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International audience; Atmospheric transport modeling has been used to interpret the unprecedented number of multi-isotope detections of radioxenons observed during the six months of the qualification process by the Comprehensive Nuclear-Test-Ban Treaty Organization of the new SPALAX-NG system (Système de Prélèvement Automatique en Ligne avec l’Analyse du Xénon - Nouvelle Génération). Highest $^{133}$Xe activity concentrations were found to be systematically associated with the concomitant measurement of several other radioxenons at the prevailing wind direction of north/northeast pointing to the Institute for Radio Elements (IRE), a medical isotope production facility located in Fleurus (Belgium). The lowest $^{133}$Xe activity concentrations were not associated with a prevailing wind direction or other radioxenons, indicating the contribution of distant sources (global background). The IRE's average source terms for $^{133}$mXe and to a lesser extent for $^{133}$Xe (slightly overestimated by a factor of 1.7) showed good agreement with the literature values, while corrections by a factor of ~23 and ~53 were proposed for $^{131}$mXe and $^{135}$Xe since the initial values were underestimated. However, detections of $^{131}$mXe alone and some low-activity concentrations of $^{133}$Xe associated with only one of the other radioxenons could not be linked to the IRE releases. Analysis of these cases suggests the contribution of local source releases that have been difficult to identify to date. In addition to the global background, releases from such local sources, if not identified, could affect the analysis of the isotopic ratios measured following a nuclear test. The characterization of these local contributions is now possible owing to the capacity of the SPALAX-NG and other new generation measurements systems.

International audience; The SPALAX-NG is a new-generation system that is designed to detect radioactive xenon at trace levels in the atmosphere following a nuclear explosion or civilian source release. This new system formed part of a validation program led by the Provisional Technical Secretary of the Comprehensive Nuclear-Test-Ban Treaty (CTBT) Organization. In this study, the first SPALAX-NG unit was tested for six months between October 2018 and April 2019 at the CEA/DIF premises near Paris, France. This test period provided an outstanding opportunity to illustrate the high level of detectability and reliability of the system. The data availability obtained over this period was approximately 99%, which was well above the CTBT Data Availability criteria of 95%. The data reliability was demonstrated by a comparison with a collocated SPALAX-1 unit (former version of SPALAX) and by re-measuring several samples at the CTBT-certified French laboratory FRL08. The high sensitivity to the detection of the four relevant radioxenon isotopes was fully demonstrated and enabled the recording of a major dataset for western Europe. A large set of isotopic ratios was measured, which enabled the discrimination criteria between civilian sources and nuclear test signatures to be refined.

Monitoring atmospheric concentrations of radioxenons is relevant to provide evidence of atmospheric or underground nuclear weapon tests. However, when the design of the International Monitoring Network (IMS) of the Comprehensive Nuclear-Test-Ban Treaty (CTBT) was set up, the impact of industrial releases was not perceived. It is now well known that industrial radioxenon signature can interfere with that of nuclear tests. Therefore, there is a crucial need to characterize atmospheric distributions of radioxenons from industrial sources—the so-called atmospheric background—in the frame of the CTBT. Two years of Xe-133 atmospheric background have been simulated using 2013 and 2014 meteorological data together with the most comprehensive emission inventory of radiopharmaceutical facilities and nuclear power plants to date. Annual average simulated activity concentrations vary from 0.01 mBq/m3 up to above 5 mBq/m3 nearby major sources. Average measured and simulated concentrations agree on most of the IMS stations, which indicates that the main sources during the time frame are properly captured. Xe-133 atmospheric background simulated at IMS stations turn out to be a complex combination of sources. Stations most impacted are in Europe and North America and can potentially detect Xe-133 every day. Predicted occurrences of detections of atmospheric Xe-133 show seasonal variations, more accentuated in the Northern Hemisphere, where the maximum occurs in winter. To our knowledge, this study presents the first global maps of Xe-133 atmospheric background from industrial sources based on two years of simulation and is a first attempt to analyze its composition in terms of origin at IMS stations.

International audience; After performing a first multi-model exercise in 2015 a comprehensive and technically more demanding atmospheric transport modelling challenge was organized in 2016. Release data were provided by the Australian Nuclear Science and Technology Organization radiopharmaceutical facility in Sydney (Australia) for a one month period. Measured samples for the same time frame were gathered from six International Monitoring System stations in the Southern Hemisphere with distances to the source ranging between 680 (Melbourne) and about 17,000 km (Tristan da Cunha). Participants were prompted to work with unit emissions in pre-defined emission intervals (daily, half-daily, 3-hourly and hourly emission segment lengths) and in order to perform a blind test actual emission values were not provided to them. Despite the quite different settings of the two atmospheric transport modelling challenges there is common evidence that for long-range atmospheric transport using temporally highly resolved emissions and highly space-resolved meteorological input fields has no significant advantage compared to using lower resolved ones. As well an uncertainty of up to 20% in the daily stack emission data turns out to be acceptable for the purpose of a study like this. Model performance at individual stations is quite diverse depending largely on successfully capturing boundary layer processes. No single model-meteorology combination performs best for all stations. Moreover, the stations statistics do not depend on the distance between the source and the individual stations. Finally, it became more evident how future exercises need to be designed. Set-up parameters like the meteorological driver or the output grid resolution should be pre-scribed in order to enhance diversity as well as comparability among model runs.

International audience; 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 99Mo 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 133Xe 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. © 2016.

The present part of the publication (Part II) deals with long range dispersion of radionuclides emitted into the atmosphere during the Fukushima Dai-ichi accident that occurred after the March 11, 2011 tsunami. The first part (Part I) is dedicated to the accident features relying on radionuclide detections performed by monitoring stations of the Comprehensive Nuclear Test Ban Treaty Organization network. In this study, the emissions of the three fission products Cs-137, I-131 and Xe-133 are investigated. Regarding Xe-133, the total release is estimated to be of the order of 6 × 1018 Bq emitted during the explosions of units 1, 2 and 3. The total source term estimated gives a fraction of core inventory of about 8 × 1018 Bq at the time of reactors shutdown. This result suggests that at least 80 % of the core inventory has been released into the atmosphere and indicates a broad meltdown of reactor cores. Total atmospheric releases of Cs-137 and I-131 aerosols are estimated to be 1016 and 1017 Bq, respectively. By neglecting gas/particulate conversion phenomena, the total release of I-131 (gas + aerosol) could be estimated to be 4 × 1017 Bq. Atmospheric transport simulations suggest that the main air emissions have occurred during the events of March 14, 2011 (UTC) and that no major release occurred after March 23. The radioactivity emitted into the atmosphere could represent 10 % of the Chernobyl accident releases for I-131 and Cs-137.

Activity concentration data from ambient radioxenon measurements in ground level air, which were carried out in Europe in the framework of the International Noble Gas Experiment (INGE) in support of the development and build-up of a radioxenon monitoring network for the Comprehensive Nuclear-Test-Ban Treaty verification regime are presented and discussed. Six measurement stations provided data from 5 years of measurements performed between 2003 and 2008: Longyearbyen (Spitsbergen, Norway), Stockholm (Sweden), Dubna (Russian Federation), Schauinsland Mountain (Germany), Bruyeres-le-Châtel and Marseille (both France). The noble gas systems used within the INGE are designed to continuously measure low concentrations of the four radioxenon isotopes which are most relevant for detection of nuclear explosions: 131mXe, 133mXe, 133Xe and 135Xe with a time resolution less than or equal to 24 h and a minimum detectable concentration of 133Xe less than 1 mBq/m3. This European cluster of six stations is particularly interesting because it is highly influenced by a high density of nuclear power reactors and some radiopharmaceutical production facilities. The activity concentrations at the European INGE stations are studied to characterise the influence of civilian releases, to be able to distinguish them from possible nuclear explosions. It was found that the mean activity concentration of the most frequently detected isotope, 133Xe, was 5–20 mBq/m3 within Central Europe where most nuclear installations are situated (Bruyeres-le-Châtel and Schauinsland), 1.4–2.4 mBq/m3 just outside that region (Stockholm, Dubna and Marseille) and 0.2 mBq/m3 in the remote polar station of Spitsbergen. No seasonal trends could be observed from the data. Two interesting events have been examined and their source regions have been identified using atmospheric backtracking methods that deploy Lagrangian particle dispersion modelling and inversion techniques. The results are consistent with known releases of a radiopharmaceutical facility.

Radioxenon concentration data collected at International Noble Gas Experiment (INGE) monitoring sites in the Northern Hemisphere are demonstrably impacted by emissions from medical isotope (MI) production facilities at Chalk River (CRL), Ontario and Fleurus, Belgium [Saey, J Environ Radioact 100(5):396–406, 2009]. Temporary cessation at these European MI facilities in the latter half of 2008 allowed an opportunity to assess the relative impact of distant MI facilities at INGE monitoring stations. In particular, the concentration distributions at the measurement sites and calculated sensitivities to the putative emission locations through atmospheric transport modelling (ATM) of meteorological Source Receptor Sensitivity (SRS) computations were used to study MI impacts.

Within the frame of Comprehensive Nuclear-Test Ban Treaty (CTBT), this paper deals with the development of the new techniques necessary for the xenon monitoring requested by the CTBT. An automatic system called SPALAX™, devoted to the on-site sampling and measurement was developed by French atomic energy commission (CEA). Analytical methods and equipments have been studied at our laboratory, using dual X-γ-spectrometry in order to get independent means with better sensitivity within a robust quality assurance program. In the case of a wide number of potential existing sources and depending on meteorological conditions, several solutions can be arrived at.

Medical and industrial fadioisotopes are fundamental tools used in science, medicine and industry with an ever expanding usage in medical practice where their availability is vital. Very sensitive environmental radionuclide monitoring networks have been developed for nuclear-security-related monitoring [particularly Comprehensive Test-Ban-Treaty (CTBT) compliance verification] and are now operational.

Berlemont, A Achim, P Chang, Z; Two different Lagrangian approaches for particle/particle collisions are described. The first model is based on the simultaneous tracking of several particles and suitable treatment is developed on particle pairs to detect collisions on each time step of the particle trajectory realization. The second method is based on a stochastic approach where one single particle is tracked, and successive random processes are applied to generate a fictitious partner of collision. In order to validate both approaches, simulations have been carried out in homogeneous isotropic turbulence and they have been compared with LES data. The particle/particle correlated motion through the surrounding fluid is proved to be a key parameter in a particle/particle collision process. (C) 2001 American Institute of Physics.