Determination of the source location of anthropogenic radionuclides collected in Finland and Sweden in June 2020 using a multi-technology analysis.

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.

A calibration procedure for beta-gamma coincidence detector-systems using four radioxenon spikes.

The determination of activity concentrations of the CTBT-relevant radioxenon relies on a robust calibration method. A procedure is outlined using four radioxenon spikes for beta-gamma detector-systems with 4π geometry. Detection efficiencies of beta-gamma coincidences in the net count calculation method, including the interference matrix between radioxenon and radon, are determined by three measurement channels: beta singles, gamma singles and beta-gamma coincidences, without reference activity values.

SAUNA III - The next generation noble gas system for verification of nuclear explosions.

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 m3 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.

A plastic scintillator and HPGe ß-γ coincidence detection system.

A network of specialist laboratories support the International Monitoring System (IMS) of the Comprehensive Nuclear-Test-Ban Treaty (CTBT) with re-measurements of radionuclide samples, including xenon gas. The measurement of four xenon fission product radionuclides (133Xe, 135Xe, 131mXe and 133mXe) can be used to detect an underground nuclear explosion. Laboratories use a range of techniques to measure the radionuclides, including beta-gamma (ß-γ) coincidence spectrometry. These highly-sensitive measurements are capable of detecting concentrations of down to 500 atoms of 133Xe in a few cm3 of xenon. In some detector systems, detection of the metastable isomers (131mXe and 133mXe) can be more challenging due to interferences between the signatures of different radionuclides. Recent work has shown that using high-purity Germanium (HPGe) high-resolution gamma detectors, these interferences can be reduced, lowering the dependence of the detection limits on radionuclide sample isotopic composition. One downside of these detectors is the reduction in detection efficiency, which impacts the overall detection sensitivity; so assessing different detector systems is a priority for radionuclide laboratories. This work presents a coincidence detector system comprising of a plastic scintillator gas cell and a large-crystal high-purity germanium detector. The energy resolution, coincidence detection efficiency, MDA and interference factors are determined from measurements of synthetic radioxenon gas samples.

Projected network performance for next generation aerosol monitoring systems.

Aerosol monitoring for radioactivity is a mature and proven technology. However, by improving key specifications of aerosol monitoring equipment, more samples per day can be collected and analyzed with the same minimum detectable concentrations as current systems. This work models hypothetical releases of 140Ba and 131I over a range of magnitudes corresponding to the inventory produced from the fission of about 100 g to 1 kiloton TNT-equivalent of 235U. The releases occur over an entire year to incorporate the natural variability in atmospheric transport. Sampling equipment located at the 79 locations for radionuclide stations identified in the Comprehensive Nuclear-Test-Ban Treaty (CTBT) for the International Monitoring System are used to determine the detections of the individual releases. Alternative collection schemes in next generation equipment that collect 2, 3, or 4 samples per day, rather than the current 1 sample per day, would result in detections in many more samples at more stations with detections for a given release level. The authors posit that next generation equipment will result in increased network resilience to outages and improved source-location capability for lower yield source releases. The application of dual-detector and coincidence measurements to these systems would significantly boost sensitivity for some isotopes and would further enhance the monitoring capability.

Investigation on atmospheric radioactivity sample association using consistency with isotopic ratio decay over time at IMS radionuclide stations.

For the enhancement of the International Data Centre's products, specifically the Standard Screened Radionuclide Event Bulletin, an important step is to establish methods to associate the detections of the Comprehensive Nuclear-Test-Ban Treaty-relevant nuclides in different atmospheric radioactivity samples with the same radionuclide release to characterize its source for the purpose of nuclear explosion monitoring. Episodes of anomalously high activity concentrations in samples at the International Monitoring System radionuclide stations are used as the primary assumption for being related to the same release. For multiple isotope observations, the consistency of their isotopic ratios in subsequent samples with radioactive decay is another plausible hint for one unique release. The radioxenon observations that are associated with the nuclear test announced by the Democratic People's Republic of Korea in 2013 serve as case study to demonstrate the effectiveness of this basic approach and how the additionally associated samples improve the source location. We use two distinct puff releases, both of short duration, for the atmospheric transport modelling simulations to gain further evidence and confidence in our sample association study by identifying the air masses that link the releases to multiple samples. This basic approach will support the definition of analysis procedures and criteria for automatic sample association to be implemented in the Standard Screened Radionuclide Event Bulletin, which is of relevance for an expert technical analysis.

Efficiency calibration and self-attenuation correction in radioxenon measurement using ß-γ coincidence method.

Measurement of the four radioxenon isotopes, namely 131mXe, 133mXe, 133Xe, and 135Xe, play a key role in underground nuclear test monitoring for ensuring compliance with the Comprehensive Nuclear-Test-Ban Treaty (CTBT). To improve detection sensitivity, a ß-γ coincidence technique is commonly used. Due to the presence of the gas matrix, such as stable xenon, nitrogen, helium, the self-attenuation effects should be taken into account when measuring different types of sample. In order to improve the accuracy of the measurement, the detection efficiencies of X-rays and γ-rays were derived by using a simulation gas calibration source with low density of sponge matrix. The detection efficiencies of ß-particles and conversion electrons (CEs) were calibrated by measuring radioxenon sample. The self-attenuation correction factors of X-rays and γ-rays were determined by Geant4 simulation method. The self-attenuation correction factors of ß-particles and CEs were provided by measuring the radioxenon samples with different volumes of xenon, nitrogen and helium.

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.

Computational and experimental optimization of 135Xe production in calibration sources.

Here we present a new method of irradiating 134Xe capsules to produce 135Xe gas standards which maximize the ratio of 135Xe to 133Xe production due to (n,g) and (n,2n) reactions, respectively. We performed "Spectral tuning" of the University of Utah TRIGA Reactor (UUTR) neutron spectrum to increase the length of time that 135Xe dominates undesirable 135Xe in the sample, so that the capsules - used for calibration and quality control testing of Xe gas detection equipment in support of the Comprehensive Test Ban Treaty (CTBT) - will remain viable for longer periods post-irradiation. Moreover, optimized methods of computation and analysis were developed yielding improved computational efficiency over standard Monte Carlo approaches. These methods provided valuable insight into the final design and manufacture of new, ex-core Teflon irradiation chambers tested in the UUTR. The methods of computation and analysis, as well as the physical irradiation chamber designs, were derived such that they could be readily applied to any reactor for spectral tuning of a specific reactor's flux profile. Results of the physical experiments employing the optimized irradiation chamber designs demonstrated sample viability time improvements of over 60% when compared to conventional, un-optimized methods of gas sample generation. Thus, use of these methods enhance both the CTBT-related calibrations and performance testing, and the continued stability of the CTBT monitoring network overall.

Using STAX data to predict IMS radioxenon concentrations.

The noble gas collection and measurement stations in the International Monitoring System (IMS) are heavily influenced by releases from medical isotope production facilities. The ability to reliably model the movement of radioxenon from the points of release to these IMS samplers has improved enough that a routine aspect of the analysis of IMS radioxenon data should be the prediction of the effect of releases from industrial nuclear facilities on the sample concentrations. Predicted concentrations at IMS noble gas systems in Germany and Sweden based on measured releases from Institute for Radioelements (IRE) in Belgium and atmospheric transport modeling for a four-month period are presented and discussed.

Uncertainty and source term reconstruction with environmental air samples.

Environmental air sampling is one of the principal monitoring technologies employed for the verification of the Comprehensive Nuclear-Test-Ban Treaty (CTBT). By combining the analysis of environmental samples with Atmospheric Transport and Dispersion Modelling (ATDM), and using a Bayesian source reconstruction algorithm, an estimate of the release location, duration, and quantity can be computed. Bayesian source reconstruction uses an uncertainty distribution of the input parameters, or priors, in a statistical framework to produce posterior probability estimates of the event parameters. The quality of the event reconstruction directly depends on the accuracy of the prior uncertainty distribution. With many of the input parameters, the selection of the uncertainty distribution is not difficult. However, with environmental samples, there is one component of the uncertainty at the interface between sample measurements and the ATDM that has been overlooked. Typically, a much smaller volume or quantity of material is sampled from the much larger domain represented in the ATDM. By examining the response of a dense network of radionuclide detectors on the West Coast of Canada during the passage of the Fukushima debris plume, an initial estimate of this uncertainty was determined to be between 20% and 30% depending on sample integration time.

Quantification of 37Ar emanation fractions from irradiated natural rock samples and field applications.

Underground-produced 37Ar can be used for underground nuclear explosions (UNE) detection and for groundwater dating. The quantification of the emanation, that is the fraction of activity produced in the rock that escapes to the pore space, is essential for predicting the background activity expected in natural environments. We propose an experiment in which artificial CaCO3 powder and natural rock particles are irradiated with neutrons in a routinely operated medical cyclotron, whose energy spectrum is experimentally measured. The produced activity was quantified and compared with the emanated activity to determine the emanating fraction. The results showed consistent and reproducible patterns with a dominance of the recoil process at small scales (<2 mm). We observed emanation values ≤1% with a dependency on the grain size and the inner geometry of particles. Soil weathering and the presence of water increased the recoil emanation. The atoms produced that were instantaneously recoiled in the intra- or inter-granular pore space left macroscopic samples by diffusion on timescales of days to weeks (Deff = 10-12 - 10-16 m2 s-1). This diffusive transport determines the activity that prevails in the fluid-filled pore space accessible for groundwater or soil gas sampling.

Projected network performance for multiple isotopes using next-generation xenon monitoring systems.

Since about 2000 (Bowyer et al., 1998), radioxenon monitoring systems have been under development and testing for the verification of the Comprehensive Nuclear Test-Ban Treaty (CTBT). Operation of the systems since then has resulted in development of a next-generation of systems that are nearly ready for operational deployment. By 2010, the need to screen out civilian sources was well known (Auer et al., 2010; Saey, 2009), and isotopic ratio approaches were soon considered (Kalinowski and Pistner, 2006) to identify specific sources. New generation systems are expected to improve the ability to verify the absence of nuclear tests by using isotopic ratios when multiple isotopes are detected. In this work, thousands of releases were simulated to compute the global detection probability of 131mXe, 133mXe, 133Xe, and 135Xe at 39 noble gas systems in the International Monitoring System (IMS) for both current and next-generation systems. Three release scenarios are defined at 1 h, 1 d, and 10 d past a 1 kt TNT equivalent 235U explosion event. Multiple cases using from one part in a million to the complete release of the xenon isotopic activity are evaluated for each scenario. Coverage maps and global integrals comparing current and next-generation monitoring systems are presented showing that next-generation noble gas systems will create measurable improvements in the IMS. The global detection probability for 133Xe is shown to be strong in all scenarios, but only modestly improved by next-generation equipment. However, the detection probability for 131mXe and 133mXe increased to about 50% in different scenarios, providing a second detectable isotope for many events. As anticipated from shorter sampling intervals, the expected number of detecting samples roughly doubled and the expected number of detecting stations rose by approximately 50% for all release scenarios. Thus, it might be anticipated that future events would consist of multiple 133Xe detections and one or more second isotope detections. Signals of this nature should increase detection confidence, tighten release location estimates, improve rejection of civilian signals, and lessen the impacts from individual systems being offline for maintenance or repair reasons.

SAUNA field - A sensitive system for analysis of radioxenon in soil gas samples.

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.

Assessment of a compton-suppressed spectrometer for measurement of radioactive xenon isotopes.

Airborne radionuclide monitoring is considered to be the most certain way to detect a clandestine nuclear weapon test. The activity concentration of radioxenon samples collected by the radionuclide stations of the International Monitoring System (IMS) for the Comprehensive Nuclear-Test-Ban Treaty (CTBT) is generally performed at the low-level, hence it is necessary to improve the detection sensitivity of the radioactivity measuring apparatus for radionuclide monitoring. The Compton-suppressed spectrometer (CSS) has the advantage of reducing the background and improving the sensitivity in the environmental level measurement. Therefore, the measurement of the relevant radioxenon sample at the environmental level is feasible by using CSS. To assess the performance of CSS for radioxenon measurements, the Compton-suppressed and unsuppressed spectra of the 133Xe and 127Xe samples have been acquired, and subsequently, the information of the full energy peaks (FEP) in the spectra were compared. The assessment indicates that CSS can provide high sensitivity, simple operation, and straightforward activity determination, and it can be regarded as an appropriate apparatus in the radioxenon measurement.

Modeling of fission and activation products in molten salt reactors and their potential impact on the radionuclide monitoring stations of the International Monitoring System.

Molten Salt Reactors (MSRs) are one of six Generation IV reactor designs currently under development around the world. Because of the unique operating conditions of MSRs, which include molten fuel and the continuous removal of gaseous fission products during operation, work was performed to model the production of activation and fission products and analyze the potential impact of emissions on the International Monitoring System (IMS) of the Comprehensive Nuclear-Test-Ban Treaty (CTBT). Simulations were performed to predict the production of IMS-relevant radionuclides in four MSR designs operating under two scenarios: (1) a sealed reactor with releases only during operational shutdown, and (2) continuous reprocessing or sparging of the fuel salt. From these production estimates the radioxenon and radioiodine signatures were extracted and compared to three current reactor designs (Boiling Water Reactor, Pressurized Water Reactor, High-Power Channel-Type Reactor). In cases where continuous reprocessing of the fuel salt occurred, both the radioxenon and radioiodine signatures were nearly indistinguishable from a nuclear explosion. Estimates were also made of the potential emission rate of radioxenon for three reactor designs and it was found that MSRs have the potential to emit radioxenon isotopes at a rate of 1015-8×1016 Bq/d for 133Xe, which may adversely affect nuclear explosion monitoring, if no abatement is used. An assessment was made of activation products using a candidate fuel salt (FLiBe) mixed with corrosion products for the Thorium Molten Salt Reactor (TMSR-LF1).

First clinical implementation of GammaTile permanent brain implants after FDA clearance.

PURPOSE: GammaTile cesium-131 (131Cs) permanent brain implant has received Food and Drug Administration (FDA) clearance as a promising treatment for certain brain tumors. Our center was the first institution in the United States after FDA clearance to offer the clinical use of GammaTile brachytherapy outside of a clinical trial. The purpose of this work is to aid the medical physicist and radiation oncologist in implementing this collagen carrier tile brachytherapy (CTBT) program in their practice. METHODS: A total of 23 patients have been treated with GammaTile to date at our center. Treatment planning system (TPS) commissioning was performed by configuring the parameters for the 131Cs (IsoRay Model CS-1, Rev2) source, and doses were validated with the consensus data from the American Association of Physicists in Medicine TG-43U1S2. Implant procedures, dosimetry, postimplant planning, and target delineations were established based on our clinical experience. Radiation safety aspects were evaluated based on exposure rate measurements of implanted patients, as well as body and ring badge measurements. RESULTS: An estimated timeframe of the GammaTile clinical responsibilities for the medical physicist, radiation oncologist, and neurosurgeon is presented. TPS doses were validated with published dose to water for 131Cs. Clinical aspects, including estimation of the number of tiles, treatment planning, dosimetry, and radiation safety considerations, are presented. CONCLUSION: The implementation of the GammaTile program requires collaboration from multiple specialties, including medical physics, radiation oncology, and neurosurgery. This manuscript provides a roadmap for the implementation of this therapy.

A new method for analysis of beta-gamma radioxenon spectra.

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.

Will 37Ar emissions from light water power reactors become an obstacle to its use for nuclear explosion monitoring?

37Ar is a promising candidate for complementing radioxenon isotopes as indicators of underground nuclear explosions. This study evaluates its potential anthropogenic background caused by emissions from commercial pressurized water reactors. Various 37Ar production pathways, which result from activation of 36Ar and of 40Ca, respectively, are identified and their emissions quantified. In-core processes include (1) the restart of operation and degassing of the primary cooling water after maintenance and refueling shutdown, (2) the replacement of primary coolant water for limiting its tritium concentrations, and (3) the leakage of 37Ar produced from calcium impurities in UO2 after fuel rod failures. Activation of air and of calcium in concrete within the biological shield are major out-of-core production pathways. Whereas emissions from in-core processes are transient, a rather constant 37Ar source term results from its out-of-core production. Generic atmospheric dispersion simulations indicate that already at moderate distances from the emitter, concentrations of 37Ar caused by routine reactor operations are far below its cosmogenic background in air. The only exception results from an inadvertent reactor re-start without operation of the primary cooling water degassing system for prolonged time. Such an event also causes high emissions of 41Ar which can be used for discriminating its 37Ar signal from an underground nuclear explosion.

Cavity-melt partitioning of refractory radionuclides and implications for detecting underground nuclear explosions.

Isotopic ratios of radioxenon captured in the atmosphere can be indicators of the occurrence of an underground nuclear explosion. However, civilian sources of xenon isotopes, such as medical isotope production facilities and nuclear reactors, can interfere with detection of signals associated with nuclear testing, according to a standard model of the evolution of radioxenon isotopic abundances in a nuclear explosion cavity. We find that this standard model is idealized by not including the effects of physical processes resulting in the partitioning of the radionuclide inventory between a gas phase and rock melt created by the detonation and by ignoring seepage or continuous leakage of gases from the cavity or zone of collapse. Application of more realistic assumptions about the state of the detonation cavity results in isotopic activity ratios that differ from the civilian background more than the idealized standard model suggests, while also reducing the quantity of radioxenon available for atmospheric release and subsequent detection. Our simulations indicate that the physical evolution of the detonation cavity during the post-detonation partitioning process strongly influences isotopic evolution in the gas phase. Collapse of the cavity potentially has the greatest effect on partitioning of the refractory fission products that are precursors to radioxenon. The model allows for the possibility that post-detonation seismicity can be used to predict isotopic evolution.