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Synthesis and characterization of Rare Earth compounds with potencial appplication in ionizing radiation detection

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Author(s):
Simone Aparecida Cicillini
Total Authors: 1
Document type: Doctoral Thesis
Press: Ribeirão Preto.
Institution: Universidade de São Paulo (USP). Faculdade de Filosofia, Ciências e Letras de Ribeirão Preto (PCARP/BC)
Defense date:
Examining board members:
Osvaldo Antonio Serra; Hermi Felinto de Brito; Rogéria Rocha Gonçalves; Ieda Lucia Viana Rosa; Elizabeth Berwerth Stucchi
Advisor: Osvaldo Antonio Serra
Abstract

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. (AU)