Phase equilibria and volumetric properties in the system water-sodium chloride-carbon dioxide were determined experimentally for pressures between about 1 to 6 kbar, temperatures of 300° to 800°C, and fluid compositions up to 40 wt% NaCl and 20 mol% carbon dioxide, both relative to water. This was accomplished by using the synthetic fluid inclusion technique in conjunction with conventional microthermometry, a hydrothermal diamond-anvil cell and Raman spectroscopy. At constant salinity, the high-pressure portion of the solvus migrates to higher pressures and temperatures with increasing carbon dioxide concentration. Immiscibility is possible in this ternary system over almost the entire range of crustal P-T conditions at salinities equal to or in excess of 20 wt% NaCl and carbon dioxide concentrations between about 30 and 70 mol% carbon dioxide. The dP/dT slopes of lines of equal homogenization temperature decrease nonlinearly with increasing homogenization temperature; at constant homogenization temperature, these slopes become steeper (higher) along pseudobinaries with addition of carbon dioxide and particularly with addition of sodium chloride. Up to concentrations of 20 wt% NaCl and 20 mol% carbon dioxide, a sharp rise in the critical temperature was observed with increasing salinity at a fixed water/carbon dioxide ratio. The critical point shifts rapidly towards higher pressures with increasing carbon dioxide concentration. Addition of carbon dioxide to an aqueous 40 wt% NaCl solution results in a slight elevation of the halite dissolution temperature under vapor-saturated conditions. A significant error can be associated with the calculation of molar volumes from measured densities of the carbonic phase of water-sodium chloride-carbon dioxide inclusions. To avoid such errors, phase diagrams were constructed based on the obtained lines of equal homogenization temperature for salinities between 6 and 40 wt% NaCl and carbon dioxide concentrations between 5 and 20 mol% relative to water. These diagrams are of direct applicability to the interpretation of natural fluid inclusions from a wide variety of geologic environments. / Ph. D.

This thesis demonstrates that geological setting, depositional facies, open system flux of hot basinal brines and descending of shallow waters have a strong impact on the distribution of the diagenetic alterations within continental and paralic/shallow marine sandstones which in turn control the quality and heterogeneities of the reservoirs. Geological setting controls the mineralogical and textural maturity of sandstone, whereas depositional facies control the pore water chemistry (marine, brackish or meteoric), sedimentary texture and sand body geometry. Eogenetic alterations in the fluvial deposits are dominated by precipitation of infiltrated clays, kaolinitization of detrital silicates, whereas the shallow marine deposits are dominated by precipitation of early calcite and kaolinite. Conversely mesogenetic alterations are dominated by clay minerals transformation, quartz overgrowths and Ferroan- carbonates, barite and anhydrite. Flux of hot basinal brines is evidenced by precipitation of mesogenetic minerals that lack of internal sources (e.g. barite, anhydrite and ferroan carbonate cements), which is evidenced by: (1) restricted occurrence of these minerals in downthrown blocks. (2) The high fluid inclusion homogenization temperatures (Th) of quartz overgrowths (Th &gt; 110-139°C), and carbonate cements (T &gt; 80-140°C), which also have light δ18OV-PDB(-17.6‰ to -6.7‰). Flux of hot basinal brines is further evidenced by occurrence of saddle Fe-dolomite along stylolites. Fluid inclusion microthermometry further revealed a dramatic shift in pore- water chemistry from NaCl dominated brines during precipitation of quartz overgrowths to NaCl-CaCl2 dominated brines during cementation by Fe-dolomite. Presence of mixed brine (NaCl+CaCl2) systems in the fluid inclusions suggests flux of descending waters, which have circulated in the overlying carbonate-evaporite successions. The restricted occurrence of oil- filled inclusion to quartz overgrowths and methane to Fe-carbonate cements suggest migration of oil during precipitation by quartz and migration of methane during precipitation by Fe- carbonate cements. The extensive mesogenetic cements in the down thrown blocks is attributed to flux of basinal brines along deep seated faults, i.e. open system diagenesis. Integration of fluid inclusion microthermometry, isotopes, Raman spectrometry and thermal tectonic evolution of basins are essential techniques for unraveling the evolution of basinal fluids, cementation conditions and relative timing of hydrocarbons migration. / <p>Errata: Felaktigt disputationsdatum på spikbladet.</p>

Un des enjeux majeurs en Science de la Terre ces dernières décennies est de comprendre les interactions entre les différentes enveloppes terrestres. Le but poursuivi par ce travail est d’aborder quelques aspects de ces interactions du point de vue des cycles géochimiques des éléments volatils H2O et CO2 en se basant sur l’étude des inclusions fluides piégées dans des roches variées de la croûte terrestre, depuis sa surface jusqu’à l’interface croûte–manteau. La première partie de mon travail présente des travaux expérimentaux effectués sur de la halite. L’étude du fractionnement isotopique de l’oxygène et des cinétiques d’équilibration entre H2O et CO2 lors de l’évaporation de saumures a montré l’importance des corrections à effectuer sur les mesures isotopiques de l’oxygène pour des solutions de haute salinité. L’élaboration d’un protocole expérimental de précipitation de halite en milieu contrôlé a permis de mettre en évidence le potentiel des inclusions fluides pour les reconstitutions paléoclimatiques. La combinaison des données microthermométriques et des compositions isotopiques de l’hydrogène et de l’oxygène des inclusions aqueuses permet d’estimer les sources et la température de l’eau de formation de la halite ainsi que la vitesse du vent à l’interface eau-air pendant la croissance du cristal. Cette méthode a été ensuite appliquée aux dépôts de halite de Sicile datés du Messinien. La deuxième partie de mon travail est consacrée à l’identification des compositions chimiques et des sources des fluides circulant dans la croûte et à l’interface croûte-manteau à travers l’analyse des compositions isotopiques des inclusions fluides des granites et granulites. / One of the major challenges in Earth Sciences during the last decades has been to improve our knowledge of the interaction between the different components of the Earth System. Key aspects to improve the understanding of these processes are the acquisition of new data and the development of models to explain both mass and energy transfer between the deep and superficial components of the Earth system. The goal of this thesis is to study these transfers through the geochemical cycle of volatile elements trapped in fluid inclusions of various materials of the Earth crust. The first part of my work presents experimental study of halite. The study of oxygen isotope fractionation and equilibrium kinetics between H2O and CO2 during the evaporation of brines shows that corrections have to be made on the oxygen isotope measurements for high salinity solutions. The elaboration of an experimental protocol to form halite in controlled environment reveals the potential of fluid inclusions for palaeo climatic reconstructions. Combination of microthermometric data plus hydrogen and oxygen isotopic compositions of aqueous inclusions allows to estimate the sources and the temperature of the parental water of halite as well as the wind speed at the water-air interface during the crystal growth. This method was then applied to the Messinian halite deposits of Sicily. The second part of my work is dedicated to the identification of both the chemical compositions and the sources of fluids circulating in the crust and at the interface crustmantle through the analysis of isotopic compositions of fluid inclusions in granites and granulites.

When and how life first emerged on the Earth is an area of intense research. Signs of the first life on Earth, including morphological fossils, are scarce and hard to interpret. An alternative approach is to study organic biomarkers, which are molecular fossils commonly considered as bona fide biosignatures. The main objective of the project is to develop an approach for analysis of single oil-bearing fluid inclusions and most importantly the detection of organic biomarkers in these inclusions. Analysis of oil-bearing fluid inclusions is advantageous since the inclusions may provide an uncontaminated sample source of Precambrian hopanes and steranes, which are key biomarkers for tracing the early evolution of life on Earth. Due to the presence of several inclusion generations, single inclusion analysis is desired in order to constrain biomarkers to specific inclusions. Time-of-flight secondary ion mass spectrometry (ToF-SIMS) could be an excellent tool for analysis of these types of samples. The development of the approach for analysis of single oil-bearing inclusions was done in a two-step process; i) a number of crude oils were analysed with ToF-SIMS and gas chromatography mass-spectrometry (GC-MS) to facilitate interpretation of ToF-SIMS spectra of these types of samples and, ii) a procedure that combines micrographs with ion etching and ToF-SIMS analysis was developed for analysis of inclusions. The feasibility of the technique was demonstrated for oil inclusions from the Siljan impact crater in which hopanes and steranes where detected. Single oil-bearing fluid inclusions trapped in mid-Proterozoic sandstones from Northern Australia were subsequently analyzed, and steranes and hopanes were detected in these inclusions. If applied on older inclusions this approach may help answer some of the questions regarding the emergence and evolution of life on Earth, and if applied on extraterrestrial samples, also the possibility of life on other planets and moons. / Livets uppkomst och tidiga utveckling på jorden är ett hett forskningsfält. Hur och när livet och dess olika domäner (arkéer, bakterier och eukaryoter) uppstod på jorden är fortfarande oklart vilket beror på att de första tecknen på liv, vilka inkluderar morfologiska fossil, spårfossil och isotoper, är få och svåra att tolka. Ett alternativt sätt att studera det tidiga livet är att studera organiska biomarkörer som är organiska molekyler som anses unika för liv. Huvudmålet med projektet är att utveckla en metod som kan detektera organiska biomarkörer i enskilda oljebärande vätskeinneslutningar. Vätskeinneslutningar, som är små mängder vätska (picoliter) infångad in en sten, är intressanta då de är en potentiell provkälla för prekambriska (äldre än 500 miljoner år) biomarkörer, som hopaner och steraner, vilka används för att utforska livets tidiga utveckling på jorden. Analys av enskilda inneslutningar är emellertid oftast nödvändigt för att kunna tidsavgränsa biomarkörer. På grund av att de flesta inneslutningar är små (10 µm i diameter) är det inte möjligt att analysera en enskild vätskeinneslutning med standardtekniken gaskromatografi-masspektrometri (GC-MS). Time-of-flight secondary ion mass spektrometri (ToF-SIMS) med sin höga känslighet, höga massupplösning och kapacitet för 2D-representation av analysdata och djupprofilering av prover är en utmärkt teknik för analys av enskilda inneslutningar. Metoden för analys av enskilda inneslutningar utvecklades i två steg. Först analyserades ett antal råoljor med ToF-SIMS och GC-MS för att underlätta förståelsen av ToF-SIMS-spektra från dessa typer av prover. Därefter utvecklades en metod som bestod av mikroskopering för att lokalisera inneslutningen, jonetsning för att öppna inneslutningen och ToF-SIMS analys av det exponerade innehållet. Metoden testades framgångsrikt på enskilda inneslutningar i hydrotermala vener av flusspat och kalcit i ordovicisk (488-443 miljoner år sedan) kalksten. Därefter användes den utvecklade metoden för att analysera enskilda vätskeinneslutningar i 1,43 miljarder år gammal sandsten från norra Australien, i vilka hopaner och steraner detekterades. De detekterade steranerna visar att trots att havet under denna tid var syrefritt existerade det lokala syrerika miljöer där eukaryoter kunde överleva. Om den utvecklade metoden används på ännu äldre inneslutningar, vilka har daterats till 3,2 miljarder år, kan den komma att svara på några de mest fundamentala frågorna kring livets uppkomst och tidiga utveckling. Om metoden används på utomjordiska prover kan den svara på frågan om det finns liv på andra planeter eller månar. / At the time of the doctoral defense, the following papers were unpublished and had a status as follows: Paper 3: Manuscript. Paper 4: Submitted.

Middle Ordovician carbonates in the Lake Simcoe area, south-central Ontario were examined to determine if: (1) The δ18O values of early-stage calcite cement in hardgrounds are useful proxies for Ordovician seawater δ18O values; (2) a regional hydrothermal event affected middle Ordovician strata in the Lake Simcoe area. Whole rock samples of middle Ordovician hardgrounds and immediately overlying limestones containing early calcite cement have δ13C values ranging from -1.7 to +2.9‰ (PDB) and δ18O values ranging from -6.9 to -2.9‰ (PDB). Hardground δ18O values and the similarity of the isotopic composition between the hardgrounds and overlying limestones are consistent with diagenetic alteration during shallow burial, which indicates the hardgrounds are not useful proxies. Late-stage calcite cements have δ13C values from -8.4 to +2.9‰ (PDB) and δ18O values from -11.4 to -6.0‰ (PDB). Late-stage microcrystalline dolomites have δ13C values from -3.9 to +0.4‰ and δ18O values from -10.7 to -7.6‰. Late-stage saddle dolomites have δ13C values from -1.7 to 1.9‰ and δ18O values from -13.8 to -8.5‰. The late-stage carbonate δ18O values are more negative than the early-stage carbonate δ18O values and are interpreted to reflect progressively deeper burial diagenesis. Four types of fluid inclusions were identified in late-stage calcite, saddle dolomite, barite, and quartz. Type 1 inclusions are aqueous liquid-rich with very consistent low to very low vapour-liquid ratios and are of primary, secondary pseudosecondary and indeterminate origins. Type 2 inclusions are aqueous liquid-only and are of primary and secondary origins. Type 3 inclusions are oil-bearing, liquid-rich with low to medium vapor-liquid ratios and are of secondary origin. Type 4 inclusions are vapour-only and are of indeterminate origin. The type 4 inclusions analyzed did not yield any microthermometric data suggesting they are empty cavities that have lost all their fluid. Fluid inclusions of primary, secondary and pseudosecondary origins in calcite, dolomite and quartz have overlapping homogenization temperatures ranging from 43 to 188°C. Fluid inclusions of indeterminate origin in calcite and barite have homogenization temperatures from 80 to greater than 200°C. Petrographic and microthermometric evidence indicates that fluid inclusion homogenization temperatures greater than 150°C most likely are caused by stretching or leaking; therefore, are discounted. Fluid inclusion types 1 and 2 represent two fluid inclusion assemblages (FIA) based on final ice melting temperatures. The high salinity (10 to 30 wt%CaCl2) inclusions in FIA 1 are of primary, secondary, pseudosecondary and indeterminate origin in calcite, dolomite, barite and quartz. Fluid inclusions in FIA 1 are interpreted as reflecting saline basin brines from which the host minerals precipitated during burial diagenesis. The low salinity (0 to 2.7 wt%CaCl2) inclusions in FIA 2 are of secondary and indeterminate origin in calcite. Fluid inclusions in FIA 2 may reflect a meteoric origin such as in a vadose or phreatic environment based on inclusions containing different phases and variable vapor-liquid ratios. Alternatively the low salinity inclusions may reflect alteration from an influx of meteoric fluids that migrated through basement faults and fractures during periods of uplift and erosion. Early and late-stage carbonates from this study precipitated from 18O-depleted pore fluids and/or at progressively higher temperatures accompanying deeper burial. The FIA 1 homogenization temperatures support burial diagenesis at 66 to 80°C if it is assumed the rocks were buried 2 km, the surface temperature was 20°C and the geothermal gradient was between 23 to 30°C/km. An alternative interpretation is mineral precipitation during a regional hydrothermal event. Burial diagenesis does not explain the fluid inclusion homogenization temperatures of 90°C and greater unless geothermal gradients are higher than 35°C/km or burial depth is increased to 3 km or more. However, thermal maturity of organic matter in the Michigan Basin suggests Ordovician strata were never buried more than 2 km. Four models for regional hydrothermal fluid migration are: (1) gravity-driven flow; (2) ‘squeegee-type’ fluid flow; (3) convection cell fluid flow; and (4) structurally-controlled fluid flow. The gravity-driven model relies on continental heat flow and an influx of meteoric water from basin catchment areas. For the ‘squeegee, convection cell and structurally controlled models, hot fluids could have entered the region from several conduits concurrently during episodic reactivation of basement faults and fracture systems in response to intracratonic stresses created by the continuous interaction of tectonic plates. Determining which of the models best explains regional hydrothermal fluid flow in the Michigan Basin is difficult for several reasons; (1) surface temperatures and maximum burial temperatures at the time of mineral precipitation in the Michigan Basin during the Ordovician are unknown; (2) the timing of mineral precipitation in relation to tectonic pulses is undetermined; (3) there is as yet no known deep-seated heat sources in the Michigan Basin for convection to occur; and (4) it is unknown whether advection is a major process in the Michigan Basin. A collaborative multi-disciplinary research project covering geology, geophysics and hydrogeology would provide much more integrated data than is currently available from stable isotopes, fluid inclusions and organic matter.

No description available.

Middle Ordovician carbonates in the Lake Simcoe area, south-central Ontario were examined to determine if: (1) The δ18O values of early-stage calcite cement in hardgrounds are useful proxies for Ordovician seawater δ18O values; (2) a regional hydrothermal event affected middle Ordovician strata in the Lake Simcoe area. Whole rock samples of middle Ordovician hardgrounds and immediately overlying limestones containing early calcite cement have δ13C values ranging from -1.7 to +2.9‰ (PDB) and δ18O values ranging from -6.9 to -2.9‰ (PDB). Hardground δ18O values and the similarity of the isotopic composition between the hardgrounds and overlying limestones are consistent with diagenetic alteration during shallow burial, which indicates the hardgrounds are not useful proxies. Late-stage calcite cements have δ13C values from -8.4 to +2.9‰ (PDB) and δ18O values from -11.4 to -6.0‰ (PDB). Late-stage microcrystalline dolomites have δ13C values from -3.9 to +0.4‰ and δ18O values from -10.7 to -7.6‰. Late-stage saddle dolomites have δ13C values from -1.7 to 1.9‰ and δ18O values from -13.8 to -8.5‰. The late-stage carbonate δ18O values are more negative than the early-stage carbonate δ18O values and are interpreted to reflect progressively deeper burial diagenesis. Four types of fluid inclusions were identified in late-stage calcite, saddle dolomite, barite, and quartz. Type 1 inclusions are aqueous liquid-rich with very consistent low to very low vapour-liquid ratios and are of primary, secondary pseudosecondary and indeterminate origins. Type 2 inclusions are aqueous liquid-only and are of primary and secondary origins. Type 3 inclusions are oil-bearing, liquid-rich with low to medium vapor-liquid ratios and are of secondary origin. Type 4 inclusions are vapour-only and are of indeterminate origin. The type 4 inclusions analyzed did not yield any microthermometric data suggesting they are empty cavities that have lost all their fluid. Fluid inclusions of primary, secondary and pseudosecondary origins in calcite, dolomite and quartz have overlapping homogenization temperatures ranging from 43 to 188°C. Fluid inclusions of indeterminate origin in calcite and barite have homogenization temperatures from 80 to greater than 200°C. Petrographic and microthermometric evidence indicates that fluid inclusion homogenization temperatures greater than 150°C most likely are caused by stretching or leaking; therefore, are discounted. Fluid inclusion types 1 and 2 represent two fluid inclusion assemblages (FIA) based on final ice melting temperatures. The high salinity (10 to 30 wt%CaCl2) inclusions in FIA 1 are of primary, secondary, pseudosecondary and indeterminate origin in calcite, dolomite, barite and quartz. Fluid inclusions in FIA 1 are interpreted as reflecting saline basin brines from which the host minerals precipitated during burial diagenesis. The low salinity (0 to 2.7 wt%CaCl2) inclusions in FIA 2 are of secondary and indeterminate origin in calcite. Fluid inclusions in FIA 2 may reflect a meteoric origin such as in a vadose or phreatic environment based on inclusions containing different phases and variable vapor-liquid ratios. Alternatively the low salinity inclusions may reflect alteration from an influx of meteoric fluids that migrated through basement faults and fractures during periods of uplift and erosion. Early and late-stage carbonates from this study precipitated from 18O-depleted pore fluids and/or at progressively higher temperatures accompanying deeper burial. The FIA 1 homogenization temperatures support burial diagenesis at 66 to 80°C if it is assumed the rocks were buried 2 km, the surface temperature was 20°C and the geothermal gradient was between 23 to 30°C/km. An alternative interpretation is mineral precipitation during a regional hydrothermal event. Burial diagenesis does not explain the fluid inclusion homogenization temperatures of 90°C and greater unless geothermal gradients are higher than 35°C/km or burial depth is increased to 3 km or more. However, thermal maturity of organic matter in the Michigan Basin suggests Ordovician strata were never buried more than 2 km. Four models for regional hydrothermal fluid migration are: (1) gravity-driven flow; (2) ‘squeegee-type’ fluid flow; (3) convection cell fluid flow; and (4) structurally-controlled fluid flow. The gravity-driven model relies on continental heat flow and an influx of meteoric water from basin catchment areas. For the ‘squeegee, convection cell and structurally controlled models, hot fluids could have entered the region from several conduits concurrently during episodic reactivation of basement faults and fracture systems in response to intracratonic stresses created by the continuous interaction of tectonic plates. Determining which of the models best explains regional hydrothermal fluid flow in the Michigan Basin is difficult for several reasons; (1) surface temperatures and maximum burial temperatures at the time of mineral precipitation in the Michigan Basin during the Ordovician are unknown; (2) the timing of mineral precipitation in relation to tectonic pulses is undetermined; (3) there is as yet no known deep-seated heat sources in the Michigan Basin for convection to occur; and (4) it is unknown whether advection is a major process in the Michigan Basin. A collaborative multi-disciplinary research project covering geology, geophysics and hydrogeology would provide much more integrated data than is currently available from stable isotopes, fluid inclusions and organic matter.

L’objectif de cette thèse est d’étudier le comportement du soufre dans des fluides hydrothermaux soumis à un métamorphisme de bas grade. Elle est séparée en trois études interconnectées couplant étude naturelle et expérimentale : i) une étude du cycle du soufre dans les évaporites carniennes de la "Nappe des Gypses" des Alpes françaises comme cas d’étude naturelle a été réalisée, ii) une étude de la spéciation du soufre dans les inclusions fluides associées à ces évaporites triasiques, et iii) une étude expérimentale du rôle de la spéciation du soufre sur le mécanisme de la Thermo-Réduction des Sulfates (TSR) et l’altération des hydrocarbures associée. La première étude repose sur le couplage d’une approche pétrographique classique et d’une étude détaillée des inclusions fluides, des isotopes stable (δ34S, δ33S, δ36S, Δ33S, Δ36S, δ13C et δ18O) et de la matière organique dans la "Nappe des Gypses". Ces études couplées ont permis d’identifier le processus de TSR comme la réaction contrôlant le comportement du soufre dans cette formation en système fermé. La seconde étude repose sur une nouvelle approche analytique couplant spectroscopie Raman in-situ et platine microthermométrique permettant de réchauffer jusqu’à 300°C les échantillons (naturel et synthétique). Ainsi, à température >100°C la présence de l’ion radicalaire S3- et d’autres espèces polymériques du soufre (Snx) a été mise en évidence dans la “Nappe des Gypses”. Cette étude confirme le rôle indispensable à la TSR de l’ion S3- et des Snx dans les fluides naturels. Cette étude naturelle a été complétée par une étude expérimentale préliminaire qui a permis de mettre en place de nouveaux protocoles expérimentaux en autoclave et en capillaires de silice couplés à des analyses spectroscopiques et isotopiques. Ceci afin de mieux comprendre le rôle de la spéciation du soufre dans les interactions entre une phase aqueuse et un fluide hydrocarboné lors de la TSR. Cette thèse conduit à une meilleure compréhension du rôle de la spéciation du soufre et son lien avec des composés organiques lors de la TSR en condition métamorphique de bas grade. Cela ouvre de nouvelles perspectives de compréhension des formations géologiques basées sur le couplage d’études géologiques classiques et d’études géochimiques plus fines / The aim of this thesis is to study the sulfur behavior in hydrothermal fluids subjected to low grade metamorphism. It is separated into three interconnected studies linking natural and experimental study: i) a study of the sulfur cycle in the Carnian evaporites of the "Nappe des Gypses" from the French Alps as a natural case study is performed, ii) a study of the sulfur speciation in fluid inclusions associated to these Triassic evaporites, and iii) an experimental study of the role of sulfur speciation on the Thermochemical Sulfate Reduction (TSR) mechanisms and the associated hydrocarbons alteration. The first study is based on the coupling of a classical petrographic approach associated to a detailed study of fluid inclusions, stable isotopes (δ34S, δ33S, δ36S, Δ33S, Δ36S, δ13C and δ18O) and organic matter in the “Nappe des Gypses”. The coupling study allows to identify the TSR process as the reaction controlling the behavior of sulfur in this formation in a closed system. The second study is based on a new analytical approach coupling in-situ Raman spectroscopy and microthermometric stage. This technique allows to heat up to 300°C samples (natural and synthetic). Thus, at temperature >100°C, the presence of the radical ion S3- and other polymeric sulfur species (Snx) is demonstrated in the “Nappe des Gypses”. This study confirms the essential role in the TSR process of S3- and Snx species in natural fluids. This study natural was completed by a preliminary experimental study allowed to set up new experimental protocols in autoclave and fused silica capillaries coupled to spectroscopic and isotopic analyses. This to better understood the role of sulfur speciation in the interactions between an aqueous phase and a hydrocarbons fluid during the TSR. This thesis leads to a better understanding of the role of sulfur speciation and its link with organic compounds during TSR under low grade metamorphic conditions. This opens new perspectives to understand geological formations based on coupling of classical geological studies and finer geochemical studies

Les principales cibles d'exploration pour les gisements d’uranium de type discordance du bassin d’Athabasca (Canada) sont les structures graphiteuses du socle. Toutes ces structures ne sont pourtant pas fertiles et elles présentent des histoires plus ou moins complexes de circulations fluides successives. Cette thèse propose de déconvoluer les caractéristiques propres à chaque évènement de circulations fluides par une étude multidisciplinaire focalisée sur l’exemple de l’environnement proche du gisement de Cigar Lake. Au cours de l’exhumation tardi-orogénique du socle, la formation de failles ductile-cassantes associées à une circulation intense de fluides à C-O-H-N a permis des enrichissements en graphite et une première évolution pétrophysique des zones endommagées. Ces structures du socle particulièrement fragilisées par la déformation cassante fini-Hudsonienne ont pu être réactivées après dépôt du bassin et devenir des lieux favorables à la convection de saumures sédimentaires. La circulation de saumures sodiques dans le socle a favorisé des interactions fluides-roches à l’origine de la solubilisation de l’uranium, d’altérations K-Mg et d’évolution de composition du fluide vers un pôle plus calcique de plus forte salinité. Enfin une méthodologie d’analyse intégrée des compositions élémentaires majeures, traces et isotopiques U-Pb-O sur oxydes d’uranium est proposée, permettant de déconvoluer les effets des évènements fluides ultérieurs sur la minéralisation primaire. Cinq évènements ont ainsi contribué aux caractéristiques actuelles du gisement de Cigar Lake : Un évènement primaire de circulation de saumures à 1290-1380 Ma, à l’origine de l’ensemble du stock d’uranium ; un événement de circulations fluides à ca. 900 Ma à l’échelle régionale qui n’est pas associé à une reprécipitation d’uranium mais a brechifié et perturbé la chimie des oxydes primaires ; deux évènements tardifs de circulations fluides à ca. 340 et 220 Ma qui ont significativement remobilisé le stock primaire d’uranium. Enfin un dernier épisode récent de circulation d’eaux météoriques est à nouveau à l’origine d’un changement de chimie des oxydes antérieurs et d’une remise à zéro des systèmes isotopiques / The main exploration targets for unconformity-related U deposits of the Athabasca Basin are the graphite-rich structures in the basement. But these are not necessarily fertile. They show distinct features expressing specific events of fluid circulations. This study aims, through a multidisciplinary approach, at unravelling the complex history of fluid flow events recorded in the vicinity of the Cigar Lake deposit. During the basement uplift, at the end of the Trans-Hudson Orogeny, the formation of ductile-brittle shear zones associated to the circulation of C-O-H-N fluids led to hydrothermal graphite enrichments and a petrophysical evolution of damages zones. These graphite-rich shear zones that were specifically weakened by the ante-Athabasca brittle reactivation have been reactivated once more after basin deposition allowing the formation of a developed damage zone especially favorable for sedimentary brine convection. Circulations of NaCl-rich brines in the basement led to brine-rock interactions, and subsequent uptake of uranium and other metals from the basement rocks. The latter have subsequently undergone strong K-Mg alteration whereas the NaCl dominated brines evolved toward a CaCl2-dominated composition with higher salinities. Finally, this thesis sets out an integrated methodology allowing to decipher the complex superimposed geochemical signatures of distinct fluid flow events on the primary uranium oxides. Five fluid flow events contributed to the present day state of the Cigar Lake deposit: a primary event of brine circulation occurred at 1290-1380 Ma and is at the origin of the main U stock; a second basin-scale event of fluid flow occurred at ca. 900 Ma, it brecciated and strongly disturbed the deposit; two later events of fluid flow strongly remobilized the deposit at ca. 340 and 220 Ma and greatly contributed to the actual state of the deposit. Finally a last, rather recent event of fluid flow was at the origin of strong chemical changes in the uranium oxides compositions and strong isotopic resetting

Submitted by Simone Souza (simonecgsouza@hotmail.com) on 2017-11-01T14:56:26Z No. of bitstreams: 1 DISS_2014_Jonas Mangoni Rambo.pdf: 9222881 bytes, checksum: 541ad16fc560f2a2f8e066273f9c5d87 (MD5) / Approved for entry into archive by Jordan (jordanbiblio@gmail.com) on 2017-11-08T15:34:43Z (GMT) No. of bitstreams: 1 DISS_2014_Jonas Mangoni Rambo.pdf: 9222881 bytes, checksum: 541ad16fc560f2a2f8e066273f9c5d87 (MD5) / Made available in DSpace on 2017-11-08T15:34:43Z (GMT). No. of bitstreams: 1 DISS_2014_Jonas Mangoni Rambo.pdf: 9222881 bytes, checksum: 541ad16fc560f2a2f8e066273f9c5d87 (MD5) Previous issue date: 2014-04-15 / A Província Aurífera Alta Floresta (PAAF) localiza-se no norte do estado de Mato Grosso, delimitada ao norte pelo Gráben do Cachimbo e ao sul pelo Gráben dos Caiabís. Se enquadra na porção sul do Cráton Amazônico, entre as províncias geocronológicas Ventuari – Tapajós e Rio Negro – Juruena. Na porção leste da PAAF foram selecionados 5 alvos para elaboração deste trabalho: (i) Mina do Edu; (ii) Garimpo do Peteca; (iii) Filão do Laje; (iv) Filão do Cocheira e (v) Filão do Vinte. O corpo mineralizado do Edu tem atitudes de N55ºE/subvertical, e é classificado como estruturas do tipo T. Essas estruturas são fraturas extensionais que ocorreram com a mesma atitude do esforço principal e, portanto, indicam a direção do esforço compressivo principal e são preenchidas por veios de quartzo. A Mina do Edu apresenta fluídos carbônicos e aquosa-carbônico. O Garimpo do Peteca e o Filão do Laje, com atitudes de E-W/subvertical, são classificados como estruturas do tipo R. Os Filões do Cocheira e do Vinte, com atitudes N-S/subvertical, são classificados como estruturas do tipo X, que são zonas confinadas de cisalhamento transcorrente geradas a partir da nucleação de fraturas de cisalhamento dextral. O Garimpo do Peteca, o Filão do Laje, Filão do Cocheira e Filão do Vinte apresentam fluídos estritamente aquosos, variando de alta a média salinidade. Esses fluídos distintos sugerem mineralizações provenientes de uma mesma fonte magmática, no entanto, devido à distância de algumas ocorrências da fonte, o fluído foi interagindo com outros fluídos, se distinguindo assim do fluído primário. / The Alta Floresta Gold Province (PAAF) is located in the northern state of Mato Grosso, bounded on the north by the Gráben do Cachimbo and on the south by Gráben dos Caiabis. The PAAF fits in the southern portion of the Amazon Craton, between the Ventuari - Tapajós and Rio Negro - Juruena geochronological provinces. In the eastern portion of PAAF 5 targets were selected for the present work: (i) Mina do Edu (ii) Garimpo do Peteca (iii) Filão do Laje , (iv) Filão do Cocheira (v) Filão do Vinte. The mineralized body of the Mina do Edu has attitude of N55ºE/subvertical, and is classified as structures of the T type. These structures are extensional fractures that occurred with the same attitude as the main effort, and therefore indicate the direction of the main compressive stress and are filled by quartz veins. The Mina do Edu presents carbonic and aqueous-carbonic fluid inclusions. The Garimpo do Peteca and Filão do Laje, with attitudes of EW/subvertical, are classified as structures of the R type. The Filão do Cocheira and Filão do Vinte, with attitudes NS/subvertical, are classified as structures of the X type, which are enclosures transcurrent shear generated from the nucleation of dextral shear fractures. The Garimpo do Peteca, Filão do Laje, Filão do Cocheira and Filão do Vinte presents strictly aqueous fluid inclusions, ranging from high to medium salinity. These different fluids suggest mineralization from the same magmatic source, however, due to the distance of the source from some instances, the fluid was interacting with other fluids, thus distinguishing from the primary fluid.