O Laboratório do Acelerador Linear do Instituto de Física da Universidade de São Paulo está desenvolvendo um estudo sobre a eficiência e a função resposta de detetores de HPGe a fótons de alta energia. Neste trabalho foi estudada a função resposta de fótons provenientes da reação 19F(p,alfa gama)16O. Na reação podem ser observados os fótons característicos de 6,1 MeV, 6,9 MeV e 7,1 MeV. Fótons com esta energia possuem um grande potencial para várias aplicações importantes, como \"Proton Induced Gamma-ray Emission\" (PIGE), gamagrafia e procedimentos de calibração. No caso de procedimentos de calibração essa reação possui um diferencial: o fluxo de fótons observado é bem maior do que em outras reações estudadas, tais como 27Al (p, gama)28Si e 23Na(p, gama)24Mg. Os experimentos foram realizados no Laboratório de Análise de Materiais por Feixes Iônicos (LAMFI) do IFUSP, utilizando um acelerador eletrostático tipo \"Pelletron-tandem\" de 1,7 MV de tensão máxima no terminal. O detetor estudado foi um HPGe do tipo coaxial \"reverse-electrode closed-end\" com 72,5 mm de diâmetro e 60,5 mm de comprimento e 60% da eficiência de um detetor de NaI para fótons de 1,332 MeV. O detetor foi posicionado a 0 grau em relação à linha de feixe. A corrente de prótons na irradiação era da ordem de 50 nA e a energia dos prótons variou entre 1,36 MeV e 1,42 MeV. O alvo utilizado consistia em 250 micro g/cm^2 de CaF2 evaporado em um suporte de Ta. Os picos dos três fótons da reação 19F(p,alfa gama)16O apresentaram deformações devido à emissão em vôo dos fótons. Essas deformações apresentam variações em função da energia dos prótons. Com o objetivo de descrever as formas dos picos foi desenvolvido um programa que utiliza a técnica de Monte Carlo para simulá-las. Os dados sobre \"yields\" relativos dos fótons e seção de choque da reação 19F(p,alfa gama)16O encontrados na literatura são imprecisos e contraditórios. Então, como parte dos resultados deste trabalho, foram obtidos os \"yields\" relativos dos fótons da reação 19F(p,alfa gama)16O para energias de prótons entre 1,360 MeV e 1,420 MeV. A função resposta do detetor para as diferentes formas dos picos foram obtidas através de simulações com o programa MCNP5. Para estas simulações foi feita uma descrição detalhada da geometria interna do detetor, obtida por meio de radiografias do mesmo. As intensidades relativas dos fótons da reação 19F(p,alfa gama)16O em função da energia dos prótons puderam ser obtidas através de um ajuste por mínimos quadrados das funções respostas simuladas aos espectros experimentais de altura de pulso. / In the 19F(p, alpha gamma)16O reaction, characteristic gamma-rays with energies: 6.1 MeV; 6.9 MeV and 7.1 keV can be observed. These photons can be used in many important applications such as Proton Induced Gamma-ray Emission (PIGE), gamma radiography and calibration purposes. It has another advantage in calibration procedures, which is the observed photon flux is greater than other reactions studied, 27Al(p, gamma)28Si and 23Na(p, gamma)24Mg. In our laboratory, we are studying the efficiency and response function of HPGe detectors for high energy photons, and for this it is necessary a source with a level scheme with a few gamma-ray transitions and known relative yields. The 19F(p, alpha gamma)16O reaction satisfies the first condition but in the literature we found relative yields for thick targets or reaction cross section for thin targets. However, we use targets of intermediate thickness, therefore in this work we measure the relative gamma-ray yields for protons with energies between 1.36 MeV and 1.42 MeV. The experiments were performed at the 1.7 MV Pelletron tandem accelerator of the Laboratório de Análise de Materiais por Feixes Iônicos (LAMFI) located at Instituto de Física da Universidade de São Paulo, using a reverse-electrode closed-end coaxial HPGe detector with 72.5 mm in diameter and 60.5 mm in length, at 0 degree. The proton irradiation current was 50 nA, and the target consisted of 250 micro g/cm^2 CaF2 evaporated on a 0.1 mm Ta backing. In this reaction the 20Ne resonant state fissions in flight, and the resulting 16O excited states have different half-lives; all observed peaks are deformed due to either Doppler broadening from 16O random velocity direction or Doppler shift from nuclei that leave the target toward the vacuum chamber. Moreover, the peak deformations vary with the proton energy. These deformations were modeled by a Monte Carlo simulation that follows the oxygen nuclei in its trajectory until photon emission, considering the changes in spatial distribution of the exact interaction point in the target with incident proton energy due to the large resonance width and proton energy loss, and 16O energy loss and multiple scattering until decay, in the different target layers. Using the detector response functions calculated by MCNP5 simulations, the relative intensities of the three gamma rays were obtained by a least square fit of the response functions, taking into account the Doppler broadening and shift for each gamma ray, to the data in the experimental pulse-height spectrum.

Ces travaux de thèse traitent de l'étude et de la validation d'un spectromètre gamma pour la mesure de la composition chimique des surfaces planétaires et ont été appliqués à la préparation d'une mission vers la planète Mercure. Ils ont permis de caractériser les performances d'un concept d'instrument basé sur un cristal de germanium ultra-pur (HPGe) refroidi activement à température cryogénique. Deux aspects critiques ont été particulièrement étudiés en liaison avec l'environnement extrême rencontré dans le Système Solaire interne. D'abord une caractérisation expérimentale et numérique des dommages radiatifs causés par les particules solaires dans les cristaux de germanium a été réalisée et a conduit à établir une procédure de récupération des performances. D'autre part, un modèle thermique numérique de l'instrument ainsi que des essais sur une maquette thermique ont été réalisés et valident le concept thermique de l'instrument.

A quantificação da atividade de radionuclídeos emissores de raios gama em amostras medidas por espectrometria gama com detectores HPGe depende da análise dos fotopicos presentes no espectro, especialmente da determinação exata das suas áreas líquidas. Tal análise é geralmente realizada com o auxílio de ferramentas de software proprietário. Este trabalho apresenta uma metodologia, descrição de algoritmos e um aplicativo de código aberto, denominado OpenGamma, para a busca e análise de fotopicos a fim de se obter seus parâmetros relevantes e as atividades dos radionuclídeos na amostra. A implementação computacional é distribuída sob licença aberta para o código principal e com o uso de pacotes de software aberto para o projeto da interface e para bibliotecas matemáticas. O procedimento para a busca de picos é realizado em três etapas. Primeiramente, executa-se uma pesquisa preliminar com o método da segunda diferença, que consiste na geração de um espectro derivado para a busca de picos candidatos. Na segunda etapa, calculam-se as larguras experimentais dos picos, dos quais escolhem-se aqueles bem formados e isolados para a obtenção da função de ajuste da largura vs. canal, por meio do método de Levenberg-Marquardt para ajustes não-lineares. Por fim, regiões do espectro com picos agrupados são delimitadas e novo ajuste não-linear é aplicado a cada região para a obtenção dos termos da linha de base e dos fotopicos. A partir destes termos, são calculadas as áreas líquidas dos picos. Para a determinação da atividade, curvas de calibração de eficiência previamente obtidas, bem como dados de transições gama dos radionuclídeos, são incorporadas ao código e aplicadas. O código foi escrito em linguagem C++ e a interface foi desenvolvida com a ferramenta Qt. Para as funções matemáticas e procedimentos de ajuste, foi usada a biblioteca científica GNU (GSL). A validação de código foi feita por meio da análise de: 1) espectros sintéticos de teste da AIEA, especialmente desenhados para a avaliação de desempenho de software; 2) espectros obtidos com amostras de exercícios de intercomparação e 3) espectros da rotina de trabalho do Laboratório de Radiometria Ambiental (LRA) do IPEN e analisados com o aplicativo comercial InterWinner. Os resultados obtidos são consistentes com os valores de referência e com aqueles obtidos pelo aplicativo citado, sugerindo que o código OpenGamma pode ser utilizado com segurança na espectrometria de raios gama de uso geral. / Radioactivity quantification of gamma-ray emitter radionuclides in samples measured by HPGe gamma-ray spectrometry relies on the analysis of the photopeaks present in the spectra, especially on the accurate determination of their net areas. Such a task is usually performed with the aid of proprietary software tools. This work presents a methodology, algorithm descriptions and an open source application, called OpenGamma, for the peak search and analysis in order to obtain the relevant peaks parameters and radionuclides activities. The computational implementation is released entirely in open-source license for the main code and with the use of open software packages for interface design and mathematical libraries. The procedure for the peak search is performed on a three step approach. Firstly a preliminary search is done by using the second-difference method, consisting in the generation of a derived spectrum in order to find candidate peaks. In the second step, the experimental peaks widths are assessed and well formed and isolated ones are chosen to obtain a FWHM vs. channel relationship, by application of the Levenberg-Marquardt minimization method for non-linear fitting. Lastly, regions of the spectrum with grouped peaks are marked and a non-linear fit is again applied to each region to obtain baseline and photopeaks terms; from these terms, peaks net areas are then assessed. For the activity determination, previously obtained efficiency calibration curves, as well as nuclides gamma-ray data, are incorporated in the code and applied. The code was developed in C++ language and the interface was developed with Qt GUI software toolkit. GNU scientific library, GSL, was employed to perform fitting procedures as needed. Validation of code was done by analyzing: 1) synthetic test spectra from IAEA, especially designed for software performance evaluation; 2) spectra obtained from samples of intercomparison exercises and 3) spectra from routine activities of the Environmental Radiometric Laboratory (LRA) at IPEN and analyzed with the commercial software package InterWinner. Results obtained are consistent with the reference values and with those obtained by the aforementioned package. The results suggest that the OpenGamma code could be safely used in general-purpose gamma-ray spectrometry.

A quantificação da atividade de radionuclídeos emissores de raios gama em amostras medidas por espectrometria gama com detectores HPGe depende da análise dos fotopicos presentes no espectro, especialmente da determinação exata das suas áreas líquidas. Tal análise é geralmente realizada com o auxílio de ferramentas de software proprietário. Este trabalho apresenta uma metodologia, descrição de algoritmos e um aplicativo de código aberto, denominado OpenGamma, para a busca e análise de fotopicos a fim de se obter seus parâmetros relevantes e as atividades dos radionuclídeos na amostra. A implementação computacional é distribuída sob licença aberta para o código principal e com o uso de pacotes de software aberto para o projeto da interface e para bibliotecas matemáticas. O procedimento para a busca de picos é realizado em três etapas. Primeiramente, executa-se uma pesquisa preliminar com o método da segunda diferença, que consiste na geração de um espectro derivado para a busca de picos candidatos. Na segunda etapa, calculam-se as larguras experimentais dos picos, dos quais escolhem-se aqueles bem formados e isolados para a obtenção da função de ajuste da largura vs. canal, por meio do método de Levenberg-Marquardt para ajustes não-lineares. Por fim, regiões do espectro com picos agrupados são delimitadas e novo ajuste não-linear é aplicado a cada região para a obtenção dos termos da linha de base e dos fotopicos. A partir destes termos, são calculadas as áreas líquidas dos picos. Para a determinação da atividade, curvas de calibração de eficiência previamente obtidas, bem como dados de transições gama dos radionuclídeos, são incorporadas ao código e aplicadas. O código foi escrito em linguagem C++ e a interface foi desenvolvida com a ferramenta Qt. Para as funções matemáticas e procedimentos de ajuste, foi usada a biblioteca científica GNU (GSL). A validação de código foi feita por meio da análise de: 1) espectros sintéticos de teste da AIEA, especialmente desenhados para a avaliação de desempenho de software; 2) espectros obtidos com amostras de exercícios de intercomparação e 3) espectros da rotina de trabalho do Laboratório de Radiometria Ambiental (LRA) do IPEN e analisados com o aplicativo comercial InterWinner. Os resultados obtidos são consistentes com os valores de referência e com aqueles obtidos pelo aplicativo citado, sugerindo que o código OpenGamma pode ser utilizado com segurança na espectrometria de raios gama de uso geral. / Radioactivity quantification of gamma-ray emitter radionuclides in samples measured by HPGe gamma-ray spectrometry relies on the analysis of the photopeaks present in the spectra, especially on the accurate determination of their net areas. Such a task is usually performed with the aid of proprietary software tools. This work presents a methodology, algorithm descriptions and an open source application, called OpenGamma, for the peak search and analysis in order to obtain the relevant peaks parameters and radionuclides activities. The computational implementation is released entirely in open-source license for the main code and with the use of open software packages for interface design and mathematical libraries. The procedure for the peak search is performed on a three step approach. Firstly a preliminary search is done by using the second-difference method, consisting in the generation of a derived spectrum in order to find candidate peaks. In the second step, the experimental peaks widths are assessed and well formed and isolated ones are chosen to obtain a FWHM vs. channel relationship, by application of the Levenberg-Marquardt minimization method for non-linear fitting. Lastly, regions of the spectrum with grouped peaks are marked and a non-linear fit is again applied to each region to obtain baseline and photopeaks terms; from these terms, peaks net areas are then assessed. For the activity determination, previously obtained efficiency calibration curves, as well as nuclides gamma-ray data, are incorporated in the code and applied. The code was developed in C++ language and the interface was developed with Qt GUI software toolkit. GNU scientific library, GSL, was employed to perform fitting procedures as needed. Validation of code was done by analyzing: 1) synthetic test spectra from IAEA, especially designed for software performance evaluation; 2) spectra obtained from samples of intercomparison exercises and 3) spectra from routine activities of the Environmental Radiometric Laboratory (LRA) at IPEN and analyzed with the commercial software package InterWinner. Results obtained are consistent with the reference values and with those obtained by the aforementioned package. The results suggest that the OpenGamma code could be safely used in general-purpose gamma-ray spectrometry.

A técnica de análise por ativação com nêutrons instrumental tem sido amplamente utilizada pelo Laboratório de Ativação Neutrônica (LAN) do IPEN, com emprego do método comparativo, utilizando-se como fonte de nêutrons o reator de pesquisa do tipo piscina IEA-R1, do Instituto de Pesquisas Energéticas e Nucleares (IPEN). Neste método uma amostra é irradiada, simultaneamente, com um padrão do elemento a ser determinado. Para contornar a dificuldade de uma análise multielementar, por ser necessário preparar vários padrões, foi desenvolvido o método k0 de ativação neutrônica. No método k0 a concentração dos elementos de interesse da amostra é calculada em relação a um elemento comparador, geralmente o ouro. Todavia, esse método requer, com precisão, a eficiência de detecção no intervalo de energia de interesse e na geometria do arranjo experimental. Para contornar o tratamento manual dos dados em planilhas eletrônicas, passíveis de incidência de erros, foi desenvolvido, então, um software web, com acesso de qualquer dispositivo com Internet, livre, para calibração da eficiência absoluta de detectores do tipo HPGe. Utilizou-se a linguagem de programação Python, livre, de baixa curva de aprendizagem e padronizada no projeto eScience, a qual o referido software faz parte, e o framework web Django. No sistema é possível realizar todos os cadastros das informações utilizadas no cálculo da eficiência. Além de calcular a eficiência, o sistema plota o gráfico com os pontos da eficiência, linha de regressão, com possibilidade de ajustes, e barra de erro representando as incertezas. Como parte integrante do projeto e-science, o software emite relatórios referentes aos dados dos espectros e da eficiência, permitindo seu compartilhamento. / The technique of instrumental neutron activation analysis has been widely used by IPEN\'s Neutron Activation Laboratory (LAN), using the comparative method, using the IEA-R1 pool-type research reactor as the neutron source Energy and Nuclear Research (IPEN). In this method a sample is simultaneously irradiated with a pattern of the element to be determined. In order to overcome the difficulty of a multielementary analysis, because it isnecessary to prepare several standards, the k0 method of neutron activation was developed. In method k0 the concentration of the elements of interest of the sample is calculated in relation to a comparator element, generally gold. However, this method accurately requires the detection efficiency in the energy range of interest and the geometry of the experimental arrangement. In order to circumvent the manual processing of the data in electronic spreadsheets, which could lead to errors, a web software was developed with access from any free Internet device for calibration of the absolute efficiency of HPGe type detectors. It was used the free and low learning curve, Python programming language, standardized in the eScience project, to which the software is part, and the Django web framework. In the softwareit is possible to carry out all the registers of the information used in the calculation of the efficiency. In addition to calculating efficiency, the software plots the graph with the efficiency points, regression line, with possibility of adjustments, and error bar representing the uncertainties. As part of the e-science project, the software issues reports on spectra and efficiency data, allowing it to share.

Abstract My thesis examines the measurement optimalization when the semiconductor HPGe detectors with a low background and a high relative efficiency are used for achieving low values of MDA (minimum detectable activity). I conducted my research in the Department of Spectrometry of SÚRO (National Radiation Protection Institute) in Prague. In this laboratory the standard geometries of detectors with lower efficiency are used. The aim of this thesis is to offer a proposal of new geometry, sizes and shapes of measurement cells which will better correspond with the demand for higher efficiency of updated detectors. The assignment was to find the best mathematical function to descibe the correlation between efficiency and the direction of the radiation point source towards the detector. This function is derived from experimentally obtained data. To conduct measurements, three kinds of detectors with high relative efficiency used for activity measurements at different geometries were selected. As the source of gamma radiation, the point sources with energies of 46 keV, 661 keV, 1332 keV in different distances and positions were used. The function was applied separatelly to each of the three detectors and to the areas above the detector and sidewards of the detector. The objective of the research was to project new measurement geometries or to optimalize the current ones which could be used also in other detectors with high efficiency. After integrating the function in the cylindrical area above the detector and the annular area sidewards of the detector, areas contributing substantially to the overall efficiency were determined. These areas may be considered to be the optimal sizes for new geometries in given positions. After combining all the optimal areas above the detector, sidewards of the detector and for selected energies and the detector, optimal sizes of a new geometry were found. The function can be used both in the front part and the side part of the detector but its validity is limited. The value of MDA for the particular geometry is in indirect proportion to the efficiency square root and thus this new geometry should lead to minimum values of MDA.

With the complex composition of the radioisotopes and waste materials, the characterization of the volumetric low-level wastes from CANDU plants is challenging. This study presents a technique to localize and quantify the contaminations presented in the CANDU waste containers. MCNP-based models are developed for an N-type coaxial HPGe detector and a LaBr3 detector to simulate the photon peak information. The simulated efficiency and the experimental count rates are combined to estimate the activity of unknown waste samples. During the spectrum collection of a 4L Marinelli beaker source and 1-quart waste samples, the MCNP algorithm showed better accuracy in activity estimation than the Mirion ISOCS/LabSOCS software. With further development, this method has the potential to outperform the popular commercial software in estimating activity for volume sources with complex geometry and uneven distribution. The multi-detector array models with hotspot designs are also studied in this work to provide real-time information about the location and activity of the contamination inside the 2.2 m3 industrial low-level waste containers. The on-site measurements show promising results as the position of the contamination was able to be located within a volume of 61×40×34 cm. Overall, this technique has good potential to be utilized in the nuclear industry for large-volume low-level waste analysis. / Thesis / Master of Science (MSc)

The CNO cycle consists of a set of nuclear reactions that convert hydrogen into helium and releases energy in stars. The cycle contributes less than 1% to our Sun's luminosity, but it is responsible for detectable neutrino fluxes that can bring direct information of the physical conditions in the solar core, provided that the nuclear reaction rate is known with sufficient precision. The 14N(p,γ)15O is the slowest reaction in the CNO cycle and estabilishes its rate. The experimental study has been performed both at the LUNA 400 kV accelerator deep underground in the Gran Sasso mountain in Italy and at a 3 MV Tandetron in the Helmholtz-Zentrum Dresden-Rossendorf. A proton beam was sent on solid TiN targets and the prompt photons were collected by a composite HPGe detector (at LUNA) or by up to four HPGe detectors (Dresden). The obtained results improve the fit of the excitation function in the R-matrix framework, that is used to extrapolate the S-factor at the very low astrophysical energies. In addition, the strength of two resonances at Ep = 430 and 897 keV of the 15N(p,αγ)12C reaction were measured, improving the precision for hydrogen depth profiling.

La spectrométrie gamma à haute résolution offre un outil d’analyse performant pour effectuer des mesurages environnementaux. Dans le cadre de la caractérisation radiologique d’un site (naturelle ou artificielle) ainsi que pour le démantèlement d’installations nucléaires, la cartographie des radionucléides est un atout important. Le principe consiste à déplacer un spectromètre HPGe sur le site à étudier et, à partir des données nucléaires et de positionnements, d’identifier, de localiser et de quantifier les radionucléides présents dans le sol. Le développement de cet outil fait suite à une intercomparaison où un exercice orienté intervention a montré les limites des outils actuels. Une partie de ce travail s’est portée sur la représentation cartographique des données nucléaires. La connaissance des paramètres d’un spectre in situ a permis la création d’un simulateur modélisant la réponse d’un spectromètre se déplaçant au-dessus d’un sol contaminé. Ce simulateur a lui-même permis de développer les algorithmes de cartographie et de les tester dans des situations extrêmes et non réalisables. Ainsi, ce travail ouvre sur la réalisation d’un prototype viable donnant en temps réel les informations nécessaires sur l’identité et la position possible des radionucléides. La recherche réalisée sur la déconvolution des données permet de rendre en post traitement une carte de l’activité du sol par radionucléide mais également une indication sur la profondeur de la source. Le prototype nommé OSCAR (Outil Spectrométrique de Cartographie de Radionucléides) a ainsi été testé sur des sites contaminés (Suisse et Japon) et les résultats obtenus sont en accord avec des mesures de référence. / The high-resolution gamma spectrometry currently provides a powerful analytical tool for performing environmental measurements. In the context of radiological characterization of a site (natural or artificial radioactivity) and for the dismantling of nuclear installations, mapping of radionuclides is an important asset. The idea is to move a HPGe spectrometer to study the site and from nuclear and position data, to identify, to locate and to quantify the radionuclides present in the soil. The development of this tool follows an intercomparaison (ISIS 2007) where an intervention / crisis exercise showed the limits of current tools. The main part of this research project has focused on mapping of nuclear data. Knowledge of the parameters of an in situ spectrum helped to create a simulator modeling the response of a spectrometer moving over contaminated soil. The simulator itself helped to develop algorithms for mapping and to test them in extreme situations and not realizable. A large part of this research leads to the creation of a viable prototype providing real-time information concerning the identity and locality as possible radionuclides. The work performed on the deconvolution of data can make in post processing a map of the activity of radionuclide soil but also an indication of the depth distribution of the source. The prototype named OSCAR was tested on contaminated sites (Switzerland and Japan) and the results are in agreement with reference measurements.

The CNO cycle consists of a set of nuclear reactions that convert hydrogen into helium and releases energy in stars. The cycle contributes less than 1% to our Sun's luminosity, but it is responsible for detectable neutrino fluxes that can bring direct information of the physical conditions in the solar core, provided that the nuclear reaction rate is known with sufficient precision. The 14N(p,γ)15O is the slowest reaction in the CNO cycle and estabilishes its rate. The experimental study has been performed both at the LUNA 400 kV accelerator deep underground in the Gran Sasso mountain in Italy and at a 3 MV Tandetron in the Helmholtz-Zentrum Dresden-Rossendorf. A proton beam was sent on solid TiN targets and the prompt photons were collected by a composite HPGe detector (at LUNA) or by up to four HPGe detectors (Dresden). The obtained results improve the fit of the excitation function in the R-matrix framework, that is used to extrapolate the S-factor at the very low astrophysical energies. In addition, the strength of two resonances at Ep = 430 and 897 keV of the 15N(p,αγ)12C reaction were measured, improving the precision for hydrogen depth profiling.