Submitted by HIGOR HENRIQUE DE SOUZA OLIVEIRA null (higor6@itelefonica.com.br) on 2016-03-14T01:11:55Z No. of bitstreams: 1 Tese de Doutorado.pdf: 10715169 bytes, checksum: 67bc136f2489ae6944e6a9db6998967a (MD5) / Approved for entry into archive by Sandra Manzano de Almeida (smanzano@marilia.unesp.br) on 2016-03-15T17:52:52Z (GMT) No. of bitstreams: 1 oliveira_hhs_dr_araiq_par.pdf: 1487328 bytes, checksum: dc6bd8f68483e98dd23a89fc9938b22d (MD5) / Made available in DSpace on 2016-03-15T17:52:52Z (GMT). No. of bitstreams: 1 oliveira_hhs_dr_araiq_par.pdf: 1487328 bytes, checksum: dc6bd8f68483e98dd23a89fc9938b22d (MD5) Previous issue date: 2016-02-24 / Luminescência é a emissão de luz decorrente da excitação de átomos, íons, moléculas ou materiais. Quando a excitação é realizada por radiações ionizantes, o material luminescente é denominado cintilador e possui aplicações tecnológicas relacionadas à detecção dessas radiações de alta energia. A conformação desses materiais tem impacto direto em seu custo e aplicabilidade e atualmente, há uma busca por novas conformações de materiais luminescentes para aplicação em diversos dispositivos. Sistemas bidimensionais, como filmes finos nanoestruturados, possuem potencial aplicação em nanotecnologia e os processos de auto-organização desses sistemas têm sido crescentemente estudados e empregados. Neste trabalho, as propriedades luminescentes do polioxometalato [Eu(W5O18)2]9- foram estudadas em função de sua conformação em sólido estendido, filmes de Langmuir e de Langmuir-Blodgett, com ênfase em medidas de luminescência com excitação por radiação ultravioleta ou raios X. O sólido Na9[Eu(W5O18)2].14H2O foi preparado pela mistura de soluções de tungstato de sódio e nitrato de európio em pH e temperatura adequados. Medidas de espectroscopia de fotoluminescência do sólido evidenciam a presença de íons Eu3+ ao menos em dois sítios não-centrossimétricos, sendo um deles de menor simetria com relação ao outro. Com o aumento da temperatura, as distorções provocadas pelas vibrações térmicas e pela saída das moléculas de água de hidratação diminuem a simetria local ao redor dos íons Eu3+ em ambos os sítios. As mudanças nas propriedades luminescentes decorrentes do aumento da temperatura são irreversíveis a partir de 100oC, temperatura na qual inicia-se a desidratação do sólido. A excitação via transferência de carga dos ligantes para os metais favorece a emissão proveniente dos íons Eu3+ nos sítios menos distorcidos enquanto a excitação direta nos níveis intraconfiguracionais dos íons Eu3+ favorece a emissão proveniente dos íons Eu3+ nos sítios mais distorcidos. O mecanismo de cintilação nesse sólido tem contribuição significativa do processo de transferência de energia de estados relacionados à transferência de carga para os níveis excitados dos íons Eu3+ e a eficiência desse processo diminui com a incidência de raios X, provavelmente devido à criação de defeitos eletrônicos nos grupos (W5O18)6-, levando à diminuição da eficiência do processo de absorção e transferência de energia para os íons Eu3+ e consequentemente, à diminuição da intensidade de emissão em função do tempo de exposição à radiação X. Os filmes de Langmuir do sistema misto surfactante/polioxometalato assumem empacotamento compacto, estável e parcialmente reversível na interface subfase-ar. O sistema projetado e montado pelo grupo de pesquisa do Laboratório de Materiais Luminescentes para a realização de medidas de espectroscopia de fotoluminescência com excitação ultravioleta in situ na cuba de Langmuir-Blodgett permite correlacionar as propriedades luminescentes de filmes de Langmuir com os diferentes níveis de organização da monocamada, sendo uma poderosa ferramenta na caracterização desses filmes. Os filmes de Langmuir-Blodgett do sistema misto surfactante/polioxometalato foram preparados com elevada taxa de transferência e apresentam intensidade de emissão linearmente dependente do número de camadas depositadas. Nestes filmes, os íons Eu3+ ocupam ao menos dois sítios não-centrossimétricos com tempos de vida distintos e a variação da temperatura provoca alterações quase completamente reversíveis em suas propriedades luminescentes. / Luminescence is the emission of light resulting from the excitation of atoms, ions, molecules or materials. When ionizing radiation is used in the excitation, the luminescent material is called scintillator and has technological applications related to the detection of these high energy radiations. The conformation of these materials has direct impact on theirs cost and applicability and currently, there is a search for new conformations of luminescent materials for application in several devices. Two-dimensional systems, as nanostructured thin films, have potential applications in nanotechnology and the self-assembly processes of these systems have been increasingly studied and employed. In this work, the luminescent properties of the polyoxometalate [Eu(W5O18)2]9- were studied as a function of its conformation in solid bulk, Langmuir and Langmuir-Blodgett films, with emphasis on X-ray- and UV-excited luminescence measurements. Solid Na9[Eu(W5O18)2].14H2O was prepared by mixing sodium tungstate and europium nitrate solutions in suitable temperature and pH. Photoluminescence measurements of the solid sample evidence the presence of Eu3+ ions at least two non-centrosymmetric sites. With increasing temperature, the distortions caused by thermal vibration and dehydration process decrease the local symmetry around the Eu3+ at both sites. Changes in the luminescent properties are irreversible after temperatures above 100°C, temperature at which it begins the solid dehydration. Ligand to metal charge transfer excitation promotes the emission from the Eu3+ ions at less distorted site while the direct excitation in intraconfigurational levels of Eu3+ ions promote the emission from the Eu3+ ions at more distorted site. The scintillation mechanism of this solid has significant contribution of the energy transfer process from charge transfer states to the excited levels of Eu3+ ions and the efficiency of this process decreases by the incidence of X-rays, probably due to the creation of electronic defects at groups (W5O18)6-, decreasing the efficiency of the absorption and energy transfer processes and consequently, decreasing the emission intensity with the exposure to X-rays. Langmuir films of the surfactant/polyoxometalate system assume compact, stable and partially reversible packaging at the subphase-air interface. The system to performing in situ photoluminescence spectroscopy at Langmuir-Blodgett trough, designed by research group of the Luminescent Materials Laboratory, allows the correlation between the luminescent properties of Langmuir films and the monolayer organization level, being a powerful tool in the characterization of these films. Langmuir-Blodgett films of the surfactant/polyoxometalate system were prepared with high transfer rate and the films present emission intensity linearly dependent on the number of deposited layers. In these films, Eu3+ ions occupy at least two non-centrosymmetric sites with different lifetimes and the temperature variation causes almost completely reversible changes in their luminescent properties.

In the present work a new synthesis route, a hybrid between solid state reaction and proteic sol-gel method, is applied to a scintillator material based on Ca2Al2SiO7 (CAS). The luminescence mechanisms for the nanostructured scintillator is studied a mechanism that describes the luminescence process, when excited with X-rays, is proposed. The same system was also prepared via other 2 different methodologies, solid state traditional route, proteic sol-gel route, and 3 different solvents were used, for comparison in the hybrid method. In all cases the CAS phase was found as indicated by X-ray powder diffraction. During the thermal evolution of CAS precursors prepared via hybrid route assisted by coconut water, intermediate oxide phases were formed and they reacted with SiO2 to form the final CAS phase. SEM images indicated that the organic molecules present in the coconut water play an important role in the nanoparticle formation defining the average size and morphology, Samples prepared via the hybrid route showed particle with spherical shape with average size of (36 ± 15) nm. Analysis carried out via photoemission spectroscopy indicated that Si ions are the most abundant cation on surface of the particles produces via hybrid methods and solid state reaction. X-ray absorption (XAS) revealed that the Si coordination environment did not change during the synthesis. The XAS technique also indicated that the main valence for the dopants in CAS structure and the emission spectra obtained via pholuminescence and X-ray excited optical luminescence (XEOL) confirmed that the main emissions are related to the dopants on the CAS matrix. Extended X-ray absorption fine structure revealed the location of the dopants in the CAS matrix, and the most probable defect generated for the dopant presence. XEOL excitation spectra showed different behaviors for the luminescence around K edge of the matrix elements. The XEOL decay time indicated that fast scintillators were produced when CAS were doped with Ce3+ with characteristic constants lower than 40 ns. The results time dependent XEOL emission also showed that the luminescence decay curves are influenced by the presence of electrons and holes shallow traps in the CAS electronic structure. / No presente trabalho uma nova rota de síntese, híbrida entre as sínteses de estado sólido e sol-gel proteico, é aplicada a um material cintilador baseado na matriz cristalina Ca2Al2SiO7 (CAS). Adicionalmente, o mecanismo de luminescência destes cintiladores nanoestruturados é estudado e um modelo é proposto. Para efeito de comparação com a rota de síntese híbrida, amostras foram também preparadas por sol-gel proteico e síntese de estado sólido, e com a variação do solvente na síntese híbrida. Os resultados de difração de raios X mostraram que as amostras apresentaram a fase cristalina de Ca2Al2SiO7 após calcinação acima de 1300°C. Durante a evolução térmica dos precursores preparados pelo método híbrido assistido por água de coco, fases cristalinas intermediárias são formadas e estas reagem com o SiO2, até a formação do CAS. As imagens obtidas por microscopia eletrônica de varredura indicaram que as moléculas orgânicas presentes na água de coco são decisivas no controle do tamanho e morfologia das nanopartículas obtidas pelo método híbrido, e as partículas apresentam formato esférico e tamanho médios de (36 ± 15) nm. A espectroscopia de fotoemissão revelou que o Si é o elemento mais abundante na superfície das amostras produzidas pelos métodos híbridos e síntese de estado sólido. Enquanto a absorção de raios X (XAS) mostrou que a coordenação do Si não muda durante a síntese. A XAS também indicou as valências mais abundantes dos íons dopantes do CAS e os espectros de emissão fotoluminescente e de luminescência óptica estimulada por raios X (XEOL) confirmaram que estes são os canais luminescentes dos materiais. Com a análise da estrutura fina de absorção de raios X foi possível localizar os sítios ocupados pelos dopantes no CAS, assim como estimar o tipo de defeito mais provável, gerado pela presença destes íons. Os espectros de excitação XEOL mostraram comportamentos diferentes para a luminescência na região das bordas K de absorção dos elementos da matriz. As medidas de tempo de decaimento da luminescência indicaram a obtenção de cintiladores muito rápidos, com constantes características menores que 40 ns em todas as amostras que contém Ce3+ e que o processo de decaimento também está associado à presença de armadilhas de portadores de cargas na estrutura eletrônica do material.

Made available in DSpace on 2014-10-09T12:28:29Z (GMT). No. of bitstreams: 0 / Made available in DSpace on 2014-10-09T13:56:14Z (GMT). No. of bitstreams: 0 / 90Y (T1/2 = 2,67 dias; Eβmáx = 2,28 MeV) é um radionuclídeo com eficácia estabelecida para diversas terapias de câncer, marcando biomoléculas e no tratamento da radiosinovectomia. Devido às suas propriedades nucleares, é obtido através do decaimento do 90Sr (T1/2 = 28 anos), na forma de um gerador. Vários tipos de geradores de 90Sr/90Y foram desenvolvidos, e os mais empregados são os que usam resinas de troca catiônica, onde Sr e Y são adsorvidos e 90Y é seletivamente eluído com acetato ou EDTA. A desvantagem deste tipo de gerador é a radiólise, que degrada o seu uso. O gerador eletroquímico é uma solução proposta devido ao fato de não haver efeitos significativos da radiação sobre o próprio gerador. Neste conceito, a diferença entre os potenciais eletroquímicos dos elementos Y e Sr é utilizada para se obter uma rápida separação do 90Y do 90Sr. A produção de 90Y via formação de colóides é o método mais simples para a separação, baseando-se na formação de colóides de Y em pH altamente alcalino, podendo ser filtrado e separado do Sr, sendo posteriormente dissolvido em HCl. O objetivo deste trabalho consistiu no desenvolvimento de tecnologias para o preparo de geradores de 90Sr/90Y, onde foram desenvolvidos três tecnologias, a saber: geradores do tipo coluna utilizando resinas catiônicas, geradores via formação de colóides e geradores eletroquímicos. Foram também avaliadas metodologias para o controle de qualidade radionuclídico do 90Y dos geradores desenvolvidos: cintilação líquida, identidade radionuclídica, cromatografia por extração em papel (EPC) utilizando complexantes para 90Y e técnica por Espectrometria de Emissão Ótica com Plasma Indutivamente Acoplado (ICPOES). Os resultados mostraram que os geradores utilizando resinas catiônicas obtiveram os melhores resultados em relação ao rendimento e eficiência (~ 83%) de eluição, reprodutibilidade e a pureza radionuclídica. O gerador eletroquímico mostrou um potencial para o desenvolvimento, tendo a vantagem de não sofrer os efeitos da radiólise do par 90Sr/90Y, como acontece com a resina. Das metodologias de controle qualidade radionuclídica estudadas, uma comparação e avaliação mostrou que a EPC é muito sensível e permite a avaliação praticamente instantânea da qualidade do 90Y eluído dos geradores. / Dissertacao (Mestrado) / IPEN/D / Instituto de Pesquisas Energeticas e Nucleares - IPEN-CNEN/SP

Luminóforos inorgânicos contendo Terras Raras (TR) apresentam um papel importante como detectores de radiação ionizante, aplicados em diagnósticos médicos por imagem, como radiologia e tomografia. A função dos luminóforos é transformar os fótons da radiação de alta energia absorvidos (raios X ou ?) em fótons de luz visível, promovendo melhor qualidade de imagem e, conseqüentemente menor tempo de exposição do paciente à radiação. Os luminóforos de TR consistem de uma matriz hospedeira onde estão presentes íons de TR como Lu, La, Y ou Gd e de um íon ativador (que emite luz na região visível do espectro) como Eu3+, Tb3+, Tm3+ ou Ce3+, por exemplo. Luminóforos contendo íons Ce3+ como ativador são alvo de várias pesquisas relacionadas com detecção de radiação ionizante, devido às rápidas transições 5 d ? 4 f (tempo de resposta de ~ 10 a 100 ns) e emissão de luz na região do azul ou verde, requisitos esperados para um eficiente luminóforo para tal aplicação. Este trabalho apresenta a preparação de luminóforos de TR, dopados com Ce3+ ou Tm3+, na forma de pó, por diferentes métodos de síntese, como os métodos de combustão e Pechini e também por processo sol-gel. Aluminatos de TR (Lu3Al5O12 e Y3Al5O12) dopados com cério ou túlio foram obtidos pela reação de combustão entre precursores nitrato com uréia ou glicina sob aquecimento, ou pela síntese de polímeros de ácido cítrico com etilenoglicol contendo íons TR e alumínio (método Pechini). Em ambos os métodos os compostos foram obtidos por calcinação a temperaturas baixas quando comparadas às dos métodos convencionais. Silicatos de TR (Gd2SiO5, Lu2SiO5 e Y2SiO5) dopados com cério ou túlio foram preparados pelo método sol-gel convencional, por reação entre tetraetóxisilano (TEOS), etanol, água e nitratos metálicos, sob catálise básica, e por um método sol-gel modificado utilizando um polímero precursor. Neste último procedimento, TEOS, etanol e água reagiram juntamente com um sal orgânico de TR, álcool polivinílico (PVA) e uréia como combustível, produzindo um gel. Posterior calcinação levou à formação do silicato. A caracterização dos compostos foi realizada por análises de difratometria de raios X pelo método do pó (DRX), microscopia de eletrônica de varredura (MEV) ou de transmissão (MET), EDX, excitação e emissão no UV-Vis e tempo de vida de luminescência. Para os aluminatos dopados com cério foram ainda realizados espectros de emissão sob excitação por raios X. Os métodos de síntese utilizados se mostraram eficientes para obtenção de luminóforos na forma de pó nanométrico, com exceção do método sol-gel modificado, pois para algumas amostras observou-se a formação de mistura de fases. Os compostos dopados com cério apresentaram excitação e emissão características desse íon na região do verde ou azul do espectro visível, dependendo da matriz, com tempos de vida menores que 100 ns. Já aqueles dopados com túlio apresentaram emissão característica do íon, na região do azul, porém com tempos de vida da ordem de microssegundos. / Rare Earth (RE) inorganic phosphors play an important role as ionizing radiation detectors when applied to medical imaging techniques like radiology and tomography. These phosphors is to convert the high energy radiation absorbed photons (X or ?-rays) into visible photons, leading to better quality images and reducing the time the patient is exposed to radiation. RE phosphors consist of a host lattice where RE ions such as Lu, La, Y, or Gd are present, as well as activator ions (which emit light in the visible range of the spectrum) such as Eu3+, Tb3+, Tm3+, or Ce3+. Cerium-doped phosphors have been the target of several researches related with ionizing radiation detection due to their 5d - 4 f fast transitions (decay time in the ~ 10 to 100 ns range) and due to the fact that they emit light in the blue or green region of the spectrum, which is required for to the efficient phosphors to be applied in the detection of X or ?-rays. This work presents the synthesis of RE phosphor powders doped with Ce3+ or Tm3+, through different synthetic methods: combustion, Pechini, and sol-gel. RE aluminates (Lu3Al5O12 and Y3Al5O12) doped with Ce or Tm were prepared by combustion reaction between nitrate precursors and urea or glycine under heating. They were also obtained via the synthesis of polymers using citric acid, ethileneglycol, RE3+ and Al3+ ions (Pechini method). In both cases, the compounds were obtained by calcination at lower temperatures than those used inconventional methods. RE silicates (Gd2SiO5, Lu2SiO5 e Y2SiO5) doped with Ce or Tm were synthesized by the conventional sol-gel method using tetraethoxisylane (TEOS), ethanol and water, under basic catalysis, and also by a modified sol-gel route that uses a polymeric precursor. In the latter one, TEOS, ethanol and water were reacted with an organic RE salt, polyvinyl alcohol (PVA), and urea was used as fuel, thus yielding a gel. After calcination, we observed silicate formation. Characterization of the compounds was performed by X-ray diffractometry (XRD ? powder method), scanning or transmission electron microscopy (SEM or TEM), energy dispersive X-ray (EDX), luminescence spectroscopy in the UV-Vis range and lifetime analyses. For the cerium doped aluminates, emission spectra under X-ray excitation were also obtained. The synthetic methods used here showed to be efficient for the preparation of nanometric phosphor powders except for the modified sol-gel route, because in this case formation of a mixture of phases was observed for some samples. The Ce-doped compounds exhibited excitation and emission features of this ion in either the green or blue region of the visible spectrum, depending on the matrix, with lifetime values lower than 100 ns. However, the Tm-doped compounds displayed the blue emission typical of Tm ions, but the lifetime values were in the range of microseconds.

Le mise en commun de la tomographie par émission de positons (TEP) et de la tomodensitométrie (TDM) sur des scanner bimodaux TEP/TDM a été un axe de recherche essentiel en imagerie ces vingt dernières années et a mené à un développement rapide de cette technique en clinique et en pré-clinique. Cependant, même si les deux modalités peuvent être juxtaposées sur le même statif, l’idée originelle de David W. Townsend prévoyait d’acquérir de manière simultanée les données TEP et TDM provenant du même champ de vue. Cela devrait permettre de connaître la position exacte du sujet lors de l’acquisition, et donc potentiellement de corriger de ses mouvements. C’est dans cet optique que nous avons développé le prototype ClearPET/XPAD : le premier scanner TEP/TDM simultané combinant les modules phoswich à scintillateurs du prototype ClearPET et un détecteur à pixels hybride développé au CPPM faisant face à une source de rayons X sur le même rotateur. Je présente les premières images TEP/CT simultanées de source ponctuelles, du fantôme Derenzo et d’une souris vivante acquises sur le prototype ClearPET/XPAD et discute les limites et les particularités de l’imagerie hybride TEP/TDM simultanée. / The combination of Positron Emission Tomography (PET) and X-ray Computerized Tomographie (CT) for PET/CT imaging has been an essential line of research in the previous decades and led to a rapid expansion of this technique in clinics and preclinics. However, even if the two modalities can be juxtaposed on the same gantry, the original concept invented by David W. Townsend foresaw to do both PET and CT imaging at the same time, while imaging a common Field-Of-View (FOV). This will allow to know the exact position of the animal during the scan and possibly to correct for the animal movements. Therefore we developed the ClearPET/XPAD prototype: the first simultaneous PET/CT scanner for mice combining on the same gantry ClearPET modules and the hybrid pixels camera XPAD3 facing an X-ray source. I present the first simultaneous PET/CT scans of point sources, of the Derenzo phantom and of a living mouse acquired with the ClearePET/XPAD prototype and discuss the limitations and prospects of simultaneous hybrid PET/CT imaging.

Es wird ein Verfahren zur Energiekalibrierung von Niedrig-Z-Szintillatoren vorgestellt. Jenes basiert dabei auf einem roboter-unterstütztem Weitwinkel-Compton-Aufbau. In diesem werden die koinzidenten Ereignisse von Compton-gestreuten Photonen in einem HPGe-Detektor und einem Niedrig-Z-Szintillator erfasst und die Messdaten zur Energiekalibrierung des letzteren genutzt. Eine Bestimmung von Compton-Kanten für das Szintillatormaterial ist dabei nicht zwingend notwendig. / A technique for the energy calibration of low-Z scintillators is being presented. It is based on a robot-supported wide-angle Compton setup. In this the coincident events of photons being Compton-scattered in a HPGe detector and a low-Z scintillator are being recorded and the generated measurement data used for energy calibration of the latter. A determination of Compton edges in the scintillator material is not necessarily needed.

Durch die Kopplung von Szintillationskristallen an Lichtwellenleiter könnten robuste Messgeräte für die spektroskopitsche Messung von Strahlungsfeldgrößen in Bohrlöchern in Betonstrukturen beim Rückbau von Kernkraftwerken realisiert werden. In dieser Arbeit wurden zwei Prototypen solcher Messgeräte entwickelt, wobei ein auf einem Gadolinium-Aluminium-Gallium-Granat-Szintillationskristall basierendes Messsystem mit einem Kunststofflichtwellenleiter mit hohem Durchmesser aufgrund seiner hohen Zählrate bevorzugt wurde. Mit diesem Messystem konnten spektroskopische Messungen von Gammastrahlung durchgeführt werden. Weiterhin konnte gezeigt werden, dass Kontaminationen einer bestimmten Aktivität bis in einen Abstand von mehreren Zentimetern von der Messsonde im Beton nachweisbar sind. Ein Schätzwert der minimale Messzeit zur Erkennung einer nachweisbaren Kontamination konnte bestimmt werden. Eine hinreichend große, gemessene Ereigniszahl ermöglicht zusätzlich die Bestimmung des Abstands einer radioaktiven, punktförmigen Kontamination eines bekannten Nuklids. Für ein bekanntes Nuklid konnte weiterhin aus der Zählrate ein Schätzwert für die Energiedosis am Ort der Messsonde mithilfe von Referenzmessungen der Dosis mittels Berylliumoxid-Detektoren bestimmt werden.:Inhaltsverzeichnis Abbildungsverzeichnis vii Tabellenverzeichnis ix 1 Einleitung 1 2 Physikalische Grundlagen 3 2.1 Radioaktiver Zerfall 3 2.2 Gröÿen des Strahlungsfelds 3 2.3 Wechselwirkungen von Photonen mit Materie 5 2.4 Lichtentstehung in anorganischen Szintillatoren 8 2.5 Lichtmessung 10 2.6 Pulshöhenverteilungen von Szintillationsdetektoren 12 2.7 Ein ussfaktoren der Lichtausbeute 14 3 Material und Methoden 16 3.1 Aufbau LSO-Sonde und Messungen mit radioaktiven Quellen 16 3.2 Aufbau Lichtkopplung mittels Linse 18 3.3 Aufbau und Versuchsablauf Quarzglaskopplungen 20 3.4 Aufbau GAGG-Sonde 21 3.5 Aufbau des Betonphantoms 24 3.5.1 Dichtebestimmung des Betonphantoms 24 3.6 Messablauf Tiefenkurven in Betonphantom 27 3.7 Datenanalyse mittels Kolmogorv-Smirnov-Test 27 4 Ergebnisse 29 4.1 Spektroskopische Eigenschaften LSO-Sonde 29 4.2 Winkelverteilung austretender Photonen aus Szintillationskristall 33 4.3 Quarzglaskopplung 36 4.4 Spektroskopische Eigenschaften GAGG-Sonde 43 4.5 Vergleich GAGG- und LSO-Sonde 47 4.6 Abstandsabhängigkeit der Zählrate 50 4.7 Abschätzung der maximalen Abschirmdicke von Beton für Kontaminationserkennung 53 4.8 Abschätzung der minimalen Messzeit zur Kontaminationserkennung 56 4.9 Abschirmungsdickenbestimmung mittels Abschirmungsparameter 57 4.10 Bestimmung der Dosis 62 5 Diskussion 64 6 Zusammenfassung 67 / A robust measuring system for spectroscopic measurementes of gamma-ray radiation in boreholes in concrete structures can be built by coupling of a scintillation crystal to a light guide. Two prototypes of such measuring systems are developed one based on a Gadolinium-Aluminium-Gallium-Garnet scintillation crystal with a plastic optical fiber with a high diameter is preferred due to the higher count rate. Spectroscopic measurements of gamma-ray radiation with this measuring system can be performed. It can be shown that contamination of a specific activity can be detected even if they are located in concrete in a distance of several centimeters from the radiation sensor. for the minimal measurement time of 38 s An estimated value to detect a traceable contamination could be determined. If a high number of events can be detected, even the distance between a point like radioaktive source of a known nuclide and the radiation sensor can be determined. An estimated value for the applied dose at the place of the radiation sensor could be determined for a known nuclide with the help of the count rate. Therefore, reference measurements of dose with berylliumoxide detectors were performed.:Inhaltsverzeichnis Abbildungsverzeichnis vii Tabellenverzeichnis ix 1 Einleitung 1 2 Physikalische Grundlagen 3 2.1 Radioaktiver Zerfall 3 2.2 Gröÿen des Strahlungsfelds 3 2.3 Wechselwirkungen von Photonen mit Materie 5 2.4 Lichtentstehung in anorganischen Szintillatoren 8 2.5 Lichtmessung 10 2.6 Pulshöhenverteilungen von Szintillationsdetektoren 12 2.7 Ein ussfaktoren der Lichtausbeute 14 3 Material und Methoden 16 3.1 Aufbau LSO-Sonde und Messungen mit radioaktiven Quellen 16 3.2 Aufbau Lichtkopplung mittels Linse 18 3.3 Aufbau und Versuchsablauf Quarzglaskopplungen 20 3.4 Aufbau GAGG-Sonde 21 3.5 Aufbau des Betonphantoms 24 3.5.1 Dichtebestimmung des Betonphantoms 24 3.6 Messablauf Tiefenkurven in Betonphantom 27 3.7 Datenanalyse mittels Kolmogorv-Smirnov-Test 27 4 Ergebnisse 29 4.1 Spektroskopische Eigenschaften LSO-Sonde 29 4.2 Winkelverteilung austretender Photonen aus Szintillationskristall 33 4.3 Quarzglaskopplung 36 4.4 Spektroskopische Eigenschaften GAGG-Sonde 43 4.5 Vergleich GAGG- und LSO-Sonde 47 4.6 Abstandsabhängigkeit der Zählrate 50 4.7 Abschätzung der maximalen Abschirmdicke von Beton für Kontaminationserkennung 53 4.8 Abschätzung der minimalen Messzeit zur Kontaminationserkennung 56 4.9 Abschirmungsdickenbestimmung mittels Abschirmungsparameter 57 4.10 Bestimmung der Dosis 62 5 Diskussion 64 6 Zusammenfassung 67

Die Grundlage vieler zukünftiger Flüssigszintillator-Neutrinoexperimente (SNO+, Daya Bay, LENA) ist das Lösungsmittel Lineare-Alkyl-Benzene (LAB, C6H5CnH2n+1, n = 10 - 13). Zusammen mit dem weit verbreiteten Szintillator 2,5-Diphenyloxazole (PPO) ist es ein farb- und geruchsloses Detektormaterial mit hohem Flammpunkt. Im Vergleich zu toluol- oder xylolbasierten Szintillatoren ist LAB+PPO preiswert und nicht gesundheitsschädlich. Die Eigenschaften von LAB machen es ebenfalls interessant für die Anwendung an nELBE, die Neutronenfugzeitanlage im Helmholtz-Zentrum Dresden - Rossendorf. Ein neuer Ansatz zur Bestimmung der Lichtausbeute im niederenergetischen Bereich (bis 2 MeV) wird vorgestellt. Kombiniert wurden Messungen mit (quasi) monoenergetischen Gammastrahlungs-Prüfstrahlern und einem in dieser Arbeit aufgebauten Compton-Spektrometer. Letzteres ermöglicht die Bestimmung der Lichtausbeute bis zu 5 keVee. Der Birks-Parameter wurde für eine Lösung von LAB + 3 g/l PPO sowie für den Flüssigszintillator NE-213 bestimmt. Die relative Lichtausbeute in Bezug auf letzteren konnte mit diesen Messmethoden ebenfalls ermittelt werden. Zur spektralen Analyse des Lumineszenzlichtes wurden Messungen an Fluoreszenz- und UV/VIS- Spektrometern durchgeführt. Die Pulsformdiskriminationsfähigkeit auf LAB basierenden Szintillatoren wurde während eines Flugzeitexperiments in einem gemischten n-gamma-Feld eines Cf(252)-Prüfstrahlers ermittelt. Dabei kamen unterschiedliche Algorithmen der semi-analogen und digitalen Pulsformdiskrimination zum Einsatz. / Linear alkyl benzene (LAB, C6H5CnH2n+1, n = 10 - 13) is the proposed solvent for the SNO+, the Daya Bay Neutrino and LENA experiment. In solution with the commonly used scintillator PPO it is a colourless, odourless and cheap liquid scintillator with a high fash point and low health hazard compared to toluene based ones. The properties of LAB make this scintillator interesting also for nELBE, the neutron time-of-fight facility at Helmholtz-Zentrum Dresden - Rossendorf. A new approach to measure the light yield in the low-energy range using a combination of quasi-monoenergetic photon sources and a Compton-spectrometer is described. The latter allows the measurement of the light yield down to 5 keVee (electron equivalent). The Birks- Parameter was determined for a homemade solution (LAB + 3 g/l PPO) and for NE-213. The light yield (relative to this standard scintillator) was confrmed by measurements using a fuorescence spectrometer. The ability of pulse-shape-discrimination in a mixed n-gamma- field of a Cf(252) source was tested using different digital and semi-analogue techniques.

- / The term Molecular Imaging (MI) can be broadly defined as the in vivo characterization and measurement of biological processes at the cellular and molecular level. In contradistinction to “classical” diagnostic imaging, it sets forth to probe the molecular abnormalities that are the basis of disease rather than to image the end effects of these molecular alterations. The underlying biology represents a new arena for many researchers. A number of technological challenges such as signal amplification, data and image processing and efficient imaging strategies, provide a fast growing scientific domain. Positron Emission Tomography (PET), Magnetic Resonance Imaging (MRI), Single Photon Emission Tomography (SPECT) and optical imaging are the main tools of clinical molecular imaging. Nuclear medicine techniques (SPECT and PET) are key players in MI. New radiopharmaceutical products are currently being developed, in order to increase the specificity and sensitivity of existing imaging techniques. Small animal imaging is the main tool for the evaluation of those derivatives, especially in dynamic in vivo studies. In this, preclinical part, high resolution and high sensitivity imaging equipment is necessary; as a result a number of such prototypes have been developed worldwide and some of them are commercialized. However, there cost is usually not affordable for small or medium size laboratories. In this work a low cost dual head PET camera, suitable for high resolution small animal studies has been developed. It is the result of the collaboration between Jefferson lab and Technological Educational Institute of Athens (TEI) and is currently evaluated in Institute of Radioisotopes and Radiodiagnostic Products (IRRP), in “Demokritos” Center. The system has a field of view of 5x5cm and is based on 2 H8500 position sensitive photomultiplier tubes (PSPMTs), coupled to two LSO crystals with 2.5x2.5mm pixel size. Then an FPGA based data acquisition system and proper data reconstruction system collect events, sort coincidences and produce images. The DAQ board consists of 16-channel DAQ modules installed on a USB2 carrier. Each channel is an independent acquisition system consisting of traditional analog pulse processing, FPGA analog control, and FPGA signal processing. After acquisition and processing, channel data are assembled into event blocks for readout by the carrier board. Application specific tasks are performed in JAVA using the Kmax interface. The GUI was designed to be easy-to-use. In order to further analyze images and process the results proper algorithms were developed in MATLAB and ImageJ. Systems evaluation has been carried out using FDG. Point sources have been used for systems calibration. Capillaries with 1.1mm inner diameter were imaged and used for resolution calculation. Finally a mouse injected with 100μCi of FDG was imaged. Spatial resolution has been measured using thin capillaries (1.1mm inner diameter) and found equal to 3,5mm in planar mode. This lower limit is determined by LSO pixels size (2.5×25mm2). Simulation studies have shown that resolution lower than 2mm will be achieved in tomographic mode. Mice injected with FDG are presented. Brain and heart are clearly imaged. Currently, a rotating base is constructed, in order to upgrade the system to a tomographic PET. PET results will be presented as well. In addition, IRRP and TEI are working on new radiopharmaceuticals based on Cu-64. It must be stated that PET market opened in Greece four years ago; This system is the first working small PET prototype in Greece and it initiates national preclinical PET research.

Current positron emission mammography (PEM) depth of interaction (DOI) enabling detectors have low scintillator to photodetector encoding ratios, RE causing high system complexity and cost. The modularized dual-ended readout block (DERB) detector combines the Anger logic block detector with dual-ended readout to increase RE while measuring DOI. To investigate the trade-off between RE and spatial resolution, scalable DERB detectors with varying RE and light guide thickness were modelled with Monte- Carlo. Simulation showed RE can increase up to six-fold compared to the dual-ended readout design without significantly degrading spatial resolution. Experimental characterization of a RE = 9 : 8 DERB detector was found to achieve super-resolution <0.5 mm for resolving crystal indices, DOI resolution of ~5 mm FWHM, and mean energy resolution of 20% without recovering photons lost to neighbouring detector modules. The model was validated by agreement of simulation results adjusted for detector quantum efficiency with experimental results.