Various fuel cycles for a sodium-cooled, subcritical, fast reactor with a fusion neutron source for the transmutation of light water reactor spent fuel have been analyzed. All fuel cycles were 4-batch, and all but one were constrained by a total fuel residence time consistent with a 200 dpa clad and structure materials damage limit. The objective of this study was to achieve greater than 90% burn up of the transuranics from the spent fuel.

Os progressos computacionais nas últimas décadas e a teoria matemática cada vez mais sólida têm possibilitado a resolução de problemas de alta complexidade, permitindo uma modelagem cada vez mais detalhada da realidade. Tal verdade aplica-se inclusive para os sistemas rígidos de Equações Diferencias Ordinárias (EDOs): existem métodos numéricos altamente performáticos para este tipo de problema, que permitem uma grande variação no tamanho do passo de integração sem impactar na sua convergência. Este trabalho apresenta um estudo sobre o conceito de rigidez e técnicas numéricas para resolução de problemas rígidos de EDOs. O que nos motivou a estudar tais técnicas foram problemas oriundos da Física Nuclear que envolvem cadeias de decaimento radioativo. Estes problemas podem ser modelados por uma cadeia fechada de compartimentos que se traduz em um sistema de EDOs. Os elementos destas cadeias podem possuir constantes de decaimento com ordens de grandeza muito distintas, caracterizando a sua rigidez e exigindo cautela na resolução das equações que as modelam. Embora seja possível determinar a solução analítica para estes problemas, o uso de métodos numéricos facilita a obtenção da solução quando consideramos sistemas com um número elevado de equações. Além disso, soluções numéricas permitem adaptações na modelagem ou em ajustes de dados com mais facilidade. Métodos implícitos são indicados para a resolução deste tipo de problema, pois possuem uma região de estabilidade ilimitada. Neste trabalho, implementamos dois métodos numéricos que possuem esta característica: o método de Radau II e o método de Rosenbrock. Estes métodos foram utilizados para obtenção de soluções numéricas robustas para problemas rígidos de decaimento radioativo envolvendo cadeias naturais e artificiais, considerando retiradas de elementos das cadeias durante o processo de decaimento e quando queremos determinar qual era o estado inicial de uma cadeia que está em decaimento. Ambos os métodos foram implementados com estratégias de controle do tamanho do passo de integração e produziram resultados consistentes dentro de uma precisão pré-fixada. / The computational progress in the last decades and the increasingly solid mathematical theory have made possible the resolution of highly complex problems allowing an ever more detailed modelling of reality. This is true even for the systems of stiff Ordinary Differential Equations (ODEs): there are highly performative numerical methods for this kind of problem which allow a wide variation in the size of integration step without impacting on their convergence. This thesis presents a study about the concept of stiffness and numerical techniques to solve stiff problems of ODEs. What motivated us to study these techniques were problems from the Nuclear Physics involving radioactive decay chains. These problems could be modelled by a closed chain of compartments which is translated into a system of ODEs. The elements of these chains could have decay constants with very different orders of magnitude which characterizes the stiffness of the problem and requires caution in solving the model equations. Although it is possible to determine the analytical solution to these problems when we consider systems with a high number of equations, calculate the solution by numerical methods becomes easier. Furthermore, numerical solutions allow adaptations in modelling or data adjustments more easily. Implicit methods are indicated to solve this kind of problem because they have an unlimited region of stability. In this study, we implemented two numerical methods which have this feature: Radau II method and Rosenbrock method. These methods were used to obtain robust numerical solutions for stiff problems of radioactive decay involving natural and artificial chains, considering the removal of elements during the decay process and when we want to determine what was the initial state of a chain which is decaying. Both methods were implemented with control strategies for integration step size providing consistent results within a pre-established accuracy.

Em cumprimento aos requisitos normativos e regulatórios, considerados os padrões nacionais e internacionais de Boas Práticas de Fabricação (BPF) de medicamentos, o ambiente de produção de radiofármacos (célula) é determinante para a qualidade do medicamento, quanto aos limites estabelecidos na legislação vigente para níveis de contaminantes, discriminados como partículas não viáveis (partículas em geral) e microrganismos viáveis, corroborado, ainda, pelo fator de decaimento radioativo, uma vez que os radiofármacos devem ser liberados e administrados aos pacientes pouco tempo após sua produção. Tão importante quanto proteger o produto contra uma possível contaminação do meio ambiente é o operador estar protegido contra a contaminação pelo manuseio do produto. Assim, o estudo, concepção e desenvolvimento de uma célula nacional implicou em análises minuciosas de cada um dos elementos de composição do ambiente de produção e de sua operação, orientado pelo conceito de Quality by Design, metodologia que vem sendo aplicada, recentemente, na indústria farmacêutica. O conhecimento do produto, a configuração do espaço de operação por meio de mockup, a abordagem quanto aos atributos críticos da qualidade, com definições claras quanto aos parâmetros do processo produtivo, validados em experimentos, definiram uma célula multipropósito para produção de radiofármacos em acordo com BPF. / In order to fulfill the normative and regulations requirements under the national and international aspects of Good Manufacturing Practices (GMP), the radiopharmaceutical production environment (called \"hot cell\") is determinant for the quality of the medicinal product, within the limits established by the current legislation for levels of contaminants, split into non-viable particles (airborne general particles) and viable microorganisms; in addition to the radioactive decay (called \"half-life\") results radiopharmaceuticals to be released and administered to patients shortly after their production. It is not sufficient to protect the product against possible contamination from the environment, but the operator must be contamination protected when handling the product. Thus, the study, design and development of a national hot cell resulted in detailed analyzes of each single elements of the production environment and its operation, guided by the concept of Quality by Design, which is the methodology that has been applied recently at the pharmaceutical industry. The features such as the product conceptual knowledge, the configuration of the operating space (by mockups), the approaches regarding the quality critical attributes, the clear definitions regarding the parameters of the productive process, and finally the experimental validation, defined a multipurpose hot cell for the production of radiopharmaceuticals according to GMP requirements.

Em cumprimento aos requisitos normativos e regulatórios, considerados os padrões nacionais e internacionais de Boas Práticas de Fabricação (BPF) de medicamentos, o ambiente de produção de radiofármacos (célula) é determinante para a qualidade do medicamento, quanto aos limites estabelecidos na legislação vigente para níveis de contaminantes, discriminados como partículas não viáveis (partículas em geral) e microrganismos viáveis, corroborado, ainda, pelo fator de decaimento radioativo, uma vez que os radiofármacos devem ser liberados e administrados aos pacientes pouco tempo após sua produção. Tão importante quanto proteger o produto contra uma possível contaminação do meio ambiente é o operador estar protegido contra a contaminação pelo manuseio do produto. Assim, o estudo, concepção e desenvolvimento de uma célula nacional implicou em análises minuciosas de cada um dos elementos de composição do ambiente de produção e de sua operação, orientado pelo conceito de Quality by Design, metodologia que vem sendo aplicada, recentemente, na indústria farmacêutica. O conhecimento do produto, a configuração do espaço de operação por meio de mockup, a abordagem quanto aos atributos críticos da qualidade, com definições claras quanto aos parâmetros do processo produtivo, validados em experimentos, definiram uma célula multipropósito para produção de radiofármacos em acordo com BPF. / In order to fulfill the normative and regulations requirements under the national and international aspects of Good Manufacturing Practices (GMP), the radiopharmaceutical production environment (called \"hot cell\") is determinant for the quality of the medicinal product, within the limits established by the current legislation for levels of contaminants, split into non-viable particles (airborne general particles) and viable microorganisms; in addition to the radioactive decay (called \"half-life\") results radiopharmaceuticals to be released and administered to patients shortly after their production. It is not sufficient to protect the product against possible contamination from the environment, but the operator must be contamination protected when handling the product. Thus, the study, design and development of a national hot cell resulted in detailed analyzes of each single elements of the production environment and its operation, guided by the concept of Quality by Design, which is the methodology that has been applied recently at the pharmaceutical industry. The features such as the product conceptual knowledge, the configuration of the operating space (by mockups), the approaches regarding the quality critical attributes, the clear definitions regarding the parameters of the productive process, and finally the experimental validation, defined a multipurpose hot cell for the production of radiopharmaceuticals according to GMP requirements.

Os progressos computacionais nas últimas décadas e a teoria matemática cada vez mais sólida têm possibilitado a resolução de problemas de alta complexidade, permitindo uma modelagem cada vez mais detalhada da realidade. Tal verdade aplica-se inclusive para os sistemas rígidos de Equações Diferencias Ordinárias (EDOs): existem métodos numéricos altamente performáticos para este tipo de problema, que permitem uma grande variação no tamanho do passo de integração sem impactar na sua convergência. Este trabalho apresenta um estudo sobre o conceito de rigidez e técnicas numéricas para resolução de problemas rígidos de EDOs. O que nos motivou a estudar tais técnicas foram problemas oriundos da Física Nuclear que envolvem cadeias de decaimento radioativo. Estes problemas podem ser modelados por uma cadeia fechada de compartimentos que se traduz em um sistema de EDOs. Os elementos destas cadeias podem possuir constantes de decaimento com ordens de grandeza muito distintas, caracterizando a sua rigidez e exigindo cautela na resolução das equações que as modelam. Embora seja possível determinar a solução analítica para estes problemas, o uso de métodos numéricos facilita a obtenção da solução quando consideramos sistemas com um número elevado de equações. Além disso, soluções numéricas permitem adaptações na modelagem ou em ajustes de dados com mais facilidade. Métodos implícitos são indicados para a resolução deste tipo de problema, pois possuem uma região de estabilidade ilimitada. Neste trabalho, implementamos dois métodos numéricos que possuem esta característica: o método de Radau II e o método de Rosenbrock. Estes métodos foram utilizados para obtenção de soluções numéricas robustas para problemas rígidos de decaimento radioativo envolvendo cadeias naturais e artificiais, considerando retiradas de elementos das cadeias durante o processo de decaimento e quando queremos determinar qual era o estado inicial de uma cadeia que está em decaimento. Ambos os métodos foram implementados com estratégias de controle do tamanho do passo de integração e produziram resultados consistentes dentro de uma precisão pré-fixada. / The computational progress in the last decades and the increasingly solid mathematical theory have made possible the resolution of highly complex problems allowing an ever more detailed modelling of reality. This is true even for the systems of stiff Ordinary Differential Equations (ODEs): there are highly performative numerical methods for this kind of problem which allow a wide variation in the size of integration step without impacting on their convergence. This thesis presents a study about the concept of stiffness and numerical techniques to solve stiff problems of ODEs. What motivated us to study these techniques were problems from the Nuclear Physics involving radioactive decay chains. These problems could be modelled by a closed chain of compartments which is translated into a system of ODEs. The elements of these chains could have decay constants with very different orders of magnitude which characterizes the stiffness of the problem and requires caution in solving the model equations. Although it is possible to determine the analytical solution to these problems when we consider systems with a high number of equations, calculate the solution by numerical methods becomes easier. Furthermore, numerical solutions allow adaptations in modelling or data adjustments more easily. Implicit methods are indicated to solve this kind of problem because they have an unlimited region of stability. In this study, we implemented two numerical methods which have this feature: Radau II method and Rosenbrock method. These methods were used to obtain robust numerical solutions for stiff problems of radioactive decay involving natural and artificial chains, considering the removal of elements during the decay process and when we want to determine what was the initial state of a chain which is decaying. Both methods were implemented with control strategies for integration step size providing consistent results within a pre-established accuracy.

Ce travail de thèse s’inscrit dans le domaine de l’énergie nucléaire, de l’aval du cycle du combustible et du calcul des incertitudes. Le CEA doit concevoir le prototype ASTRID, réacteur à neutrons rapides refroidi au sodium (RNR), qui est l’un des concepts retenus au sein du forum Génération IV et dont la puissance résiduelle et l’estimation de son incertitude ont un impact important. Ce travail consiste à développer un code de propagation des incertitudes des données nucléaires sur la puissance résiduelle dans les RNR.La démarche s’est déroulée en trois temps.La première étape a permis de limiter le nombre de paramètres intervenant dans le calcul de la puissance résiduelle. Pour cela, un essai de puissance résiduelle sur le réacteur PHENIX (PUIREX 2008) a été interprété de façon à valider expérimentalement le formulaire d’évolution DARWIN pour les RNR et à quantifier les termes sources de la puissance résiduelle.La deuxième étape a eu pour but de développer un code de propagation des incertitudes : CyRUS (Cycle Reactor Uncertainty and Sensitivity). Une méthode de propagation déterministe a été retenue car elle permet des calculs rapides et fiables. Les hypothèses de linéarité et de normalité qu’elle entraîne ont été validées théoriquement. Le code a également été comparé avec succès à un code stochastique sur l’exemple de la fission élémentaire thermique de l’235U.La dernière partie a été une application du code sur des expériences de puissance résiduelle d’un réacteur, de bilan matière d’une aiguille combustible et d’une fission élémentaire de l’235U. Le code a démontré des possibilités de retour d’expériences sur les données nucléaires impactant l’incertitude de cette problématique.Deux résultats principaux ont été mis en évidence. Tout d’abord, les hypothèses simplificatrices des codes déterministes sont compatibles avec un calcul précis de l’incertitude de la puissance résiduelle. Ensuite, la méthode développée est intrusive et permet un retour d’expérience sur les données nucléaires des expériences du cycle. En particulier, ce travail a montré qu’il est déterminant de mesurer précisément les rendements de fission indépendants et de déterminer leurs matrices de covariances afin d’améliorer la précision du calcul de la puissance résiduelle. / This PhD study is in the field of nuclear energy, the back end of nuclear fuel cycle and uncertainty calculations. The CEA must design the prototype ASTRID, a sodium cooled fast reactor (SFR) and one of the selected concepts of the Generation IV forum, for which the calculation of the value and the uncertainty of the decay heat have a significant impact. In this study is developed a code of propagation of uncertainties of nuclear data on the decay heat in SFR.The process took place in three stages.The first step has limited the number of parameters involved in the calculation of the decay heat. For this, an experiment on decay heat on the reactor PHENIX (PUIREX 2008) was studied to validate experimentally the DARWIN package for SFR and quantify the source terms of the decay heat.The second step was aimed to develop a code of propagation of uncertainties : CyRUS (Cycle Reactor Uncertainty and Sensitivity). A deterministic propagation method was chosen because calculations are fast and reliable. Assumptions of linearity and normality have been validated theoretically. The code has also been successfully compared with a stochastic code on the example of the thermal burst fission curve of 235U.The last part was an application of the code on several experiments : decay heat of a reactor, isotopic composition of a fuel pin and the burst fission curve of 235U. The code has demonstrated the possibility of feedback on nuclear data impacting the uncertainty of this problem.Two main results were highlighted. Firstly, the simplifying assumptions of deterministic codes are compatible with a precise calculation of the uncertainty of the decay heat. Secondly, the developed method is intrusive and allows feedback on nuclear data from experiments on the back end of nuclear fuel cycle. In particular, this study showed how important it is to measure precisely independent fission yields along with their covariance matrices in order to improve the accuracy of the calculation of the decay heat.

<p>U ovoj disertaciji su prikazani rezultati kompleksnih istraživanja uticaja<br />kosmičkog zračenja na nuklearne spektre na nivou mora.<br />Utvrđivanje specifičnih vremenskih intervala u vremenskom spektru,<br />kojima odgovaraju tačno određene grupe događaja indukovane<br />kosmičkim mionima, omogućava adekvatno odbacivanje ometajućih<br />događaja u željenim energetskim oblastima detektovanih spektara, pri<br />antikoincidentnom režimu rada ultraniskofonskih sistema. U prvom<br />eksperimentu prikazanom u ovoj disertaciji,&nbsp; istraživana je mogućnost<br />vremenskog razlaganja detektovanih događaja,&nbsp; pomoću koincidentnog<br />sistema u čijem sklopu se nalazi HPGe detektor i&nbsp; plastični scintilator, u<br />povr&scaron;inskoj laboratoriji. Ustanovljeno je da se promptni i zakasneli<br />koincidentni događaji između plastičnog &ldquo;veto&rdquo; detektora i<br />germanijumskog detektora mogu jasno razdvojiti u dve grupe, za oko<br />100 ns. Dodatno, zakočno zračenje i&nbsp; anihilacioni događaji mogu se<br />razdvojiti u vremenu od (n,n&rsquo;) događaja, iako svi ovi događaji pripadaju<br />grupi zakasnelih događaja. Takođe, registrovani su&nbsp; i&nbsp; značajno zakasneli<br />anihilacioni događaji, koji nastaju usled raspada zaustavljenih pozitivnih<br />miona.<br />Drugi eksperiment prikazan u ovoj disertaciji baziran je na ultra-niskofonskom HPGe spektrometru relativne efikasnosti 100%.<br />Dodatkom dva plastična scintilatora i brzo-sporog koincidentnog kola,<br />istraživani su koincidentni događaji između plastičnih scintilatora i<br />HPGe spektrometra. Ovaj spektrometarski sistem MIREDO <em>(Muon<br />Induced Rare Event Dynamic Observatory</em>) prvenstveno je namenjen<br />proučavanju procesa indukovanih kosmičkim mionima u različitim<br />materijalima. Analiza ovakvih interakcija može biti od značaja za ultra-niskofonske eksperimente. Rezultati dobijeni za tri ispitivana materijala,<br />pakovana u<em> Marinelli</em> sud, prezentovani su i diskutovani.<br />U trećem eksperimentu prikazanom u ovoj disertaciji ispitan je<br />potencijalni uticaj solarnih&nbsp; neutrina&nbsp; na izmerenu brzinu&nbsp; radioaktivnog<br />raspada,&nbsp; merenjem varijacija u brzini brojanja<br />³H&nbsp; metodom tečnog&nbsp;scintilacionog brojanja. Kori&scaron;ćenjem sofisticiranog tečnog scintilacionog&nbsp;spektrometra&nbsp;<em> Quantulus</em>&nbsp; ustanovljeno je da na merenje<br />visokoenergetskog dela&nbsp;³H spektra može značajno uticati nestabilnost<br />instrumenta. Oscilatorni karakter izmerenog visokoenergetskog dela<br />³H&nbsp;spektra&nbsp; je registrovan, ali sa veoma malom amplitudom (manjom od<br />0.5%), koja se ne može jednostavno objasniti samo nestabilno&scaron;ću<br />instrumenta.&nbsp; Kada je meren ukupan&nbsp;³H spektar, nisu nađene značajne<br />varijacije u brzini brojanja.<br />Već duže vreme je poznato da je niskoenergetsko gama zračenje<br />kontinualne distribucije prisutno na otvorenom prostoru, u vazduhu na<br />povr&scaron;ini Zemlje. U prethodnim istraživanjima pretpostavljano je da&nbsp; ovo<br />zračenje potiče skoro isključivo od gama fotona koji su emitovani usled<br />prirodne radioaktivnosti i potom rasejani u nazad od strane vazduha<br />iznad zemlje. U četvrtom eksperimentu prikazanom u ovoj disertaciji<br />pokazano je da&nbsp; je&nbsp; ovo zračenje (u energetskom regionu 30 keV-300<br />keV), sa maksimumom na oko&nbsp; 90 keV, u značajnoj meri&nbsp; proizvedeno<br />kosmičkim zračenjem, sa fluksom fotona od oko 3000 m^-2s^-1. Takođe,<br />ustanovljeno je da dozama op&scaron;te populacije doprinosi ovo sveprisutno<br />niskoenergetsko gama zračenja kosmičkog porekla, zajedno sa<br />odgovarajućim fluksom niskoenergetskih elektrona i da ove komponente<br />ukupnih doza indukovanih kosmičkim zračenjem na nivou mora nisu<br />zanemarljive.</p> / <p>In this dissertation results of complex research on cosmic-ray impact on&nbsp;nuclear spectra at sea level are shown.&nbsp; The appropriate selection of&nbsp;coincidence time interval &nbsp;in low-background experiments that are based&nbsp;on the rejection of anticoincidence background events is very important&nbsp;for reducing the influence of cosmic-ray muons on acquired spectral&nbsp;data. In&nbsp; the first&nbsp; experiment&nbsp; presented in this dissertation,&nbsp; performed by&nbsp;the coincidence system of an HPGe detector and a plastic detect or&nbsp; in a&nbsp;surface laboratory, the time resolution of the detected events is explored.&nbsp;It is&nbsp; found that the prompt and delayed coincidence events between a&nbsp;plastic veto detector and a &nbsp;Ge detector can be sharply divided for&nbsp;approximately 100 ns in two groups. In addition, the bremsstrahlung&nbsp;and annihilation events can&nbsp; be time-resolved from the (n,n&rsquo;) events,&nbsp;although all of these events belong to the group of delayed events. Also,&nbsp;substantially delayed annihilation events, which are caused by the&nbsp;<br />decays of stopped positive muons, were detected.<br />The second experiment shown in this dissertation is based on the 100%&nbsp;relative efficiency ultra-low-background HPGe spectrometer. With the&nbsp;addition of two plastic scintillators and a fast-slow coincidence circuit,&nbsp;the coincidence events between the plastic detectors and the HPGe&nbsp;spectrometer have been investigated. This&nbsp; MIREDO (Muon Induced&nbsp;Rare Event Dynamic Observatory) spectrometer system is primarily&nbsp;<br />developed for the study of cosmic muon induced processes in different&nbsp;materials. Exploration of such interactions can be important for ultra-low&nbsp;background experiments. Results derived for three samples, placed in a&nbsp;Marinelli beaker, are presented and discussed.<br />In third experiment shown in this dissertation,&nbsp; the potential influence of&nbsp;solar neutrinos on measured decay rate is investigated by&nbsp; the liquid&nbsp;scintillation measurement of the count rate variations of&nbsp;³H. Making use of the sophisticated Quantulus liquid scintillation spectrometer, it is&nbsp;found that the&nbsp; measurement of the high-energy tail of&nbsp;³H spectrum may be significantly influenced by instrumental&nbsp; instability.&nbsp; The oscillatory behavior of measured high-energy tail of ³H spectrum&nbsp; is registered, but&nbsp;with very small amplitude (less than 0.5%), which cannot&nbsp; be easily&nbsp;<br />explained only by instrumental instability. When the total&nbsp;³H spectrum was measured, no significant variations in the count rate were found.&nbsp;<br />For a long time, it has been known that low-energy continuous gamma&nbsp;radiation is present in open air at the Earth&rsquo;s surface. In previous&nbsp;investigations it was assumed that this radiation is produced almost&nbsp;exclusively by gamma photons emitted due to the natural radioactivity,&nbsp;which are backscattered by air above ground.&nbsp; In the fourth experiment&nbsp;presented in this dissertation, it is&nbsp; shown&nbsp; that significant amount of this&nbsp;<br />radiation (related to energy region 30&nbsp; keV-300&nbsp; keV) that peaks at about&nbsp;90 keV, is produced by cosmic-rays, with the photon flux of about 3000&nbsp;m^-2s^-1.&nbsp; Also, it is found&nbsp; that the contribution of this omnipresent low&nbsp;energy gamma radiation of cosmic-ray origin, including the&nbsp;corresponding low-energy electron flux, to the doses of general&nbsp;<br />population are non-negligible components of overall doses induced by&nbsp;cosmic rays near sea level.</p>