Impacts of future nuclear power generation on the international monitoring system.

Many countries are considering nuclear power as a means of reducing greenhouse gas emissions, and the IAEA (IAEA, 2022) has forecasted nuclear power growth rates up to 224% of the 2021 level by 2050. Nuclear power plants release trace quantities of radioxenon, an inert gas that is also monitored because it is released during nuclear explosive tests. To better understand how nuclear energy growth (and resulting Xe emissions) could affect a global nonproliferation architecture, we modeled daily releases of radioxenon isotopes used for nuclear explosion detection in the International Monitoring System (IMS) that is part of the Comprehensive Nuclear Test-Ban Treaty: 131mXe, 133Xe, 133mXe, and 135Xe to examine the change in the number of potential radioxenon detections as compared to the 2021 detection levels. If a 40-station IMS network is used, the potential detections of 133Xe in 2050 would range from 82% for the low-power scenario to 195% for the high-power scenario, compared to the detections in 2021. If an 80-station IMS network is used, the potential detections of 133Xe in 2050 would range from 83% of the 2021 detection rate for the low-power scenario to 209% for the high-power scenario. Essentially no detections of 131mXe and 133mXe are expected. The high growth scenario could lead to a 2.5-fold increase in 135Xe detections, but the total number of detections is still small (on the order of 1 detection per day in the entire network). The higher releases do not pose a health issue, but better automated methods to discriminate between radioactive xenon released from industrial sources and nuclear explosions will be needed to offset the higher workload for people who perform the monitoring.

Set up and test of an anticoincidence system for the detection of radioactive xenon by gamma spectrometry system.

The aim of this work is based on the optimisation of a gamma spectrometry system in anticoincidence for the detection of noble gases, in particular the radioactive isotopes of xenon. These four radionuclides are of particular interest for the Comprehensive Nuclear Test-Ban Treaty (CTBT). The Laboratory of the ENEA Research Centre of Brasimone, where the experimental apparatus has been set up to carry out the measurements of 131mXe, 133Xe, 133mXe and 135Xe, is able to provide, if necessary, data and analysis on noble gases. The apparatus provides for the sampling of outdoor air, the passage through filters and in activated carbons maintained at cryogenic temperatures to allow xenon absorption. Finally, gas extraction and xenon volumes are analyzed by means of gas chromatography and a thermal conductivity detector. At the end of the extraction an aluminium cylinder containing radioxenon is analyzed by high resolution gamma spectroscopy using a High Purity Germanium Detector P-type. The signals produced by the interaction of cosmic rays with the crystal have been recognized as the main cause of the increase of the detector background because they give rise to the Compton continuum and, as a result, they affect the value of the minimum detectable activity (MDA). In order to overcome this effect, a system in anticoincidence has been developed using two plastic scintillators, placed over the shielding of the HPGe detector, which send pulses recording within a time delay window located in the germanium multichannel analyzer: at the time the signal arrives from the scintillator, the gate blocks data acquisition to avoid recording pulses generated by cosmic radiation. For both configurations of the system (with and without the anticoincidence apparatus operating) the energy, and efficiency calibrations have been carried out using a certified multigamma-ray calibration source to assess the performance.

Phase II testing of Xenon International on Mount Schauinsland, Germany.

Station RN33 on Mount Schauinsland near Freiburg, Germany, is part of the International Monitoring System monitoring radioxenon in air (131mXe, 133Xe, 133mXe, and 135Xe) for verification of the Comprehensive Nuclear Test Ban Treaty. Here, we present data from phase II testing of a new system, Xenon International at RN33, July 14th, 2021 to Jan 22nd, 2022, together with SPALAX data from the same time period. Radioxenon could be detected in 473 of 719 samples, among them many multiple isotope detections. Activity concentrations of spiked and selected environmental samples were verified by laboratory reanalysis. The sensitivity of Xenon International for radioxenons is up to one order of magnitude better for the metastable isotopes than that of the SPALAX, with a shorter sampling duration of 6 h.

First STAX detector installation at the National Institute for Radioelements (IRE).

The Source Term Analysis of Xenon (STAX) project has been installing stack detectors at medical isotope production facilities to measure radioxenon emissions to investigate the effect of radioxenon releases on nuclear explosion monitoring. This paper outlines the installation of the first STAX detection system at the National Institute for Radioelements (IRE) in Fleurus, Belgium which has been operating for over three years and transferring collected data to the STAX repository. Information about the equipment installed, the data flow established, and calculations for determination of radioxenon releases from the facility are presented. Data quality was investigated to confirm values reported by STAX automated data processing and in a comparison of collected STAX data with data collected by IRE for regulatory reporting.

Source Term Analysis of Xenon (STAX): An effort focused on differentiating man-made isotope production from nuclear explosions via stack monitoring.

An overview of the hardware and software developed for the Source Term Analysis of Xenon (STAX) project is presented which includes the data collection from two stack monitoring systems installed at medical isotope production facilities, infrastructure to transfer data to a central repository, and methods for sharing data from the repository with users. STAX is an experiment to collect radioxenon emission data from industrial nuclear facilities with the goal of developing a better understanding of the global radioxenon background and the effect industrial radioxenon releases have on nuclear explosion monitoring. A final goal of this work is to utilize collected data along with atmospheric transport modeling to calculate the contribution of a peak or set of peaks detected by the International Monitoring System (IMS) to provide desired discriminating information to the International Data Centre (IDC) and National Data Centers (NDCs). Types of data received from the STAX equipment are shown and collected data was used for a case study to predict radioxenon concentrations at two IMS stations closest to the Institute for RadioElements (IRE) in Belgium. The initial evaluation of results indicate that the data is very valuable to the nuclear explosion monitoring community.

Effect of dentine site on resin and cement adaptation tested using X-ray and electron microscopy to evaluate bond durability and adhesive interfaces.

Glass ionomer (GI) cements and self-etch (SE) or universal adhesives after etching (ER) adapt variably with dentine. Dentine characteristics vary with depth (deep/shallow), location (central/peripheral), and microscopic site (intertubular/peritubular). To directly compare adhesion to dentine, non-destructive imaging and testing are required. Here, GI, ER, and SE adapted at different dentine depths, locations, and sites were investigated using micro-CT, xenon plasma focused ion beam scanning electron microscopy (Xe PFIB-SEM), and energy dispersive X-ray spectroscopy (EDS). Extracted molars were prepared to deep or shallow slices and treated with the three adhesives. Micro-CT was used to compare changes to air volume gaps, following thermocycling, and statistically analysed using a quantile regression model and Fisher's exact test. The three adhesives performed similarly across dentine depths and locations, yet no change or overall increases and decreases in gaps at all dentine depths and locations were measured. The Xe PFIB-SEM-milled dentine-adhesive interfaces facilitated high-resolution characterization, and element profiling revealed variations across the tooth-material interfaces. Dentine depth and location had no impact on adhesive durability, although microscopic differences were observed. Here we demonstrate how micro-CT and Xe PFIB-SEM can be used to compare variable dental materials without complex multi-stage specimen preparation to minimize artefacts.

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.

Determining the source of unusual xenon isotopes in samples.

Three unusual radioactive isotopes of xenon-125Xe, 127Xe, and 129mXe-have been observed during testing of a new generation radioxenon measurement system at the manufacturing facility in Knoxville, Tennessee. These are possibly the first detections of these isotopes in environmental samples collected by automated radioxenon systems. Unfortunately, the new isotopes detected by the Xenon International sampler can interfere with quantification of the radioactive xenon isotopes used to monitor for nuclear explosions. Xenon International sampling data collected during February through September 2020 were combined with an atmospheric transport model to identify the possible release location. A source-location analyses using sample counts dominated by 125Xe strongly supports the conclusion that the release point is near (within 20 km) the sampler location. Wind patterns are not consistent with releases coming from more distant nuclear power plants. The High Flux Isotope Reactor (HFIR) and the Spallation Neutron Source (SNS) at Oak Ridge National Laboratory are located in the region of most likely source locations. The source-location analysis cannot rule out either facility as a release location, and some of the samples may contain a combination of releases from both facilities. The source-location results using 125Xe are not unexpected because Klingberg et al. (2013) previously published the production rate of radioactive xenon isotopes from neutron activation of stable xenon in the air at the HFIR. Up to 1012 Bq of 125Xe could be produced per operational day and other xenon isotopes would be produced in lesser quantities.

Deep-mantle krypton reveals Earth's early accretion of carbonaceous matter.

Establishing when, and from where, carbon, nitrogen and water were delivered to Earth is a fundamental objective in understanding the origin of habitable planets such as Earth. Yet, volatile delivery to Earth remains controversial1-5. Krypton isotopes provide insights on volatile delivery owing to their substantial isotopic variations among sources6-10, although pervasive atmospheric contamination has hampered analytical efforts. Here we present the full suite of krypton isotopes from the deep mantle of the Galápagos and Iceland plumes, which have the most primitive helium, neon and tungsten isotopic compositions11-16. Except for 86Kr, the krypton isotopic compositions are similar to a mixture of chondritic and atmospheric krypton. These results suggest early accretion of carbonaceous material by proto-Earth and rule out any combination of hydrodynamic loss with outgassing of the deep or shallow mantle to explain atmospheric noble gases. Unexpectedly, the deep-mantle sources have a deficit in the neutron-rich 86Kr relative to the average composition of carbonaceous meteorites, which suggests a nucleosynthetic anomaly. Although the relative depletion of neutron-rich isotopes on Earth compared with carbonaceous meteorites has been documented for a range of refractory elements1,17,18, our observations suggest such a depletion for a volatile element. This finding indicates that accretion of volatile and refractory elements occurred simultaneously, with krypton recording concomitant accretion of non-solar volatiles from more than one type of material, possibly including outer Solar System planetesimals.

Real-Time Measurement of Xenon Concentration in a Binary Gas Mixture Using a Modified Ultrasonic Time-of-Flight Anesthesia Gas Flowmeter: A Technical Feasibility Study.

BACKGROUND: Xenon (Xe) is an anesthetic gas licensed for use in some countries. Fractional concentrations (%) of gases in a Xe:oxygen (O2) mixture are typically measured using a thermal conductivity meter and fuel cell, respectively. Speed of sound in such a binary gas mixture is related to fractional concentration, temperature, pressure, and molar masses of the component gases. We therefore performed a study to assess the feasibility of developing a novel single sterilizable device that uses ultrasound time-of-flight to measure both real-time flowmetry and fractional gas concentration of Xe in O2. METHODS: For the purposes of the feasibility study, we adapted an ultrasonic time-of-flight flowmeter from a conventional anesthetic machine to additionally measure real-time fractional concentration of Xe in O2. A total of 5095 readings of Xe % were taken in the range 5%-95%, and compared with simultaneous measurements from the gold standard of a commercially available thermal conductivity Xe analyzer. RESULTS: Ultrasonic measurements of Xe (%) showed agreement with thermal conductivity meter measurements, but there was marked discontinuity in the middle of the measurement range. Bland-Altman analysis (95% confidence interval in parentheses) yielded: mean difference (bias) 3.1% (2.9%-3.2%); lower 95% limit of agreement -4.6% (-4.8% to -4.4%); and upper 95% limit of agreement 10.8% (10.5%-11.0%). CONCLUSIONS: The adapted ultrasonic flowmeter estimated Xe (%), but the level of accuracy is insufficient for clinical use. With further work, it may be possible to develop a device to perform both flowmetry and binary gas concentration measurement to a clinically acceptable degree of accuracy.

Design and development of radioactive xenon gas purification and analysis system based on molecular sieves.

The dynamic adsorption of xenon on molecular sieve packed columns was investigated. The modified Wheeler-Jonas equation was used to describe adsorption parameters such as adsorption capacity and adsorption rate coefficient. Different experimental conditions were accomplished to study their effects and to touch appropriate adsorbing circumstances. Respectable consistency was reached between experimental and modeled values. A purification and analysis setup was developed for radioactive xenon gas determination. Standard sample analysis results approved acceptable quantification accuracy.

Elucidation of transformation pathway of ketoprofen, ibuprofen, and furosemide in surface water and their occurrence in the aqueous environment using UHPLC-QTOF-MS.

The identification and determination of transformation products (TPs) of pharmaceuticals is essential nowadays, in order to track their fate in the aqueous environment and, thus, to estimate the actual pollution. However, this is a challenging task due to the necessity to apply high-resolution instruments enable to detect known and unknown compounds. This work presents the use of liquid chromatography quadrupole time-of-flight mass spectrometry (LC-QTOF-MS) as a powerful tool for the identification of three selected pharmaceuticals, furosemide (FUR), ibuprofen (IBP), and ketoprofen (KET), and their TPs in various water samples. Laboratory degradation experiments were performed using xenon lamp as a source of the irradiation in order to simulate phototransformation processes which may occur in the environment. Furthermore, the photodegradation kinetics of three selected compounds were assessed in a reactor equipped with xenon lamp in river water samples. Five TPs of IBP, seven of KET, and five of FUR were identified; some of them are presented here for the first time. Accurate mass measurements and fragmentation pattern obtained during an LC-QTOF-MS analysis allowed for structure elucidation of TPs followed by the creation of transformation pathway of selected pharmaceuticals. Finally, different water samples (wastewater influent and effluent, river water, untreated and treated water) were analyzed in order to estimate the presence of parent and transformed compounds. Only KET was detected in untransformed form in considered samples. Most of the TPs of selected drugs were found at least once in all water samples. Although IBP and FUR were not present in water samples as parent compounds, their different TPs occur. A great potential of LC-QTOF-MS in the identification and structural elucidation of TPs in the environment, allowing the recognition of the fate of pharmaceuticals in the environment through the determination of transformation pathway, has been presented.

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

Observations made in April 2013 of the radioxenon isotopes (133)Xe and (131m)Xe 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 (131m)Xe 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.

Inference and analysis of xenon outflow curves under multi-pulse injection in two-dimensional chromatography.

Multidimensional gas chromatography is widely applied to atmospheric xenon monitoring for the Comprehensive Nuclear-Test-Ban Treaty (CTBT). To improve the capability for xenon sampling from the atmosphere, sampling techniques have been investigated in detail. The sampling techniques are designed by xenon outflow curves which are influenced by many factors, and the injecting condition is one of the key factors that could influence the xenon outflow curves. In this paper, the xenon outflow curves of single-pulse injection in two-dimensional gas chromatography has been tested and fitted as a function of exponential modified Gaussian distribution. An inference formula of the xenon outflow curve for six-pulse injection is derived, and the inference formula is also tested to compare with its fitting formula of the xenon outflow curve. As a result, the curves of both the one-pulse and six-pulse injections obey the exponential modified Gaussian distribution when the temperature of the activated carbon column's temperature is 26°C and the flow rate of the carrier gas is 35.6mLmin(-1). The retention time of the xenon peak for one-pulse injection is 215min, and the peak width is 138min. For the six-pulse injection, however, the retention time is delayed to 255min, and the peak width broadens to 222min. According to the inferred formula of the xenon outflow curve for the six-pulse injection, the inferred retention time is 243min, the relative deviation of the retention time is 4.7%, and the inferred peak width is 225min, with a relative deviation of 1.3%.

Deep fracture fluids isolated in the crust since the Precambrian era.

Fluids trapped as inclusions within minerals can be billions of years old and preserve a record of the fluid chemistry and environment at the time of mineralization. Aqueous fluids that have had a similar residence time at mineral interfaces and in fractures (fracture fluids) have not been previously identified. Expulsion of fracture fluids from basement systems with low connectivity occurs through deformation and fracturing of the brittle crust. The fractal nature of this process must, at some scale, preserve pockets of interconnected fluid from the earliest crustal history. In one such system, 2.8 kilometres below the surface in a South African gold mine, extant chemoautotrophic microbes have been identified in fluids isolated from the photosphere on timescales of tens of millions of years. Deep fracture fluids with similar chemistry have been found in a mine in the Timmins, Ontario, area of the Canadian Precambrian Shield. Here we show that excesses of (124)Xe, (126)Xe and (128)Xe in the Timmins mine fluids can be linked to xenon isotope changes in the ancient atmosphere and used to calculate a minimum mean residence time for this fluid of about 1.5 billion years. Further evidence of an ancient fluid system is found in (129)Xe excesses that, owing to the absence of any identifiable mantle input, are probably sourced in sediments and extracted by fluid migration processes operating during or shortly after mineralization at around 2.64 billion years ago. We also provide closed-system radiogenic noble-gas ((4)He, (21)Ne, (40)Ar, (136)Xe) residence times. Together, the different noble gases show that ancient pockets of water can survive the crustal fracturing process and remain in the crust for billions of years.

The total release of xenon-133 from the Fukushima Dai-ichi nuclear power plant accident.

The accident at the Fukushima Dai-ichi nuclear power plant (FD-NPP) on 11 March 2011 released large amounts of radioactivity into the atmosphere. We determine the total emission of the noble gas xenon-133 ((133)Xe) using global atmospheric concentration measurements. For estimating the emissions, we used three different methods: (i) using a purely observation-based multi-box model, (ii) comparisons of dispersion model results driven with GFS meteorological data with the observation data, and (iii) such comparisons with the dispersion model driven by ECMWF data. From these three methods, we have obtained total (133)Xe releases from FD-NPP of (i) 16.7 ± 1.9 EBq, (ii) 14.2 ± 0.8 EBq, and (iii) 19.0 ± 3.4 EBq, respectively. These values are substantially larger than the entire (133)Xe inventory of FD-NPP of about 12.2 EBq derived from calculations of nuclear fuel burn-up. Complete release of the entire (133)Xe inventory of FD-NPP and additional release of (133)Xe due to the decay of iodine-133 ((133)I), which can add another 2 EBq to the (133)Xe FD-NPP inventory, is required to explain the atmospheric observations. Two of our three methods indicate even higher emissions, but this may not be a robust finding given the differences between our estimates.

Measurement of radon and xenon binding to a cryptophane molecular host.

Xenon and radon have many similar properties, a difference being that all 35 isotopes of radon ((195)Rn-(229)Rn) are radioactive. Radon is a pervasive indoor air pollutant believed to cause significant incidence of lung cancer in many geographic regions, yet radon affinity for a discrete molecular species has never been determined. By comparison, the chemistry of xenon has been widely studied and applied in science and technology. Here, both noble gases were found to bind with exceptional affinity to tris-(triazole ethylamine) cryptophane, a previously unsynthesized water-soluble organic host molecule. The cryptophane-xenon association constant, K(a)=42,000 ± 2,000 M(-1) at 293 K, was determined by isothermal titration calorimetry. This value represents the highest measured xenon affinity for a host molecule. The partitioning of radon between air and aqueous cryptophane solutions of varying concentration was determined radiometrically to give the cryptophane-radon association constant K(a)=49,000 ± 12,000 M(-1) at 293 K.

Myocardial blood flow during general anesthesia with xenon in humans: a positron emission tomography study.

BACKGROUND: Xenon has only minimal hemodynamic side effects and induces pharmacologic preconditioning. Thus, the use of xenon could be an interesting option in patients at risk for perioperative myocardial ischemia. However, little is known about the effects of xenon anesthesia on myocardial blood flow (MBF) and coronary vascular resistance in humans. METHODS: Myocardial blood flow was noninvasively quantified by H2¹5O positron emission tomography in six healthy volunteers (age: 38 ± 8 yr). MBF was measured at baseline and during general anesthesia induced with propofol and maintained with xenon, 59 ± 0%. Absolute quantification of MBF was started after the calculated plasma concentration of propofol had decreased to less than 1.5 µg · ml⁻¹. RESULTS: Compared with baseline (MBFbaseline, 1.03 ± 0.09 ml · min⁻¹ · g⁻¹; mean ± SD), MBF was decreased insignificantly by xenon (MBFxenon, 0.80 ± 0.22 ml · min⁻¹ · g⁻¹; -21%, P = 0.11). Xenon decreased the rate-pressure product (RPP; heart rate × systolic arterial pressure), an indicator of cardiac work and myocardial oxygen consumption (-15%, P < 0.04). When correcting for the RPP, the decrease in MBF observed during xenon anesthesia was reduced to -9% (MBFcorr-xenon, 1.42 ± 0.28 ml · g⁻¹ · mmHg⁻¹ vs. MBFcorr-baseline, 1.60 ± 0.28 ml · g⁻¹ · mmHg⁻¹, P = 0.32). Xenon did not affect the dependency of MBF on the RPP. Coronary vascular resistance did not significantly change (+15 ± 23%, P = 0.18) during xenon anesthesia. CONCLUSIONS: In healthy subjects, xenon has only minimal effects on coronary flow dynamics. These effects are probably of indirect nature, reflecting the decrease in myocardial oxygen consumption induced by the effects of xenon anesthesia on cardiac work.

Spatially uniform calibration of a liquid xenon detector at low energies using (83m)Kr.

A difficult task with many particle detectors focusing on interactions below approximately 100 keV is to perform a calibration in the appropriate energy range that adequately probes all regions of the detector. Because detector response can vary greatly in various locations within the device, a spatially uniform calibration is important. We present a new method for calibration of liquid xenon (LXe) detectors, using the short-lived (83m)Kr. This source has transitions at 9.4 and 32.1 keV, and as a noble gas like Xe, it disperses uniformly in all regions of the detector. Even for low source activities, the existence of the two transitions provides a method of identifying the decays that is free of background. We find that at decreasing energies, the LXe light yield increases, while the amount of electric field quenching is diminished. Additionally, we show that if any long-lived radioactive backgrounds are introduced by this method, they will present less than 67x10(-6) events kg(-1) day(-1) keV(-1) in the next generation of LXe dark matter direct detection searches.

Scalable synthesis of cryptophane-1.1.1 and its functionalization.

Cryptophanes, cage molecules for which xenon exhibits a high affinity, are good candidates for xenon biosensing. Cryptophane-1.1.1 (1) exhibits the highest binding constant for xenon encapsulation in organic solution determined to date. This property suggests that the cryptophane-1.1.1 core (1) is optimal for sensing applications. A high-yielding scalable synthesis of compound 1 is reported as well as an easy way to functionalize it.