The Comprehensive Nuclear Test Ban Treaty verification regime mandates atmospheric monitoring for the four radioxenon isotopes that are produced in high abundance in a nuclear explosion: [superscript 131m]Xe, [superscript 133m]Xe, [superscript 133g]Xe, and [superscript 135g]Xe. This mandate has driven the development of improved xenon detectors, including a phoswich detector, which has potential to replace the ARSA detector in the International Monitoring System. In this experiment, the four relevant radioxenon isotopes were produced through neutron activation and the phoswich detector was used to attain spectra from the gas. Spectral characteristics and resolution of the phoswich spectra were compared to an ARSA-type [beta]-[gamma] coincidence detector to perform an overall evaluation of the phoswich detector. The results indicated that spectral characteristics and resolutions for the phoswich were comparable to the ARSA-type detector, with slightly improved beta detection. As an additional test of the new detector's capabilities, a tailored spectrum designed to mimic a nuclear explosion signature was produced and analyzed with the detector. / text

For verifying the Comprehensive Nuclear-Test-Ban Treaty (CTBT), different monitoring technologies (seismic, infrasound, hydroacoustic, and radionuclide detection) are combined. The monitoring of radioactive xenon isotopes is one of the principal methods for the determination of the nuclear nature of an explosion. After an underground nuclear detonation the radioxenon isotopes [superscript 131m]Xe, [superscript 133m]Xe, ¹³³Xe, and ¹³⁵Xe, and the radioargon isotope ³⁷Ar have an increased probability of detection. In order to effectively utilize these isotopes as indicators of nuclear testing, an accurate background must be calculated. This work examines the fission products produced by spontaneous fission of ²³⁸U, which is naturally present in the earth's crust, and of ²⁴⁰Pu which is present as a product of nuclear weapons and nuclear reactor accidents. These calculations provide a range of production values for radioxenon in a variety of geologies as well as at various historic locations. The activation of geologic calcium and potassium by cosmic ray neutrons is considered for a variety of properties effecting the neutron flux. These calculations provide a range of radioargon production values across a selection of geologies. The impact of latitude and the solar activity cycle are also examined. In order to examine the transport of the isotopes through soil a model of the transport of xenon and argon through various geologies was developed. This model incorporates both the introduction of xenon from the atmosphere and that produced by spontaneous fission. This is then considered in light of what might be observed in an on-site inspection (OSI). What this work finds is that the radioxenon natural background does exceed detection limits in particular locations and geologies, however, a careful examination of the location and the ideal sampling depths can minimize the impact during an OSI. Radioargon, however, has a much larger natural background at shallow depths which are the realm of OSI sampling. Should radioargon sampling be used in an OSI the sampling time is crucial in distinguishing a nuclear explosion from the natural background. In some scenarios the natural background production of radioargon may be sufficient to interfere with the detection of an underground nuclear weapon test. This information may be beneficial in the development of future OSI noble gas monitoring techniques. / text

Atmospheric monitoring of radionuclides as part of the International Monitoring System requires the capability to differentiate between a radionuclide signature emanating from peaceful nuclear activity and one emanating from a well-contained underground nuclear explosion. While the radionuclide signatures of nuclear weapons are generally well known, radionuclides must first pass through hundreds of meters of earth to reach the surface where they can be detected and analyzed. Less well known is the affect that subsurface vertical transport has on the isotopic signatures of nuclear explosions. In this work, a model is developed, and tested, simulating the detonation of a simple underground nuclear explosion and the subsequent vertical transport of resulting radioxenon to the surface. First, the fast-fission burn of a fissile spherical core surrounded by a layer of geologic media is modeled, normalized to 1 kton total energy. The resulting source term is then used in the testing and evaluation of the constructed vertical transport model, which is based on the double-porosity model of underground fluid transport driven by barometric pumping. First, the ability of the vertical transport code to effectively model the underground pressure response from a varying surface pressure is demonstrated. Next, a 100-day simulation of the vertical migration of a static source is examined, and the resulting cumulative outflow of roughly 1% initial inventory outflow per cycle is found to closely follow the analytical predictions. Finally, calculated radioxenon source terms are utilized to model the resulting vertical transport and subsequent surface outflow. These results are found to be consistent with the physical expectations of the system, and lastly a cursory sensitivity analysis is conducted on several of the physical parameters of the model. The result is that the vertical transport model predicts isotopic fractionation of radioxenon that can potentially lie outside of currently accepted standard bounds. / text

This thesis investigates the ability of transparent surface coatings to reduce xenon diffusion into plastic scintillators. The motivation for the work is improved radioxenon monitoring equipment, used with in the framework of the verification regime of the Comprehensive Nuclear-Test-Ban Treaty. A large part of the equipment used in this context incorporates plastic scintillators which are in direct contact with the radioactive gas to be detected. One problem with such setup is that radioxenon diffuses into the plastic scintillator material during the measurement, resulting in an unwanted memory effect consisting of residual activity left in the detector. In this work coatings of Al2O3 and SiO2, with thicknesses between 20 and 400 nm have been deposited onto flat plastic scintillator samples, and tested with respect to their Xe diffusion barrier capabilities. All tested coatings were found to reduce the memory effect, and 425 nm of Al2O3 showed the most promise. This coating was deposited onto a complete detector. Compared to uncoated detectors, the coated one presented a memory effect reduction of a factor of 1000. Simulations and measurements of the expected light collection efficiency of a coated detector were also performed, since it is important that this property is not degraded by the coating. It was shown that a smooth coating, with a similar refractive index as the one of the plastic, should not significantly affect the light collection and resolution. The resolution of the complete coated detector was also measured, showing a resolution comparable to uncoated detectors. The work conducted in this thesis proved that this coating approach is a viable solution to the memory effect problem, given that the results are reproducible, and that the quality of the coating is maintained over time.

The significance of the radioxenon memory effect in the context of the International Monitoring System of the Comprehensive Nuclear-Test-Ban Treaty is introduced as motivation for the project. Existing work regarding xenon memory effect reduction and thin film diffusion barriers is surveyed. Experimental techniques for radioxenon production and exposure, as well as for thin film deposition on plastic by plasma enhanced chemical vapor deposition (PECVD), are detailed. A deposition rate of 76.5 nm min⁻¹ of SiO₂ is measured for specific PECVD parameters. Relative activity calculations show agreement within 5% between identically exposed samples counted on parallel detectors. Memory effect reductions of up to 59±1.8% for 900 nm SiO₂ films produced by plasma enhanced chemical vapor deposition and of up to 77±3.7% for 50 nm Al₂O₃ films produced by atomic layer deposition are shown. Future work is suggested for production of more effective diffusion barriers and expansion to testing in operational monitoring stations. / text

This thesis investigates surface coatings as xenon diffusion barriers on plastic scintillators. The motivation for the work is improved radioxenon detection systems, used within the verification regime of the Comprehensive Nuclear-Test-Ban Treaty (CTBT). One type of radioxenon detection systems used in this context is the Swedish SAUNA system. This system uses a cylindrical plastic scintillator cell to measure the beta decay from radioxenon isotopes. The detector cell also acts as a container for the xenon sample during the measurement. One problem with this setup is that part of the xenon sample diffuses into the plastic scintillator material during the measurement, resulting in residual activity left in the detector during subsequent measurements. This residual activity is here referred to as the memory effect. It is here proposed, and demonstrated, that it is possible to coat the plastic scintillator material with a transparent oxide coating, working as a xenon diffusion barrier. It is found that a 425 nm Al2O3 coating, deposited with Atomic Layer Deposition, reduces the memory effect by a factor of 1000, compared an uncoated detector. Furthermore, simulations show that the coating might also improve the light collection in the detector. Finally, the energy resolution of a coated detector is studied, and no degradation is observed. The focus of the thesis is measurements of the diffusion barrier properties of Al2O3 films of different thicknesses deposited on plastic scintillators, as well as an evaluation of the expected effect of a coating on the energy resolution of the detector. The latter is studied through light transport simulations. As a final step, a complete coated plastic scintillator cell is evaluated in terms of memory effect, efficiency and energy resolution. In addition, the xenon diffusion process in the plastic material is studied, and molecular dynamics simulations of the Xe-Al2O3 system are performed in order to investigate the reason for the need for a rather thick coating to significantly reduce the memory effect.

When a nuclear explosion occurs certain radionuclides are emitted, notably xenon. Due to the fact that xenon is a noble gas, it is hard to contain and can therefore be detected far from the explosion site. There are four isotopes of xenon that are of interest in the detection of a nuclear explosion: 131mXe, 133mXe, 133Xe and 135Xe. By constantly measuring the amount of these isotopes in the air, changes in the concentration in an indication that a nuclear explosion has occurred. In this thesis a detector was modelled in GEANT4 and focuses on one kind of noble gas detector: SAUNA - the Swedish Automatic Unit for Noble gas Acquisition. SAUNA uses the coincidence technique in order to determine the concentration of xenon there is in the air. By using the coincidence technique, it is possible to reduce the impact of the background radiation and therefore increase the efficiency of the detector. 133Xe has a coincidence when it first undergoes beta decay, with an endpoint energy of 346 keV, and then emits a 80 keV gamma particle. 135Xe has also a dual coincidence, a beta decay with an endpoint energy of 910 keV together with a 250 keV gamma-ray. However both these isotopes have a triple coincidence decay that also can be exploited: for 133Xe, a beta particle with endpoint energy of 346 keV, a 30 keV X-ray and a 45 keV conversion electron, while for 135Xe there is instead of the gamma particle a 30 keV X-ray and a 214keV conversion electron that can be emitted together with the beta particle. The 30 keV X-ray together with the beta particle for 133Xe can also be used as a dual coincidence, in that case the conversion electron is ignored. For 133Xe, when a beta particle, a 45 keV conversion electron, and a 30 keV X-ray are emitted, the model was able to detect all three particles in 69.2% ± 0.1 of the cases. However, when only the particles with a detected energy within a 5 keV interval of their generated energies are considered to be in coincidence, then for 133Xe triple coincidence occurs in 22.9% ± 0.2 of the cases. For 135Xe the model was able to detect the triple coincidence (between a beta, 214 keV CE and 30 keV X-ray) in 63.5% ± 0.1 of the cases. This work shows that adding another particle in a coincidence reduces the chance to detect the coincidence. The positive effect of adding another particle in a coincidence is that the minimum detectable concentration of xenon should be smaller. The goal for future detectors should be to make it possible for the detector to take advantage of the triple coincidences but at the same time be also able to use the dual coincidences.

Dans le cadre du Traité d'Interdiction Complète des Essais Nucléaires (TICE), le Système de Surveillance International (SSI) a été développé. Ce réseau consiste en plusieurs centaines de stations de mesures dont le rôle est de détecter la signature d'un essai nucléaire clandestin. Quatre types de mesures sont effectués: sismique, hydro-acoustique, infrason et radionucléide. Dans le cas particulier d'un essai nucléaire souterrain, seule la mesure des radionucléides est adéquate pour mettre en évidence le caractère nucléaire de l'explosion. Quatre radionucléides du xénon sont produits en masse lors d'un essai nucléaire: le 131m-Xe, le 133m-Xe, le 133-Xe, et le 135-Xe. Une faible proportion de ces gaz parvient à diffuser à travers les fissures de la cavité et se retrouver dans l'atmosphère. A cause de la dilution atmosphérique, les concentrations de ces quatre radionucléides sont extrêmement faibles et par conséquent difficiles à détecter. De plus, le bruit de fond atmosphérique ne cesse d'augmenter car ces gaz radioactifs sont également produits et relâchés par les usines de production de radio-isotopes médicaux et les centrales nucléaires. Afin de renforcer le réseau de surveillance, le CEA-DAM a proposé de développer un système de détection des radionucléides du xénon ultra-compact et mobile, afin de pouvoir effectuer des mesures de vérification directement sur site suspect, et ainsi contourner la contrainte de dilution atmosphérique. Ces travaux présentent le développement et l'optimisation de ce système. Le système a d'abord été modélisé sur ordinateur et ses performances en terme d'efficacité de détection ont été simulées par méthode de Monte-Carlo avec le logiciel Geant4. Les mesures se font en utilisant la technique de mesure en coïncidences électron/photon. En parallèle, une chaîne d'acquisition ultra-compacte a été développée, ainsi qu'un réseau de communication permettant de synchroniser en temps les différents spectromètres numériques utilisés pour le traitement du signal (protocole IEEE 1588 PTP). Les concentrations minimales détectables de ce système sont inférieures à 5 mBq/m³ pour une acquisition de 12 h, et ce pour les quatre radionucléides du xénon d'intérêt. / As part of the Comprehensive nuclear Test Ban Treaty (CTBT), an International Monitoring System (IMS) has been developed. This network consists of several hundred measuring stations whose role is to detect the signatures of a clandestine nuclear test. Four types of measurements are carried out: seismic, hydroacoustic, infrasound and radionuclide. In the particular case of an underground nuclear test, only the radionuclide measurement is adequate to detect the explosion and quantify its yield. Four xenon radionuclides with long half-lives are produced during a nuclear test: the 131m-Xe, the 133m-Xe, the 133-Xe and the 135-Xe. A small proportion of these gases may diffuse through the cracks in the cavity and end up in the atmosphere. Due to atmospheric dilution, the concentrations of these four radionuclides are extremely low and therefore difficult to detect. In addition, atmospheric background continues to increase as these radioactive gases are also produced by medical radioisotope facilities and nuclear power plants. In order to strengthen the IMS, the CEA-DAM has proposed to develop an ultra-compact and mobile system for detecting xenon radionuclides, in order to be able to carry out verification measurements directly on site, and thus to avoid the problem of atmospheric dilution. This work presents the development and optimization of this system. The system was first modelled on a computer and its performances in terms of detection efficiency were simulated by the Monte-Carlo method using Geant4 software. Measurements are made in electron-photon coincidence mode. In parallel, an ultra-compact acquisition chain has been developed, as well as a communication network to synchronize in time the various digital spectrometers used for signal processing (IEEE 1588 PTP protocol). The minimum detectable concentrations of this system are less than 5 mBq/m³ for a 12 h acquisition, for the four xenon radionuclides of interest.