The 187Re–187Os systematics, abundances of highly siderophile elements (HSE: Re, platinum group elements and Au), Te, Se and S as well as major and minor elements were determined in separated ...components of two unequilibrated L chondrites QUE 97008 (L3.05) and Ceniceros (L3.7). The 187Re–187Os systematics are disturbed in the components of both meteorites, most likely due to open system behavior of Re during terrestrial weathering of QUE 97008 and alteration on the L chondrite parent body as indicated by an internal errorchron generated for components of Ceniceros. The HSE abundance patterns suggest that the bulk rock abundances were mainly controlled by two different end members. Non-magnetic fractions display lower Re/Os and HSE/Ir than CI chondrites. Chondrules, metal-troilite spherules and fine magnetic fractions, are depleted in refractory HSE and show higher Rh/Ir, Pd/Ir and Au/Ir than in CI chondrites. The different HSE compositions indicate the presence of unequilibrated alloys and loss of refractory HSE-rich carrier phases from the precursors of some L chondrite components. Gold is decoupled from other HSE in magnetic fractions and shows chalcophile affinities with a grain size dependent variation similar to S and Se, presumably inherited from preaccretionary processes. Tellurium is depleted in all components compared to other analysed siderophile elements, and its abundance was most likely controlled by fractional condensation and different geochemical affinities. The volatility dependent depletion of Te requires different physical and chemical conditions than typical for the canonical condensation sequence as represented by carbonaceous chondrites. Tellurium also shows variable geochemical behavior, siderophile in Ceniceros, predominantly chalcophile in QUE 97008. These differences may have been inherited from element partitioning during chondrule formation. Selenium and S on the other hand are almost unfractionated from each other and only show complementary S/Se in a few components, presumably due to the effects of volatility or metal–silicate partitioning during chondrule formation. Terrestrial weathering had negligible effects on the S, Se and Te systematics.
Mass fractions of S, Cu, Se, Mo, Ag, Cd, In, Te, Ba, Sm, W and Tl were determined by isotope dilution sector field ICP‐MS in the same sample aliquot of reference materials using HF‐HNO3 digestion in ...PFA beakers in pressure bombs and glassy carbon vessels in a high‐pressure asher (HPA‐S) for comparison. Additionally, Bi was determined by internal standardisation relative to Tl. Because isobaric and oxide interferences pose problems for many of these elements, efficient chromatographic separation methods in combination with an Aridus desolvator were employed to minimise interference effects. Repeated digestion and measurement of geological reference materials (BHVO‐1, BHVO‐2, SCo‐1, MAG‐1, MRG‐1 and UB‐N) gave results with < 5% relative intermediate precision (1s) for most elements, except Bi. Replicates of NIST SRM 612 glass digested on a hot plate were analysed by the same methods, and the results agree with reference values mostly within 2% relative deviation. Data for the carbonaceous chondrites Allende, Murchison, Orgueil and Ivuna are also reported. Digestion in a HPA‐S was as efficient as in pressure bombs, but some elements displayed higher blank levels following HPA‐S treatment. Pressure bomb digestion yielded precise data for volatile S, Se and Te, but may result in high blanks for W.
Les fractions de masse du S, Cu, Se, Mo, Ag, Cd, In, Te, Ba, Sm, W et Tl ont été déterminées par dilution isotopique couplée à un ICP‐MS à secteur magnétique pour le même aliquot de matériaux de référence en utilisant la méthode de digestion HF‐HNO3 dans des béchers PFA placés dans des bombes de pression et dans des récipients en carbone vitreux dans un minéralisateur de haute pression (HPA‐S) pour comparaison. En outre, le Bi a été déterminé par standardisation interne par rapport à Tl. Parce que les interférences isobariques et d'oxydes posent des problèmes pour beaucoup de ces éléments, des méthodes efficaces de séparation chromatographique en combinaison avec un nébuliseur Aridus ont été utilisées pour minimiser les effets de ces interférences. La digestion et la mesure répétées des matériaux géologiques de référence (BHVO‐1, BHVO‐2, SCO‐1, MAG‐1, MRG‐1 et UB‐N) ont donné des résultats avec une précision intermédiaire (1s) < 5% pour la plupart des éléments, à l'exception du Bi. Des répliquats du verre NIST SRM 612 digérés sur une plaque chauffante ont été analysés par les mêmes méthodes et les résultats sont pour la plupart en accord avec les valeurs de référence avec un coefficient de variation de 2%. Les données pour les chondrites carbonées Allende, Murchison, Orgueil et Ivuna sont également présentées. La technique de digestion dans un HPA‐S est aussi efficace que celle utilisant les bombes de pression, mais certains éléments présentent des niveaux de blancs élevés après le traitement par HPA‐S. La digestion dans les bombes de pression produit des données précises pour les éléments volatils S, Se et Te, mais peut entraîner des blancs élevés pour le W.
Chromium isotopic data of physically separated components (chondrules, CAIs, variably magnetic size fractions) of the carbonaceous chondrites Allende and Murchison and bulk rock data of Allende, ...Ivuna, and Orgueil are reported to evaluate the origin of isotopic heterogeneity in these meteorites. Allende components show ε53Cr and ε54Cr from −0.23 ± 0.07 to 0.37 ± 0.05 and from −0.43 ± 0.08 to 3.7 ± 0.1, respectively. In components of Murchison, ε53Cr and ε54Cr vary from −0.06 ± 0.08 to 0.5 ± 0.1 and from 0.7 ± 0.2 to 1.7 ± 0.1, respectively. The non‐systematic variations of ε53Cr and 55Mn/52Cr in the components of Allende and Murchison were likely caused by small‐scale, alteration‐related redistribution of Mn >20 Ma after formation of the solar system. Chondrule fractions show the lowest 55Mn/52Cr and ε54Cr values of all components, consistent with evaporation of Mn and ε54Cr‐rich carrier phases from chondrule precursors. Components other than the chondrules show higher Mn/Cr and ε54Cr, suggestive of chemical and isotopic complementarity between chondrules and matrix‐rich fractions. Bulk rock compositions calculated based on weighted compositions of components agree with measured Cr isotope data of bulk rocks, in spite of the Cr isotopic heterogeneity reported by the present and previous studies. This indicates that on a sampling scale comprising several hundred milligrams, these meteorites sampled isotopically and chemically homogeneous nebular reservoirs. The linear correlation of 55Mn/52Cr with ε53Cr in bulk rocks likely was caused by variable fractionation of Mn/Cr, subsequent mixing of phases in nebular domains, and radiogenic ingrowth of 53Cr.
The abundances of elements and their isotopes in our Galaxy show wide variations, reflecting different nucleosynthetic processes in stars and the effects of Galactic evolution. These variations ...contrast with the uniformity of stable isotope abundances for many elements in the Solar System, which implies that processes efficiently homogenized dust and gas from different stellar sources within the young solar nebula. However, isotopic heterogeneity has been recognized on the subcentimetre scale in primitive meteorites, indicating that these preserve a compositional memory of their stellar sources. Small differences in the abundance of stable molybdenum isotopes in bulk rocks of some primitive and differentiated meteorites, relative to terrestrial Mo, suggest large-scale Mo isotopic heterogeneity between some inner Solar System bodies, which implies physical conditions that did not permit efficient mixing of gas and dust. Here we report Mo isotopic data for bulk samples of primitive and differentiated meteorites that show no resolvable deviations from terrestrial Mo. This suggests efficient mixing of gas and dust in the solar nebula at least to 3 au from the Sun, possibly induced by magnetohydrodynamic instabilities. These mixing processes must have occurred before isotopic fractionation of gas-phase elements and volatility-controlled chemical fractionations were established.
Mass fractions of the siderophile volatile elements S, Se, and Te were determined together with highly siderophile elements (HSE) and osmium isotope ratios in multiple aliquots of five lunar mafic ...impact melt breccias. The impactites were sampled from presumably Imbrium‐related ejecta deposits at the Apollo 14, 15, and 16 landing sites. As in many mafic impact melt breccias, all studied impactites display fractionated siderophile element patterns characteristic of differentiated metal, interpreted to reflect metal‐rich impactor material from the core of a differentiated planetesimal. The compositional record of Fra Mauro crystalline matrix breccias and recent constraints on the time of their formation suggest that the admixture of this differentiated metal component to the Procellarum KREEP Terrane occurred before the Imbrium basin was formed. The impact melt rock portion of dimict breccia 61015 displays fractionations of HSE like other mafic impact melt breccias, but CI chondrite‐like ratios of S, Se, Te, and Ir. Preservation of these contrasting impactor signatures in a single impactite sample demonstrates mixing of differentiated metal and CI chondrite‐like impactor material and their homogenization in an impact melt sheet. Correlations of highly siderophile element ratios between impactites from different Apollo landing sites suggest that siderophile element inventories of many lunar impactites were affected by similar mixing processes. Mass fractions and ratios of S, Se, and Te in other mafic impact melt breccias closely resemble those of pristine mafic target rocks.
Silicon and iron isotope compositions of different physically separated components of enstatite chondrites (EC) were determined in this study to understand the role of nebular and planetary scale ...events in fractionating Si and Fe isotopes of the terrestrial planet‐forming region. We found that the metal–sulfide nodules of EC are strongly enriched in light Si isotopes (δ30Si ≥ −5.61 ± 0.12‰, 2SD), whereas the δ30Si values of angular metal grains, magnetic, slightly magnetic, and non‐magnetic fractions become progressively heavier, correlating with their Mg# (Mg/(Mg+Fe)). White mineral phases, composed primarily of SiO2 polymorphs, display the heaviest δ30Si of up to +0.23 ± 0.10‰. The data indicate a key role of metal–silicate partitioning on the Si isotope composition of EC. The overall lighter δ30Si of bulk EC compared to other planetary materials can be explained by the enrichment of light Si isotopes in EC metals along with the loss of isotopically heavier forsterite‐rich silicates from the EC‐forming region. In contrast to the large Si isotope heterogeneity, the average Fe isotope composition (δ56Fe) of EC components was found to vary from −0.30 ± 0.08‰ to +0.20 ± 0.04‰. A positive correlation between δ56Fe and Ni/S in the components suggests that the metals are enriched in heavy Fe isotopes whereas sulfides are the principal hosts of light Fe isotopes in the non‐magnetic fractions of EC. Our combined Si and Fe isotope data in different EC components reflect an inverse correlation between δ30Si and δ56Fe, which illustrates that partitioning of Si and Fe among metal, silicate, and sulfidic phases has significantly fractionated Si and Fe isotopes under reduced conditions. Such isotope partitioning must have occurred before the diverse components were mixed to form the EC parent body. Evaluation of diffusion coefficients of Si and Fe in the metal and non‐metallic phases suggests that the Si isotope compositions of the silicate fractions of EC largely preserve information of their nebular processing. On the other hand, the Fe isotopes might have undergone partial or complete re‐equilibration during parent body metamorphism. The relatively uniform δ56Fe among different types of bulk chondrites and the Earth, despite Fe isotope differences among their components, demonstrates that the chondrite parent bodies were not formed by random mixing of chondritic components from different locations in the disk. Instead, the chondrite components mostly originated in the same nebular reservoir and Si and Fe isotopes were fractionated either due to gas–solid interactions and associated changes in physicochemical environment of the nebular reservoir and/or during parent body processing. The heavier Si isotope composition of the bulk silicate Earth may require accretion of chondritic and/or isotopically heavier EC silicates along with cumulation of refractory forsterite‐rich heavier silicates lost from the EC‐forming region to form the silicate reservoir of the Earth.
Reconstructing the building blocks that made Earth and the Moon is critical to constrain their formation and compositional evolution to the present. Neodymium (Nd) isotopes identify these building ...blocks by fingerprinting nucleosynthetic components. In addition, the
Sm-
Nd and
Sm-
Nd decay systems, with half-lives of 103 million years and 108 billion years, respectively, track potential differences in their samarium (Sm)/Nd ratios. The difference in Earth's present-day
Nd/
Nd ratio compared with chondrites
, and in particular enstatite chondrites, is interpreted as nucleosynthetic isotope variation in the protoplanetary disk. This necessitates that chondrite parent bodies have the same Sm/Nd ratio as Earth's precursor materials
. Here we show that Earth and the Moon instead had a Sm/Nd ratio approximately 2.4 ± 0.5 per cent higher than the average for chondrites and that the initial
Nd/
Nd ratio of Earth's precursor materials is more similar to that of enstatite chondrites than previously proposed
. The difference in the Sm/Nd ratio between Earth and chondrites probably reflects the mineralogical distribution owing to mixing processes within the inner protoplanetary disk. This observation simplifies lunar differentiation to a single stage from formation to solidification of a lunar magma ocean
. This also indicates that no Sm/Nd fractionation occurred between the materials that made Earth and the Moon in the Moon-forming giant impact.
Osmium isotopic compositions, abundances of highly siderophile elements (HSE: platinum group elements, Re and Au), the chalcogen elements S, Se and Te and major and minor elements were analysed in ...physically separated size fractions and components of the ordinary chondrites WSG 95300 (H3.3, meteorite find) and Parnallee (LL3.6, meteorite fall). Fine grained magnetic fractions are 268-65 times enriched in HSE compared to the non-magnetic fractions. A significant deviation of some fractions of WSG 95300 from the 4.568 Ga 187Re-187Os isochron was caused by redistribution of Re due to weathering of metal. HSE abundance patterns show that at least four different types of HSE carriers are present in WSG 95300 and Parnallee. The HSE carriers display (i) CI chondritic HSE ratios, (ii) variable Re/Os ratios, (iii) lower than CI chondritic Pd/Ir and Au/Ir and (iv) higher Pt/Ir and Pt/Ru than in CI chondrites. These differences between components clearly indicate the loss of refractory HSE carrier phases before accretion of the components. Tellurium abundances correlate with Pd and are decoupled from S, suggesting that most Te partitioned into metal during the last high-temperature event. Tellurium is depleted in all fractions compared to CI chondrite normalized Se abundances. The depletion of Te is likely associated with the high temperature history of the metal precursors of H and LL chondrites and occurred independent of the metal loss event that depleted LL chondrites in siderophile elements. Most non-magnetic and slightly magnetic fractions have S/Se close to CI chondrites. In contrast, the decoupling of Te and Se from S in magnetic fractions suggests the influence of volatility and metal-silicate partitioning on the abundances of the chalcogen elements. The influence of terrestrial weathering on chalcogen element systematics of these meteorites appears to be negligible.
Ejecta at North Ray crater (Apollo 16) sampled a unique section of the lunar highlands not accessible at most other landing sites and provide important constraints on the composition of late accreted ...materials. New data on multiple aliquots of four fragmental matrix breccias and a fragment‐laden melt breccia from this site display a variety of highly siderophile element patterns which may represent the signatures of volatile element‐depleted carbonaceous chondrite‐like material, primitive achondrite, differentiated metal, and an impactor component that cannot be related to known meteoritic material. The latter component is prevalent in these rocks besides characterized by depletions in Re and Os compared to Ir, Ru and Pt, chondritic Re/Os, and a gradual depletion of Pd and Au. The observed characteristics are more consistent with fractionations by nebular processes, like incomplete condensation or evaporation, than with lunar crustal processes, like partial melting or volatilization. The impactor signature preserved in these breccias may stem from primitive meteorites with a refractory element composition moderately different from known chondrites. The presence of distinct impactor components within the North Ray crater breccias together with observed correlations of characteristic element ratios (e.g., Re/Os, Ru/Pt, Pd/Ir) in different impact lithologies of four Apollo landing sites constrains physical mixing processes ranging from the scale of gram‐sized samples to the area covered by the Apollo missions.
Different solar system objects display variable abundances of neutron‐rich isotopes such as 54Cr, 50Ti, and 48Ca, which are commonly attributed to a heterogeneous distribution of presolar grains in ...different domains of the solar system. Here, we show that the heterogeneity of 54Cr/52Cr and the correlation of 54Cr/52Cr with Fe/Cr in metal fractions of EH3 chondrites and in inner solar system bodies can be attributed to variable irradiation of dust grains by solar energetic particles and variable mixing of irradiated material in the different domains of the inner solar nebula. The isotope variations in inner solar system objects can be generated by ~300 y long local irradiation of mm‐ to cm‐sized solids with average solar energetic particle fluxes of ~105 times the modern value. The relative homogeneity of 53Cr/52Cr in inner solar system objects can be a consequence of the production of 53Mn by the early irradiation of dust, evaporation, and nebula‐wide homogenization of Mn due to high temperatures, followed by Mn/Cr fractionation within the first few million years of the solar system. The 54Cr/52Cr of the Earth can be produced by irradiated pebbles and <15 wt% of CI chondrite like material. Alternatively, Earth may contain only a few % of CI chondrite like material but then must have an Fe/Cr ratio 10–15% higher than CI chondrites.
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