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Incorporating civilian radioxenon background estimates in anomaly detection

A nuclear explosion screening exercise in 2023 (Maurer et al., 2023) found challenges with discerning anomalous radioxenon activity concentrations relative to elevated background concentrations. Research has continued into methods to detect anomalous radioxenon concentrations by comparing samples to estimates of atmospheric radioxenon background concentrations caused by releases at nuclear reactors or medical isotope production facilities. A new approach estimates the sample concentrations using time-varying radioxenon release rates obtained using optimization techniques that constrain the facility release rates to plausible amounts based on historical data or facility knowledge. The purpose of the optimization is to determine whether any combination of plausible release rates from emitting facilities can explain a series of radioxenon measurements at one or more sampling stations. A case study uses radioxenon data collected at three locations in western Europe for a month in 2021 and considers releases from 77 locations. Fewer samples are identified as being anomalous using a simplistic flagging rule than from an application of the current International Monitoring System (IMS) activity concentration-level rule.

Environmental sciences

Analysis of measurements from an array of radioxenon samplers near to Hartlepool Nuclear Power Station

As part of a scientific research and development project, the radionuclide fingerprint of an operating advanced gas-cooled reactor 25 (AGR) has been studied across several facets (Goodwin et al., 2024). One part of this project was to deploy an array of 26 radioxenon samplers to the region for a period of around 1 year, to measure any radioxenon emissions from the reactors of the 27 Hartlepool nuclear power station at a range of tens of kilometres away. The array of 3 sensors was operational for around 12 28 months from March 2022 and detected many occurrences of isotopes of radioxenon. Here we provide a detailed analysis and 29 interpretation of the data and where possible, attribution of detections to a source or region. Whilst a key part of this work is to 30 measure any emissions of radioxenon from Hartlepool, this work presents one of the most comprehensive efforts to determine the 31 source of a great number of (mostly) 133Xe detections. A combination of different types of atmospheric dispersion modelling 32 techniques, including the use of stack monitoring data from nearby civil radioxenon-emitting nuclear facilities has enabled the 33 majority of detections to be attributed to one or more possible sources. Whilst emissions from Hartlepool have been detected on 34 the systems, the majority of detections are associated with a medical isotope production facility in Fleurus, Belgium (IRE).

Advanced gas-cooled reactor

A flow-through gamma detection system for sub-surface radioxenon tracer measurements in LYNM PE1

A continuous flow-through, real-time radioxenon sensor array has been designed to monitor either 127 Xe or 133 Xe tracer gas as part of a series of underground chemical explosions in the Low-Yield Nuclear Monitoring (LYNM) Physics Experiment 1 (PE1). The sensors are pairs of shielded thallium-doped sodium iodide gamma-ray detectors that surround a gas measurement chamber. Each measurement chamber is connected to a sampling location in the geology surrounding the chemical explosion or in the access tunnel. The first experiment in the series, PE1 A, occurred in 2023 and the system quantified the 127 Xe tracer gas in the gas sampling lines for four weeks following the experiment execution. The array generated a set of radioxenon concentration time series with a 15-minute resolution that will be used to refine subsurface gas transport models.

Gamma-ray coincidence detection

Measurements of radioxenon activities during periods of gaseous release from an advanced gas-cooled reactor

Activities of radioxenon isotopes are reported from an Advanced Gas-cooled Reactor (AGR) during periods of gaseous release. Xenon isotopes are relevant to the monitoring regime of the Comprehensive Nuclear-Test-Ban Treaty (CTBT). These releases may affect detections from the International Monitoring System (IMS) by influencing the radioxenon background. Time series activity plots have been produced from both in-core monitoring and direct measurement at the point of release using a stack monitor system. Ratio plots using both data sets have been produced with results compared with a commonly chosen nuclear explosion “discrimination line.” The reported results improve the understanding of radionuclide emissions from civil nuclear power plants. This work is being performed as part of the Xenon Environmental Nuclide Analysis at Hartlepool (XENAH) collaboration between the Atomic Weapons Establishment (AWE, UK), EDF Energy (UK), Pacific Northwest National Laboratory (PNNL, USA), and the Swedish Defence Research Agency (FOI).

22 GENERAL STUDIES OF NUCLEAR REACTORS

A target for production of radioxenons

A liquid cesium target has been developed which permits the production and identification of the neutron deficient isotopes of xenon. The thick target yields of Xe-127 and Xe-129 m were measured for proton energies between 28 and 40 MeV. Production of Xe-129 m, as indicated by the presence of a 196 keV line in the gamma ray spectra, occurred at all proton energies; Xe-127 was produced at proton energies above 33 MeV. Both accumulated on the target with the same time constant, and the cross sections were comparable in magnitude. The radioxenons were removed from the target by a stream of carrier gas so that chemical separation was unnecessary.

Blue, J. W.

A target for production of radioxenons

A liquid cesium target has been developed which allows the production and separate identification of the neutron deficient isotopes of xenon. The present report describes irradiations utilizing 34 to 41 MeV protons to produce millicurie quantities of Xe-127 and Xe-129m. At higher energies, however, the target could be used without modification to produce xenon isotopes as light as 119.

Blue, J. W.

127 Xe quantification method development and intercomparison exercise

Monitoring of the atmosphere for fission products ( 131m Xe, 133m Xe, 133 Xe, and 135 Xe) is performed by various laboratories to detect nuclear explosions. Quantification of 127 Xe is not routinely performed by laboratories measuring atmospheric radioxenon because it is not a fission product. 127 Xe was recently detected by a ground-based beta-gamma air monitoring system. When measured using beta-gamma coincidence detector systems, such as those in use on the International Monitoring System (IMS) of the Comprehensive Nuclear-Test-Ban Treaty (CTBT), 127 Xe can interfere with the quantification of fission product radioxenon due to overlap of the 127 Xe beta-gamma coincidence signatures with those of fission product radioxenon. Here, this work demonstrates quantification of 127 Xe at different laboratories with different measurement techniques. Production and purification of 127 Xe was performed by neutron activation of enriched 126 Xe. The purified 127 Xe was then split between laboratories, and detection and quantification methods were developed. At Idaho National Laboratory, a quantification method involving high purity germanium detectors was devised that included self-attenuation correction. At AWE, a beta-gamma coincidence counting method, as used in support of the IMS, was modified to enable the measurement and analysis of the 127 Xe samples. Corrections were made for self-attenuation, which showed a strong xenon volume dependency, for some coincidence signatures. The gas sample activity concentration was used as the comparison metric and it showed excellent agreement between the methods.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P

Computational Optimization of 133m Xe Production via Neutron Irradiation in a TRIGA Reactor

Here, the Comprehensive Nuclear-Test-Ban Treaty bans all nuclear tests worldwide. As part of treaty compliance, the concentration of radioactive nuclides in the atmosphere is monitored to detect nuclear weapons tests. Radioactive noble gas fission products, specifically radioxenon, can vent into the atmosphere after a nuclear weapons test, even if the test is well contained underground or underwater. Radioxenon thus serves as a signal for nuclear weapons tests. All atmospheric monitoring systems require samples of radioxenon isotopes for detector calibration, quality control, and certification. Here, we present a novel, improved method for creating samples of 133m Xe via neutron irradiation of 132 Xe in the Washington State University TRIGA reactor. 132 Xe neutron absorption results in either 133 Xe or 133m Xe—thermal neutron absorption results in 133m Xe 12% of the time, while fast neutron absorption (above ~1 MeV) results in 133m Xe ~50% of the time. To optimize the production of 133m Xe via neutron absorption in 132 Xe in the thermal TRIGA reactor, spectral tuning using an irradiation chamber is required to maximize the fraction of fast neutrons being absorbed and minimize the number of thermal neutrons interacting with the 132 Xe. We used MCNP to tally 132 Xe absorptions with the isotopic tally function, flux tallies and neutron attenuation to estimate the number of neutrons reaching the 132 Xe through the irradiation chamber, and the adjoint importance function to improve the source strength estimate. Additionally, we performed a heat transfer analysis for safety considerations. It was determined that the use of a 96% enriched 10 B boron carbide chamber, placed next to the fuel elements in reactor position D8, increases the 133m Xe/ 133 Xe activity ratio from a baseline value of 0.3 to 1.0, a 233% increase. Additionally, it was determined that the alpha heating produced in the boron does not become an unmanageable problem in the Washington State University reactor.

37 - INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL C

Explosive Byproduct Gas Transport Through Sorptive Geomedia

Current underground nuclear explosion (UNE) detection strategies rely heavily on atmospheric noble gas sampling of radioxenon. However, discriminating nuclear weapons testing programs from civilian sources is difficult due to highly variable atmospheric radioxenon backgrounds and processes affecting subsurface transport of parent radionuclides. Here, we aim to study the transport of gases produced by subsurface explosions as novel stable signatures for underground nuclear explosion (UNE) monitoring. These gases may be produced in large quantities with distinct molecular ratios, which will be impacted by subsurface transport processes. To demonstrate how ratios of gases produced by explosions can change during transport in geomaterials, we conducted laboratory benchtop experiments on the transport of carbon dioxide (CO 2 ) and hydrogen (H 2 ) gases through variably saturated zeolitic tuff, which is abundant at the historic US testing site. We observed that zeolitic tuff sorbs substantial quantities of CO 2 while allowing H 2 to transport more freely, leading to changes in the molecular ratios of the two gases along the transport pathway. Gas uptake in the dry zeolitic tuff core was 72.3% for CO 2 , compared with 53.4% for xenon and 7.6% for H 2 . The presence of 20% water saturation disrupted the CO 2 sorption process, though to a lesser extent than observed for noble gases, with a 36.7% drop in xenon sorption compared with a 21.9% drop for CO 2 . These results represent the first observations of zeolite sorption altering explosive gas ratios during transport through geomedia relevant to nuclear proliferation monitoring.

54 ENVIRONMENTAL SCIENCES

Preferential adsorption of noble gases in zeolitic tuff with variable saturation: A modeling study of counter-intuitive diffusive-adsorptive behavior

Noble gas transport through geologic media has important applications in the prediction and characterization of measured gas signatures related to underground nuclear explosions (UNEs). Retarding processes such as adsorption can cause significant species fractionation of radionuclide gases, which has implications for measured and predicted signatures used to distinguish radioxenon originating from civilian nuclear facilities or from UNEs. Accounting for the effects of variable water saturation in geologic media on tracer transport is one of the most challenging aspects of modeling gas transport because there is no unifying relationship for the associated tortuosity changes between different rock types, and reactive transport processes such as adsorption that are affected by the presence of water likewise behave differently between gas species. In this study, we perform numerical diffusive-adsorptive transport simulations to estimate gas transport parameters associated with bench-scale laboratory diffusion cell experiments measuring breakthrough in zeolitic and non-zeolitic rocks for a gaseous mixture of xenon, krypton, and SF 6 at varying degrees of water saturation (S w ). Counter-intuitive transport behavior was observed in the zeolitic rock experiments whereby breakthrough concentrations were significantly higher when the core was partially saturated (S w = 17 %) than under dry (S w = 0 %) conditions. Breakthrough of xenon was especially retarded in the dry core – likely due to comparatively high affinity of xenon for zeolitic adsorption sites – and estimated effective diffusion coefficients for all gases were approximately an order of magnitude lower than what is predicted by porosity-tortuosity models. We propose the counter-intuitive behavior observed is because water infiltration of zeolite nanopores reduces both the adsorptive capacity of the rock and the tortuosity of connected flow paths. We developed a two-site competitive kinetic Langmuir adsorption reaction for the porous media transport simulator in order to constrain transport parameters within zeolitic tuff, where differential adsorption to zeolite and non-zeolite pores was observed. We determined that liquid saturation-dependent diffusive-adsorptive transport is affected by subtle and at times competing processes that are specific to different gases, which have a significant overall influence on effective transport parameters.

58 GEOSCIENCES

A statistical approach to screening isotopic signatures in monitoring for underground nuclear explosions

The ability to differentiate between atmospheric radionuclide signatures from underground nuclear explosions (UNEs) and signals from other sources, such as medical isotope-production facilities and nuclear reactors, can be critical to the detection and monitoring of unannounced, low-yield nuclear events. Signatures having anomalously high amplitudes, compared to background levels, remain the best indicator in screening for a UNE. However, isotopic composition can further validate a suspected UNE signature, but separation from any atmospheric background composition is first necessary. To date, evaluating the challenges of performing this separation has typically involved comparing an observed background with a highly idealized deterministic model of radioxenon signature production by a UNE that does not consider the influence of post-detonation chemical/physical processes in the detonation cavity or the subsequent gas transport mechanisms that can also affect the isotopic composition of the detected gas signature. In addition, purely deterministic models, as previously employed, overlook the uncertainty inherent in estimating critical parameters characterizing the UNE and its detonation environment. In this paper, we create detailed, multi-parameter models of radionuclide evolution using the widely accepted England and Rider post-detonation radionuclide decay-chain network coupled to detailed models simulating physical production and transport processes affecting the gas signature. Because these models are governed by uncertain parameters including barometric fluctuations, realistic ranges of variation for each of the parameters influencing isotopic composition are then defined. A Latin-Hypercube sampling approach is used to obtain a random distribution of isotopic production and gas transport results associated with a given value of each parameter. We apply these results to background histories of two stations, one providing 4-isotope background measurements and the other providing two-isotope measurements associated with the 2013 DPRK announced UNE.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P

Deployment of portable, modular gas samplers as part of an atmospheric tracer experiment

Underground nuclear explosions release noble gases into the atmosphere that can be detected to support international monitoring efforts. Atmospheric transport models help predict the movement of these gases over long distances, but struggle to predict the movement in the atmosphere local to the release. A field experiment was designed to monitor the movement of 127 Xe within a 5-km radius. Four gas samplers were deployed as part of this experiment to collect atmospheric samples at various distances from the release point. In conclusion, these samples were then analyzed in a near-field lab using a NaI detector and in an off-site lab using gamma-gamma coincidence and beta-gamma coincidence counting.

Radioxenon

Detecting 127 Xe in an atmospheric tracer experiment

The Xcounts algorithm for calculating air concentrations of radioactive xenon isotopes (Eslinger et al., 2023) has been extended to estimate 127 Xe in addition to 131m Xe, 133m Xe, 133 Xe, and 135 Xe. The algorithm was applied to 119 samples collected with a SAUNA Q B system (Ringbom et al., 2023) during a two-month atmospheric tracer release experiment. Finally, the algorithm identified two samples with 127 Xe present from a single 1.5 h release about 3.5 km upwind of the sampler and no false detections of 127 Xe were observed in the other samples.

127Xe calibration

Analysis of 127 Xe tracer measurements using a net counts method

A suite of measurement systems were deployed as part of the Physical Experiment 1 series of experiments, which involved detonating chemical explosives along with radionuclide tracers in an underground cavity, at the Nevada National Security Site (NNSS) in the United States. One of the radionuclide tracers, 127 Xe was released from the containment following the explosion and detected on a SAUNA Q B sampler situated approximately 3.5 km away. The system uses a beta-gamma coincidence detector system to measure fission product radioisotopes of xenon relevant to nuclear explosion monitoring. In this work we use the coincidence measurement data to analyse and interpret the results from the SAUNA Q B system, to calculate the measured 127 Xe activity concentration(s).

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P

Influence of background sources and topographic resolution in the Weather Research and Forecasting Model on xenon plume characteristics at monitoring stations

For many atmospheric monitoring applications, networks of measurement sites—such as the radionuclide stations of the International Monitoring System—can be sparse. With measurement locations potentially hundreds to thousands of kilometers from a release it is important to quantify the effects of physical processes on transport and dispersion of plumes between source and measurement locations. This study addresses the effects of background sources and topography resolution near the release location of radionuclides. We use the Weather Research and Forecasting (WRF) model with inline chemistry to investigate (1) how an additional, time-varying source of 133 Xe, such as an operational medical isotope production facility, contributes to activity concentration measurements at monitoring sites, and (2) how complex topography influences on atmospheric conditions near emission sources impact plume concentrations at varying distances from the source. Two 133 Xe emission sources, including (1) a high flux rate of short duration representing an explosive event, and (2) a variable and continuous background source, are simulated. The continuous background source contributes significantly to total 133 Xe concentrations at several monitoring stations. Further, a WRF simulation at 9 km horizontal resolution is compared with a nested grid simulation, where the innermost domain has a resolution of 1 km. Increased topographic resolution leads to an improved representation of plume responses to local winds, with topographic influences greatest at locations closest to the sources. Differences between the two domain resolutions decrease at greater distances from the sources, as plumes have time to spread and mix and are influenced by synoptic scale circulation patterns that are represented similarly in both simulations.

54 ENVIRONMENTAL SCIENCES