Global emission inventory of 131mXe, 133Xe, 133mXe, and 135Xe from all kinds of nuclear facilities for the reference year 2014.

Global radioactivity monitoring for the verification of the Comprehensive Nuclear-Test-Ban Treaty (CTBT) includes the four xenon isotopes 131mXe, 133Xe, 133mXe and 135Xe. These four isotopes are serving as important indicators of nuclear explosions. The state-of-the-art radioxenon emission inventory uses generic release estimates for each known nuclear facility. However, the release amount can vary by several orders of magnitude from year to year. The year 2014 was selected for a single year radioxenon emission inventory with minimized uncertainty. Whenever 2014 emissions reported by the facility operator are available these are incorporated into the 2014 emission inventory. This paper summarizes this new emission inventory. The emissions are compared with previous studies. The global radioxenon emission inventory for 2014 can be used for studies to estimate the contribution of this anthropogenic source to the observed ambient concentrations at IMS noble gas sensors to support CTBT monitoring activities, including calibration and performance assessment of the verification system as described in the Treaty as well as developing and validating methods for enhanced detection capabilities of signals that may indicate a nuclear test. One specific application is the 1st Nuclear Explosion Signal Screening Open Inter-Comparison Exercise announced end of 2021.

Overview of temporary radioxenon background measurement campaigns conducted for the CTBTO between 2008 and 2018.

The Comprehensive Nuclear-Test-Ban Treaty (CTBT) specifies that an overall network of at least 40 International Monitoring System (IMS) stations should monitor the presence of radioxenon in the atmosphere upon its entry into force. The measurement of radioxenon concentrations in the air is one of the major techniques to detect underground nuclear explosions. It is, together with radionuclide particulate monitoring, the only component of the network able to confirm whether an event originates from a nuclear test, leaving the final proof to on-site inspection. Correct and accurate interpretation of radioxenon detections by State Signatories is a key parameter of the verification regime of the Preparatory Commission for the Comprehensive Nuclear-Test-Ban Treaty Organization (CTBTO). In this context, the discrimination between the highly variable radioxenon background generated by normal operations of nuclear facilities and CTBT-relevant events is a challenging, but critical, task. To this end, the radioxenon background that can be expected at IMS noble gas systems must be sufficiently characterized and understood. All activities conducted to study the global radioxenon background are focused on the calibration and performance of the verification system as described in the Treaty. The unique CTBTO noble gas system network is designed to optimally covering the globe. By the end of 2019, 31 systems were put in operation, 25 of which being already certified. It took two decades from the first experimental setup of noble gas system in the field to reach this stage of maturity. In the meantime, it was an urgent need to gain empirical evidence of atmospheric radioxenon concentrations with the full spectrum of characteristics that IMS noble gas systems may be observing. This experience was significantly advanced through temporary measurement campaigns. Their objective was to gain the additional necessary knowledge for a correct understanding and categorization of radioxenon detections. The site selection for these campaigns put emphasis on regions with low coverage by the initially few experimental noble gas systems at IMS locations or where potential interferences with normal background might be observed. Short-term measurements were first initiated in 2008. Sites of potential interest were identified, and campaigns up to few weeks were performed. Based on the findings of these short campaigns, transportable systems were procured by the CTBTO. Longer temporary measurement campaigns were started afterwards and operated by local hosts in different regions of the globe. Site selections were based on purely scientific criteria. Objectives of the measurement campaigns were continually reassessed, and projects were designed to meet the scientific needs for radioxenon background understanding as required for nuclear explosion monitoring. As of today, several thousands of samples have been collected and measured. Spectra of temporary measurement campaigns were (and are still) analysed in the International Data Centre (IDC). As they are not part of the CTBT monitoring system, no IDC product is generated. Analysis results are stored in a non-operational database of the CTBTO and made available, together with raw data, to authorized users of States Signatories through a Secure Web Portal (SWP) and to scientific institutions for approved research projects through a virtual Data Exploitation Centre (vDEC) after signing a cost-free confidentiality agreement (https://www.ctbto.org/specials/vdec). This paper aims at providing an overview of the temporary measurement campaigns conducted by the CTBTO since the very first field measurements. It lays out scientific results in a systematic approach. This overview demonstrates the asset of radioxenon background measurement data that have been collected with a wide variety of characteristics that may be observed at IMS stations. It bears a tremendous opportunity for development, enhancement and validation of methodologies for CTBT monitoring. In 2018, a campaign started in Japan with transportable noble gas systems in the vicinity of the IMS station RN38 in Takasaki. It will be described separately once the measurements are completed.

On the usability of event zero time determinations using radioxenon isotopic activity ratios given the real atmospheric background observations.

This work focuses on the usability of event zero time determination using xenon isotopic activity ratios. Two data sets from Nevada underground nuclear test and Fukushima accident debris were used to calculate the age of radioxenon release by considering three kinds of radioactivity release radionuclide sources: nuclear explosion scenarios, nuclear power reactor release and medical isotopes production facilities release. Typical nuclear power reactor releases were characterized and reference values are proposed for six isotopic activity ratios, which data can be considered as reference point of nuclear reactor effluents at the time of their release obtained from real observations. The same reference values of isotopic activity ratio are given for medical isotopes production facilities releases. The purpose of this study is to evaluate the use of zero-time calculation for source characterization under the assumption that a hypothesis about the event time is made. The event time information may come from a seismo-acoustic event of interest or an inverse atmospheric transport simulation or other context information. For both data sets used in this study, the age precisions are calculated and the time precision difference is evaluated and used as a parameter for the characterization of each radionuclide event. Almost all radioxenon isotopic activity ratios are found to correctly identifying the source type of the radionuclide events studied in this work. The results from this radionuclide events characterization study may be helpful for event screening activities of the Comprehensive Nuclear Test Ban Treaty Organization (CTBTO).

Nuclear event zero time determination using analytical solutions of radioxenon activities under in-growth condition.

Motivated by simplifying the calculation process of radioxenon isotopic activity used by scientist community in nuclear event characterization, the analytical formulas of the numbers of nuclides and isotopic activities of CTBT relevant radioxenon Xe-135, Xe-133m, Xe-133 and Xe-131m proposed in this work can be useful and incorporated in the calculation algorithms for nuclear event studies. The calculated ages using analytical formulas and radioxenon activity data from real observations compare well with the reported ages and show good results of event timing precision.

Setting the baseline for estimated background observations at IMS systems of four radioxenon isotopes in 2014.

Worldwide monitoring of radionuclides is an essential part of the verification system of the Comprehensive Nuclear-Test-Ban Treaty (CTBT) as it can provide a direct evidence of the nuclear nature of an explosion. In the case of underground nuclear testing, the radioactive noble gases, specifically radioxenon, have the highest probability to escape to the atmosphere. The detection capability of the CTBT noble gas network, which is being built, is weakened due to the presence of a worldwide civilian radioxenon background. Improving the understanding and knowledge of civilian radioxenon sources and their impact on the noble gas systems background is crucial to strengthen their verification capabilities. Two major civilian radioxenon sources have been identified in past research, namely: Medical Isotope Production Facilities (MIPFs) and Nuclear Power Plants (NPPs). In this study, a 2014 baseline radioxenon emission inventory is proposed for all four CTBT relevant radioxenon isotopes (Xe-131m, Xe-133m, Xe-133 and Xe-135) on the basis of a literature review for both the Medical Isotopes Productions Facilities and Nuclear Power Plants. This 2014 baseline radioxenon emission inventory relies on peer-reviewed information on the facility location and corresponding radioxenon emission. The baseline radioxenon emission inventory is used along with Atmospheric Transport Modelling (ATM) to estimate the radioxenon activity concentrations at the noble gas systems. The results reveal the complexity and the geographical dependence of the civilian radioxenon background. The estimations are compared to the observations for CTBT noble gas systems that were operational in 2014. It is demonstrated that the estimated Xe-133 activity concentrations are, for most systems, in the same order of magnitude than observed detections. Non-detections of Xe-131m, Xe-133m, Xe-133 and Xe-135 are, for most samples, well reproduced by the estimation. To our best knowledge, this study is the first attempt to propose, a baseline emission inventory for all four CTBT relevant radioxenon isotopes and compare the estimated Xe-131m, Xe-133m, Xe-133 and Xe-135 activity concentrations with all observations at CTBT noble gas systems during the full 2014 calendar year.

Fast and accurate dating of nuclear events using La-140/Ba-140 isotopic activity ratio.

This study reports on a fast and accurate assessment of zero time of certain nuclear events using La-140/Ba-140 isotopic activity ratio. For a non-steady nuclear fission reaction, the dating is not possible. For the hypothesis of a nuclear explosion and for a release from a steady state nuclear fission reaction the zero-times will differ. This assessment is fast, because we propose some constants that can be used directly for the calculation of zero time and its upper and lower age limits. The assessment is accurate because of the calculation of zero time using a mathematical method, namely the weighted least-squares method, to evaluate an average value of the age of a nuclear event. This was done using two databases that exhibit differences between the values of some nuclear parameters. As an example, the calculation method is applied for the detection of radionuclides La-140 and Ba-140 in May 2010 at the radionuclides station JPP37 (Okinawa Island, Japan).

Update and improvement of the global krypton-85 emission inventory.

Krypton-85 is mainly produced in nuclear reactors by fission of uranium and plutonium and released during chopping and dissolution of spent fuel rods in nuclear reprocessing facilities. As noble gas it is suited as a passive tracer for evaluation of atmospheric transport models. Furthermore, research is ongoing to assess its quality as an indicator for clandestine reprocessing activities. This paper continues previous efforts to compile a comprehensive historic emission inventory for krypton-85. Reprocessing facilities are the by far largest emitters of krypton-85. Information on sources and calculations used to derive the annual krypton-85 emission is provided for all known reprocessing facilities in the world. In addition, the emission characteristics of two plants, Tokai (Japan) and La Hague (France), are analysed in detail using emission data with high temporal resolution. Other types of krypton-85 sources are power reactors, naval reactors and isotope production facilities. These sources contribute only little or negligible amounts of krypton-85 compared to the large reprocessing facilities. Taking the decay of krypton-85 into account, the global atmospheric inventory is estimated to about 5500 PBq at the end of 2009. The correctness if the inventory has been proven by meteorological simulations and its error is assumed to be in the range of a few percent.

A novel vacuum ultra violet lamp for metastable rare gas experiments.

We report on a new design of a vacuum ultra violet (VUV) lamp for direct optical excitation of high laying atomic states, e.g., for excitation of metastable rare gas atoms. The lamp can be directly mounted to ultra-high vacuum vessels (p ≤ 10(-10)mbar). It is driven by a 2.45 GHz microwave source. For optimum operation, it requires powers of ~20 W. The VUV light is transmitted through a magnesium fluoride window, which is known to have a decreasing transmittance for VUV photons with time. In our special setup, after a run-time of the VUV lamp of 550 h the detected signal continuously decreased to 25% of its initial value. This corresponds to a lifetime increase of two orders of magnitude compared to previous setups or commercial lamps.

Characterisation of prompt and delayed atmospheric radioactivity releases from underground nuclear tests at Nevada as a function of release time.

A database with information on about 500 cases of atmospheric radioactivity releases from underground nuclear tests is analysed. The data are statistically evaluated and systematically aggregated in order to characterise prompt uncontrolled as well as delayed operational releases of radioactivity into the atmosphere. The focus is put on the latter. The reported data compare well with theoretically derived xenon activities for reasonable nuclear test scenarios. Conclusions are drawn on the main features of releases that can be expected from underground nuclear tests as a function of release time. These findings are relevant for developing and validating methods to be applied in global monitoring of atmospheric radioactivity with respect to indications of an underground nuclear explosion.

Global radioxenon emission inventory based on nuclear power reactor reports.

Atmospheric radioactivity is monitored for the verification of the Comprehensive Nuclear-Test-Ban Treaty, with xenon isotopes 131mXe, 133Xe, 133mXe and 135Xe serving as important indicators of nuclear explosions. The treaty-relevant interpretation of atmospheric concentrations of radioxenon is enhanced by quantifying radioxenon emissions released from civilian facilities. This paper presents the first global radioxenon emission inventory for nuclear power plants, based on North American and European emission reports for the years 1995-2005. Estimations were made for all power plant sites for which emission data were unavailable. According to this inventory, a total of 1.3PBq of radioxenon isotopes are released by nuclear power plants as continuous or pulsed emissions in a generic year.

Isotopic signature of atmospheric xenon released from light water reactors.

A global monitoring system for atmospheric xenon radioactivity is being established as part of the International Monitoring System to verify compliance with the Comprehensive Nuclear-Test-Ban Treaty (CTBT). The isotopic activity ratios of (135)Xe, (133m)Xe, (133)Xe and (131m)Xe are of interest for distinguishing nuclear explosion sources from civilian releases. Simulations of light water reactor (LWR) fuel burn-up through three operational reactor power cycles are conducted to explore the possible xenon isotopic signature of nuclear reactor releases under different operational conditions. It is studied how ratio changes are related to various parameters including the neutron flux, uranium enrichment and fuel burn-up. Further, the impact of diffusion and mixing on the isotopic activity ratio variability are explored. The simulations are validated with reported reactor emissions. In addition, activity ratios are calculated for xenon isotopes released from nuclear explosions and these are compared to the reactor ratios in order to determine whether the discrimination of explosion releases from reactor effluents is possible based on isotopic activity ratios.

Conclusions on plutonium separation from atmospheric krypton-85 measured at various distances from the Karlsruhe reprocessing plant.

For wide-area atmospheric monitoring, krypton-85 is the best indicator for clandestine plutonium separations. The detection and false alarm rates were determined from weekly samples at five different distances from the Karlsruhe reprocessing plant between 1985 and 1988. The detection rate for the separation of 4 kg of plutonium per week was found to be as high as 80-90% at a distance of less than 1 km, 70% at 5 km, 40% at 39 km, and 15% at 130 km. At distances up to 40 km, the false alarm rate is less than 3.5%. On average, the fuel released 28 TBq krypton-85 per kg plutonium. For weapons-grade plutonium, the krypton signal would be lower by a factor of 2. Hence, the given percentages correspond to the detection probabilities for the separation of a significant quantity (8 kg) of plutonium per weekly sample under the specific meteorological conditions of the WAK. The minimum separation rates that could have been detected are 2 gram of weapons-grade plutonium per week at a distance of less than 1 km, 40 g/week at 5 km, 200 g/week at 39 km, and 1000 g/week at 130 km.