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<p>Nearly mono-energetic, high intensity (~10<super>7</super> gamma/s), and approximately 100% linearly polarized gamma-ray beams at energies between 5.15 and 7.60 MeV were used to induce photofission of <super>232</super>Th, <super>233,235,238</super>U, <super>237</super>Np, and <super>239,240</super>Pu. Prompt fission neutron yields parallel and perpendicular to the plane of beam polarization were measured using arrays of 12-18 liquid scintillator detectors. Prompt neutron polarization asymmetries close to zero were found for the even-odd actinides (<super>233,235</super>U, <super>237</super>Np, and <super>239</super>Pu), while significant asymmetries were found for the even-even actinides (<super>232</super>Th, <super>238</super>U, and <super>240</super>Pu). Predictions based on previously measured fission fragment angular distributions combined with a model of prompt neutron emission agree well with our experimental results. Finally, we describe a new method of measuring the enrichment of special nuclear material based on our results.</p> / Dissertation

La gestion des colis de déchets radioactifs représente un enjeu majeur pour l’industrie nucléaire. La solution de gestion d’un colis est déterminée en fonction de ses caractéristiques radiologiques. L’une de ces principales caractéristiques est l’activité α qui est principalement due aux actinides. Les méthodes non destructives actives, reposant sur le principe de la réaction de fission, permettent de quantifier les actinides. Ces méthodes sont mises en œuvre lorsque les techniques non-destructives passives deviennent inapplicables. Dans un premier temps, les méthodes actives consistent à irradier le colis afin d’entraîner des réactions de fission sur les actinides. Dans un second temps, les particules promptes et retardées émises suite aux réactions de fission sont détectées. Cette thèse a pour objectif d’optimiser le flux de neutrons, destiné à interroger les colis, en étudiant la possibilité d’utiliser un accélérateur d’électrons comme source de neutrons en lieu et place d’un générateur de type deutérium-tritium (gain attendu de l’ordre de deux décades en termes d’intensité d’émission). Un accélérateur d’électrons permettrait par ailleurs d’améliorer la caractérisation des colis de déchets radioactifs en rendant compatible, à l’aide du même dispositif d’irradiation, les mesures par interrogation neutronique active, par interrogation photonique active, et l’imagerie haute énergie.Dans un premier temps, nous avons caractérisé et optimisé le flux de photoneutrons émis par un accélérateur d’électrons en utilisant les codes de calculs Monte Carlo MCNPX et TRIPOLI-4. Nous avons considéré des cibles de conversion en tungstène ou en tantale et avons déterminé les paramètres suivants : intensité moyenne d’émission ; spectre en énergie ; et distribution angulaire. La cohérence de nos résultats a été évaluée par comparaison entre calculs et mesures d’activation neutronique. Nous avons ensuite évalué la faisabilité des mesures par interrogation neutronique active, en utilisant la cible d’un accélérateur d’électrons de 17 MeV en tant que générateur de neutrons, sur des échantillons d’uranium et de plutonium. Nous nous sommes intéressés à la détection des neutrons prompts, des neutrons retardés, et des gamma retardés. Nous avons également réalisé l’association de résultats de mesures par interrogations neutronique et photonique actives non-simultanées. Nous avons appliqué cette technique à la mesure de l’enrichissement de l’uranium. Enfin, nous avons dimensionné par simulation MCNPX une cellule de mesure, basée sur un accélérateur d’électrons, dédiée à l’interrogation neutronique active. La cellule a ensuite été construite et une campagne d’expérimentations a permis d’évaluer les performances de cette dernière lors de mesures réalisées sur des colis de déchets radioactifs maquettes de type 220 L contenant différentes matrices. / Management of nuclear waste packages is a crucial task for the nuclear industry. The solution for management of a nuclear waste package is chosen according to its radiological characteristics. One of the most important of these features is the α-activity which is mainly due to actinides. Non-destructive active methods based on the fission process enable to quantify the actinides. These methods are implemented when non-destructive passive methods become inapplicable. First, these methods consist in irradiating a package in order to induce fission reactions on the actinides, and then, to detect the prompt and delayed particles which are emitted further to these reactions. This thesis aims at optimizing the neutron flux, which is intended to interrogate a package, by studying the potentialities of using an electron accelerator as a neutron source instead of a deuterium-tritium neutron generator (expected gain in terms of emission intensity on the order of two decades higher). Furthermore, an electron accelerator would enable to improve nuclear waste packages characterization by making compatible, on the same irradiation setup, neutron interrogation measurements, photon interrogation measurements, and high-energy imaging.First, we characterized and optimized the photoneutron flux emitted by an electron accelerator using MCNPX and TRIPOLI-4 Monte Carlo codes. We considered tungsten and tantalum conversion targets and focused on the following parameters: average emission intensity; mean energy; and angular distribution. The consistency of our results has been verified by comparing neutron activation calculations and measurements. We have then evaluated the feasibility of neutron interrogation measurements on uranium and plutonium samples using the target of a 17 MeV electron accelerator as a neutron generator. We detected prompt neutrons, delayed neutrons, and delayed gamma-rays. We also combined photon and neutron interrogation non-simultaneous measurements. We applied such technique to the measurement of uranium enrichment. Finally, we designed by MCNPX simulation a neutron interrogation setup based on an electron accelerator. The cell was then built and an experimentation campaign enabled to evaluate performances of the latter. Measurements were carried out on 220 liter nuclear waste mock-up drums containing different matrices.

The e-linac beam that will serve the ARIEL Electron Target East (AETE) has an energy range from 30 MeV to 50 MeV with a power up to 500 kW. The beam electrons are to be converted into photons by means of an electron-to-gamma converter with the purpose of inducing photonuclear reactions in a target to produce exotic isotopes. In the process of conversion, the primary electron beam power deposition in the converter causes a significant increase of the temperature that must be dissipated. The converter performance contributes notably to the overall isotope production and extraction efficiency. This thesis describes the work to optimize and verify the conceptual design of the electron-to-gamma converter through simulations and experimental measurements. / Graduate

Nosso objetivo e estudar os principais mecanismos de foto absorção no ANTPOT.232 TH entre 7 e 60 Mev, ressonâncias gigantes e mecanismo do quase-deuteron, associados ao decaimento por fissão. Para isso, fizemos medidas da seção de choque de eletrofissão no ANTPOT.232 TH, entre as energias de 7 a 60 Mev, no laboratório do acelerador linear do IFUSP. Utilizamos, na analise, o formalismo dos fótons virtuais, que relaciona a seção de choque de fotofissão a seção de choque de eletrofissão. Foi utilizada a seção de choque de fotofissão medida em livermore e calculamos a seção de choque de fotoabsorção e2 (t=0 e t=1), além da seção de choque de fotoabsorção obtida via quase-deuteron. Verificamos que a contribuição predominante para a seção de choque de eletrofissão e a da componente de dipolo elétrico, sendo as demais contribuições (quadrupolo elétrico e modelo modificado do quase-deuteron) uma ordem de grandeza inferior a esta. / Our objective is to study the main photoabsorption mechanisms in 232T]n between 7 and 60 Mev, namely, Giant Resonances and Quasi-Deuteron, associated to fission decay. We performed electrofission measurements at the linear accelerator of IFUSP. In the analysis, the Virtual Photon Formalism, that relates the photofission cross section to the electrofission cross section, was used. In the calculations, the photofission cross section measured at Livermore Laboratory was used. The E2 photoabsorption and quasi-deuteron photoabsorption cross sections were calculated. We concluded that the most important contribution to the electrofission cross section comes from the El- giant resonance component, the other ones (E2 giant resonance component and quasi-deuteron mechanisms) being 1 or 2% of total electrofission cross section.

Este trabalho é dedicado ao estudo de reações de fissão de núcleos pesados induzidas por fótons e prótons a energias intermediárias e altas, fazendo uso, para tanto, do código de Monte Carlo CRISP, sendo um trabalho inteiramente computacional. Estudou-se um novo conjunto de parâmetros para a fórmula de massa semi-empírica proposta por Pearson em seu trabalho de 2001, a partir da qual se passou à simulação de reações de fissão induzidas por fótons dos núcleos 208Pb, 232Th, 237Np e 238U, e fissão induzida por prótons nos núcleos 197Au, 208Pb, 237Np e 241Am. Os modelos de Bohr e Wheeler para fissão, de 1939, e o modelo de Weisskopf para emissão de partículas de 1937 foram empregados na simulação. Para os parâmetros de densidade de níveis, um conjunto de parâmetros foi obtido para as fórmulas empíricas de Dostrovsky de 1958 e para a razão de fissão. Foram calculadas seções de choque de fotofissão para os núcleos 208Pb, 232Th, 237Np e 238U, produtos de reações de spallation induzidas por prótons nos núcleos 208Pb e 197Au, e distribuições de massa dos fragmentos de fissão em reações de Bremsstrahlung com o 238U e em reações induzidas por prótons com os núcleos 197Au, 208Pb, 237Np e 241Am. São apresentadas comparações a dados experimentais de todos os cálculos realizados. Também se obteve um modelo para aproximar os valores de barreira de fissão obtidos pelo método ETFSI (Extended Thomas-Fermi plus Strutinsky Integral). / This work is dedicated to the study of heavy nuclei fission induced by intermediate- and high-energy photons and protons, by using to this end the Monte Carlo code CRISP, therefore being an entirely computacional work. A new set of parameters for the 2001 semi-empirical mass formula proposed by Pearson is studied. Then we simulate fission reactions induced by photons and protons on 208Pb, 232Th, 237Np and 238U, and fission induced by protons on 197Au, 208Pb, 237Np e 241Am. The Bohr-Wheeler model for describing the fission process and the Weisskopf model for the emission probability of particles were used to perform the calculation. Regarding the level density parameters, a set of parameters is presented for the empirical formulas of Dostrovsky and for the fission ratio. This work also presents calculated fotofission cross section for induced reactions on 208Pb, 232Th, 237Np and 238U nuclei, spallation products of proton induced reactions on 208Pb and 197Au, and fragment mass distributions of Bremsstrahlung reactions with 238U and of proton induced reactions on 197Au, 208Pb, 237Np and 241Am. Comparisons to experimental data are shown for all calculations. A model to aproximate the fission barrier values obtaind by the ETFSI - Extended Thomas-Fermi plus Strutinsky Integral method is also presented.

Este trabalho é dedicado ao estudo de reações de fissão de núcleos pesados induzidas por fótons e prótons a energias intermediárias e altas, fazendo uso, para tanto, do código de Monte Carlo CRISP, sendo um trabalho inteiramente computacional. Estudou-se um novo conjunto de parâmetros para a fórmula de massa semi-empírica proposta por Pearson em seu trabalho de 2001, a partir da qual se passou à simulação de reações de fissão induzidas por fótons dos núcleos 208Pb, 232Th, 237Np e 238U, e fissão induzida por prótons nos núcleos 197Au, 208Pb, 237Np e 241Am. Os modelos de Bohr e Wheeler para fissão, de 1939, e o modelo de Weisskopf para emissão de partículas de 1937 foram empregados na simulação. Para os parâmetros de densidade de níveis, um conjunto de parâmetros foi obtido para as fórmulas empíricas de Dostrovsky de 1958 e para a razão de fissão. Foram calculadas seções de choque de fotofissão para os núcleos 208Pb, 232Th, 237Np e 238U, produtos de reações de spallation induzidas por prótons nos núcleos 208Pb e 197Au, e distribuições de massa dos fragmentos de fissão em reações de Bremsstrahlung com o 238U e em reações induzidas por prótons com os núcleos 197Au, 208Pb, 237Np e 241Am. São apresentadas comparações a dados experimentais de todos os cálculos realizados. Também se obteve um modelo para aproximar os valores de barreira de fissão obtidos pelo método ETFSI (Extended Thomas-Fermi plus Strutinsky Integral). / This work is dedicated to the study of heavy nuclei fission induced by intermediate- and high-energy photons and protons, by using to this end the Monte Carlo code CRISP, therefore being an entirely computacional work. A new set of parameters for the 2001 semi-empirical mass formula proposed by Pearson is studied. Then we simulate fission reactions induced by photons and protons on 208Pb, 232Th, 237Np and 238U, and fission induced by protons on 197Au, 208Pb, 237Np e 241Am. The Bohr-Wheeler model for describing the fission process and the Weisskopf model for the emission probability of particles were used to perform the calculation. Regarding the level density parameters, a set of parameters is presented for the empirical formulas of Dostrovsky and for the fission ratio. This work also presents calculated fotofission cross section for induced reactions on 208Pb, 232Th, 237Np and 238U nuclei, spallation products of proton induced reactions on 208Pb and 197Au, and fragment mass distributions of Bremsstrahlung reactions with 238U and of proton induced reactions on 197Au, 208Pb, 237Np and 241Am. Comparisons to experimental data are shown for all calculations. A model to aproximate the fission barrier values obtaind by the ETFSI - Extended Thomas-Fermi plus Strutinsky Integral method is also presented.