Krypton-85 datasets of the northern and southern hemisphere collected over the past 60 years.

With a half-life of 10.7 years, the noble gas radioisotope 85Kr is perfectly suited as a tracer to date ice and water that formed during the past half century. Furthermore, due to its inhomogeneous input into the atmosphere, it is a useful tool to investigate atmospheric circulation and back-trajectory analysis. The data presented here represent a comprehensive time series of atmospheric 85Kr activity concentrations in ground level air that can be used to model northern and southern hemispheric input functions, which is essential to apply 85Kr as a dating tracer. The collection comprises 11 datasets from 4 monitoring stations in the northern and 7 monitoring stations in the southern hemisphere, respectively. In total, it contains about 8000 measurements performed over the past 60 years, making it the largest published 85Kr record.

Half a century of Krypton-85 activity concentration measured in air over Central Europe: Trends and relevance for dating young groundwater.

For almost half a century weekly samples for the measurement of krypton-85 (85Kr) activity concentrations in surface air have been collected by the Bundesamt für Strahlenschutz (BfS), Germany. Sampling started at Freiburg (230m asl) in 1973, Mt Schauinsland (1205m asl) in 1976 and Mt Jungfraujoch in Switzerland (3454 asl) in 1990. Distinct maxima in the time series of atmospheric 85Kr activity concentration are caused by emissions from nuclear reprocessing plants in Europe, mainly the La Hague, France, and Sellafield, UK, reprocessing plants. Between 1970 and 1990 peak activity concentrations measured in winter along the Rhine Rift in Freiburg are often higher than at Mt Schauinsland, due to emissions from the operating pilot reprocessing plant in Karlsruhe - approximately 130 km to the north - and large-scale inversions that inhibit exchange of air masses within the Rhine Rift with those at higher altitudes. From the early 1990s onwards, after the shut-down of the pilot plant, differences between Freiburg and Schauinsland are much smaller. Activity concentrations measured at Jungfraujoch are generally lower and close to baseline levels, due to its location in the free troposphere. Weekly baseline and average 85Kr activity concentration in the atmosphere in Central Europe were modelled from almost 12,000 individual measurements at 11 stations. The baseline and average have continuously increased, interrupted by a relatively stable period between 2009 and the end of 2014 with a baseline activity concentration of about 1.39 Bq/m3. Depending on the geographical location and hydrological conditions, the modelled baseline or average 85Kr activity concentration time series can be used as input functions for the dating of young groundwater.

Simulating the mesoscale transport of krypton-85.

Due to its half-life, chemical inertness and low solubility in water, radioactive 85Kr is a valuable tracer for testing the performance of atmospheric dispersion models in simulating long-range transport of pollutants. This paper evaluates the capability of simulating the dispersion of radiokrypton emitted by a nuclear fuel reprocessing plant in north-west France. Three time periods during which elevated activity concentrations of 85Kr in ground level air were detected in south-west Germany are chosen. Simulations have been performed using the HYSPLIT code and the European Centre for Median-Range Weather Forecasts (ECMWF) data base. Although their results show a slight trend of underestimating the measured 85Kr concentrations, there is a significant correlation and moderate scatter between observations and simulations with about 50% of the results being within a factor of two of the measured concentrations. The simulated travel time distributions provided a valuable tool for providing additional insight into the dispersion of the tracer radionuclides and for identifying potential causes of deviations between measured and calculated concentrations.

Variation in airborne 134Cs, 137Cs, particulate 131I and 7Be maximum activities at high-altitude European locations after the arrival of Fukushima-labeled air masses.

The Fukushima-labeled air mass arrival, and later the cesium-134 (134Cs), cesium-137 (137Cs) and particulate iodine-131 (hereafter noted 131Ip) maximum levels were registered in Europe at different dates depending on the location. Most of those data were obtained at low-altitude sampling areas. Here, we compare the airborne levels registered at different high-altitude European locations (from 850 m to about 3500 m). The integrated 137Cs activity concentration was not uniform with regard to the altitude even after a long travel time/distance from Japan. Moreover, the relation of integrated 137Cs vs. altitude showed a linear decrease up to an altitude of about 3000 m. A similar trend was noticed for 131Ip (particulate fraction) while it increased above 3000 m. Comparison with 7Be activity concentration showed that, as far as the high altitude location is concerned, the 137Cs and 134Cs maximum concentrations corresponded to the 7Be maximum, suggesting downdraft movements from high tropospheric or stratospheric layers to be responsible for 137,134Cs increase and peak values. This was also confirmed by high potential vorticity and low relative humidity registered during the peak values.

International challenge to predict the impact of radioxenon releases from medical isotope production on a comprehensive nuclear test ban treaty sampling station.

The International Monitoring System (IMS) is part of the verification regime for the Comprehensive Nuclear-Test-Ban-Treaty Organization (CTBTO). At entry-into-force, half of the 80 radionuclide stations will be able to measure concentrations of several radioactive xenon isotopes produced in nuclear explosions, and then the full network may be populated with xenon monitoring afterward. An understanding of natural and man-made radionuclide backgrounds can be used in accordance with the provisions of the treaty (such as event screening criteria in Annex 2 to the Protocol of the Treaty) for the effective implementation of the verification regime. Fission-based production of (99)Mo for medical purposes also generates nuisance radioxenon isotopes that are usually vented to the atmosphere. One of the ways to account for the effect emissions from medical isotope production has on radionuclide samples from the IMS is to use stack monitoring data, if they are available, and atmospheric transport modeling. Recently, individuals from seven nations participated in a challenge exercise that used atmospheric transport modeling to predict the time-history of (133)Xe concentration measurements at the IMS radionuclide station in Germany using stack monitoring data from a medical isotope production facility in Belgium. Participants received only stack monitoring data and used the atmospheric transport model and meteorological data of their choice. Some of the models predicted the highest measured concentrations quite well. A model comparison rank and ensemble analysis suggests that combining multiple models may provide more accurate predicted concentrations than any single model. None of the submissions based only on the stack monitoring data predicted the small measured concentrations very well. Modeling of sources by other nuclear facilities with smaller releases than medical isotope production facilities may be important in understanding how to discriminate those releases from releases from a nuclear explosion.

Detection of (133)Xe from the Fukushima nuclear power plant in the upper troposphere above Germany.

After the accident in the Japanese Fukushima Dai-ichi nuclear power plant in March 2011 large amounts of radioactivity were released and distributed in the atmosphere. Among them were also radioactive noble gas isotopes which can be used as tracers to test global atmospheric circulation models. This work presents unique measurements of the radionuclide (133)Xe from Fukushima in the upper troposphere above Germany. The measurements involve air sampling in a research jet aircraft followed by chromatographic xenon extraction and ultra-low background gas counting with miniaturized proportional counters. With this technique a detection limit of the order of 100 (133)Xe atoms in liter-scale air samples (corresponding to about 100 mBq/m(3)) is achievable. Our results provide proof that the (133)Xe-rich ground level air layer from Fukushima was lifted up to the tropopause and distributed hemispherically. Moreover, comparisons with ground level air measurements indicate that the arrival of the radioactive plume at high altitude over Germany occurred several days before the ground level plume.

The influence on the radioxenon background during the temporary suspension of operations of three major medical isotope production facilities in the Northern Hemisphere and during the start-up of another facility in the Southern Hemisphere.

Medical isotope production facilities (MIPF) have recently been identified to emit the major part of the environmental radioxenon measured at many globally distributed monitoring sites deployed to strengthen the radionuclide component of the Comprehensive Nuclear-Test-Ban Treaty (CTBT) verification regime. Efforts to raise a global radioxenon emission inventory revealed that the yearly global total emission from MIPF's is around 15 times higher than the total radioxenon emission from nuclear power plants (NPP's). Given that situation, from mid 2008 until early 2009 two out of the ordinary hemisphere-specific events occured: 1) In the Northern hemisphere, a joint temporary suspension of operations of the three largest MIPF's made it possible to quantify the effects of the emissions related to NPP's. The average activity concentrations of (133)Xe measured at a monitoring station close to Freiburg, Germany, went down significantly from 4.5 +/- 0.5 mBq/m(3) to 1.1 +/- 0.1 mBq/m(3) and in Stockholm, Sweden, from 2.0 +/- 0.4 mBq/m(3) to 1.05 +/- 0.15 mBq/m(3). 2) In the Southern hemisphere the only radioxenon-emitting MIPF in Australia started up test production in late November 2008. During eight test runs, up to 6.2 +/- 0.2 mBq/m(3) of (133)Xe was measured at the station in Melbourne, 700 km south-west from the facility, where no radioxenon had been observed before, originating from the isotopic production process. This paper clearly confirms the hypothesis that medical isotope production facility are at present the major emitters of radioxenon to the atmosphere. Suspension of operations of these facilities indicates the scale of their normal contribution to the European radioxenon background, which decreased two to four fold. This also gives a unique opportunity to detect and investigate the influence of other local and long distance sources on the radioxenon background. Finally the opposing effect was studied: the contribution of the start-up of a renewed radiopharmaceutical facility to the build up of a radioxenon background across Australia and the Southern hemisphere.

Spatial and temporal variations of atmospheric 85Kr observed during 1995-2001 in Japan: estimation of atmospheric 85Kr inventory in the Northern Hemisphere.

Atmospheric 85Kr concentrations have been continuously monitored since 1995 at the Meteorological Research Institute (MRI) in Tsukuba, Japan. They have also been observed once a year at several stations over the Japanese islands since 1995. The annual growth rate of the background atmospheric 85Kr concentrations in Tsukuba was 0.03 Bq x m(-3) x yr(-1) during 1996-2001. The atmospheric 85Kr concentrations at several stations over Japan were within the range of the annual variations in Tsukuba. However, higher and lower 85Kr concentrations in early winter, compared with those in Tsukuba (36.1 degrees N, 140.1 degrees E), occurred in Sapporo (43.1 degrees N, 141.3 degrees E) and Ishigaki (24.3 degrees N, 124.2 degrees E), respectively. The reason for this is that Sapporo is covered by a continental air mass, some from European sources, whereas Ishigaki is still covered by a subtropical air mass. The Northern Hemispheric background 85Kr concentrations from 1994 to 2001 was calculated from the 85Kr inventory and the release rate of 85Kr from the nuclear fuel reprocessing plants in Europe. Calculated 85Kr concentrations in surface air were in good agreement with annual average observed values at the MRI, Tsukuba. The global atmospheric inventory of 85Kr in December 2001 was also estimated to be approximately 5 EBq by using observed data in Tsukuba.