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Radionuclides are monitored in the atmosphere for the signatures of nuclear explosions, as part of the verification of the Comprehensive Nuclear-Test-Ban Treaty (CTBT). Civil nuclear facilities, such as Nuclear Power Plants (NPPs) and Isotope Production Facilities (IPFs) are sources of anthropogenic radionuclides in the atmosphere and these signatures are sometimes indistinguishable to those of a nuclear explosion. In order to improve the understanding of civil radionuclide-emitting facilities and their impact on the International Monitoring System (IMS) of the CTBT, a group of scientists from the UK, US and Sweden are collaborating with EDF Energy UK to measure radionuclide emissions from an Advanced Gas-cooled Reactor (AGR) nuclear power station. Emissions are being measured at the source, via a stack monitor and high-resolution gamma spectrometry measurements of filters and also at tens of kilometres away via three sensitive radioxenon atmospheric samplers. The timing, isotopic composition, activity magnitudes and other release parameters of interest are investigated, to improve the discrimination between a civil radionuclide release and an explosive nuclear test. This paper outlines the work of the Xenon and Environmental Nuclide Analysis at Hartlepool (XENAH) collaboration, describes the equipment fielded and provides initial results from each measurement campaign.

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.

We introduce a new concept in radioxenon detection - the radioxenon Array, defined as a system where air sampling and activity measurement is performed at multiple locations, using measurement units that are less sensitive, but on the other hand less costly, and easier to install and operate, compared to current state-of-the-art radioxenon systems. The inter-unit distance in the Array is typically hundreds of kilometres. Using synthetic nuclear explosions together with a parametrized measurement system model, we argue that, when such measurement units are combined into an Array, the aggregated verification performance (detection, location, and characterization) can be high. The concept has been realized by developing a measurement unit named SAUNA QB, and the world's first radioxenon Array is now operating in Sweden. The operational principles and performance of the SAUNA QB and the Array is described, and examples of first measured data are presented, indicating a measurement performance according to expectations.

The SAUNA III represent the next generation of the SAUNA systems designed for detection of low levels of radioactive xenon in the atmosphere, with the main purpose of detecting underground nuclear explosions. The system automatically collects, processes and measures 40 m(3) atmospheric samples every 6 h, increasing both the sensitivity and time resolution as compared the systems currently in use. The higher sensitive increases the number of detections, especially for samples were more than one isotope of xenon are detected. This improves the understanding of the background and the possibility to screen out signal from civilian sources. The increased time resolution of the new system also provides a more detailed picture of the plumes, especially important for near-by sources. The design of the system as well as data from the first two years of operation are presented.

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.

A high throughput system for processing and detection of low levels of radioxenon in soil gas samples has been developed. Processing and analysis of sub-soil noble gas samples puts high demands on the gas separation part of the system since the samples might contain high levels of Rn, CO2 as well as other gases. The gas process is optimized to remove all CO2, H2O and Rn with a high recovery yield of the xenon in the sample to ensure a high sensitivity even for small samples. The system is designed to handle multiple samples per day with a high level of automation and sample traceability to be suitable for use in an on-site inspection (OSI) an important component in the verification of the Comprehensive Nuclear Test Ban Treaty. To ensure a rapid deployment the system could be pre-installed in a flight container.

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.

An analysis of a data set consisting of 3 years of high time resolution radioxenon stack measurements from the three nuclear reactors at the Forsmark nuclear power plant in Sweden, as well as measurements of atmospheric radioxenon in Stockholm air, 110 km away, is presented. The main causes for the stack releases, such as the function of the xenon mitigation systems, presence of leaking fuel elements, and reactor operations such as shutdown and startup, are discussed in relation to the stack data. The relation between radioxenon releases and reactor operation is clearly illustrated by the correlation between the stack measurements and thermal reactor power. In general, the isotopic ratios of the Stockholm measurements, which are shown to mainly originate from Forsmark releases, agree well with stack measurements, and with a modeled reactor operational sequence. Results from a forward atmospheric dispersion calculation agree very well with observed plume arrival times and widths, and with some exceptions, also with absolute activity concentrations. The results illustrates the importance of detailed knowledge of radioxenon emissions from nuclear power plants when interpreting radioxenon measurements for nuclear test ban verification, and provide new input to this kind of analysis. Furthermore, it demonstrates the possibility to use sensitive radioxenon detection systems to remotely detect and verify reactor operation.

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.

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.

PNNL developed a beta–gamma simulator (BGSim) that incorporated GEANT-modeled data sets from radioxenon decay chains, as well as functionality to use nuclear detector-acquired data sets to create new beta–gamma spectra with varying amounts of background, 133 Xe, 131m Xe, 133m Xe, 135 Xe, and 222 Rn and its decay products. After BGSim was developed, additional uses began to be identified for the program output: training sets of two-dimensional spectra for data analysts at the IDC and other NDC, and spectra for exercises such as the Integrated Field Exercise 2014 held in Jordan at the Dead Sea.

The general characterisation of the global radioxenon background is of interest for the verification of the Comprehensive Nuclear-Test-Ban Treaty. Since the major background sources are only a few isotope production facilities, their source term has an emphasized influence on the worldwide monitoring process of radioxenon. In this work, two different datasets of source terms are applied through atmospheric transport modelling, to estimate the concentration at two radioxenon detection stations in Germany and Sweden. One dataset relies on estimated average annual emissions; the other includes monthly resolved measurements from an isotope production facility in Fleurus, Belgium. The quality of the estimations is then validated by comparing them to the radioxenon concentrations that have been sampled at two monitoring stations over the course of 1 year.

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.

Observations made in April 2013 of the radioxenon isotopes Xe-133 and Xe-131m 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 131mXe 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. (C) 2013 The Authors. Published by Elsevier Ltd. All rights reserved.

A cylindrical plastic scintillator cell, used for radioxenon monitoring within the verification regime of the Comprehensive Nuclear-Test-Ban Treaty, has been coated with 425 nm Al 2 O 3 using low temperature Atomic Layer Deposition, and its performance has been evaluated. The motivation is to reduce the memory effect caused by radioxenon diffusing into the plastic scintillator material during measurements, resulting in an elevated detection limit. Measurements with the coated detector show both energy resolution and efficiency comparable to uncoated detectors, and a memory effect reduction of a factor of 1000. Provided that the quality of the detector is maintained for a longer period of time, Al 2 O 3 coatings are believed to be a viable solution to the memory effect problem in question.

Radioxenon emissions of the TRIGA Mark II research reactor in Vienna were investigated with respect to a possible impact on the verification of the Comprehensive Nuclear Test-Ban-Treaty. Using the Swedish Automatic Unit for Noble Gas Acquisition (SAUNA II), five radioxenon isotopes 125Xe, 131mXe, 133mXe, 133Xe and 135Xe were detected, of which 125Xe is solely produced by neutron capture in stable atmospheric 124Xe and hence acts as an indicator for neutron activation processes. The other nuclides are produced in both fission and neutron capture reactions. The detected activity concentrations ranged from 0.0010 to 190 Bq/m³. The source of the radioxenon is not yet fully clarified, but it could be micro-cracks in the fuel cladding, fission of 235U contaminations on the outside of the fuel elements or neutron activation of atmospheric Xe. Neutron deficient 125Xe with its highly complex decay scheme was seen for the first time in a SAUNA system. In many experiments the activity ratios of the radioxenon nuclides carry the signature of nuclear explosions, if 131mXe is omitted. Only if 131mXe is included into the calculations of the isotopic activity ratios, the majority of the measurements revealed a “civil” signature (typical for a NPP). A significant contribution of the TRIGA Vienna to the global or European radioxenon inventory can be excluded. Due to the very low activities, the emissions are far below any concern for human health.

Detailed deterministic calculations of electron–photon coincidence spectra for 131mXe and 133mXe, 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 131mXe show good agreement with observed features in electron spectra. The results can be used in the development of radioxenon calibration and concentration analysis techniques.

The Comprehensive Nuclear-Test-Ban Treaty (CTBT) specifies that radioxenon measurements should be performed at 40 or more stations worldwide within the International Monitoring System (IMS). Measuring radioxenon is one of the principle techniques to detect underground nuclear explosions. Specifically, presence and ratios of different radioxenon isotopes allows determining whether a detection event under consideration originated from a nuclear explosion or a civilian source. However, radioxenon monitoring on a global scale is a novel technology and the global civil background must be characterized sufficiently. This paper lays out a study, based on several unique measurement campaigns, of the worldwide concentrations and sources of verification relevant xenon isotopes. It complements the experience already gathered with radioxenon measurements within the CTBT IMS programme and focuses on locations in Belgium, Germany, Kuwait, Thailand and South Africa where very little information was available on ambient xenon levels or interesting sites offered opportunities to learn more about emissions from known sources. The findings corroborate the hypothesis that a few major radioxenon sources contribute in great part to the global radioxenon background. Additionally, the existence of independent sources of 131mXe (the daughter of 131I) has been demonstrated, which has some potential to bias the isotopic signature of signals from nuclear explosions.