. On 11 March 2011, an earthquake occurred about 130 km off the Pacific coast of Japan's main island Honshu, followed by a large tsunami. The resulting loss of electric power at the Fukushima Dai-ichi nuclear power plant developed into a disaster causing massive release of radioactivity into the atmosphere. In this study, we determine the emissions into the atmosphere of two isotopes, the noble gas xenon-133 (133Xe) and the aerosol-bound caesium-137 (137Cs), which have very different release characteristics as well as behavior in the atmosphere. To determine radionuclide emissions as a function of height and time until 20 April, we made a first guess of release rates based on fuel inventories and documented accident events at the site. This first guess was subsequently improved by inverse modeling, which combined it with the results of an atmospheric transport model, FLEXPART, and measurement data from several dozen stations in Japan, North America and other regions. We used both atmospheric activity concentration measurements as well as, for 137Cs, measurements of bulk deposition. Regarding 133Xe, we find a total release of 15.3 (uncertainty range 12.2–18.3) EBq, which is more than twice as high as the total release from Chernobyl and likely the largest radioactive noble gas release in history. The entire noble gas inventory of reactor units 1–3 was set free into the atmosphere between 11 and 15 March 2011. In fact, our release estimate is higher than the entire estimated 133Xe inventory of the Fukushima Dai-ichi nuclear power plant, which we explain with the decay of iodine-133 (half-life of 20.8 h) into 133Xe. There is strong evidence that the 133Xe release started before the first active venting was made, possibly indicating structural damage to reactor components and/or leaks due to overpressure which would have allowed early release of noble gases. For 137Cs, the inversion results give a total emission of 36.6 (20.1–53.1) PBq, or about 43% of the estimated Chernobyl emission. Our results indicate that 137Cs emissions peaked on 14–15 March but were generally high from 12 until 19 March, when they suddenly dropped by orders of magnitude at the time when spraying of water on the spent-fuel pool of unit 4 started. This indicates that emissions may not have originated only from the damaged reactor cores, but also from the spent-fuel pool of unit 4. This would also confirm that the spraying was an effective countermeasure. We explore the main dispersion and deposition patterns of the radioactive cloud, both regionally for Japan as well as for the entire Northern Hemisphere. While at first sight it seemed fortunate that westerly winds prevailed most of the time during the accident, a different picture emerges from our detailed analysis. Exactly during and following the period of the strongest 137Cs emissions on 14 and 15 March as well as after another period with strong emissions on 19 March, the radioactive plume was advected over Eastern Honshu Island, where precipitation deposited a large fraction of 137Cs on land surfaces. Radioactive clouds reached North America on 15 March and Europe on 22 March. By middle of April, 133Xe was fairly uniformly distributed in the middle latitudes of the entire Northern Hemisphere and was for the first time also measured in the Southern Hemisphere (Darwin station, Australia). In general, simulated and observed concentrations of 133Xe and 137Cs both at Japanese as well as at remote sites were in good quantitative agreement. Altogether, we estimate that 6.4 PBq of 137Cs, or 18% of the total fallout until 20 April, were deposited over Japanese land areas, while most of the rest fell over the North Pacific Ocean. Only 0.7 PBq, or 1.9% of the total fallout were deposited on land areas other than Japan.

Xenon-133 and caesium-137 releases into the atmosphere from the Fukushima Dai-ichi nuclear power plant: determination of the source term, atmospheric dispersion, and deposition

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A global monitoring system for atmospheric xenon radioactivity is being established as part of the International Monitoring System that will verify compliance with the Comprehensive Nuclear-Test-Ban Treaty (CTBT) once the treaty has entered into force. This paper studies isotopic activity ratios to support the interpretation of observed atmospheric concentrations of 135Xe, 133mXe, 133Xe and 131mXe. The goal is to distinguish nuclear explosion sources from civilian releases. Simulations of nuclear explosions and reactors, empirical data for both test and reactor releases as well as observations by measurement stations of the International Noble Gas Experiment (INGE) are used to provide a proof of concept for the isotopic ratio based method for source discrimination.

Discrimination of Nuclear Explosions against Civilian Sources Based on Atmospheric Xenon Isotopic Activity Ratios

The influence of radiopharmaceutical isotope production on the global radioxenon background.

Radioxenon detections in the CTBT international monitoring system likely related to the announced nuclear test in North Korea on February 12, 2013.

Global radioxenon emission inventory based on nuclear power reactor reports

Monitoring of radioactive noble gases, in particular xenon isotopes, is a crucial element of the verification of the Comprehensive Nuclear-Test-Ban Treaty (CTBT). The capability of the noble gas network, which is currently under construction, to detect signals from a nuclear explosion critically depends on the background created by other sources. Therefore, the global distribution of these isotopes based on emissions and transport patterns needs to be understood. A significant xenon background exists in the reactor regions of North America, Europe and Asia. An emission inventory of the four relevant xenon isotopes has recently been created, which specifies source terms for each power plant. As the major emitters of xenon isotopes worldwide, a few medical radioisotope production facilities have been recently identified, in particular the facilities in Chalk River (Canada), Fleurus (Belgium), Pelindaba (South Africa) and Petten (Netherlands). Emissions from these sites are expected to exceed those of the other sources by orders of magnitude. In this study, emphasis is put on 133Xe, which is the most prevalent xenon isotope. First, based on the emissions known, the resulting 133Xe concentration levels at all noble gas stations of the final CTBT verification network were calculated and found to be consistent with observations. Second, it turned out that emissions from the radioisotope facilities can explain a number of observed peaks, meaning that atmospheric transport modelling is an important tool for the categorization of measurements. Third, it became evident that Nuclear Power Plant emissions are more difficult to treat in the models, since their temporal variation is high and not generally reported. Fourth, there are indications that the assumed annual emissions may be underestimated by factors of two to ten, while the general emission patterns seem to be well understood. Finally, it became evident that 133Xe sources mainly influence the sensitivity of the monitoring system in the mid-latitudes, where the network coverage is particularly good.

Computation and Analysis of the Global Distribution of the Radioxenon Isotope 133Xe based on Emissions from Nuclear Power Plants and Radioisotope Production Facilities and its Relevance for the Verification of the Nuclear-Test-Ban Treaty

Verification of the Comprehensive Nuclear-Test-Ban Treaty is a complex undertaking. A monitoring system comprising a global network of 321 seismic, hydroacoustic, infrasound and radionuclide stations is used to detect signals that could indicate a possible nuclear explosion. This system daily sends more than 10 GB of raw data to the Vienna based International Data Centre for further processing and analysis to answer a simple question: have any indications for a possible nuclear explosion been sensed? We will focus on the 40 stations in charge for global radioxenon monitoring and discuss the complexity of solving the nuclear source attribution problem. © 2008 Wiley Periodicals, Inc. Complexity, 2008.

The views expressed herein are those of the authors and do not necessarily reflect the views of the CTBTO Preparatory Commission.

https://onlinelibrary.wiley.com/doi/pdf/10.1002/cplx.20228

Matthias P. Tuma

Papers

Global radioxenon emission inventory based on nuclear power reactor reports

Computation and Analysis of the Global Distribution of the Radioxenon Isotope 133Xe based on Emissions from Nuclear Power Plants and Radioisotope Production Facilities and its Relevance for the Verification of the Nuclear-Test-Ban Treaty

The complexity of CTBT verification. Taking noble gas monitoring as an example

The complexity of CTBT verification. Taking noble gas monitoring as an example