - 1978) in the Republic of Sakha (Yakutia), Russia. In 2001-2002, background levels of 137Cs surface contamination densities on control forest plots varied from 0.73 to 0.97 kBq m(-2) with an average of 0.84+/-0.10 kBq m(-2) and a median of 0.82 kBq m(-2). 137Cs ground contamination densities at the "Crystal" site ranged from 1.3 to 64 kBq m(-2); the activity gradually decreased with distance from the borehole. For "Kraton-3", residual surface contamination density of radiocaesium varied drastically from 1.7 to 6900 kBq m(-2); maximal 137Cs depositions were found at a "decontaminated" plot. At all forest plots, radiocaesium activity decreased throughout the whole vertical soil profile. Vertical distributions of 137Cs in soil for the majority of the plots sampled (n=18) can be described using a simple exponential function. Despite the fact that more than 20 years have passed since the main fallout events, more than 80% of the total deposited activity was found in the first 5 cm of the vegetation-soil cores from most of the forested landscapes. The low annual temperatures, clay-rich soil type with neutral pH, and presence of thick lichen-moss carpet are the factors which may hinder 137Cs transport down the soil profile.     

Elevated concentrations of primordial radionuclides in sediments from the Reedy River and surrounding creeks in Simpsonville, South Carolina

A gamma-ray survey and analysis of 16 riverbed samples from the Reedy River watershed near Simpsonville, SC were conducted and compared with national and international studies of primordial radionuclides. The study reported here follows on a recent discovery of anomalously high uranium concentrations in several private well waters in the area. An HPGe spectrometer was used for quantification of gamma emitting radionuclides in the sediments. All sediments contained radionuclides from the uranium and thorium series as well as (40)K. Uranium-238 concentrations in sediment samples ranged from 11.1 to 74.2Bqkg(-1). The measured radionuclide concentrations were compared with data from UNSCEAR and NURE reports. The river and stream sediment data were augmented by in situ NaI(Tl) gamma-ray spectrometer measurements. Comparisons between the ex situ and in situ measurements indicate equivalently distributed uranium in the surface soils and stream sediments, the source of which is likely attributed to the monazite belts that are known to exist in the area.     

An analysis of the environmental mobility of radiostrontium from weapons testing and Chernobyl in Finnish river catchments

The mobility of radiostrontium within the Arctic environment and surrounding area has been studied by analysing the mobility of 90Sr in river catchments that are within Finland. The environmental mobility of 90Sr deposited by both nuclear weapons testing and the Chernobyl accident has been investigated in five Finnish river catchments. Different models assessing the time-dependent mobility of 90Sr have been evaluated. No significant differences were found between the mobility of 90Sr from nuclear weapons tests and from the Chernobyl accident. Model parameters obtained by fitting to the measurements of the deposition and runoff rates of the nuclear weapons test fallout gave predictions which were consistent with the mid- and long-term contamination by the Chernobyl fallout. A comparison of 90Sr with 137Cs showed that they had similar mobility on deposition but, as time passed, the relative mobility of 90Sr increased with respect to 137Cs over a period of 5-8 years. Once the relative migration of 90Sr with respect to 137Cs reached equilibrium, its runoff rate was, on average, approximately an order of magnitude greater than 137Cs.     

Radioisotope contaminations from releases of the Tomsk-Seversk nuclear facility (Siberia, Russia)

Soils have been sampled in the vicinity of the Tomsk-Seversk facility (Siberia, Russia) that allows us to measure radioactive contaminations due to atmospheric and aquatic releases. Indeed soils exhibit large inventories of man-made fission products including 137Cs (ranging from 33,000 to 68,500 Bq m(-2)) and actinides such as plutonium (i.e. 239+240Pu from 420 to 5900 Bq m(-2)) or 241Am (160-1220 Bq m(-2)). Among all sampling sites, the bank of the Romashka channel exhibits the highest radioisotope concentrations. At this site, some short half-life gamma emitters were detected as well indicating recent aquatic discharge in the channel. In comparison, soils that underwent atmospheric depositions like peat and forest soils exhibit lower activities of actinides and 137Cs. Soil activities are too high to be related solely to global fallout and thus the source of plutonium must be discharges from the Siberian Chemical Combine (SCC) plant. This is confirmed by plutonium isotopic ratios measured by ICP-MS; the low 241Pu/239Pu and 240Pu/239Pu atomic ratios with respect to global fallout ratio or civil nuclear fuel are consistent with weapons grade signatures. Up to now, the influence of Tomsk-Seversk plutonium discharges was speculated in the Ob River and its estuary. Isotopic data from the present study show that plutonium measured in SCC probably constitutes a significant source of plutonium in the aquatic environment, together with plutonium from global fallout and other contaminated sites including Tomsk, Mayak (Russia) and Semipalatinsk (Republic of Kazakhstan). It is estimated that the proportion of plutonium from SCC source can reach 45% for 239Pu and 60% for 241Pu in the sediments.