The ranges and stragglings of fission fragments from the thermal neutron fission of U-235 have been measured. Particular attention was given to the preparation of very thin uranium sources, the design of a well collimated recoil system and the preparation of the fragment catcher. The ranges and range distributions in aluminum of fission products of mass numbers 95, 140, 141 and 147 have been obtained. The range values obtained agree with previous determinations within the experimental error. The refined techniques developed in this work have enabled differential range distributions to be obtained which are more precise than any previous determinations. / Thesis / Master of Science (MSc)

The present study is focused on evaluating higher actinides beyond uranium that are capable of supporting power and propulsion requirements in robotic deep space and interstellar exploration. The central technology in this thesis is based on utilizing advanced actinides for direct fission fragment energy conversion coupled with magnetic collimation. Critical fission configurations are explored which are based on fission fragment energy conversion utilizing a nano-scale layer of the metastable isotope 242mAm coated on carbon fibers. A 3-D computational model of the reactor core is developed and neutron properties are presented. Fission neutron yield, exceptionally high thermal fission cross sections, high fission fragment kinetic energy and relatively low radiological emission properties are identified as promising features of 242mAm as a fission fragment source. The isotopes 249Cf and 251Cf are found to be promising candidates for future studies. Conceptual system integration, deep space mission applicability and recommendations for future experimental development are introduced.

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.

La fission nucléaire est le mécanisme de séparation d'un noyau lourd en deux noyaux appelés fragments de fission. Ces fragments excités émettent des neutrons et des gammas dits prompts pour rejoindre leur état fondamental ou métastable. L'énergie libérée lors de la fission est utilisée dans les centrales nucléaires pour fournir de l'électricité. La durée de vie et le contrôle des réacteurs nucléaires dépendent entre autres des observables de fission telles que les rendements en masse des fragments, la multiplicité et l'énergie des neutrons et des gammas prompts. La première partie de cette thèse est dédiée à l'étude du processus de désexcitation des fragments de fission avec le code de simulation Monte-Carlo FIFRELIN. Ce code, constitué de plusieurs modèles nucléaires permettant de décrire les fragments, prédit les propriétés (multiplicité, énergie) des particules promptes émises lors de la désexcitation. Lors de ce travail de thèse l'influence des modèles sur les prédictions du code a été étudiée. Les modèles étudiés sont ceux définissant le moment angulaire initial, la densité de niveaux et les fonctions de force gamma des fragments. Les résultats de ces études permettent d'identifier les modèles qui influencent significativement les prédictions du code et donc, de sélectionner la combinaison des modèles reproduisant le maximum d'observables et d'améliorer la description nucléaire des fragments. Ces études sont d'abord menées sur la fission spontanée du 252Cf pour laquelle de nombreuses données expérimentales existent ce qui permet de contraindre fortement les modèles. Des études sur la fission rapide (énergie des neutrons incidents de l'ordre du MeV) de 238U et 237Np sont ensuite réalisées. Elles sont motivées, entre autres, par le développement de nouveaux concepts de réacteurs rapides, dits de quatrième génération, permettant de réduire les quantités de déchets nucléaires et d'utiliser les réserves abondantes de 238U pour fournir de l'électricité. Les données expérimentales relatives à la fission rapide sont rares. De nouveaux dispositifs expérimentaux sont actuellement en développement afin d’étudier l’évolution des différentes observables de fission sur un large domaine en énergie d’excitation. Le dispositif FALSTAFF qui fait l'objet de la deuxième partie de cette thèse est l'un d'entre eux. Dans cette seconde partie les étapes de développement, d'optimisation et de caractérisation du premier bras du dispositif expérimental FALSTAFF sont présentées. Ce spectromètre, installé auprès de l'installation NFS (Neutrons For Science), permettra d'étudier la fission rapide en cinématique directe de nombreux actinides. La détection des deux fragments de fission en coïncidence permettra de caractériser leur énergie, leurs masses (avant et après évaporation des neutrons) et leur charge. La multiplicité des neutrons émis sera alors déterminée et nous renseignera sur le partage de l'énergie d’excitation entre les fragments. Les données mesurées serviront ultérieurement de données d'entrée au code FIFRELIN. La mesure de la vitesse des deux fragments en coïncidence (méthode 2V), avec des détecteurs de temps de vol MWPC-SeD donnent accès à la masse avant évaporation. Une chambre à ionisation axiale placée après ces détecteurs permet de mesurer l'énergie cinétique et le profil de perte d'énergie des fragments, ce qui permet de déterminer respectivement la masse après évaporation (méthode EV) et la charge nucléaire des fragments.La partie expérimentale de cette thèse est dédiée au développement des programmes de simulation et d'analyse des données, à la mise en place du système d'acquisition, à la caractérisation et à l'optimisation des détecteurs. Ce dernier point concerne essentiellement l'étude des performances de la chambre à ionisation axiale. / Nuclear fission is the process in which a heavy nucleus splits into two nuclei called fission fragments. These excited fragments emit prompt neutrons and gammas to reach their ground or a metastable state. The energy released during fission is used in nuclear power plants to provide electricity. The nuclear reactor lifespan and control depend partly on fission observables such as the fragment mass yields, the neutron and gamma multiplicity and energy. The first part of this thesis is dedicated to the study of the fission fragment de-excitation process with the FIFRELIN Monte-Carlo code. This code, containing many nuclear models describing the fragments, predicts the prompt particle properties (multiplicity, energy).During this PhD work the impact of different models on the code predictions was investigated. The models which are studied are those defining the initial angular momentum, the level density and the radiative strength function of fragments. These studies identified those nuclear properties that have a significant impact on the code predictions, and as a consequence permitted selection of the model combination suited to reproduce the maximum number of fission observables, and improving our understanding about the nuclear description of fission fragments. These studies are firstly performed on the spontaneous fission of 252Cf for which numerous experimental data are available allowing constraints to be set on the models. Studies on fast fission (incident neutron with an energy around MeV) of 238U and 237Np are then performed. They are motivated partly by the development of new fast reactor concepts, called Generation IV reactors, that will reduce the quantity of nuclear waste and burn the large amount of natural uranium to provide electricity. Experimental data concerning fast fission are scarce. As a consequence new experimental setups are currently under development. They will measure fission observables over a large excitation energy domain. One of them, called FALSTAFF, is the topic of the second part of this thesis. In the second part of this PhD thesis, the different steps concerning the development, the optimization and the characterization of the first arm of the FALSTAFF setup are presented. This spectrometer, placed at the NFS facility (Neutrons For Science), will study fast fission in direct kinematic for various actinides. The detection of both fragments in coincidence will allow characterization of their energy, their masses (before and after neutron evaporation) and their nuclear charge. The neutron multiplicity will be deduced and will provide information on the energy sharing between the fragments. This data will be later used as input for the FIFRELIN code. The velocity determination of both fragments (2V method), with MWPC-SeD time-of-flight detectors, will provide pre-neutron emission fragment masses. An axial ionization chamber, placed after those detectors, will measure the kinematic energy and the energy loss profile of fragments, which will provide respectively the post-neutron emission mass (EV method) and the nuclear charge. The experimental part of this thesis is dedicated to the development of simulation and data analysis software, the configuration of the data acquisition system, the characterization and the optimization of the detectors. This last item mainly concerns the axial ionization chamber.

The general fission process is well known and is applied in nuclear power plants all over the world. However many properties of fission fragments are still not well understood. The angular momentum distribution of fission fragments is an important property to gain a better understanding of the fission process, and that can be derived indirectly from isomeric yield ratios. The goal of this project has been to develop a script in Python that runs the nuclear reaction code TALYS with the Total Monte Carlo method to calculate the isomeric yield ratio. The script generates a matrix consisting of excitation energies and angular momenta that is provided to TALYS. One matrix corresponds to one calculation of the isomeric ratio. Thus, the dependency of the isomeric yield ratio on these matrices can be observed. After looking into the matrices, the dependencies of the isomeric yield ratios on the excitation energies and the angular momentum distribution are observed. In this project, the calculated isomeric yield ratios are compared with the experimental value obtained from an experiment conducted in August of 2019 at the IGISOL-JYFLTRAP facility in Jyväskylä, Finland. It is worth mentioning that, fission system is of Uranium-238 which was induced by a proton beam at an energy of 25 MeV. The dependency of the isomeric yield ratio (IYR) on the angular momentum and the excitation energy has been investigated. However, it has proved more difficult than expected, to deduce an estimation for the angular momentum distribution. Another finding of this project is that the two codes used, GEF and TALYS sometimes produce inconstant results.

[pt] Um espectrômetro de massa PDMS-252Cf-TOF (Time-of-Flight Plasma Dessorption Mass Spectrometry) foi usado para analisar amostras condensadas de água pura e misturas de H2O:C2H2, H2O:C2H6 e H2O:N2O, em temperaturas entre 10 e 100 K. Os íons dessorvidos devido ao impacto foram identificados e seus rendimentos de dessorção determinados. Observa-se que a distribuição desses rendimentos em função da massa dos íons pode ser descrita pela soma de duas exponenciais. Este resultado sugere fortemente que ocorrem dois processos de formação de agregados: um, via emissão direta de fragmentos do sólido e outro, via recombinação de fragmentos na fase gasosa. Para H2O puro, os principais agregados dessorvidos são: ((H2O)nH2O+, (H2O)nH3O+, On +, (H2O)nO−, (H2O)nOH− e On −. Para misturas de gelos H2O:C2H2 e H2O:C2H6, são observadas as séries (C2H2)n + e (C2H6)n +. Para H2O:N2O, as séries Nn +, (O)nN2 +, (O)nN2−, (O)nN4−, e (N2)nNO+ são as mais abundantes. A Teoria do Funcional da Densidade (DFT), no nível B3LYP/6-31G, foi usada para calcular a estabilidade molecular dos íons moleculares secundários emitidos. Cálculos para as estruturas C2Hm + (com m = 1 a 6) geraram 26 estruturas estáveis. As curvas de estabilidade por massa/carga obtidas são comparadas com aquelas obtidas experimentalmente para os rendimentos de dessorção por massa/carga para os mesmos íons. Tal metodologia é utilizada para prever as conformações mais prováveis dos íons dessorvidos. / [en] A PDMS-252Cf-TOF (Time-of-Flight Plasma Desorption Mass Spectrometry) mass spectrometer was used to analyze condensed samples of pure water and mixtures of H2O:C2H2, H2O:C2H6 and H2O:N2O, at temperatures between 10 and 100 K. The ions desorbed due to the projectile impact were identified and their desorption yields determined. It is observed that the yield distributions as a function of the mass of the ions can be described by the sum of two exponentials. This result strongly suggests that two processes of aggregate formation occur: one, via direct emission of fragments from the solid and the other, via recombination of fragments in the gas phase. For pure H2O, the main desorbed aggregates are: ((H2O)nH2O+, (H2O)nH3O+, On +, (H2O)nO−, (H2O)nOH− and On −. For mixtures of ices H2O:C2H2 and H2O:C2H6, the series (C2H2)n + and (C2H6)n + are observed. For H2O:N2O, the series Nn +, (O)nN2 +, (O)nN2−, (O)nN4−, and (N2)nNO+ are the most abundant. Density Functional Theory (DFT), at the B3LYP/6-31G level, was used to calculate the molecular stability of emitted secondary molecular ions. Calculations for the C2Hm + structures (with m = 1 to 6) generated 26 stable structures. The stability curves per mass/charge obtained are compared with those obtained experimentally for the desorption yields per mass/charge for the same ions. Such methodology is used to predict the most likely conformations of the desorbed ions.

[pt] Um espectrômetro de massa tipo tempo-de-vôo, montado no Laboratório Nacional de Luz Síncrotron (Campinas - SP), foi utilizado para analisar os íons dessorvidos de uma amostra de amônia condensada (temperaturas de análise: 25 a 150 K) ao ser impactada por fragmentos de fissão do 252Cf. O espectrômetro permite identificar e determinar as abundâncias das espécies iônicas dessorvidas. Quanto à parte teórica, foram feitos cálculos para determinar as estruturas mais estáveis dos agregados de NH3 e para determinar suas dinâmicas de emissão de íons secundários observados na parte experimental. A amônia foi escolhida por sua semelhança com a água, uma molécula muito bem estudada. Outra razão é o atual interesse em determinar a formação de compostos orgânicos nas superfícies de corpos interestelares, uma vez que está comprovada a presença da amônia naquelas superfícies. Nos espectros obtidos observa-se a formação de agregados de amônia que podem ser representados por (NH3)nNHm ± com n = 0-30 e m = 0-5, para íons positivos, e com n = 0- 3 para íons negativos. Uma forma de evidenciar a possibilidade de formação de novos compostos foi realizar experiências com a mistura NH3-CO, com a mesma montagem experimental utilizada para a amônia. Observa-se no espectro obtido (antes da sublimação do CO a 30 K) linhas de massa resultantes de reações primárias que correspondem a íons moleculares híbridos com estrutura CnOmHl+.Os cálculos teóricos referentes às estruturas dos agregados foram realizados través do programa Jaguar 5.5 e Jaguar 6.0. O objetivo é determinar as estruturas mais estáveis dos agregados iônicos da amônia através da teoria DFT (Teoria do Funcional de Densidade) por meio da minimização da energia. Encontrou-se uma relação direta entre as estabilidades determinadas e as abundâncias relativas no espectro de massa. Finalmente foram realizados cálculos com o modelo teórico de dessorção iônica induzida por elétrons. Os resultados de distribuição de velocidades e energias foram comparados com os dados experimentais dos agregados da amônia (n = 0, 4), apresentando uma concordância razoável em valor absoluto, mas moderada em forma. / [en] A time-of-flight mass spectrometer, mounted at the Laboratório National de Luz Síncrotron (Campinas - SP), was used to analyze desorbed ions of a condensed ammonia sample (analyzing temperatures: 25 - 150 K) being impacted by 252Cf fission fragments . The spectrometer allows identifying and determining the relative yields of ionic desorbed species. Besides, it had been made theoretical calculations to determine the most stable cluster structures as well as to determine the emission dynamics of NH3 clusters observed in the experimental part. The ammonia was chosen because of its similarity with the water molecule (very well studied). Another reason is the current interest in determining the organic compounds formation in the interstellar surfaces, now that it is proven the presence of ammonia in those surfaces. The measured spectra show the formation of ammonia clusters that can be represented by (NH3)nNHm ± with n = 0 - 30 and m = 0 - 5 for positive ions, and n = 0 - 3 for negative ones. One way to evidence the formation possibility of new compound is to perform experiments with CO-NH3 mixture samples, using the same experimental set up used for the ammonia. In the spectrum measured before CO sublimation (30 K), mass lines, product of primary reactions, corresponding to hybrid molecular ions having the CnOmHl + structure were observed. Theoretical calculations referring to cluster structures had been carried out using the programs Jaguar 5,5 and Jaguar 6.0. The objective is to determine the most stable structures of the ammonia clusters through the Density Functional Theory (DFT) by means of energy minimizations. A direct relation between the computed stabilities and the relative abundances in the mass spectra was found. Finally calculations with the Secondary Electron Induced Desorption (SEID) model had been carried out. Results of velocity and energy distributions had been compared with the experimental data of ammonia clusters (n = 0, 4), presenting a good agreement in absolute values but moderate agreement in shape.

Energy resolution characteristics of silicon surface barrier detector signals amplified by different preamplifiers and spectroscopic amplifiers have been studied. The characterization has been done using alpha particles from an 241Am source and spontaneous fission fragments from two Cf sources. The alpha and spontaneous fission activities of the sources have been measured and the isotopic compositions, ages, and initial activities of the two Cf sources have been calculated using the results from the activity measurements. 82.3% and 82.5% of the spontaneous fission activity of the two sources is found to originate from 252Cf. Heavy ion detection properties of two Si detector setups have been determined by measuring spontaneous fission fragments from one of the Cf sources in coincidence. The mass distribution of fission fragments is derived from the pulse spectra of the coincidence measurements. The conditions for future time resolution measurements have been established. Inquiries on commercially available ultra-thin Si detectors have been made. The purpose is to upgrade detector telescopes to lower the energy threshold of ΔE-ΔE-E identification of particles from neutroninduced nuclear reactions. Three manufacturers of Si detectors with thickness 20-25 µm and active area around 450 mm2 have been listed together with properties of the three offered detectors.

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.