ABSTRACT
In June 2020, observations of anthropogenic radionuclides in Estonia, Finland, and Sweden that were not related to any acknowledged environmental release led to a comprehensive investigation on the source and cause of the unusual emissions. Several of the observed radionuclides were on the list of Comprehensive Nuclear-Test-Ban Treaty (CTBT) relevant radionuclides as an indicator of a potential nuclear test, and warranted detailed investigation. While analysis of aerosol samples coupled with Atmospheric Transport and Dispersion Modelling (ATDM) is a standard approach for environmental particulate releases, several new techniques were employed to better characterize the samples that allowed for useful inferences to be made. These inferences were crucial in forming the ultimate hypothesis for determining the facility type and location of the release.
Subject(s)
Air Pollutants, Radioactive , Radiation Monitoring , Finland , Sweden , Radiation Monitoring/methods , Air Pollutants, Radioactive/analysis , Radioisotopes/analysis , EstoniaABSTRACT
In 2015 and 2016, atmospheric transport modeling challenges were conducted in the context of the Comprehensive Nuclear-Test-Ban Treaty (CTBT) verification, however, with a more limited scope with respect to emission inventories, simulation period and number of relevant samples (i.e., those above the Minimum Detectable Concentration (MDC)) involved. Therefore, a more comprehensive atmospheric transport modeling challenge was organized in 2019. Stack release data of Xe-133 were provided by the Institut National des Radioéléments/IRE (Belgium) and the Canadian Nuclear Laboratories/CNL (Canada) and accounted for in the simulations over a three (mandatory) or six (optional) months period. Best estimate emissions of additional facilities (radiopharmaceutical production and nuclear research facilities, commercial reactors or relevant research reactors) of the Northern Hemisphere were included as well. Model results were compared with observed atmospheric activity concentrations at four International Monitoring System (IMS) stations located in Europe and North America with overall considerable influence of IRE and/or CNL emissions for evaluation of the participants' runs. Participants were prompted to work with controlled and harmonized model set-ups to make runs more comparable, but also to increase diversity. It was found that using the stack emissions of IRE and CNL with daily resolution does not lead to better results than disaggregating annual emissions of these two facilities taken from the literature if an overall score for all stations covering all valid observed samples is considered. A moderate benefit of roughly 10% is visible in statistical scores for samples influenced by IRE and/or CNL to at least 50% and there can be considerable benefit for individual samples. Effects of transport errors, not properly characterized remaining emitters and long IMS sampling times (12-24 h) undoubtedly are in contrast to and reduce the benefit of high-quality IRE and CNL stack data. Complementary best estimates for remaining emitters push the scores up by 18% compared to just considering IRE and CNL emissions alone. Despite the efforts undertaken the full multi-model ensemble built is highly redundant. An ensemble based on a few arbitrary runs is sufficient to model the Xe-133 background at the stations investigated. The effective ensemble size is below five. An optimized ensemble at each station has on average slightly higher skill compared to the full ensemble. However, the improvement (maximum of 20% and minimum of 3% in RMSE) in skill is likely being too small for being exploited for an independent period.
Subject(s)
Air Pollutants, Radioactive , Radiation Monitoring , Humans , Xenon Radioisotopes/analysis , Air Pollutants, Radioactive/analysis , Radiation Monitoring/methods , Canada , International CooperationABSTRACT
Over 40 soil gas samples were collected both in post-industrial areas as well as in undisturbed areas in the region of Kvarntorp, Sweden. Radioxenon (133Xe) was detected in 15 samples and radioargon was detected in 7 from 10 samples analysed. The concentration of radioxenon and radioargon in soil gas ranged up to 109 mBq/m3 and 19 mBq/m3, respectively. During sample collection other soil gases such as radon, CO2 and O2 were also measured and soil samples were taken along with dose rate measurements. The field experiment presented here shows that it is possible to detect naturally occurring radioxenon and radioargon in soil gas simultaneously.
Subject(s)
Air Pollutants, Radioactive/analysis , Radiation Monitoring , Radon/analysis , Soil Pollutants, Radioactive/analysis , Xenon Radioisotopes/analysis , Gases/analysis , Soil , SwedenABSTRACT
A new method for calculation of isotope-specific activities and activity concentrations in measurement systems for atmospheric radioxenon is presented. The method results in simple matrix-vector equations, and requires the definition of fewer spectral regions-of-interest than previous algorithms. The most important difference compared to the current method is however the calculation of decision limits, which results in false detection rates closer to the selected confidence level of 95% compared to the methods used today. This is achieved by introducing a Bayesian correction of the background estimate. The results have implications for the understanding of the atmospheric radioxenon background, for example for the observed low levels of 133mXe, an important isotope in the area of nuclear explosion detection.
ABSTRACT
Motivated by the need for consistent use of concepts central to the reporting of results from measurements of atmospheric radioactivity, we discuss some properties of the methods commonly used. Different expressions for decay correction of the activity concentration for parent-daughter decay pairs are presented, and it is suggested that this correction should be performed assuming parent-daughter ingrowth in the sample during the entire measurement process. We note that, as has already been suggested by others, activities rather than activity concentrations should be used when nuclide ratios are calculated. In addition, expressions that can be used to transform activity concentrations to activity ratios are presented. Finally we note that statistical uncertainties for nuclide ratios can be properly calculated using the exact solution to the problem of confidence intervals for a ratio of two jointly normally distributed variables, the so-called Fieller׳s theorem.
Subject(s)
Air Pollutants, Radioactive/analysis , Air Pollutants, Radioactive/chemistry , Algorithms , Artifacts , Models, Chemical , Radiation Monitoring/methods , Radioisotopes/analysis , Radioisotopes/chemistry , Computer Simulation , Half-Life , Reproducibility of Results , Sensitivity and SpecificityABSTRACT
Observations made in April 2013 of the radioxenon isotopes (133)Xe and (131m)Xe at measurement stations in Japan and Russia, belonging to the International Monitoring System for verification of the Comprehensive Nuclear-Test-Ban Treaty, are unique with respect to the measurement history of these stations. Comparison of measured data with calculated isotopic ratios as well as analysis using atmospheric transport modeling indicate that it is likely that the xenon measured was created in the underground nuclear test conducted by North Korea on February 12, 2013, and released 7-8 weeks later. More than one release is required to explain all observations. The (131m)Xe source terms for each release were calculated to 0.7 TBq, corresponding to about 1-10% of the total xenon inventory for a 10 kt explosion, depending on fractionation and release scenario. The observed ratios could not be used to obtain any information regarding the fissile material that was used in the test.
Subject(s)
Nuclear Weapons , Xenon/analysis , Democratic People's Republic of Korea , Japan , Radiation Monitoring , Russia , Xenon Radioisotopes/analysisABSTRACT
Detailed deterministic calculations of electron-photon coincidence spectra for (131m)Xe and (133m)Xe, including Auger electrons and X-rays from atomic relaxation, have been performed in order to increase the understanding of observed features in spectra produced by radioxenon measurement systems used in nuclear explosion monitoring. Energies and intensities of Auger electrons and X-rays agree well with earlier calculations, and the predicted intensities and energies for (131m)Xe show good agreement with observed features in electron spectra. The results can be used in the development of radioxenon calibration and concentration analysis techniques.
ABSTRACT
Radioactive xenon monitoring is one of the main technologies used for the detection of underground nuclear explosions. Precise and reliable measurements of (131m)Xe, (133g)Xe, (133m)Xe, and (135g)Xe are required as part of the International Monitoring System for compliance with the Comprehensive Nuclear-Test-Ban Treaty (CTBT). For the first time, simultaneous testing of four highly sensitive and automated fieldable radioxenon measurement systems has been performed and compared to established laboratory techniques. In addition to an intercomparison of radioxenon monitoring equipment of different design, this paper also presents a set of more than 2000 measurements of activity concentrations of radioactive xenon made in the city of Freiburg, Germany in 2000. The intercomparison experiment showed, that the results from the newly developed systems agree with each other and the equipment fulfills the fundamental requirements for their use in the verification regime of the CTBT. For 24-h measurements, concentrations as low as 0.1 mBqm(-3) were measured for atmospheric samples ranging in size from 10 to 80 m(3). The (133)Xe activity concentrations detected in the ambient air ranged from below 1 mBqm(-3) to above 100 mBqm(-3).