SuperNEMO est un projet de détecteur de nouvelle génération pour la recherche de la décroissance double bêta sans émission de neutrinos. La technique expérimental déployée est dans la lignée du son prédécesseur NEMO3, combinant un trajectographe et un calorimètre, afin d’identifier non seulement les électrons des décroissances double bêta, mais également pour mesurer l’ensemble des composantes de bruit de fond du détecteur. Le projet vise ainsi une sensibilité de 10^26 ans sur la période du 82Se, ce qui permettrait de sonder une masse effective du neutrino de 50 meV. Pour atteindre cette sensibilité, le projet prévoit notamment de mettre en place un calorimètre composé d’un millier de compteur à scintillation de basse radioactivité, dont la résolution en énergie serait meilleure que 8 % FWHM pour des électrons de 1 MeV.Ce travail de thèse apporte une contribution importante dans les travaux de Recherche et Développements pour améliorer les performances des scintillateurs et photomultiplicateurs, et pour réduire leur radioactivité, avec notamment la conception d’un nouveau photomultiplicateur en collaboration avec Photonis. / SuperNEMO is a next generation double beta decay experiment which will extend the successful “tracko-calo” technique employed in NEMO 3. The main characteristic of this type of detector is to identify not only double beta decays, but also to mesure its own background components. The projet aims to reach a sensitivity up to 1026 years on the half-life of 82Se. One of the main challenge of the Research and Development is to achieve an unprecedented energy resolution for the electron calorimeter, better than 8 % FWHM at 1 MeV.This thesis contributes to improve scintillators and photomultiplicators performances and reduce their radioactivity, including in particular the development of a new photomultiplier in collaboration with Photonis.

This thesis describes the measurement technique of fast-neutron tomography for assessing spatial distributions of steam and water in two-phase flows. This so-called void distribution is of importance both for safe operation and for efficient use of the fuel in light water reactors, which compose the majority of the world’s commercial nuclear reactors. The technique is aimed for usage at thermal-hydraulic test loops, where heated two-phase flows are being investigated under reactor-relevant conditions. By deploying portable neutron generators in transmission tomography, the technique becomes applicable to stationary objects, such as thermal-hydraulic test loops. Fast neutrons have the advantage of high transmission through metallic structures while simultaneously being relatively sensitive to the water/void content. However, there are also challenges, such as the relatively low yield of commercially available fast-neutron generators, the tendency of fast neutrons to scatter in the interactions with materials and the relatively low efficiency encountered in fast-neutron detection. The thesis describes the design of a prototype instrument, FANTOM, which has been assembled and demonstrated. The main design parameters have been optimized to achieve maximal signal count rate in the detector elements, while simultaneously reaching an image unsharpness of ≤0.5 mm. Radiographic projections recorded with the assembled instrument are presented, and the performance parameters of FANTOM are deduced. Furthermore, tomographic reconstruction methods for axially symmetric objects, which is relevant for some test loops, have been developed and demonstrated on measured data from three test objects. The attenuation distribution was reconstructed with a radial resolution of 0.5 mm and an RMS error of 0.02 cm-1, based on data recorded using an effective measurement time of 3.5 hours per object. For a thermal-hydraulic test loop, this can give a useful indication of the flow mode, but further development is desired to improve the precision of the measurements. Instrument upgrades are foreseen by introducing a more powerful neutron generator and by adding detector elements, speeding up the data collection by several orders of magnitude and allowing for higher precision data. The requirements and performance of an instrument for assessment of arbitrary non-symmetric test loops is discussed, based on simulations.

The importance of gamma-ray spectroscopy – the science of determining the distribution of energy in a gamma field – can rarely be overstated. High performance scintillators for gamma-ray spectroscopy in Nuclear Nonproliferation applications and homeland security require excellent energy resolution to distinguish neighboring element and isotope lines while minimizing the time and exposure to do so. Semiconductor detectors operate by converting incident photons directly into electrical pulses, but often have problems of high costs due to constituent segregation and surface states as is the case for Cadmium Zinc Telluride. The ideal scintillator material for gamma spectrometer will therefore requires high light yield, excellent proportionality between light yield and gamma photon energy, and material uniformity. A scintillator should possess the following properties; it should convert the kinetic energy of the generated charged particles (typically K-shell electrons) into detectable visible light. This conversion should be linear-the light yield should be proportional to deposited energy over as wide a range as possible. For good light collection, the medium should be transparent to the wavelength of its own emission. The decay time of the induced luminescence should be short so that fast signal pulses can be generated. The medium should be of good optical quality and subject to manufacture in sizes large enough to be of interest as a practical detector. Its index of refraction should be near that of glass (~1.5) to permit efficient coupling of scintillation light to a photomultiplier tube or other photo-sensor. In the past decade, inorganic scintillator research has focused less on improving the characteristics of known scintillators, but rather on the search for new hosts capable of fast response and high energy resolution. Extensive searches have been made for hosts doped with lanthanide activators utilizing the allowed 5d-4f transition. These 5d-4f transitions are dipole-allowed and thus are about 106 times stronger than the more frequently observed 4f-4f transition in the trivalent rare earth ions. Ce3+, Nd3+ and Pr3+ have been investigated for fast response applications while Ce3+, Eu2+ and Yb2+ stand out as the most promising activators offering high light yield, and high energy resolution. Using a modified Bridgman growth technique we have grown crystals with a low energy resolution of 2.6% at 662 keV, which is lower than the previous 2.8% reported for SrI2:Eu2+. The modified technique (called so for its vertical crystal growth orientation) is necessary due to the anisotropic thermal expansion coefficient of Strontium Iodide. The problem plaguing the growth of the crystal is spontaneous cracking, which usually appear during cooling in the bulk. With the use of a zone separating shield, one can achieve more control of the temperature gradient between the two zones without compromising the actual temperature of the two zones. Additionally the use of codopants, in particular divalent magnesium improved the crystalline quality by acting as a gathering for iodine ions, which led to reduction of defect density.

The starting SNO+ experiment, successor to the Sudbury Neutrino Observatory, is a neutrino detector using LAB based liquid scintillator as active medium. Situated in the SNOLab deep underground laboratory in Sudbury, Canada, the rock overburden amounts to about 6 km.w.e., providing an effective shielding against cosmic rays. The residual muon rate is 63 μ/day going through the detector volume. About 780 t of an LAB mixture inside an acrylic sphere with a 6 m radius will be observed by ≈ 9300 photomultipliers, surrounded by a ≈ 7000 t water shielding. SNO+ will be searching for low energy solar-, geo-, reactor- and supernova neutrinos, but the main goal is the observation of the neutrinoless double beta decay in Te-130. Under operating conditions, the scintillator will be cooled to about 12° C. This work investigated the effect of temperature changes on the light output of LAB based liquid scintillator in a range from -5° C to 30° C with α-particles and electrons in a small scale setup. Assuming a linear behaviour, a combined negative temperature coefficient of (−0.29 ± 0.01) %/° C is found. Considering hints for a particle type dependency, electrons show (−0.17 ± 0.02) %/° C whereas the temperature dependency seems stronger for α-particles (−0.35 ± 0.03) %/° C. A pulse shape analysis shows increased strength of a slow decay component at lower temperatures, pointing to reduced non-radiative triplet state de-excitations at lower temperatures. Furthermore, this work found upper bounds for the in-situ muon-induced isotope production via scaling calculations and simulations with Geant4 based software. For the most concerning isotope C-11, an upper limit of about 1.3 × 10^3 decays/kt/yr is found and a reduction technique, developed by the Borexino collaboration, can be effectively applied for SNO+. Also a muon reconstruction algorithm is implemented, performing reasonably well, but not good enough to improve the background reduction scheme. / Das zukünftige SNO+ experiment, Nachfolger des Sudbury Neutrino Observatory, ist ein Neutrino-Detektor mit LAB basierten Flüssigszintillator als aktivem Medium. Im SNOLab Untertagelabor (Sudbury, Kanada) gelegen, ist es durch die Felsüberdeckung von 6 km.w.e. hervorragend gegen kosmische Strahlung abgeschirmt. Die Rate der übrigen Myonen die das Detektorvolumen durchdringen beträgt ca. 63 μ/Tag. In einer Acrylkugel, mit einem Radius von 6 m, wird eine LAB Mischung von ≈ 9300 Photomultipliern beobachtet und von einer Wasserabschirmung von ≈ 7 kt umgeben. SNO+ wird nach niederenergetischen solaren-, Geo-, Reaktor- und Supernova Neutrinos suchen, aber das Hauptziel ist die Beobachtung von neutrinolosen doppelten Betazerfällen in Te-130. Unter den Betriebsbedingungen wird der Flüssigszintillator eine Temperatur von ca. 12° C annehmen. Diese Arbeit hat den Einfluss von Temperaturveränderungen in einem Bereich von -5° C to 30° C auf die erzeugte Lichtmenge untersucht. Dazu wurden α-Teilchen und Elektronen in einem kleineren Versuchaufbau beobachtet. Unter der Annahme eines linearen Verhaltens, wurde ein globaler negativer Temperaturkoeffizient von (−0.29 ± 0.01) %/° C gefunden. Unter Berücksichtigung von Hinweisen auf eine Teilchenartabhängigkeit, findet sich für Elektronen ein Koeffizient von (−0.17 ± 0.02) %/° C, wohingegen α-Teilchen eine stärkere Abhängikeit von (−0.35 ± 0.03) %/° C aufweisen. Eine Pulsformanalyse zeigt eine bei tieferen Temperaturen stärker ausgeprägte langsame Zerfallskomponente, was darauf hinweist dass die nicht-radiativen Abregungen der Triplet-Zustände bei niedrigeren Temperaturen reduziert sind. Weiterhin wurden in dieser Arbeit obere Ausschlußgrenzen für in-situ Myon-induzierte Isotopenproduktion gefunden, wozu Skalierungsrechnungen und Simulation mit auf Geant4 basierender Software benutzt wurden. Für das wichtigste Isotop C-11 wurde eine obere Grenze von 1.3 × 10^3 Ereignisse/kt/Jahr gefunden und eine Technik zur Reduzierung des Untergrundes, entwickelt von der Borexino Kollaboration, kann effektiv für SNO+ angewendet werden. Darüber hinaus wurde eine Myon Spurrekonstruktion implementiert, die sinnvolle Ergebnisse liefert, aber nicht gut genug ist um die Untergrund Reduzierung zu unterstützen.

O conhecimento preciso do espectro energético de fótons é de extrema importância na radioterapia no que se refere à escolha adequada das doses a que os pacientes são submetidos. Os dados de saída dos detectores de radiação são apenas espectros de altura de pulso (PHD), ao invés de espectros de energia, que correspondem a informações distorcidas sobre a fonte e seus decaimentos devido a diversos erros associados ao processo de cintilação do cristal e à eletrônica. Os resultados medidos foram obtidos com o uso de um detector cintilador de NaI(Tl) e as simulações Monte Carlo foram feitas com o uso do programa EGSnrc. A partir das características do detector obtidas experimentalmente, nossas simulações puderam ser validadas para se aproximarem o mais próximo possível do caso real em laboratório. Dessas medidas experimentais de fontes radioativas de calibração e simulações, foi montada uma matriz resposta inversa que transforma PHD em espectro de energia de fótons. Uma vez que a faixa energética das fontes radioativas medidas teve um limite de 1.6MeV, a matriz resposta também o apresenta, mas que pode ser contornado de acordo com a geometria usada para a obtenção do PHD a ser corrigido. Observa-se que a resposta do detector é diretamente proporcional à energia e assim, dependendo da energia incidente a ser estudada, dois tipos de matriz resposta inversa podem ser aplicadas. Os resultados desta transformação de PHD para espectro de energia de fótons são apresentados. / The accurate knowledge of the photon energy spectrum in radiotherapy is of extremely importance when it comes to the appropriate choice for doses whose patients are submitted. The output data from the radiation detectors is described as pulse high distributions, instead of energy spectra, that correspond to distorted information about the source and its decays due to many errors associated to the crystal scintillation process and the electronics. The measured results were obtained with a NaI(Tl) scintillation detector and Monte Carlo simulations were performed by the EGSnrc program. From the detector characteristics obtained experimentally, the simulations were validated so they could approximate the more real as possible as in laboratory. Using these simulated and experimental calibration sources, an inverse response matrix was built and transforms pulse high distributions in photons energy spectrum. Once the correction energy limit due to the radiation sources used is approximately 1.6 MeV, so the response matrix has a limit, but it can be overcame by the beam incident angle and the geometry used when the pulse high distributions to be corrected is going to be measured. One can realize that the detector response is directly proportional to the incident energy and, when it is intense as in a LINAC or weak as in a calibration source, different types of matrix can be applied. The results from these transformations are presented.

Les progrès réalisés dans la maîtrise de la physique et de la détection des neutrinos ouvrent aujourd'hui la porte à la physique appliquée des antineutrinos. Dans cette optique, cette particule a en effet la particularité fondamentale de porter l'information de son lieu d'émission sans perturbation. Comme les neutrinos sont liés aux processus faibles tels que la désintégration nucléaire beta les applications se trouvent dans la surveillance des matières radioactives et des réacteurs nucléaires. Dans ce contexte, le projet Nucifer vise à construire et opérer un détecteur miniature d'antineutrinos de réacteur nucléaire, à installer au maximum à quelques dizaines de mètres d'un réacteur de puissance pour suivre sa puissance thermique et évaluer la quantité de plutonium produite. De plus, une réanalyse récente des mesures précédentes réalisées à proximité de réacteurs ces 40 dernières années montrent un écart significatif entre les taux de détection neutrinos attendus et mesurés. Parmi les hypothèses variées qui permettent d'expliquer cette anomalie se trouve une nouvelle oscillation entre neutrinos, impliquant nécessairement l'existence d'un quatrième neutrino, stérile. Pour mettre en évidence les antineutrinos et mesurer leur énergie, la détection beta inverse dans environ 850 kg de liquide scintillant dopé au gadolinium est utilisée. Toute la difficulté expérimentale provient des bruits de fond, qui peuvent être très importants lorsque le détecteur est installé ) proximité du réacteur ou de la surface. Le détecteur est maintenant intégré sur le réacteur nucléaire de recherche Osiris du CEA, situé à Saclay, et a commencé la prise de données en avril 2012. Malheureusement, une faible longueur d'atténuation du liquide et un niveau de bruit de fond gamma inattendu nous empêchent de distinguer les neutrinos. Nous attendons maintenant le remplacement du liquide et la construction d'un nouveau mur de plomb pour continuer l'étude du suivi du réacteur et pour tester l'hypothèse de neutrino stérile. / The major advances done in the understanding of neutrinos properties and in detector technology have opened the door to a new discipline: the Applied Antineutrino Physics. Indeed, this particle has the great advantage to carry information from its emission place without perturbation. Because neutrinos are inextricably linked to nuclear processes, new applications are in nuclear safeguards. In this context, the Nucifer project aims to test a small electron-antineutrino detector to be installed a few 10 meters from a reactor core for monitoring its thermal power and for testing the sensitivity to the plutonium content. Moreover, recent re-analysis of previous short-distance reactor-neutrino experiments shows a significant discrepancy between measured and expected neutrino count rates. Among the various hypotheses a new phenomenon as the existence of a fourth sterile neutrino can explain this anomaly. To be able to count neutrinos and get the corresponding energy spectrum, the detection is based on the inverse beta decay in about 850 kg of doped liquid scintillator. The experimental challenge is to operate such a small detector in a high background place, due to the closeness with the surface and the reactor radiations. The detector is now finished and data taking has begun at the Osiris research reactor in Saclay since april 2012. Sadly, unexpected low liquid attenuation length and high gamma background level prevented us to highlight neutrinos. We are now waiting for a liquid change and a new lead wall to study reactor monitoring and to test the sterile neutrino hypothesis.

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.

It has been shown that neutrons emitted from the same 252Cf fission event are preferentially detected within small angles of each other and at angles around 180 degrees. The distribution of this angular anisotropy is dependent upon the nuclide emitting the neutrons. Coincident neutrons can be detected from a shielded source, so a study of the angular anisotropy between coincident neutrons is useful for this context. This could allow for the dynamic determination of the ratio of the rate of (alpha,n) neutron production to the spontaneous fission neutron production (designated alpha) used in neutron coincidence counting for safeguards. This could also be used to identify neutron emitting isotopes in a homeland security application. An angular frequency distribution for coincident neutrons was produced via experiments using an array of cylindrical liquid scintillators and a 252Cf source. It was found, in accordance with previous experiments, that the angular frequency distribution peaks at small angles and at angles around 180 degrees. A Monte Carlo, physics-based simulation program was created to simulate the distribution of angles between neutrons from the same fission event from 252Cf and 240Pu sources. The resulting distributions were clearly distinguishable from each other. The code was benchmarked to measured results from a 252Cf source at Lawrence Livermore National Laboratory. Knowledge of the unique angular distributions of coincident neutrons from various fissioning sources is useful for identification and verification purposes. Another practical application of angular anisotropy information for coincident neutrons from a given source is determining the ratio of the (alpha,n) to spontaneous fission rates for a source undergoing neutron coincidence counting. The utility of this was verified by using measurements made by faculty and students of the University of Michigan Nuclear Engineering Department for a MOX fuel pin at the Joint Research Center in Ispra, Italy. Good agreement between the predicted and declared values for alpha was found.

In recent years, the United States Departments of Homeland Security (DHS) and Customs and Border Protection (CBP) have been charged with the task of scanning every cargo container crossing domestic borders for illicit radioactive material. This is accomplished by using gamma-ray detection systems capable of discriminating between non-threatening radioisotopes, such as Cs-137, which is often used in nuclear medicine, and fissile material, such as U-238, that can be used to make nuclear weapons or "dirty" bombs. Scintillation detector systems, specifically thallium-doped sodium iodide (NaI(Tl)) single crystals, are by far the most popular choice for this purpose because they are inexpensive relative to other types of detectors, but are still able to identify isotopes with reasonable accuracy. However, increased demand for these systems has served as a catalyst for the research and development of new scintillator materials with potential to surpass NaI(Tl). The focus of a majority of recent scintillator materials research has centered on sintered transparent ceramics, phosphor-doped organic matrices, and the development of novel single crystal compositions. Some of the most promising new materials are glass-ceramic nanocomposites. By precipitating a dense array of nano-scale scintillating crystals rather than growing a single monolith, novel compositions such as LaBr₃(Ce) may be fabricated to useful sizes, and their potential to supersede the energy resolution of NaI(Tl) can be fully explored. Also, because glass-ceramic synthesis begins by casting a homogeneous glass melt, a broad range of geometries beyond the ubiquitous cylinder can be fabricated and characterized. Finally, the glass matrix ensures environmental isolation of the hygroscopic scintillating crystals, and so glass-ceramic scintillators show potential to serve as viable detectors in alpha- and neutron-spectroscopy in addition to gamma-rays. However, for the improvements promised by glass-ceramics to become reality, several material properties must be considered. These include the degree of control over precipitated crystallite size, the solubility limit of the glass matrix with respect to the scintillating compounds, the variation in maximum achievable light yield with composition, and the peak wavelength of emitted photons. Studies will focus on three base glass systems, sodium-aluminosilicate (NAS), sodium-borosilicate (NBS), and alumino-borosilicate (ABS), into which a cerium-doped gadolinium bromide (GdBr₃(Ce)) scintillating phase will be incorporated. Scintillator volumes of 50 cubic centimeters or greater will be fabricated to facilitate comparison with NaI(Tl) crystals currently available.

A dual neutron and gamma detection system has been developed for online measurements. The system consists of a single crystal mounted on a photomultiplier tube to detect simultaneously gamma radiation as well as thermal neutrons. A compact data acquisition system has been used for neutron and gamma discrimination. The system has been tested with different gamma energies and with an Am-Be neutron source at the University of Ontario Institute of Technology neutron facility. This thesis presents the characteristics of the developed detector, and experimental data carried out in different experiments in different fields. / UOIT