Dissertations / Theses on the topic 'Fission products Analysis'

Simultaneous measurements of the angular distribution, mass distribution and average total kinetic energy of fission fragments produced by the neutron-induced fission of 235U and 232Th have been made using a gridded ionisation chamber. The neutron energy range used was thermal to 1.9 MeV for 235U and 1.4 to 1.7 MeV for 232Th. The following topics were investigated: the interdependence of the fission fragment angular and mass distribution; the anomalous behaviour of fragment anisotropy for 235U(n,f) at neutron energies En below 150 keV; the possible existence of a third symmetric mass peak for 232Th(n,f); the mass fine structure in 235U(n,f) and 232Th(n,f); and the dependence of the fission fragment average total kinetic energy on the excitation energy of the fissioning nucleus. For this study, mono-energetic neutrons were produced by the and reactions. Four signals produced by the fission chamber were fed into a data acquisition system and processed by a specially modified comprehensive computer program. The results indicate that there is no interdependence between the angular and mass distributions of fragments for 235U(n,f) and for 232Th(n,f). The angular distribution of 235U fission fragments showed an anisotropy of less than one for En below 150 keV. For 232Th, the expected minimum in the anisotropy near En = 1.6 MeV was confirmed. No evidence for a third peak in the mass symmetry region of 232Th(n,f) was observed, within the yield sensitivity limitation of the chamber. Fine structure was observed in the mass yield distributions for 235U(n,f) and 232Th(n,f) at mass locations predicted by theory. The fission fragment average total kinetic energy for 235U(n,f) and 232Th(n,f) showed no significant dependence on the excitation energy of the fissioning nucleus. Possible reasons for some of these results are advanced.

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Tese (Doutoramento)
IPEN/T
Instituto de Pesquisas Energeticas e Nucleares - IPEN/CNEN-SP

Dans les nouvelles centrales nucléaires dites 4ème génération, comme d’ailleurs les anciennes, le dioxyde d’uranium devra opérer dans des milieux hostiles de températures et d’irradiation avec la présence des produits de fission (PF) et des particules alpha (α). Le fonctionnement dans ces conditions extrêmes induira des déplacements d’atomes et dégradera les propriétés thermiques et mécaniques du combustible UO2. La compréhension du comportement des défauts lacunaires, des PF et de l’hélium est cruciale pour prévoir le comportement du dioxyde d’uranium au sein de ces futures installations nucléaires. La première partie de cette thèse est consacrée à l’étude des défauts lacunaires induits par l’implantation de krypton et d’iode (quelques MeV) dans l’UO2 polycristallin et leurs stades de recuits. L’analyse par spectroscopie d’annihilation de positons (PAS) a permis de mettre en évidence la création de défauts de Schottky VU-2VO dans le cas des implantations iode et la formation de clusters lacunaires contenant du gaz pour les implantations krypton. L’évolution en température de ces défauts générés dépend des paramètres d’implantation (nature des ions, énergie, fluence). Cette étude a montré les rôles importants que peuvent jouer les défauts lacunaires et la présence des gaz de fission dans l’évolution du matériau UO2. Ensuite, nous nous sommes intéressés à l’étude et à la caractérisation, par PAS et les techniques d’analyse par faisceau d’ions (NRA/C et RBS/C), du comportement de l’hélium dans l’UO2. Les mesures de NRA/C et RBS/C révèlent une localisation d’une grande fraction d’hélium dans les sites interstitiels octaédriques de la matrice UO2. La localisation de l’hélium reste stable dans ces sites pour T< 600°C, évoluent légèrement entre 600 et 700°C et devient aléatoire à 800°C. Les mesures PAS mettent en évidence trois stades d’évolution des défauts lacunaires : la recombinaison par migration des interstitiels d’oxygène, l’agglomération des défauts entre 600 et 800°C et leur dissociation et élimination lorsque la température augmente. Ces résultats suggèrent que le transport d'hélium est assisté par les défauts lacunaires
In the new fourth generation nuclear plants, as in the old ones, uranium dioxide must operate in hostile environments of temperature and irradiation with the presence of fission products (FP) and alpha particles (α). Operation in these extreme conditions will induce atoms displacements and degrade the thermal and mechanical properties of UO2 fuel. Understanding the behavior of induced vacancy defects, FP and helium is crucial to predict the uranium dioxide behavior in the future nuclear reactors. The first part of this thesis is dedicated to the study of vacancy defects induced by krypton and iodine implantation (a few MeV) in the UO2 polycrystalline and of their evolution under annealing. Analysis by positron annihilation spectroscopy (PAS) has highlighted the creation of Schottky defects VU-2VO in the case of iodine implantations and formation of vacancy clusters containing the gas for krypton implantation. The temperature evolution of these defects depends on the implantation parameters (nature of the ion energy, fluence). This study showed the important roles that can play vacancy defects and the presence of fission gases in the evolution of UO2 material. Then we were interested in the study of the helium behavior in UO2 its location and migration, agglomeration and interaction with vacancy defects by using PAS and ion beam analysis (NRA/C and RBS/C). The NRA/C and RBS/C characterizations showed a localization of a large helium fraction in the octahedral interstitial sites of the UO2 matrix. The helium location in these sites remains stable for T <600°C, changing slightly between 600 and 700°C and becomes random at 800°C. Positron annihilation spectroscopy reveals three stages of vacancy defects evolution : The recombination with oxygen interstitial migration, defects agglomeration between 600 and 800°C and their dissociation and elimination when the temperature increases. These results suggest that the He transport is assisted by the vacancy defects

A análise por ativação com nêutrons é um método utilizado na determinação de diversos elementos em diferentes tipos de matrizes. Entretanto, quando a amostra contém altos teores de U ocorre o problema de interferência devido aos produtos de fissão do isótopo 235U. Um dos métodos de tratar este problema é fazer a correção usando fatores de interferência devido à fissão do U para os radionuclídeos utilizados nas análises dos elementos. No presente estudo foram determinados os valores dos fatores de interferência devido à fissão do U para os radioisótopos 141Ce, 143Ce,140La, 99Mo, 147Nd, 153Sm e 95Zr no reator nuclear de pesquisas IEA-R1 do IPEN-CNEN/SP. Esses fatores de interferência foram determinados experimentalmente, por meio da irradiação dos padrões sintéticos em uma determinada posição do reator, e teoricamente, determinando a razão dos fluxos de nêutrons epitérmicos e térmicos na mesma posição onde os padrões sintéticos foram irradiados e utilizando parâmetros nucleares da literatura. Os fatores de interferência obtidos foram comparados com os valores reportados em outros estudos. Para avaliar esses fatores de interferência, eles foram aplicados em análises dos elementos alvo deste estudo, nos materiais de referência certificados NIST 8704 Buffalo River Sediment, IRMM BCR-667 Estuarine Sediment e IAEA-SL-1 Lake Sediment.
Neutron activation analysis is a method used in the determination of several elements in different kinds of matrices. However, when the sample contains high U levels the problem of 235U fission interference occurs. A way to solve this problem is to perform the correction using the interference factor due to U fission for the radionuclides used on elemental analysis. In this study, the interference factors due to U fission for the radioisotopes 141Ce, 143Ce, 140La, 99Mo, 147Nd, 153Sm and 95Zr in the research nuclear reactor IEA-R1 at IPEN-CNEN/SP were determined. These interference factors were determined experimentally, by irradiation of synthetic standards in a selected position in the reactor, and theoretically, determining the epithermal to neutron fluxes ratio in the same position where synthetic standards were irradiated and using reported nuclear parameters on the literature. The obtained interference factors were compared with values reported by other works. To evaluate the reliability of these factors they were applied in the analysis of studied elements in the certified reference materials NIST 8704 Buffalo River Sediment, IRMM BCR- 667 Estuarine Sediment e IAEA-SL-1 Lake Sediment.

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Dissertação (Mestrado)
IPEN/D
Instituto de Pesquisas Energeticas e Nucleares - IPEN-CNEN/SP

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Dissertação (Mestrado em Tecnologia Nuclear)
IPEN/D
Instituto de Pesquisas Energeticas e Nucleares - IPEN-CNEN/SP

Thesis (S.B.)--Massachusetts Institute of Technology, Dept. of Physics, 2004.
MIT Institute Archives copy: leaves 92-111 bound in reverse order.
Includes bibliographical references (leaf 57).
The current analysis of the MITR core radioactivity inventory eliminates unnecessary assumptions made in previous estimates of the inventory, and revises the list of contributory isotopes to include all actinide and fission product isotopes necessary for a proper accident source term calculation. The result is a power-history-dependent inventory that increases with bum-up, and comprises 41 actinide isotopes and 596 fission product isotopes. The analysis uses the ORIGEN2 depletion code to calculate the activity of actinide and fission product isotopes for eight MITR input models at 32 intervals over a period of 5376MWD. The input models simulate a MITR core loaded with high- enrichment, U-Alx cermet fuel or low-enrichment, monolithic U-Mo fuel, and operated at 6MW with a continuous-burn-up or cyclic-burn-up-and-decay power history. Reorganization of the ORIGEN2 output file, and application of an element reduction criterion creates the condensed matrix file for each MITR input model. This file lists the contribution of each isotope to the core radioactivity inventory at each output interval, and is the basis for all inventory analysis. The inventory analysis yields three important conclusions. First, the assumption of an equilibrium inventory of isotopes in the fuel is accurate to within 3% for all time after 10% fuel bum-up, and conservative over the entire fuel cycle. The equilibrium fuel assumption is invalid for the actinides due to a slow rate of inventory growth. Second, the cyclic-bum-up-and-decay power history yields a lower core inventory than the continuous-burn-up power history for both fuel enrichments. The difference is minimized by increasing the ratio of irradiation time to decay time.
(cont.) Finally, the analysis indicates that conversion to a U-Mo fuel will produce an actinide inventory 18 times greater than that of the current U-Alx fuel, with no significant change in the fission product inventory. However, the actinide inventory is a small fraction of the fission product inventory. The worst-case core inventory available for release is 2.91 E+7Ci for the high-enrichment fuel, and 2.94E+7Ci for the low-enrichment fuel, with a core loading of 24 elements in each case. The best-estimate core inventory available for release is 2.83E+7Ci, and 2.82E+7Ci respectively, and accounts for typical cyclic operation of the MITR.
by William B. Kennedy.
S.B.

Dans les nouvelles centrales nucléaires dites 4ème génération, comme d'ailleurs les anciennes, le dioxyde d'uranium devra opérer dans des milieux hostiles de températures et d'irradiation avec la présence des produits de fission (PF) et des particules alpha (α). Le fonctionnement dans ces conditions extrêmes induira des déplacements d'atomes et dégradera les propriétés thermiques et mécaniques du combustible UO2. La compréhension du comportement des défauts lacunaires, des PF et de l'hélium est cruciale pour prévoir le comportement du dioxyde d'uranium au sein de ces futures installations nucléaires. La première partie de cette thèse est consacrée à l'étude des défauts lacunaires induits par l'implantation de krypton et d'iode (quelques MeV) dans l'UO2 polycristallin et leurs stades de recuits. L'analyse par spectroscopie d'annihilation de positons (PAS) a permis de mettre en évidence la création de défauts de Schottky VU-2VO dans le cas des implantations iode et la formation de clusters lacunaires contenant du gaz pour les implantations krypton. L'évolution en température de ces défauts générés dépend des paramètres d'implantation (nature des ions, énergie, fluence). Cette étude a montré les rôles importants que peuvent jouer les défauts lacunaires et la présence des gaz de fission dans l'évolution du matériau UO2. Ensuite, nous nous sommes intéressés à l'étude et à la caractérisation, par PAS et les techniques d'analyse par faisceau d'ions (NRA/C et RBS/C), du comportement de l'hélium dans l'UO2. Les mesures de NRA/C et RBS/C révèlent une localisation d'une grande fraction d'hélium dans les sites interstitiels octaédriques de la matrice UO2. La localisation de l'hélium reste stable dans ces sites pour T< 600°C, évoluent légèrement entre 600 et 700°C et devient aléatoire à 800°C. Les mesures PAS mettent en évidence trois stades d'évolution des défauts lacunaires : la recombinaison par migration des interstitiels d'oxygène, l'agglomération des défauts entre 600 et 800°C et leur dissociation et élimination lorsque la température augmente. Ces résultats suggèrent que le transport d'hélium est assisté par les défauts lacunaires.

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Dissertacao (Mestrado)
IPEN/D
Instituto de Pesquisas Energeticas e Nucleares - IPEN/CNEN-SP

Les noyaux riches en neutrons de masse A=100-110 constituent une région de grand intérêt pour l'étude de la structure nucléaire loin de la stabilité. De précédentes études de cette région de masse ont déjà révélé la complexité de l'évolution de la collectivité et de la déformation dans les chaînes isotopiques de Zr, Mo, Ru et Pd. Afin d'étendre les données expérimentales sur la collectivité à des états de plus haut spin et à des noyaux plus riches en neutrons, des temps de vie d'états excités ont été mesurés dans des noyaux produits par une réaction de fusion-fission en cinématique inverse au GANIL. Les fragments de fission étaient séparés et identifiés en A et Z grâce au spectromètre magnétique de grande acceptance VAMOS tandis que le rayonnement gamma était détecté dans l'ensemble de détecteurs germanium EXOGAM. Environ vingt temps de vie d'états 2+, 4+ et 6+ ont été extraits à l'aide du plunger de Cologne. Cette expérience représente la première mesure RDDS dans des fragments de fission identifiés évènement par évènement à la fois en A et Z.Cette étude des noyaux de masse A=100-110 est complétée par des calculs auto-cohérents de champ moyen et au-delà avec la force de Gogny (D1S). La structure des états fondamentaux et excités est décrite dans le cadre du modèle de Hartree-Fock-Bogoliubov avec des contraintes sur les déformations axiale et triaxiale. Les excitations individuelles sont étudiées par des calculs bloqués et les états de haut spin sont décrits dans l'approximation du champ tournant. Enfin, la méthode de la coordonnée génératrice approchée par un hamiltonien collectif en cinq dimensions (5DCH) est appliquée aux états collectifs de basse énergie. Les résultats sont comparés aux mesures de la collectivité
Neutron-rich nuclei of mass A=100-110 are of great interest for the study of nuclear structure far from stability. Previous experimental and theoretical studies suggest a complex evolution of deformation and collectivity in the isotopic chains of Zr, Mo, Ru and Pd.In order to extend information on the evolution of the collectivity towards higher spin states and more neutron-rich nuclei, lifetimes of excited states were measured in nuclei produced through a fusion-fission reaction in inverse kinematic at GANIL. Fission fragments were separated and identified in both A and Z with the high acceptance magnetic spectrometer VAMOS while the EXOGAM germanium detectors array was used for the coincident gamma-ray detection. Lifetimes of about twenty excited states were extracted using the plunger device of Cologne. This is the first RDDS measurement on fission fragments which are identified in A and Z on an event-by-event basis. The study of this mass region is completed by theoretical calculations using self consistent mean field and beyond mean field methods implemented with the Gogny force (D1S). The structure of the ground states and the excited states is described with Hartree-Fock-Bogoliubov calculations with constraints placed on the axial and triaxial deformations. Individual excitations are investigated through blocking calculations and the high spin states are studied through cranking calculations. Finally, an approximated generator coordinate method (GCM+GOA) using the 5DCH hamiltonian is used to describe the low energy collective states and to interpret the experimental evolution of the collectivity

Les réacteurs à neutrons rapides refroidis au sodium sont en développement en vue d'assurer une quatrième génération de réacteurs répondant à la demande énergétique, tout en assurant la préservation des ressources d'uranium par un fonctionnement en surgénérateur. L'objectif de la filière est également d'améliorer la gestion de la radiotoxicité des déchets produits par transmutation des actinides mineurs et de contrôler la non-prolifération par un fonctionnement en cycle fermé. Une instrumentation de surveillance et de contrôle de ce type de réacteur a été étudiée dans cette thèse. La spectrométrie gamma de nouvelle génération permet, par les hauts taux de traitement aujourd'hui accessibles, d'envisager de nouvelles approches pour suivre avec une précision accrue la puissance neutronique et de détecter plus précocement des ruptures de gaine combustible. Des simulations numériques ont été réalisées et une campagne d'essai a été menée à bien sur le réacteur Phénix de Marcoule. Des perspectives prometteuses ont été mises en exergue pour ces deux problématiques.

samples were irradiated for approximately 45 minutes to allow for the saturation of fission products. The first method used the beam port shutter and allowed for longer counting and irradiation times, but was unsuitable for examining fission products with half-lives below 10 seconds. The on/off method used a cycle of equal irradiation and counting times of one minute. The second method is able to measure track the production of fission products with half-lives of less than 10 seconds. This method used a borated aluminum wheel beam chopper to stop the irradiation of the sample during counting. The beam chopper was set to cycle for approximately one second of counting following half a second of irradiation. The spectra from both methods were analyzed and the peaks were assigned to the appropriate fission products. The majority of the peaks were composed of gamma-rays from multiple nuclides. The peaks created by gamma-rays from decays of a single nuclide were used to calculate the detection limits of the system. Using the beam chopper system, 21 peaks would be above the detection limits of our system 95% of the time for uranium samples of less than one kilogram.
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A high-efficiency gamma-ray counting system has been built at Los Alamos National Laboratory for use in analyzing nuclear forensics samples. This system consists of two clover high-purity germanium detectors and is surrounded by a thallium-doped sodium iodide annulus. Special precautions have been taken to ensure the system has a low background. The system is connected to XIA Pixie-4 fast digitizers and collects data in list-mode. This work is split into two main parts. The first part describes the proper steps and techniques to initialize the settings of a detector system connected to fast digitizers in order to optimize the system for resolution and throughput. The various counting modes for this particular system are described in detail, including the benefits and drawbacks of each mode. Steps are then shown to characterize the system by obtaining efficiency curves for various counting modes and sample geometries. Because of the close counting geometry involved with this system, true-coincidence summing factors must be calculated, and are done so in part by measuring the peak-to-total ratios of the system in its various counting modes across a wide energy range. The dead-time for the system can be complicated due to the multiple inputs of the system. Techniques for calculating the dead-time of multiple-detector systems are discussed. The second part of this work shows the system's usefulness in analyzing nuclear forensics samples, specifically irradiated enriched uranium. Three fission product parent-daughter pairs of different lifetimes are analyzed over a course of six months. The activities of each nuclide are calculated at each time step. Age dating techniques using the parent-daughter pairs are discussed, as well as the detection limits of each nuclide for a range of sample ages. Finally, avenues for further research are presented, as well as potential sources of error or uncertainty for this work.
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It is important to have a method of experimentally calculating fission product yields. Statistical calculations and simulations produce very large uncertainties. Experimental calculations, depending on the methods used, tend to produce lower uncertainties. This work set up a method to calculate fission product yields using gamma ray spectroscopy. In order to produce a method that was theoretically sound, a simulation was set up using OrigenArp to calculate theoretical concentrations of fission products from the irradiation of natural uranium. From these concentrations, the fission product yields were calculated to verify that they would agree with expected values. Moving forward in the work, the total flux at the point of irradiation, in the pneumatic transfer system, was calculated and determined to be 3.9070E+11 ± 6.9570E+10 n/cm^2/s at 100 kW. Once the flux was calculated, the method for calculating fission product yields was implemented and yields were calculated for 10 fission products. The yields calculated were in very good agreement (within 10.04%) with expected values taken from the ENDF-349 library. This method has strong potential in nuclear forensics as it can provide a means for developing a library of experimentally-determined fission product yields, as well as rapid post-nuclear detonation analysis.
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The work presented here develops a gamma-ray spectral construction and analysis software tool that was used to analyze multi-detector data collected using a digital spectrometer with list mode capabilities. The tool was used to parse the output from three detectors and generate new spectra that the user chooses from post-processing suppression routines, such as simulated anticoincidence and coincidence spectra. Part of this research was also to characterize the improvements in the detection limits and the various detector efficiencies from this method as opposed to creating these spectra using traditional electronic gating systems. A focus is placed on the detection capability improvements for nuclear forensics purposes, particularly the identification and quantification of fission product samples, and structuring the code framework for handling these types of time-dependent samples while increasing the versatility of the detector system. Improvements to the minimum detectable activity for a series of fission products was accomplished through post-processing suppression methods and multi-dimensional spectral data structures are now achievable.
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