No description available.

This study presents a petrographic description and a classification of ordinary chondrite NWA 6514 and aims to establish the first high-precision Pb-Pb age of a single ordinary chondrite chondrule. Furthermore, the distribution of different isotopic Pb signatures among chondritic components will be investigated by Laser Ablation Inductively Coupled Plasma Mass Spectrometry (LA-ICP-MS). This study shows that NWA 6514 can be classified as a highly unequilibrated (subtype 3.10) L or LL chondrite that has experienced moderate terrestrial weathering (W2) and a low degree of shock (S2). The LA-ICP-MS measurements suggest that radiogenic Pb signatures have been locally preserved in chondrules. However, the Pb isotopic compositions of leaches from a large chondrule obtained by thermal ionization mass spectrometry show an anomalous distribution that indicates the presence of an exotic Pb component. The best estimate for the chondrule formation age is a model age of the last leach (4566.8 ± 2.6 Myr).

This study presents a petrographic description and a classification of ordinary chondrite NWA 6514 and aims to establish the first high-precision Pb-Pb age of a single ordinary chondrite chondrule. Furthermore, the distribution of different isotopic Pb signatures among chondritic components will be investigated by Laser Ablation Inductively Coupled Plasma Mass Spectrometry (LA-ICP-MS). This study shows that NWA 6514 can be classified as a highly unequilibrated (subtype 3.10) L or LL chondrite that has experienced moderate terrestrial weathering (W2) and a low degree of shock (S2). The LA-ICP-MS measurements suggest that radiogenic Pb signatures have been locally preserved in chondrules. However, the Pb isotopic compositions of leaches from a large chondrule obtained by thermal ionization mass spectrometry show an anomalous distribution that indicates the presence of an exotic Pb component. The best estimate for the chondrule formation age is a model age of the last leach (4566.8 ± 2.6 Myr).

This study investigates the pre-accretionary formation conditions of individual minerals within chondrules and whole-rock parent asteroid processes from the Renazzo-like carbonaceous (CR) chondrites. It presents a comprehensive work on the whole-rock O-isotope composition, sulfide-bearing opaque minerals, and type-II chondrules within the CR chondrites. Whole-rock O-isotope composition and minerals present in type-II chondrules are found to be related to the degree of parent asteroid aqueous alteration. Primary minerals within chondrules, formed prior to accretion of the CR chondrite parent asteroid, are used to constrain both the environment and the conditions present during chondrule formation.Chondrule formation, as recorded by chondrules in the CR chondrites, took place under dust- and ice-rich conditions relative to solar values. Type-II (FeO-rich) chondrules contain FeO-poor fragments compositionally similar to type-I (FeO-poor) chondrules; the formation of type-II chondrules may have occurred after the formation of type-I chondrules. The dust and ice abundances present during type-II chondrule formation were higher than those of type-I chondrules, although both populations probably exchanged with the same ¹⁶O-poor gas reservoir. Both the oxygen fugacity (fo₂) and sulfur fugacity (fs₂) appear to have increased from type-I to type-II chondrule formation, and between individual type-II chondrules. The increase in fo₂ and fs₂ may be due to the dissipation of H2 in the early Solar System. Gas-solid oxidation/sulfidation of Fe,Ni metal is recorded in both type-I and type-II chondrules. This corrosion occurred either during chondrule cooling after formation, or during chondrule reheating events, and suggests that S was present in the gas phase. After chondrule formation the CR chondrite parent asteroid accreted ¹⁶O-poor ice and experienced variable degrees of aqueous alteration, possibly due to heterogeneity in accreted ice or ammonia abundances and/or differing depth within the asteroid. Individual regions of the asteroid experienced different degrees of brecciation, perhaps a result of impacts, which fragmented chondrules and mixed together material that experienced different degrees of aqueous alteration. This process resulted in the heterogeneous nature of the CR chondrites.These observations constrain the formation conditions of a minor body, the CR chondrite parent asteroid, a remnant from the earliest stages of planet formation.

No description available.

Les météorites les plus primitives, appelées chondrites, sont les témoins privilégiés de la formation des premiers solides du système solaire et des processus qui ont conduit à la naissance des premiers corps planétaires. Les chondres, qui sont des sphérules ferromagnésiennes ignées, et leur matrice finement cristallisée constituent l’essentiel du volume des chondrites primitives. L’origine des chondres comme celle de la matrice est encore largement débattue. Cette thèse interroge les relations qui existent entre les chondres et la matrice à grains fins qui les auréole fréquemment, notamment dans les chondrites carbonées. En prenant l’exemple de la chondrite Vigarano (CV3) nous explorons la piste d’un continuum des conditions physico-chimiques pour former les chondres et leurs auréoles de matrice à grain fin. La thèse aborde cette problématique par une double approche : une approche expérimentale consacrée à la quantification des vitesses de dissolution de l’olivine dans des liquides silicatés caractéristiques des chondres de type I et une approche de caractérisation détaillée de la minéralogie, des fabriques et de la composition isotopique de l’oxygène des chondres et de leurs auréoles de matrice à grains fins dans Vigarano. Ces travaux suggèrent que chondre et matrice pourraient enregistrer une continuité d’interaction avec le gaz environnant, d’abord de type liquide/gaz (solubilité) pour la formation des chondres, puis de type solide/gaz (condensation) à plus basse température pour la formation des auréoles de matrice à grains fins / The most primitive meteorites, the chondrites, are our best witnesses of solar system birth and formation of first solids as well as processes that formed the first planetary bodies. Both chondrules, which are ferromagnesian igneous spherules, and fine-grained matrix, constitute the largest volume fraction of primitive chondrites. Their origin still constitutes a matter of debate. This thesis questions the relationship between chondrules and fine-grained matrix, called fine-grained rims, that frequently overlay chondrules in primitive carbonaceous chondrites. By taking the example of Vigarano (CV3), we explore the idea that chondrules and fine-grained rims could form in a continuum of physical and chemical conditions. This thesis combines both experimental and characterization approaches, with an experimental determination of olivine dissolution rates in molten silicates representative of type I chondrule melts and a detailed petrographic characterization of mineralogy, fabrics and oxygen isotopic composition of chondrules and their fine-grained rims in Vigarano. This work suggests that chondrules and their fine-grained rims could register a continuous interaction with surrounding gas, with first, chondrule formation from liquid/gas interaction (solubility) and then fine-grained rim formation, at lower temperature and from solid/gas interaction (condensation)

207Pb*/206Pb* chronometry was used to obtain the ages of Ca,Al-rich inclusions (CAIs) and chondrules found in ancient meteorites. Assuming a 238U/235U=137.88, Pb/Pb ages of chondrules in NWA801 (a CR2 meteorite) are 4564.6±1.0 Ma, chondrules in Mokoia (a CV3 chondrite) are 4564.2±1.1Ma, and CAIs in Mokoia are 4567.9±5.4 Ma. The Pb/Pb age of NWA801 chondrules is concordant with 26Al/26Mg ages of CR chondrules. However if a 238U/235U < 137.88 is used, the age for NWA801 chondrules becomes younger by ~1Ma and discordant with 26Al/26Mg ages of CR chondrules. This suggests either a discrepancy with the U compositions or the initial Mg isotopic compositions of NWA801 chondrules. The shapes of NWA801 chondrules, and blebs of FeNi metal in the meteorite matrix, were further studied by 3D X-ray micro-computed tomography (CT). Most chondrules (92%) were ‘armoured’ with one discontinuous layer of FeNi metal. Two layers of FeNi metal (one on the exterior and one concentric through the interior separated by silicate) were rare <8%. Chondrules and matrix blebs occur as oblates, prolate, spheres and triaxial spheroids. It is proposed that the shapes were made free-floating in the nebula likely by flash-melting precursors into molten droplets that were vibrating as harmonic oscillators that ‘froze-in’ their shapes during cooling. Parent-body metamorphism and shock are not likely processes affecting the matrix-bleb and chondrule shapes. Chondrules with ≥2 FeNi metal layers were likely formed by mergers and not by successive deposition and annealing of metal in multiple flash-melting events. Attempts to obtain 207Pb*/206Pb* ages from chondrules and CAIs by thermal extraction (TE)- TIMS were unsuccessful. However LA-ICP-MS was shown to be useful for rapidly determining Pb isotopic trends in meteorites and unknown objects. In particular, it was shown that 137La (T1/2=60ky) should be detectable in recently fallen meteorites using LaF−4 to suppress the 137Ba isobar during tandem accelerator mass spectrometry combined with a novel instrumental technique for isobar separation.

207Pb*/206Pb* chronometry was used to obtain the ages of Ca,Al-rich inclusions (CAIs) and chondrules found in ancient meteorites. Assuming a 238U/235U=137.88, Pb/Pb ages of chondrules in NWA801 (a CR2 meteorite) are 4564.6±1.0 Ma, chondrules in Mokoia (a CV3 chondrite) are 4564.2±1.1Ma, and CAIs in Mokoia are 4567.9±5.4 Ma. The Pb/Pb age of NWA801 chondrules is concordant with 26Al/26Mg ages of CR chondrules. However if a 238U/235U < 137.88 is used, the age for NWA801 chondrules becomes younger by ~1Ma and discordant with 26Al/26Mg ages of CR chondrules. This suggests either a discrepancy with the U compositions or the initial Mg isotopic compositions of NWA801 chondrules. The shapes of NWA801 chondrules, and blebs of FeNi metal in the meteorite matrix, were further studied by 3D X-ray micro-computed tomography (CT). Most chondrules (92%) were ‘armoured’ with one discontinuous layer of FeNi metal. Two layers of FeNi metal (one on the exterior and one concentric through the interior separated by silicate) were rare <8%. Chondrules and matrix blebs occur as oblates, prolate, spheres and triaxial spheroids. It is proposed that the shapes were made free-floating in the nebula likely by flash-melting precursors into molten droplets that were vibrating as harmonic oscillators that ‘froze-in’ their shapes during cooling. Parent-body metamorphism and shock are not likely processes affecting the matrix-bleb and chondrule shapes. Chondrules with ≥2 FeNi metal layers were likely formed by mergers and not by successive deposition and annealing of metal in multiple flash-melting events. Attempts to obtain 207Pb*/206Pb* ages from chondrules and CAIs by thermal extraction (TE)- TIMS were unsuccessful. However LA-ICP-MS was shown to be useful for rapidly determining Pb isotopic trends in meteorites and unknown objects. In particular, it was shown that 137La (T1/2=60ky) should be detectable in recently fallen meteorites using LaF−4 to suppress the 137Ba isobar during tandem accelerator mass spectrometry combined with a novel instrumental technique for isobar separation.

La Terre contient une quantité significative d’eau et son manteau est très oxydé par rapport aux conditions canoniques de la nébuleuse solaire, ce qui est contradictoire avec l’existence de son noyau métallique et sa position dans le Système solaire. Ceci implique que l’état rédox de la Terre ait augmenté au début de son histoire. Aujourd’hui, de nombreuses études suggèrent que cette évolution se soit faite à travers une accrétion hétérogène. Ainsi les premières briques élémentaires de notre planète seraient constituées de matériel très réduit et une grande partie de la différenciation précoce (extraction du noyau et différenciation silicatée) se seraient donc déroulées en conditions très réductrices (entre IW-5.5 et IW-2). L’objectif de cette thèse est de mesurer l’impact de ces conditions sur le comportement des terres rares (REE) et des éléments fortement chargés (HSFE), et de modéliser leur répartition dans les différents réservoirs lors de la différenciation précoce de la Terre. Nous réalisons une soixantaine d’expériences de fusion – cristallisation à l’équilibre de matériel chondritique à basse (5 GPa) et haute (26 GPa) pression, dans une gamme de conditions rédox allant de IW (tampon fer – wüstite) à IW-8. Afin de caractériser le paramètre fO 2 dans ces conditions extrêmes, nous développons un formalisme thermodynamique adapté, basé sur l’équilibre Si-SiO 2 . En analysant les différentes phases à l’équilibre dans les différents échantillons, nous calculons et établissons la première banque de données de partage cristal (enstatite, bridgmanite = pérovskite silicatée, majorite) – liquide silicaté, métal-silicate et sulfure-silicate pour les HFSE et les REE en conditions très réductrices. Grâce aux données enstatite – liquide nous développons un proxy de la fO 2 , basé sur le rapport D(Cr)/D(V) et grâce auquel nous mesurons la fO 2 de chondres de type I comme étant similaires aux conditions canoniques de la nébuleuse (IW-7). Nos données de partage métal – silicate prouvent que l’extraction du noyau terrestre n’est pas à l’origine d’un fractionnement des terres rares. Au contraire, en mesurant pour la première fois le spectre XANES du Nb 2+ et du Ta 3+ dans des verres silicatés à des teneurs de l’ordre du ppm, nous prouvons que le comportement de Nb et Ta est contrôlé par la fO 2 . En intégrant nos données de partage à un modèle d’accrétion hétérogène nous montrons que la signature sous-chondritique en Nb/Ta de la Terre silicatée peut être le résultat de l’accrétion d’un matériel chondritique évoluant avec le temps combinée à l’extraction du noyau en conditions réductrices, ce qui réfute l’hypothèse d’une Terre se formant à partir d’un matériel oxydé. Nos expériences de haute pression montrent que le partage des REE et des HFSE dans la majorite et la bridgmanite est très sensible à la fO 2. De plus, le processus de dismutation du fer, invoqué pour expliquer l’augmentation de la fO 2 du manteau lors de la cristallisation de l’océan magmatique, ne semble pas être un mécanisme efficace en-dessous de IW. Enfin, nos données montrent que Ti, V, Cr, Mn, Nb et Ta sont chalcophiles en conditions très réductrices. L’extraction précoce d’un liquide sulfuré dans ces conditions a donc pu modifier les rapports élémentaires supposés chondritiques dans la Terre silicatée. L’extraction d’une importante quantité de FeS pourrait aussi être à l’origine d’un découplage Zr/Hf. / The Earth contains significant amounts of water and its mantle is highly oxidized compared to the solar nebula canonical conditions, which is inconsistent with the existence of its metallic core and its location in the Solar System. This implies the redox state of the Earth has increased during its early history as suggested in heterogeneous accretion models. Thus, the first building blocks of our planet would have been made of highly reduced material, and the early Earth’s differentiation (core extraction and silicate differentiation) would have taken place under highly reducing conditions (between IW-5.5 and IW-2). The aim of this thesis is to measure the impact of these conditions on rare earth elements (REE) and high field strength elements (HFSE) behavior, and model their distribution into the main reservoirs formed early in Earth’s history. We run about sixteen melting – crystallization experiments, starting from chondritic material and equilibrating it at low (5 GPa) and high (26 GPa) pressure, spanning a redox range going from IW (iron – wüstite buffer) to IW-8. In order to characterize the fO 2 parameter in these extreme conditions, we develop an adapted thermodynamic formalism, based on Si-SiO 2 equilibrium. Analyzing the various equilibrated phases within our experimental samples, we calculate and propose the first crystal (enstatite, bridgmanite = Mg-perovskite, majorite) – silicate liquid, metal – silicate, sulfide – silicate partition coefficients database for HFSE and REE under highly reducing conditions. Using our enstatite-liquid data we develop a fO 2 proxy based on D(Cr)/D(V) ratio and we measure type I chondrule fO 2 as being similar to canonical nebular conditions (IW-7). Our metal-silicate partitioning data prove that Earth core extraction is not responsible for REE fractionation. On the contrary, recording for the first time Nb 2+ and Ta 3+ XANES spectra in silicate glasses and at ppm level concentrations, we prove that Nb and Ta behavior is mainly controlled by fO 2 . Using our partitioning data in a heterogeneous accretion model, we show that sub-chondritic Nb/Ta signature of the silicate Earth (14 ± 0.3) can be the result of the accretion of chondritic material changing with time, combined with the progressive extraction of the core in reducing conditions. This refutes the hypothesis of an oxidized material building the Earth. Our high-pressure experiments show that REE and HFSE partitioning in majorite and bridgmanite is very sensitive to fO 2 . Moreover, iron dismutation process, invoked to explain mantle fO 2 increase during magma ocean crystallization, does not seem to be an efficient mechanism below IW. Finally, our data show that Ti, V, Cr, Mn, Nb and Ta are chalcophiles under highly reducing conditions. Consequently, early extraction of a sulfide melt at an early and reduced stage could have modified chondritic elementary ratios in the silicate Earth. Extraction of a substantial amount of FeS may also cause a Zr/Hf decoupling.