A performance estimate for the detection of undeclared nuclear-fuel reprocessing by atmospheric 85Kr

To test the sensitivity of using atmospheric (85)Kr to detect undeclared separation of plutonium from irradiated nuclear-reactor fuel, measurements of atmospheric (85)Kr taken in Tsukuba, Japan are analyzed to determine: (1) a lower limit of detection for discovering anthropogenic (85)Kr emissions, (2) the probability of detecting plutonium separation at the Tokai Reprocessing Plant, and (3) the extent to which these results can be generalized to other sites. A LLD of at least 3.4 sigma=0.14 Bq/m(3) with a theoretical false-positive rate of 0.05% is recommended for safeguards' purposes. At this threshold, the continuous separation of 100, 300, and 900 g equivalent weapon-grade plutonium per day was found to correspond to 10%, 50%, and 80% probability of detection, respectively. The smallest detected concentration was for the continuous separation of 45 g/day, with a probability of detection of about 0.6%. It was found that the detection rate is determined predominantly by the weather.     

Krypton-85 in the atmosphere 1950–1977: a data review

For over 20 years the radioactive noble gas ⁸⁵Kr, the product of nuclear industry, has been released to the environment mainly from nuclear fuel reprocessing plants. Owing to its relatively long half-life $\text{T(}\text{1}\text{2}\text{= 10.76}\text{y}\text{)}$ and the absence of other appreciable sinks, a cumulative buildup of ⁸⁵Kr in the atmosphere is observed. The mean ⁸⁵Kr surface air activity in the northern hemisphere has increased from about 20 dpm/mmol Kr in 1950 to about 750 dpm/mmol Kr in 1977. In recent years, a substantial slow-down of the ⁸⁵Kr emission rate to the atmosphere has been observed. The published data indicate rather good mixing of ⁸⁵Kr in the northern hemisphere, but a gradient is observed in the southern hemisphere due to the fact that all nuclear fuel reprocessing plants are situated in the northern hemisphere and due to poor mixing of the atmosphere in the meridional direction.This paper summarizes nearly all of the data on ⁸⁵Kr activity in the atmosphere published up to the middle of 1978. The spatio-temporal distribution of ⁸⁵Kr atmospheric activity is discussed. Some forecasts of future ⁸⁵Kr concentration in the atmosphere and its possible ecological consequences are also presented.     

In situ metrology of 85Kr plumes released by the COGEMA La Hague nuclear reprocessing plant

The IRSN (Institut de Radioprotection et de S?reté Nucléaire, France) has started an in situ study of the behaviour of atmospheric releases close-by the COGEMA La Hague nuclear reprocessing plant. The study is designed to improve information on the dispersion of radioactive pollutants very close to the emission point--a 100 m height chimney. In this situation, close to the emission and height of the emission, Gaussian models generally used to predict the behaviour of atmospheric releases are not well adapted. The study is based on the characterisation of the 85Kr emitted during normal operations of the reprocessing process. Temporal and spatial variations of the plume shape were investigated with intensive in situ measurements. Live in situ techniques to measure the electrons and the photons emitted by the 85Kr have been implemented and will be described. Preliminary results showing the interest of the techniques were presented. Variations of the dose rates created by the photon flux of a plume were directly measured and correlated to other quantities.     

The Bulgarian Emergency Response System for dose assessment in the early stage of accidental releases to the atmosphere

The Bulgarian Emergency Response System (BERS) is being developed in the Bulgarian National Institute of Meteorology and Hydrology since 1994. BERS is based on numerical weather forecast meteorological information and a numerical long-range dispersion model accounting for the transport, dispersion, chemical and radioactive transformations of pollutants. In the present paper, the further development of this system for a mixture of radioactive gaseous and aerosol pollutants is described. The basic module for the BERS, the numerical dispersion model EMAP, is upgraded with a “dose calculation block”. Two scenarios for hypothetical accidental atmospheric releases from two NPPs, one in Western, and the other in Eastern Europe, are numerically simulated. The effective doses from external irradiation, from air submersion and ground shinning, effective dose from inhalation and absorbed dose by thyroid gland formed by 37 different radionuclides, significant for the early stage of a nuclear accident, are calculated as dose fields for both case studies and discussed.     

The simulation of long-range transport of ¹³⁷Cs from East Asia to Japan in 2002 and 2006

To evaluate the quantities of ¹³⁷Cs from past nuclear tests being transported to and deposited in Japan by naturally-occurring phenomena, the authors developed long-range transport models for ¹³⁷Cs considering Asian dust. The simulation using these models backed the observed recent increase of ¹³⁷Cs deposition along the coast of the Sea of Japan in early spring. For the sake of public safety, it is vital to ascertain whether an increase of radioactive deposition is caused by natural phenomena or a nuclear accident. The observations in recent years have suggested that dust and soil containing ¹³⁷Cs is transported from the regions around Inner Mongolia to Japan by the wind. In this paper, using observation data from the early spring of 2002 and 2006, the authors have found good agreement between the simulations and the measurements. The simulations reproduced the entrainment of ¹³⁷Cs and subsequent transport to Japan caused by strong winds associated with low pressure areas around the Inner Mongolian grasslands. The most likely cause of high-level ¹³⁷Cs deposition over northern Japan during March 2002 was ¹³⁷Cs associated with particles transported at low-altitude (1 km) and subjected to precipitation on the 22nd to 24th.     

Mesoscale modelling of radioactive contamination formation in Ukraine caused by the Chernobyl accident

This work is devoted to the reconstruction of time-dependent radioactive contamination fields in the territory of Ukraine in the initial period of the Chernobyl accident using the model of atmospheric transport LEDI (Lagrangian-Eulerian DIffusion model). The modelling results were compared with available 137Cs air and ground contamination measurement data. The 137Cs atmospheric transport over the territory of Ukraine was simulated during the first 12 days after the accident (from 26 April to 7 May 1986) using real aerological information and rain measurement network data. The detailed scenario of the release from the accidental unit of the Chernobyl nuclear plant has been built (including time-dependent radioactivity release intensity and time-varied height of the release). The calculations have enabled to explain the main features of spatial and temporal variations of radioactive contamination fields over the territory of Ukraine on the regional scale, including the formation of the major large-scale spots of radioactive contamination caused by dry and wet deposition.     

A new compilation of the atmospheric 85krypton inventories from 1945 to 2000 and its evaluation in a global transport model

This paper gives the yearly (85)Kr emissions of all known reprocessing facilities, which are the main sources of (85)Kr in the atmosphere since 1945, for the years 1945 until 2000. According to this inventory 10,600 PBq (Peta=10(15)) of (85)Kr have been globally emitted from the year 1945 until the end of 2000. The global atmospheric inventory at the end of the year 2000 amounts to 4800 PBq. These emissions have been incorporated into the ECHAM4 atmospheric general circulation model as point sources. Monthly mean model results are compared with measurements made at different locations and times. The influence of each source on the measured concentrations at various locations is studied. The calculated concentrations are found to give reasonably good agreement with the observations, indicating that the emission inventory is realistic. Although, at all northern hemispheric observation sites the model tends to slightly overestimate the concentrations. A possible reason for this overestimation can be found in model features (coarse resolution in time and space). The most prominent discrepancy that is consistently repeated at all northern hemispheric stations occurs in the early 1990s. This could most likely be related to an overestimate of sources. Possibly, the Russian emissions declined earlier than assumed in the current database. Another discrepancy between observations and simulations indicating an incompleteness of the release data is found at some southern hemispheric sites. The variability of their observations could only be explained by regional sources. However, several spikes occur after 1992 when no reprocessing facility is known to be in operation in the southern hemisphere. Production of isotopes for radiopharmaceuticals like technetium-99m from highly enriched uranium is the most likely explanation.     

A study of the atmospheric dispersion of a high release of krypton-85 above a complex coastal terrain, comparison with the predictions of Gaussian models (Briggs, Doury, ADMS4)

Atmospheric releases of krypton-85, from the nuclear fuel reprocessing plant at the AREVA NC facility at La Hague (France), were used to test Gaussian models of dispersion. In 2001-2002, the French Institute for Radiological Protection and Nuclear Safety (IRSN) studied the atmospheric dispersion of 15 releases, using krypton-85 as a tracer for plumes emitted from two 100-m-high stacks. Krypton-85 is a chemically inert radionuclide. Krypton-85 air concentration measurements were performed on the ground in the downwind direction, at distances between 0.36 and 3.3 km from the release, by neutral or slightly unstable atmospheric conditions. The standard deviation for the horizontal dispersion of the plume and the Atmospheric Transfer Coefficient (ATC) were determined from these measurements. The experimental results were compared with calculations using first generation (Doury, Briggs) and second generation (ADMS 4.0) Gaussian models. The ADMS 4.0 model was used in two configurations; one takes account of the effect of the built-up area, and the other the effect of the roughness of the surface on the plume dispersion. Only the Briggs model correctly reproduced the measured values for the width of the plume, whereas the ADMS 4.0 model overestimated it and the Doury model underestimated it. The agreement of the models with measured values of the ATC varied according to distance from the release point. For distances less than 2 km from the release point, the ADMS 4.0 model achieved the best agreement between model and measurement; beyond this distance, the best agreement was achieved by the Briggs and Doury models.     

Artificial radionuclides in the atmosphere over Lithuania

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

Global Radioactive Contamination Background in Terrestrial Ecosystems 13 Years after the Chernobyl Accident

The contents of ¹³⁷Cs in the soil, plant, and animal samples collected in the ecosystems of protected areas from the White Sea to the Black Sea in 1999 slightly differ from those in the period between 1980 and 1984. As a result of global fallout after the Chernobyl accident, the content of radioactive cesium in the soil has increased only on the territory of the Biological Station of Moscow State University at the White Sea, whereas that in the litter and plants has increased in virtually all areas studied. The isotope content in animals is actually equal to that recorded between 1980 and 1984. The mobility of ¹³⁷Cs in the soil–plant link has increased, which may be due to fallout after the accident. The duration of a complete radionuclide cycle in ecosystems decreases from 10 half-life periods in northern regions to 2.5 half-life periods in the southern regions. The Chernobyl disaster has caused no significant changes in the global radioactive background in the European part of the Russian Federation.     

Reconstruction of (131)I radioactive contamination in Ukraine caused by the Chernobyl accident using atmospheric transport modelling

The evaluation of (131)I air and ground contamination field formation in the territory of Ukraine was made using the model of atmospheric transport LEDI (Lagrangian-Eulerian DIffusion model). The (131)I atmospheric transport over the territory of Ukraine was simulated during the first 12 days after the accident (from 26 April to 7 May 1986) using real aerological information and rain measurement network data. The airborne (131)I concentration and ground deposition fields were calculated as the database for subsequent thyroid dose reconstruction for inhabitants of radioactive contaminated regions. The small-scale deposition field variability is assessed using data of (137)Cs detailed measurements in the territory of Ukraine. The obtained results are compared with available data of radioiodine daily deposition measurements made at the network of meteorological stations in Ukraine and data of the assessments of (131)I soil contamination obtained from the (129)I measurements.     

Calculation of the depletion of airborne pollutant plumes through dry deposition processes

The depletion of airborne pollutant plumes resulting from dry deposition on ground surfaces should be taken into account when estimating pollutant concentrations in air at distances downwind from their sources. This can be done by using a reduced release rate instead of the actual release rate for the pollutant in atmospheric dispersion equations. The reduced release rate is the actual rate of release multiplied by a depletion fraction. Depletion fractions for use with the Gaussian atmospheric dispersion equation of Pasquill and Gifford were calculated by numerical integration for downwind distances ranging from 35 to 90 000 m for release heights from 1 to 400 m, and they are tabulated for convenient interpolation for intermediate values of distance and release height. Pasquill atmospheric stability categories A-G are included. The listed values are for a deposition velocity of 0.01 m/s and a wind speed of 1 m/s but can be easily converted to apply to other deposition velocities and wind speeds. The tabulated values may be applied for downwind distances close enough to the point of release that the Gaussian model may be assumed to be realistic and where the vertical dispersion of the plume has not yet been significantly affected by the overlying atmospheric lid.     

A model for radiological consequences of nuclear power plant operational atmospheric releases

A dynamic dose and risk assessment model is developed to estimate radiological consequences of atmospheric emissions from nuclear power plants. Internal exposure via inhalation and ingestion, external exposure from clouds and radioactivity deposited on the ground are included in the model. The model allows to simulate interregional moves of people and multi-location food supply in the computational domain. Any long-range atmospheric dispersion model which yields radionuclide concentrations in air and on the ground at predetermined time intervals can easily be integrated into the model. The software developed is validated against radionuclide concentrations measured in different environmental media and dose values estimated after the Chernobyl accident. Results obtained using the model compare well with dose estimates and activities measured in foodstuffs and feedstuffs.     

Apparent 85Kr ages of groundwater within the Royal watershed, Maine, USA

Specific 85Kr activity is mapped from 264 domestic and municipal wells sampled during 2002-2004 in the Royal watershed (361 km2), Maine. Gas samples are collected at 20 m, 40 m, and > 50 m interval depths within the unconfined aquifers. Gas extraction for 85Kr from wells is obtained directly via a wellhead methodology avoiding conventional collection of large sample volumes. Atmospheric 85Kr input to the recharge environment is estimated at 1.27 Bq m(-3) by time-series analyses of weighted monthly precipitation (2001-2004). Numerical simulation of Kr gas transport through the variable unsaturated zones to the water table suggests up to 12-year time lags locally, thus biasing the 85Kr groundwater ages. Apparent 85Kr ages suggest that approximately 70% of groundwater near 20 m depth was recharged less than 30 years BP (2004). Mass-age transport modeling suggests that post mid-1950s recharge penetrates to part of the basin's floor and that older groundwater seeps from the underlying fractured bedrock may occur.     

Analysis of Factors Determining Accumulation of 137Cs by Woody Plants

The accumulation of ¹³⁷Cs by coniferous (Pinus sylvestris) and deciduous (Betula pendula) trees was studied in the area contaminated with radioactive products after the Chernobyl accident. The availability of ¹³⁷Cs to woody plants is determined by its vertical distribution in the soil profile, the proportion of its exchangeable form, and the distribution of tree roots in the soil. The index of biological availability of ¹³⁷C in the soil is proposed, and its linear dependence on the coefficients of ¹³⁷Cs transfer to wood is demonstrated.     

Global and local cancer risks after the Fukushima Nuclear Power Plant accident as seen from Chernobyl: A modeling study for radiocaesium (134Cs & 137Cs)

The accident at the Fukushima Daiichi Nuclear Power Plant (NPP) in Japan resulted in the release of a large number of fission products that were transported worldwide. We study the effects of two of the most dangerous radionuclides emitted, ¹³⁷Cs (half-life: 30.2 years) and ¹³⁴Cs (half-life: 2.06 years), which were transported across the world constituting the global fallout (together with iodine isotopes and noble gasses) after nuclear releases. The main purpose is to provide preliminary cancer risk estimates after the Fukushima NPP accident, in terms of excess lifetime incident and death risks, prior to epidemiology, and compare them with those occurred after the Chernobyl accident. Moreover, cancer risks are presented for the local population in the form of high-resolution risk maps for 3 population classes and for both sexes. The atmospheric transport model LMDZORINCA was used to simulate the global dispersion of radiocaesium after the accident. Air and ground activity concentrations have been incorporated with monitoring data as input to the LNT-model (Linear Non-Threshold) frequently used in risk assessments of all solid cancers. Cancer risks were estimated to be small for the global population in regions outside Japan. Women are more sensitive to radiation than men, although the largest risks were recorded for infants; the risk is not depended on the sex at the age-at-exposure. Radiation risks from Fukushima were more enhanced near the plant, while the evacuation measures were crucial for its reduction. According to our estimations, 730–1700 excess cancer incidents are expected of which around 65% may be fatal, which are very close to what has been already published (see references therein). Finally, we applied the same calculations using the DDREF (Dose and Dose Rate Effectiveness Factor), which is recommended by the ICRP, UNSCEAR and EPA as an alternative reduction factor instead of using a threshold value (which is still unknown). Excess lifetime cancer incidents were estimated to be between 360 and 850, whereas 220–520 of them will be fatal. Nevertheless, these numbers are expected to be even smaller, as the response of the Japanese official authorities to the accident was rapid. The projected cancer incidents are much lower than the casualties occurred from the earthquake itself (> 20,000) and also smaller than the accident of Chernobyl.     

重庆市主城区空气污染天气特征研究

利用2003～2008年重庆市主城区大气污染监测资料,分析了轻度污染以上天气的变化特征。结果表明重庆主城区的主要污染物为PM10,PM10浓度具有独特的“双峰双谷”日变化特征;污染天气具有明显的季节特征,主要污染期为秋末到初春;污染天气具有连续性特征,污染天气持续时间尺度主要集中在2～7 d;污染天气过程具有典型的大气环流和天气特征,本地地面天气类型主要以低压或均压场为主,中高纬度高空以纬向环流或西北气流为主,天气以阴天或阴晴相间为主;污染天气过程中本地气象要素变化呈现规律性,地面24 h气压变化总趋势为负变压,24 h变温为正变温,平均相对湿度维持在72%～85%,风速的变化趋势不大,基本维持在1～2 m/s,低层逆温明显。污染天气过程结束时气压明显回升,温度显著下降,相对湿度显著增加。     

Sources and pathways of Sr in the North Atlantic–Arctic region: present day and global warming

The spatial and temporal distributions of the anthropogenic radionuclides ¹³⁷Cs and ⁹⁰Sr, originating from nuclear bomb testing, the Sellafield reprocessing plant in the Irish Sea (UK), and from the Ob and Yenisey river discharges to the Arctic Ocean, have been simulated using the global version of the Miami Isopycnic Coordinate Ocean Model (MICOM). The physical model is forced with daily atmospheric re-analysis fields for the period of 1948–1999. Comparison of the temporal evolution of the observed and the simulated concentrations of ⁹⁰Sr has been performed in the Kara Sea. The relative contributions of the different sources on the temporal and spatial distributions of the surface ⁹⁰Sr are quantified over the simulated period. It follows that the Ob river discharge dominated the surface ⁹⁰Sr over most of the Arctic Ocean and along the eastern and western coasts of Greenland before 1960. During the period of 1980–1990, the atmospheric fallout and the Ob river discharge were equally important for the ⁹⁰Sr distribution in the Arctic Ocean. Furthermore, an attempt has been made to explore the possible dispersion of accidental released ⁹⁰Sr from the Ob and Yenisey rivers under a global warming scenario (2 × CO₂). The difference between the present-day and the global warming scenario runs indicates that more of the released ⁹⁰Sr from the Ob and Yenisey rivers is confined to the Arctic Ocean in the global warming run, particularly in the near coastal, non-European part of the Arctic Ocean.     

Atmospheric xenon radioactive isotope monitoring

The Comprehensive Nuclear Test Ban Treaty (CTBT) organisation is implementing a world-wide monitoring network in order to check that the State Signatories comply with the treaty. One of the monitoring facilities consists of an atmospheric noble gas monitoring equipment. According to the requirements annexed in the treaty, the French Atomic Energy Commission (CEA) developed a device, called SPALAX, which automatically extracts xenon from ambient air and makes in situ measurements of the activities of four xenon radioisotopes (131mXe, 133mXe, 133Xe, 135Xe). The originality of this device is noticeable essentially in the gas sample processing method: thanks to the coupling of a gas permeator and of a noble gas specific adsorbent, it can selectively extract and concentrate xenon to more than 3 x 10 E6. This process is carried out continuously without cryogenic cooling, without any regeneration time. The detection of the xenon radioactive isotopes is done automatically by high spectral resolution gamma spectrometry, a robust technology well-suited for on-field instrumentation. In the year 2000, a prototype was involved in an international evaluation exercise directed by the CTBT organisation (CTBTO). This exercise demonstrated that the SPALAX equipment perfectly met the requirements of the CTBTO for such systems. On the basis of the continuous 24-h resolution record of the atmospheric xenon radioactive isotopes concentrations, the SPALAX system also demonstrated that ambient levels of 133Xe can fluctuate quickly from less than the detection limit to over 40 x 10(-3) Bq m(-3). In order to build an industrial version of this equipment, the CEA entered into a partnership with a French engineering company (S.F.I., Marseille, France), which is now able to produce an industrial version of SPALAX, i.e. more compact and more efficient than the prototypes. The 133Xe minimum detectable concentration is 0.15 x 10(-3) Bq m(-3) air per 24 h sampling cycle.