Fractional crystallization, magma mixing, assimilation of continental crust, and how those processes modify volatile budgets, control the evolution of magma. As a consequence, the understanding of these processes, their magnitudes, and timescales is critical for interpreting ancient magma systems, their eruptions, and the potential future volcanic activity. In this dissertation I present the results of three projects. The first explores how magmatic processes affect magma reservoirs and eruption dynamics. The second explores where in the storage system and how often these processes occur. The third explores how volatile budgets are modified by processes such as crystallization, mixing, and assimilation. Volcán Popocatépetl (central México) erupted ~14100 14C yr BP producing the Tutti Frutti Plinian Eruption (TFPE). The eruption tapped two different silicic magmas that mixed just prior and during the eruption. The influx of mass and volatiles generated during the mixing of both magmas overpressured the reservoir, which was weakened at the top. The weakened reservoir relaxed while magma was tapped and collapsed to form a caldera at the surface. Although it is known that fractional crystallization, mixing, and assimilation can greatly modify magmas, the frequency and intensity of these events is not known. I investigated the magmatic processes responsible for the evolution of magmas erupted during five Plinian events of Popocatépetl volcano. Results show that during the last 23 ky magma was stored in two different zones, and was variably modified by replenishments of mafic magma. Interestingly, little evidence for large mafic inputs triggering explosive eruptions was found. Each of these processes alters the abundances of volatiles and introduces different types of volatiles to the system. Hence, the volatile budget of magma can have a rich and complex history. To investigate how volatile budgets evolve in active magma systems, I analyzed the abundances of volatiles (H2O, CO2, F, Cl, and S) in numerous glass inclusions trapped in phenocrysts. Results show that the magmas that produced the last five Plinian eruptions at Popocatépetl volcano evolved by crystallization and magma mixing, assimilation of the local carbonate basement is not chemically appreciable. Mixing with mafic magmas added substantial CO2 and S to the system, dewatered the magma, yet produced little change in the F contents of the magmas. / text

The Miocene rhyolites of the Spor Mountain Formation hosts the world's largest beryllium deposit which produced 85% of the world's beryllium in 2010. The fresh lava is extremely enriched in Be (up to 75 ppm in matrix glass). We have examined the rhyolite to understand the Be enrichment. The Spor Mountain rhyolite contains ~40% quartz, ~40% sanidine, ~10% biotite, and ~10% plagioclase, along with accessory fluorite, columbite, euxenite, fergusonite, monazite, thorite, and zircon. Two types of rhyolite erupted within the Spor Mountain Formation, a less evolved magma (1150 ppm Rb, 42 ppm Be, 0.68 wt% F in matrix glass) and an evolved magma (1710 ppm Rb, 75 ppm Be, 1.56 wt% F in matrix glass). Eruption temperatures estimated using zircon saturation, feldspar-liquid, two feldspar, and Ti-in-quartz geothermometers converge on 718 °C for the less evolved magma and 682 °C for the evolved magma. Using the Ti-in-Qz equation of Huang and Audetat (2012), the pressure of the Spor Mountain rhyolite system is estimated to be around 2 kbar at 700°C. Water content of the rhyolite melt was less than <5 wt%, based on the presence of all four major mineral phases at 700°C and the magma was water undersaturated (Webster et al., 1987). Viscosity of the rhyolite was about 6.2 log Pa·s for the less evolved rhyolite and 5.8 log Pa·s for the evolved rhyolite. Magma viscosities calculated using the Einstein-Roscoe question suggest the evolved magma has a slightly higher viscosity than the less evolved magma (7.0 log Pa·s in the evolved magma vs 6.7 log Pa·s in the less evolved magma) because of higher phenocryst content. Fluorine lowered the melt viscosity, though not by a significant amount (less than 0.5 log units at 1.7 wt% F). Partition coefficients for 32 elements have been calculated for biotite, for 21 elements for sanidine and plagioclase, and for 6 elements for quartz, using data acquired by laser ablation inductively coupled plasma mass spectrometry. Partition coefficients for feldspars in the Spor Mountain rhyolite are generally higher than other silicic magmas, and lower for biotite. Beryllium is one of the most incompatible trace elements in the Spor Mountain rhyolite, with a bulk partition coefficient <0.1. Volatile content of the melt (specifically F), melt composition, and the low temperature of crystallization act as the major controls of trace element partitioning. Trace element models using these partition coefficients suggests that crystal fractionation is the dominant magmatic enrichment process within the rhyolite, requiring ~45% crystallization (f = 55%) of the observed phenocrysts to get compositions from the less evolved to evolved rhyolite. Accumulation of batches of melt formed by different degrees of partial melting cannot explain the great depletion of compatible elements.

Mafic and intermediate intrusions commonly accompany Variscan granitoid plutons in Europe. They are documented from different localities of Iberian Peninsula, from the French Massif Central, Schwarzwald, from different parts of the Bohemian Massif, in Romania, Greece, Corsica and Sardinia. They comprise wide petrographic varieties from quartz gabbros, diorites, granodiorites to monzonites. They usually constitute small bodies or veins, they often occur as mafic microgranular enclaves (MME) in granodiorites and in some granites. Dioritic intrusions are characterized by a relatively high amounts of lithophile elements (Rb, Sr, Ba, Cs, LREE), and they are simultaneously high in compatible elements (Ni, Cr, V a Co). Their isotopic ratios 87 Sr/86 Sr are in all compared locations similar and are close to the Bulk Earth (0.704 - 0.708). εNd values show larger scatter, some intrusions have more crustal composition (to -8), on the other hand, another intrusions have εNd positive, that points to a contribution of basic magma. The age of dioritic intrusions differs according to individual locality suggesting more than one magmatic episode. The oldest occur in the French Massif Central (361 - 365 Ma), whereas the youngest are documented in Iberia (312 - 310 Ma). The oldest mafic intrusions in the Bohemian...

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Composition and texture of the Middle and Late Eocene volcanic, volcaniclastic, and volcanic-sedimentary rocks in the Bijgerd-Kuh e Kharchin area, in the Uromieh-Dokhtar zone northwest of Saveh, Iran, suggest the complexity of the magmatic system that involved multiple eruptions from one or more sources. Hydrated volcanic fragments in hyaloclastic rocks, and the presence of a sequence of shallow and intermediate-depth marine microfossils, suggest that the Middle Eocene units were erupted in a marine basin. The bimodal volcanism of the Late Eocene is distinguished by the presence of four alternating sequences of hyaloclastite lava and ignimbrite. The REE patterns show spatial homogeneity and temporal heterogeneity in the composition of all the Late Eocene sequences, suggesting origination of magma from varying sources that erupted at different times. The trace element distributions of the hyaloclastites and ignimbrites are compatible with those evolved through fractional crystallization of the lower and upper continental crust, respectively.

The purpose of this work was to explore the use of fractional evaporative crystallization as a technology that can be used to separate medium-curie waste from the Hanford Site tank farms into a high-curie waste stream, which can be sent to a Waste Treatment and Immobilization Plant (WTP), and a low-curie waste stream, which can be sent to Bulk Vitrification. Experimental semi-batch crystallizations of sodium salts from simulant solutions of double-shell tank (DST) feed demonstrated that the recovered crystalline product met the purity requirement for exclusion of cesium and nearly met the requirement on sodium recovery. Batch fractional evaporative crystallization involves the removal of multiple solutes from a feed solution by the progressive achievement of supersaturation (through evaporation) and concomitant nucleation and growth of each species. The slurry collected from each of these crystallization stages was collected and introduced to filtration and washing steps. The product crystals obtained after washing were sampled for analysis by polarized light microscopy (PLM), dried, and sieved. The PLM results aided in identification of species crystallized in each stage. Carbonation was used as a supplemental method to evaporative crystallization in order to increase the sodium recovery in DST experiments. Carbonation was necessary due to the high aluminum ion concentration in the solution, which leads to formation of a viscous gel during evaporation. This gel was avoided by reacting carbon dioxide with hydroxyl ions, which modified the system behavior. Through two stages of carbonation, each followed by evaporation, the effect of carbonation on sodium recovery was demonstrated.

Coordenação de Aperfeiçoamento de Pessoal de Nível Superior / Diques de basaltos toleíticos de baixo-TiO2 ocorrem na porção oriental do Enxame de Diques da Serra do Mar, na Região dos Lagos, entre Niterói e Búzios. Eles têm direções, preferencialmente, NE-SW, subordinadamente, NNE-SSW e mais raramente, NW-SE, e formas intrusivas variáveis. Os basaltos são holocristalinos a hipocristalinos, inequigranulares a equigranulares, intergranulares e intersertais. Eles são constituídos essencialmente de plagioclásio, augita e/ou pigeonita, com olivina corroída, minerais opacos e apatita como minerais acessórios e biotita, bowlingita, idingisita, uralita e saussurita como minerais secundários. A assembléia de fenocristais destas rochas foi estimada em 15% de olivina, 40% de augita e 45% de plagioclásio. Os rochas inserem-se numa série basáltica subalcalina de afinidade toleítica de baixo-TiO2 pouco expandida (MgO= 8,13-5,91%peso), não tendo sido encontradas amostras representativas de líquidos basálticos primários. Esta suíte predominante foi denominada Suíte Costa Azul. No entanto, os dados litogeoquímicos apontam para a existência de mais que uma suíte de baixo-TiO2 na área de estudo que, segundo modelos de fusão parcial em equilíbrio modal, poderiam ter sido geradas por diferentes quantidades de fusão a partir de uma mesma fonte com granada residual. Em termos regionais, a suíte Costa Azul pode ser relacionada com a Suíte Esmeralda que ocorre na subprovíncia Sul de Paraná-Etendeka, muito embora abrangendo um espectro mais amplo de razões Ti/Y. As rochas da suíte Costa Azul evoluíram por 42% de cristalização fracionada envolvendo uma assembléia de fenocristais composta por 15% de olivina, 40% de augita e 45% de plagioclásio, sem mudança de assembléia fracionante. Misturas de componentes mantélicos empobrecidos (mínimo de 72% de D-MORB) e enriquecidos (máximo de 28% de manto litosférico subcontinental) estão associadas à petrogênese desta suíte. Misturas entre componentes do tipo pluma e litosféricos não conseguem explicar as composições parentais da suíte. Os modelos petrogenéticos permitiram a proposição de um modelo geodinâmico envolvendo delaminação do manto litosférico subcontinental englobado por células convectivas ascendentes do manto sublifosférico subjacente em níveis astenosféricos pouco profundos durante um estágio avançado de rifteamento do supercontinente Gondwana. / Low-TiO2, tholeiitic basalt dykes occur eastwards the Serra do Mar Dyke Swarm within the Região dos Lagos from Niterói up to Búzios city. The dykes strike preferentially NE-SW bearing variable intrusive structures. The basalts are holo- to hypocrystaline, equigranular to inequigranular rocks with mostly intergranular and intersertal textures. They are composed mostly by plagioclase, augite and/or pigeonite and have corroded olivine, opaque minerals and apatite as accessory phases. Secondary mineralas are represented by biotite, bowlingite, iddingisite, uralite and saussurite. The phenocrysts assemblage comprise 15% olivine, 40% augite and 45% plagioclase. The rocks comprise a low-TiO2, subalkaline, tholeiitic basaltic suite hereafter called the Costa Azul suite. Nevertheless, lithogeochemical data point to the existence of more than one low-TiO2 suite in the study area. Geochemical modelling has shown that these suites can be related by different degrees of partial melting from a similar mantle source with residual garnet. The Costa Azul suite can be related with the Esmeralda low-TiO2 basaltic suite within the Paraná-Etendeka CFB province due south Brazil although comprising a wider Ti/Y ratio range. The rocks of the Costa Azul suite evolved by 42% of fractional crystallisation involving a phenocryst assemblage with 15% de olivine, 40% augite and 45% plagioclase. Binary mixing modelling point to at least 72% of a D-MORB component and 28% of a subcontinental lithospheric mantle (SCLM) component in the petrogeneses of the Costa Azul basalts. Models involving mixing between plume-like asthenospheric and SCLM components cannot explain the geochemistry of parental liquids in the Costa Azul suite. A geodynamic model involving continental lithosphere delamination and entrainment by ascending convection cells from the underlying asthenospheric depleted mantle during an advanced stage of Gondwana rifting is depicted on the basis of the petrogenetic models proposed for the Costa Azul suite.

Coordenação de Aperfeiçoamento de Pessoal de Nível Superior / Diques de basaltos toleíticos de baixo-TiO2 ocorrem na porção oriental do Enxame de Diques da Serra do Mar, na Região dos Lagos, entre Niterói e Búzios. Eles têm direções, preferencialmente, NE-SW, subordinadamente, NNE-SSW e mais raramente, NW-SE, e formas intrusivas variáveis. Os basaltos são holocristalinos a hipocristalinos, inequigranulares a equigranulares, intergranulares e intersertais. Eles são constituídos essencialmente de plagioclásio, augita e/ou pigeonita, com olivina corroída, minerais opacos e apatita como minerais acessórios e biotita, bowlingita, idingisita, uralita e saussurita como minerais secundários. A assembléia de fenocristais destas rochas foi estimada em 15% de olivina, 40% de augita e 45% de plagioclásio. Os rochas inserem-se numa série basáltica subalcalina de afinidade toleítica de baixo-TiO2 pouco expandida (MgO= 8,13-5,91%peso), não tendo sido encontradas amostras representativas de líquidos basálticos primários. Esta suíte predominante foi denominada Suíte Costa Azul. No entanto, os dados litogeoquímicos apontam para a existência de mais que uma suíte de baixo-TiO2 na área de estudo que, segundo modelos de fusão parcial em equilíbrio modal, poderiam ter sido geradas por diferentes quantidades de fusão a partir de uma mesma fonte com granada residual. Em termos regionais, a suíte Costa Azul pode ser relacionada com a Suíte Esmeralda que ocorre na subprovíncia Sul de Paraná-Etendeka, muito embora abrangendo um espectro mais amplo de razões Ti/Y. As rochas da suíte Costa Azul evoluíram por 42% de cristalização fracionada envolvendo uma assembléia de fenocristais composta por 15% de olivina, 40% de augita e 45% de plagioclásio, sem mudança de assembléia fracionante. Misturas de componentes mantélicos empobrecidos (mínimo de 72% de D-MORB) e enriquecidos (máximo de 28% de manto litosférico subcontinental) estão associadas à petrogênese desta suíte. Misturas entre componentes do tipo pluma e litosféricos não conseguem explicar as composições parentais da suíte. Os modelos petrogenéticos permitiram a proposição de um modelo geodinâmico envolvendo delaminação do manto litosférico subcontinental englobado por células convectivas ascendentes do manto sublifosférico subjacente em níveis astenosféricos pouco profundos durante um estágio avançado de rifteamento do supercontinente Gondwana. / Low-TiO2, tholeiitic basalt dykes occur eastwards the Serra do Mar Dyke Swarm within the Região dos Lagos from Niterói up to Búzios city. The dykes strike preferentially NE-SW bearing variable intrusive structures. The basalts are holo- to hypocrystaline, equigranular to inequigranular rocks with mostly intergranular and intersertal textures. They are composed mostly by plagioclase, augite and/or pigeonite and have corroded olivine, opaque minerals and apatite as accessory phases. Secondary mineralas are represented by biotite, bowlingite, iddingisite, uralite and saussurite. The phenocrysts assemblage comprise 15% olivine, 40% augite and 45% plagioclase. The rocks comprise a low-TiO2, subalkaline, tholeiitic basaltic suite hereafter called the Costa Azul suite. Nevertheless, lithogeochemical data point to the existence of more than one low-TiO2 suite in the study area. Geochemical modelling has shown that these suites can be related by different degrees of partial melting from a similar mantle source with residual garnet. The Costa Azul suite can be related with the Esmeralda low-TiO2 basaltic suite within the Paraná-Etendeka CFB province due south Brazil although comprising a wider Ti/Y ratio range. The rocks of the Costa Azul suite evolved by 42% of fractional crystallisation involving a phenocryst assemblage with 15% de olivine, 40% augite and 45% plagioclase. Binary mixing modelling point to at least 72% of a D-MORB component and 28% of a subcontinental lithospheric mantle (SCLM) component in the petrogeneses of the Costa Azul basalts. Models involving mixing between plume-like asthenospheric and SCLM components cannot explain the geochemistry of parental liquids in the Costa Azul suite. A geodynamic model involving continental lithosphere delamination and entrainment by ascending convection cells from the underlying asthenospheric depleted mantle during an advanced stage of Gondwana rifting is depicted on the basis of the petrogenetic models proposed for the Costa Azul suite.

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