Structure-Property-Composition Correlations in Rare-Earth Alumino-silicate Glasses
Abstract: Rare earth (RE) alumino-silicate (AS) glasses exhibit favorable physical, mechanical and optical properties, such as high values of the glass transition temperature, Vickers hardness, and refractive index. RE2O3-Al2O3-SiO2 glasses have found several industrial applications, for example as components of optical amplifiers and lasers. Many of these features stem from the high cation field-strength (CFS) of the trivalent RE ions (proportional to the valence of the ion divided by the square of its radius), which affects not only the physical properties of the glass, but also their structures.This thesis deals with investigations of four different RE2O3-Al2O3-SiO2 systems, where RE represents either of La, Y, Lu or Sc. The glass forming regions of the latter two were reported by us for the first time. Within each system, glasses were prepared for variable RE, Si and Al contents.The glass structures were investigated by solid-state 29Si and 27Al nuclear magnetic resonance (NMR) spectroscopy that informs about the local Si and Al environments in the glass network, which is built from interlinked SiO4 and AlO4 groups. Higher Al coordination numbers were also revealed by 27Al NMR: their amounts were observed to increase markedly as the CFS of the RE ion increases, i.e., along the series La<Y<Lu<Sc. This thesis discusses such structure/composition relationships, as well as the correlations between the glass composition and its physical properties of density, molar volume, compactness, glass transition temperature, Vickers hardness and refractive index. Some of these properties, for example the glass transition temperature and Vickers hardness, were observed to enhance as the RE3+ CFS increased.
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