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Microstructural data on the orientation and distribution of minerals can be utilized to better understand the processes controlling mineral crystallization during metamorphism and the extent to which equilibrium versus kinetic factors control the evolution of metamorphic rocks. Four studies in this dissertation address this, finding that: i) garnet crystals crystallize via epitaxial nucleation in which garnet crystallizes by templating on the crystal structure of muscovite; ii) the distribution of grain boundary void space at quartz-quartz and garnet-quartz grain boundaries is a function of the orientation of quartz crystals on either side of the grain boundary. There are more voids, and in some cases larger voids, at grain boundaries in which the a-axis of a neighboring quartz grain is perpendicular to the grain boundary than any other orientation; iii) the chemical potentials of garnet-forming components evolve differently in samples in which garnet growth either significantly or minimally overstepped equilibrium garnet-forming reactions; iv) the southwestern Meguma Terrane, Nova Scotia, experienced peak metamorphic conditions of ~630ºC and 4.0 kbar, likely resulting from regional metamorphism during the Neoacadian orogeny. A case study on the mechanisms controlling garnet crystallization in one Nova Scotian sample reveals that the rate limiting step of garnet crystallization was probably the diffusional transport of Al through the intergranular matrix. Taken together, this work has implications for understanding: i) the properties of grain boundaries in metamorphic rocks and ii) the extent to which equilibrium versus kinetic factors impact metamorphic petrogenesis. / Doctor of Philosophy / A fundamental question in the development of metamorphic rocks, or rocks that form due to changes in pressure and temperature conditions deep in the Earth's mountain belts, is: what controls the crystallization of new minerals? While pressure, temperature, and bulk composition likely play a major role in this, it is also possible that the distribution of reactant minerals and the transport of elements through the rock may also play a role in mineral crystallization. This dissertation explores several projects related to this broad topic. In one example, garnet, an important metamorphic mineral, was found to crystallize by utilizing the atomic structure of another mineral in the rock. This creates a favorable pathway for the crystallization of garnet, which preferentially grows on this 'parent' mineral. Further, the distribution of porosity, or void space, at the interfaces between mineral grains in metamorphic rocks is found to be controlled by the orientation of those minerals. This porosity likely formed when the rocks were exhumed from deep in the Earth towards its surface. Metamorphic rocks can also tell the story of continental plates colliding millions of years ago. In an example from the formation of the Appalachian Mountains ~400 million years ago, a combination of collisional tectonic forces and the heat from magmas in the shallow crust resulted in metamorphic rock, which make up much of southern Nova Scotia today. This work has important implications for understanding: i) porosity in metamorphic rocks and ii) how minerals crystallize during metamorphism.

Garnet porphyroblasts are commonly used to determine P-T conditions in metamorphic rock assemblages. However, the actual process of porphyroblast nucleation is still poorly understood and garnet growth may occur at different conditions than those predicted by equilibrium thermodynamics. It is typically assumed that the Gibbs free energy of a system can be used to predict the growth of garnet at a given P and T, but here a new idea is proposed that in nature, growth does not occur until the chemical potential of each garnet-forming component departs from its equilibrium (pre-nucleation) state. Similar thermodynamic modeling results from a variety of metamorphic settings, rock types and apparent degrees of overstep indicate these deviations likely control the extent of overstep in the garnet-forming reaction in many natural samples. The process of metamorphic differentiation is then used to explain microstructures observed in the Haimanta Group, NW India that contain quartz-rich and mica-rich layers, with numerous garnet porphyroblasts appearing solely in the quartz-rich layers. This process is deformation-controlled, allowing the microstructures to be used as kinematic indicators to determine the deformation history of the Haimanta Group. The Elle Microstructural Modeling Program, the Basil deformation code and observed chemical zoning of garnets are used to prove metamorphic differentiation as the process responsible for garnet growth, meaning a singular, prograde event resulted in garnet growth in the Haimanta Group, in agreement with published monazite data for theses samples. / Master of Science

京都大学 / 新制・課程博士 / 博士(人間・環境学) / 甲第25388号 / 人博第1130号 / 新制||人||263(附属図書館) / 京都大学大学院人間・環境学研究科相関環境学専攻 / (主査)教授 田部 勢津久, 教授 吉田 寿雄, 教授 中村 敏浩, 教授 田中 勝久 / 学位規則第4条第1項該当 / Doctor of Human and Environmental Studies / Kyoto University / DFAM

Pažangių medžiagų bei technologijų kūrimas ir taikymas - tai labai svarbus šiandieninės informacinės visuomenės uždavinys. Granato kristalinės struktūros medžiagos, pasižymėdamos ypatingomis fizikinėmis bei cheminėmis savybėmis, yra plačiai naudojamos informacinių technologijų, kietafazių lazerių, optikos įrenginių gamybose, medicinos įrangose, bei daugelyje kitų sričių. Todėl jos dėl savo unikalių savybių ir plačiai tebetyrinėjamos iki šiol. Šiame darbe pirmą kartą buvo susintetinti Ce-Al-O, Pr-Al-O, Nd-Al-O, Tb-Al-O, Dy-Al-O, Ho-Al-O, Er-Al-O, Tm-Al-O, Yb-Al-O, Lu-Al-O, Y(Nd)-Al-O ir Y(Sm)-Al-O acetatiniai-nitratiniai-glikoliatiniai geliai zolių-gelių metodu vandeniniuose tirpaluose. Jie buvo panaudoti pradinėmis medžiagomis atitinkamų lantanoidų aliuminio granatų sintezei. Vienfaziai terbio aliuminio granatas (Tb3Al5O12), disprozio aliuminio granatas (Dy3Al5O12), holmio aliuminio granatas (Ho3Al5O12), erbio aliuminio granatas (Er3Al5O12), tulio aliuminio granatas (Tm3Al5O12), iterbio aliuminio granatas (Yb3Al5O12) ir liutecio aliuminio granatas (Lu3Al5O12) buvo gauti, terbio jonų šaltiniu naudojant terbio oksidą, disprozio – disprozio oksidą, holmio – holmio oksidą, erbio – erbio oksidą, tulio – tulio oksidą, iterbio – iterbio oksidą, lutecio – liutecio oksidą, kompleksus sudarančiu reagentu 1,2-etandiolį. Tyrimų rezultatai parodė, kad šių lantanoidų aliuminio granatai gauti santykinai žemoje temperatūroje (1000°C). Zolių-gelių metodu sintetinant cerio aliuminio granatą... [toliau žr. visą tekstą] / The development and application of advanced materials is a very important task of today's information society. Garnet crystal structure compounds because of their specific physical and chemical properties are widely used in information technology, manufacturing of solid-state lasers and optical equipments, medical equipments and many other areas. Therefore, these materials because of their unique properties and characteristics are of high interest so far. For the first time Ce-Al-O, Pr-Al-O, Nd-Al-O, Tb-Al-O, Dy-Al-O, Ho-Al-O, Er-Al-O, Tm-Al-O, Yb-Al-O, Lu-Al-O, Y(Nd)-Al-O and Y(Sm)-Al-O acetate-nitrate-glycolate gels have been synthesized using environmentally friendly, economical and simple aqueous sol-gel method. They were used as starting materials for the synthesis of appropriate lanthanide aluminium garnets. The results of X-ray difraction analysis have indicated that single-phase terbium aluminium garnet (Tb3Al5O12), dysprosium aluminium garnet (Dy3Al5O12), holmium aluminium garnet (Ho3Al5O12), erbium aluminium garnet (Er3Al5O12), thulium aluminium garnet (Tm3Al5O12), ytterbium aluminium garnet (Yb3Al5O12) and lutetium aluminium garnet (Lu3Al5O12) have been synthesized by annealing Tb-Al-O, Dy-Al-O, Ho-Al-O, Er-Al-O, Tm-Al-O, Yb-Al-O and Lu-Al-O precursor gels for 10 hours at 1000 °C, respectively. For the first time these garnet structure compounds were synthesized using sol-gel method. Moreover, these lanthanide aluminium garnets were synthesized at relatively low... [to full text]

The development and application of advanced materials is a very important task of today's information society. Garnet crystal structure compounds because of their specific physical and chemical properties are widely used in information technology, manufacturing of solid-state lasers and optical equipments, medical equipments and many other areas. Therefore, these materials because of their unique properties and characteristics are of high interest so far. For the first time Ce-Al-O, Pr-Al-O, Nd-Al-O, Tb-Al-O, Dy-Al-O, Ho-Al-O, Er-Al-O, Tm-Al-O, Yb-Al-O, Lu-Al-O, Y(Nd)-Al-O and Y(Sm)-Al-O acetate-nitrate-glycolate gels have been synthesized using environmentally friendly, economical and simple aqueous sol-gel method. They were used as starting materials for the synthesis of appropriate lanthanide aluminium garnets. The results of X-ray difraction analysis have indicated that single-phase terbium aluminium garnet (Tb3Al5O12), dysprosium aluminium garnet (Dy3Al5O12), holmium aluminium garnet (Ho3Al5O12), erbium aluminium garnet (Er3Al5O12), thulium aluminium garnet (Tm3Al5O12), ytterbium aluminium garnet (Yb3Al5O12) and lutetium aluminium garnet (Lu3Al5O12) have been synthesized by annealing Tb-Al-O, Dy-Al-O, Ho-Al-O, Er-Al-O, Tm-Al-O, Yb-Al-O and Lu-Al-O precursor gels for 10 hours at 1000 °C, respectively. For the first time these garnet structure compounds were synthesized using sol-gel method. Moreover, these lanthanide aluminium garnets were synthesized at relatively low... [to full text] / Pažangių medžiagų bei technologijų kūrimas ir taikymas - tai labai svarbus šiandieninės informacinės visuomenės uždavinys. Granato kristalinės struktūros medžiagos, pasižymėdamos ypatingomis fizikinėmis bei cheminėmis savybėmis, yra plačiai naudojamos informacinių technologijų, kietafazių lazerių, optikos įrenginių gamybose, medicinos įrangose, bei daugelyje kitų sričių. Todėl jos dėl savo unikalių savybių ir plačiai tebetyrinėjamos iki šiol. Šiame darbe pirmą kartą buvo susintetinti Ce-Al-O, Pr-Al-O, Nd-Al-O, Tb-Al-O, Dy-Al-O, Ho-Al-O, Er-Al-O, Tm-Al-O, Yb-Al-O, Lu-Al-O, Y(Nd)-Al-O ir Y(Sm)-Al-O acetatiniai-nitratiniai-glikoliatiniai geliai zolių-gelių metodu vandeniniuose tirpaluose. Jie buvo panaudoti pradinėmis medžiagomis atitinkamų lantanoidų aliuminio granatų sintezei. Vienfaziai terbio aliuminio granatas (Tb3Al5O12), disprozio aliuminio granatas (Dy3Al5O12), holmio aliuminio granatas (Ho3Al5O12), erbio aliuminio granatas (Er3Al5O12), tulio aliuminio granatas (Tm3Al5O12), iterbio aliuminio granatas (Yb3Al5O12) ir liutecio aliuminio granatas (Lu3Al5O12) buvo gauti, terbio jonų šaltiniu naudojant terbio oksidą, disprozio – disprozio oksidą, holmio – holmio oksidą, erbio – erbio oksidą, tulio – tulio oksidą, iterbio – iterbio oksidą, lutecio – liutecio oksidą, kompleksus sudarančiu reagentu 1,2-etandiolį. Tyrimų rezultatai parodė, kad šių lantanoidų aliuminio granatai gauti santykinai žemoje temperatūroje (1000°C). Zolių-gelių metodu sintetinant cerio aliuminio granatą... [toliau žr. visą tekstą]

Orientador: Luiz Sérgio Amarante Simões / Resumo: Na Nappe de Passos, unidade tectônica pertencente à Faixa Brasília Meridional, em seu segmento intermediário (Unidades E e G), ocorrem megaporfiroblastos de granada (diâmetro ≥ 3 cm, alcançando até 8 cm), hospedados em cianita-mica xistos, que contrastam com os de tamanho usual (0,2 a 1,5 cm) comumente encontrados nos xistos granadíferos desta nappe. Este trabalho, como uma primeira iniciativa de estudo dessa peculiar feição metamórfica, investiga a ocorrência desses megaporfiroblastos através de levantamento de campo, análise microtectônica e determinação de perfis químicos. Parte do trabalho foi voltada para buscar ocorrências de megaporfiroblastos na porção NW da Nappe de Passos, a norte da cidade de Cássia (MG). Com o levantamento de campo, que incluiu trinta perfis seccionando as Unidades E, F G, H e I, não foi encontrada nenhuma ocorrência de camadas ricas em megaporfiroblastos neste setor da nappe. Ao longo desse levantamento, foi possível realizar uma melhor caracterização geométrica do fechamento NW da Braquissinformal de Passos e demonstrar o caráter braquiantiformal da Antiforma de Itaú de Minas. Para o estudo dos megaporfiroblastos, selecionou-se uma ocorrência no segmento SE da Nappe de Passos, no topo da Unidade E. Eles se encontram hospedados em camadas decimétricas de biotita-cianita-granada-quartzo-muscovita xistos, que se alternam com camadas de composições semelhantes, porém contendo porfiroblastos de tamanho usual. Os megaporfiroblastos têm forma elipsoida... (Resumo completo, clicar acesso eletrônico abaixo) / Abstract: The Passos Nappe is an important tectonic unit of the Southern Brasília Belt. In the intermediate segment of the Passos Nappe, represented by E and G Units, occurs megaporphyroblasts of garnet (diameter 3 to 8 cm). The megaporphyroblasts are hosted in kyanite-mica schists and contrast with the usual size (from 0.2 to 1.5 cm) commonly found in the granadiferous schists of this nappe. This work provides the first study of this peculiar metamorphic feature and aims to investigate the occurrence of these megaporphyroblasts based on field work, microtectonic analysis and determination of chemical profiles. Part of the work focused on identifying the occurrence of megaporphyroblasts to the north of the Cássia city (Minas Gerais State), within the NW sector of the Passos Nappe. Thirty transects were produced along the E, F G, H and I Units, however, no occurrence of megaporphyroblasts rich layers was found in this sector of the nappe. The improvement on the geometric characterization of the northwest closure of the Passos Brachisyncline and the demonstration of the brachianticline aspect of Itaú de Minas Antiform were possible with the transect work. For the study of megaporphyroblasts, it was selected an occurrence located in the SE sector of the Passos Nappe, situated at the top of the E Unit. The study carried out in this sector shows that megaporphyroblasts are hosted in decimetric layers of biotite-kyanite-garnet-quartz-muscovite schists, which alternate with layers of similar ... (Complete abstract click electronic access below) / Mestre

Les attentes pour les prochaines générations de batteries pour le véhicule électrique sont grandes, que ce soit en termes d’autonomie, d’impact environnemental, de vitesse de charge et de coût. Les systèmes dits tout solide comprenant un électrolyte, non plus liquide, mais solide et non-inflammable pourrait répondre à ces attentes.La céramique de type grenat Li7La3Zr2O12 (LLZO) est un électrolyte solide prometteur au vue de sa bonne conductivité, stabilité chimique et électrochimique. La contrainte majeure réside dans le besoin de densifier la céramique à haute température afin de la rendre conductrice. Aucune méthode standard d’assemblage/mise en forme n’existe pour obtenir une cellule tout solide dense avec des interfaces peu résistives.Dans cette optique, les travaux de thèse ont permis d’optimiser le protocole de synthèse par voie « tout solide » de l’oxyde LLZO et sa mise en forme grâce à la technique de compression uniaxiale à chaud (CUC). Les conditions d’assemblage de cellules symétriques Li/LLZO/Li ont permis d’étudier l’interface Li-métal/LLZO et son impact sur la dissolution/redéposition du lithium. La faisabilité de densifier une « demi-cellule » (cathode composite/LLZO) en une seule étape a également été étudiée en ajustant les paramètres de température et pression du protocole de CUC. / Next generation batteries expectations for electric vehicle are significant, whether in terms of autonomy, environmental impact, charging speed and cost. The all solid-state batteries with a non-flammable solid electrolyte, rather than the conventional liquid one, could meet those criteria.Garnet-type ceramic Li7La3Zr2O12 (LLZO) is a promising solid electrolyte given its good Li-ion conductivity, chemical and electrochemical stability. The major constraint is the need to densify the ceramic at high temperature in order to make it conductive. No standard method exists to build a dense all-solid cell with low interfacial resistance.In this context, the PhD work managed to optimize the solid-state synthesis protocol of the LLZO oxide and his densification by the hot-pressing technique. The conditions of symmetrical Li/LLZO/Li cell assembly allowed to study the Li-metal/LLZO interface and its impact on lithium plating/striping behavior. Feasibility of densifying a “half-cell” (composite cathode/LLZO) in one single step was also studied by adjusting the hot-pressing temperature and pressure parameters.