Bulk Chondrites Research Articles

Identification of a primordial high D/H component in the matrix of unequilibrated ordinary chondrites

Deuterium to hydrogen isotope ratios in unequilibrated ordinary chondrites (UOCs) which have undergone little-to-no thermal metamorphism pose an interesting problem when looking at water in the early Solar System. Bulk chondrite studies have shown that UOCs of the lowest subtypes have D/H ratios as high as comets from the outer Solar System, which, along with bulk UOC water abundances, decrease with thermal metamorphism. Since bulk UOC analyses represent a complex mixture of organic and hydrated phases, it is not clear what phase(s) is responsible for the high bulk D/H values. In this study, we report in situ secondary ion mass spectrometry (SIMS) measurements of the H isotope composition of the fine-grained matrix of UOCs with petrological subtypes ranging from 3.00 to 3.9. We find that for matrix areas in UOCs of petrologic subtype ≥3.2, correlations between D-rich organic material and D-poor phyllosilicates give relatively D-poor intrinsic water isotopic compositions, with δD values between −320 ± 91 ‰ and −71 ± 71 ‰, which are inherited from parent body accretion. Therefore, we conclude that OC parent bodies accreted D-poor water ice that had an H isotopic composition similar to that of CM and CV chondrite parent bodies. We find that matrix in UOCs of the lowest subtypes (Semarkona, Bishunpur, and Ngawi) show similar water and organic H isotope compositions to higher type UOCs. Our in situ analyses also show that matrix areas in these pristine UOCs contain a third, thus far unidentified, component that carries the high D/H signature, with δD values up to ∼6000 ‰. We propose that this component is pristine amorphous silicates preserved from the molecular cloud or early protoplanetary disc that is extremely sensitive to thermal and aqueous alteration on asteroidal parent bodies.

Insights on the origin of oldhamite in enstatite meteorites from Ca stable isotopes

In order to understand the origin of oldhamite (CaS) in enstatite meteorites, we report Ca isotopic compositions (δ44/40Ca) of oldhamite (obtained from water leachate of bulk chondrites and aubrites and mineral separates from the Norton County aubrite) and silicate minerals from different types of enstatite chondrites and aubrite. The δ44/40Ca of the bulk enstatite chondrites range from 1.05 ‰ to 1.24 ‰, with an average of 1.13 ± 0.12 ‰, higher than that of the estimate of the bulk silicate earth (∼0.94 ‰). Major and trace element analyses show that the water leachates of enstatite chondrites are mainly composed of oldhamite, and they take over 20.6–68.5 % Ca of the bulk meteorite Ca budget. The Ca isotope fractionation between oldhamite and residual silicate (Δ44/40Caoldhamite-silicate) for the studied enstatite chondrites is minimum (−0.44 ‰) for Abee (impact-melt breccia) and maximum (+0.16) for St.Marks (EH5). The Ca isotope fractionation between oldhamite (individual mineral grains and leachate) and silicates in Norton County varies from −0.47 ‰ to −0.31 ‰ with an average of −0.41 ‰. These Δ44/40Caoldhamite-silicate correlate well with previous theoretical calculation and suggests that the oldhamites in Norton County are in isotopic equilibrium with co-existing silicates, and therefore were formed during magmatic processes. However, in enstatite chondrites, the large variation on Δ44/40Caoldhamite-silicate and its negative correlation with metamorphic temperature reflects the redistribution and equilibration of Ca isotopes during metamorphism. The variable Δ44/40Caoldhamite-silicate found in unequilibrated chondrites reflect kinetic Ca isotope fractionation between oldhamite and nebular gas and therefore is evidence for the formation of oldhamite by condensation in the solar nebula.

Silicon and iron isotopes in components of enstatite chondrites: Implications for metal–silicate–sulfide fractionation in the solar nebula

AbstractSilicon 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.

High precision nickel isotope measurements of early Solar System materials and the origin of nucleosynthetic disk variability

Various chemical elements including nickel (Ni) exhibit mass-independent isotope heterogeneity on a bulk meteorite level, which is generally accepted to reflect the heterogeneous distribution of presolar carrier(s) from different nucleosynthetic sources. Thus, understanding the nature of the carriers can help decipher the origin of the observed nucleosynthetic variability, which remains elusive. In this study, we present the first high precision measurements of mass-independent and mass-dependent Ni isotope compositions for step-leaches of the CI chondrite Ivuna and Efremovka CAIs supplemented by bulk chondrite measurements. Step-leaches record highly anomalous Ni isotope signatures that can be attributed to at least four diverse nucleosynthetic sources. The most anomalous leachates show either large deficits (up to 0.1 %) in the neutron-poor 58Ni and 60Ni nuclides (L11, thought to contain mainly s-process derived Ni) or minor enrichments and deficits (∼100 ppm) in 60Ni or 64Ni (L6, L8, L9 and L10, all thought to derive mainly from supernovae). Pristine CAIs record Ni isotope compositions typified by enrichments in 58Ni of up to 400 ppm. Our new data for bulk chondrites agree with earlier work and emphasize the appropriateness of using the 62Ni/61Ni ratio for internal normalization. Based on the compositional relations between the step-leaches data, CAIs, and bulk meteorites, we show that 60Ni variability is consistent with being of nucleosynthetic origin as opposed to reflecting variable Fe/Ni ratios in the presence of live 60Fe. Finally, we infer that the observed Ni nucleosynthetic disk variability is predominantly driven by a combination of processes separating different nucleosynthetic carriers in the disk from each other, including thermal processing and size-based sorting.

Lifetime of the Outer Solar System Nebula From Carbonaceous Chondrites

AbstractThe evolution and lifetime of protoplanetary disks (PPDs) play a central role in the formation and architecture of planetary systems. Astronomical observations suggest that PPDs evolve in two timescales, accreting onto the star for up to several million years (Myr) followed by gas dissipation within ≲1 Myr. Because solar nebula magnetic fields are sustained by the gas of the protoplanetary disk, we can use paleomagnetic measurements to infer the lifetime of the solar nebula. Here, we use paleomagnetic measurements of meteorites to constrain this lifetime and investigate whether the solar nebula had a two‐timescale evolution. We report on paleomagnetic measurements of bulk subsamples of two CO carbonaceous chondrites: Allan Hills A77307 and Dominion Range 08006. If magnetite in these meteorites can acquire a crystallization remanent magnetization that recorded the ambient field during aqueous alteration, our measurements suggest that the local magnetic field strength at the CO parent body location was <0.9 μT at some time between 2.7 and 5.1 Myr after the formation of calcium‐aluminum‐rich inclusions. Coupled with previous paleomagnetic studies, we conclude that the dissipation of the solar nebula in the 3–7 AU region occurred <1.5 Myr after the dissipation of the nebula in the 1–3 AU region, suggesting that protoplanetary disks go through a two‐timescale evolution in their lifetime, consistent with dissipation by photoevaporation and/or magnetohydrodynamic winds. We also discuss future directions necessary to obtain robust records of solar nebula fields using bulk chondrites, including obtaining ages from meteorites and experimental work to determine how magnetite acquires magnetization during chondrite parent body alteration.

The effects of bulk composition on planetesimal core sulfur content and size

This study explores the compositions and sizes of metallic cores that result from planetesimals forming from a range of chondritic bulk compositions. Our models examine the influence of starting bulk composition on core size and composition, how oxygen fugacity (fO2), temperature, pressure, and bulk composition affect sulfur partitioning between the core and silicate mantle of planetesimals, and the formation and fate of immiscible sulfur-rich liquid during core solidification. We apply experimentally-derived equations for the sulfur distribution coefficient to the bulk compositions of ordinary chondrites (H,L,LL) and carbonaceous chondrites (CM, CI, CO, CK, CV) under conditions appropriate for melting planetesimals.The sulfur content of all modeled cores is above 6 wt% S, which is greater than the amount of sulfur needed to form an immiscible sulfide liquid in the presence of other light elements (e.g., C, Si, and/or P). We concluded that early planetesimal cores likely formed either an immiscible sulfide liquid, a eutectic sulfide liquid, or most surprisingly, were composed of mostly monosulfide solid solution, [(Fe, Ni)1-xS].

An exploration of whether Earth can be built from chondritic components, not bulk chondrites

Here, two of a range of possible models are explored that assume that: (i) two of the main chondritic components (chondrules and refractory inclusions) dominated the Earth’s building blocks, (ii) that their relative abundances differed from those of known chondrites, and (iii) that the elemental compositions of all components, as well as the isotopic compositions of refractory inclusions, resembled those of the components in carbonaceous chondrites.In terms of the elemental abundances, the chondrules can explain the moderately volatile element fractionations in the Bulk Silicate Earth (BSE), except for a few elements like F and In, while the refractory inclusions explain the BSE’s refractory lithophile element enrichment. Accretion of a CM- or EL-like late veneer reproduces the S, Se, Te and highly siderophile element abundances in the BSE. The accretion of CI- or CM-like material prior to the late veneer, along with small amounts of cometary and implanted solar wind material, can explain the BSE elemental and isotopic abundances of the noble gases as well as the elemental abundances of most other highly volatile elements (e.g., H, C and N) provided that variable fractions of them can be sequestered into the core or into hidden mantle reservoirs. This CI- or CM-like material provides an upper limit for the contribution to the BSE from matrix that is much less than in any chondrites. In the models, Si, O and S are the dominant light elements in the core, in that order, and their abundances are constrained to be consistent with the first principles calculations of Umemoto and Hirose (2020). The core compositions of the models are also consistent with most geochemical constraints.Satisfying all isotopic constraints is a challenge. The BSE Os isotopes are consistent with an EL dominated late veneer, but Ru isotopic evidence is best explained by the addition of CM-like material in the late veneer. Either CI- or CM-like material, in combination with small amounts of cometary and implanted solar wind material, can reproduce the BSE Ne, Ar and Kr isotopic compositions. CM-like, but not CI-like, material can roughly reproduce the BSE’s H and C isotopic compositions, but neither material can explain the BSE N isotopic composition. The BSE composition requires that the O isotopic compositions of the refractory inclusions (initially Δ17O ≤ −20‰) in Earth’s building blocks were reset in the nebula by interaction with high Δ17O H2O, perhaps during chondrule formation. To plot on the inner Solar System ε54Cr vs. ε50Ti (or ε48Ca) trend, either the average Cr content of the chondrules was roughly half of that assumed here or most of the CI/CM-like and refractory-inclusion-rich materials were accreted late.

Chromium Stable Isotope Panorama of Chondrites and Implications for Earth Early Accretion

Abstract We investigated the stable isotope fractionation of chromium (Cr) for a panorama of chondrites, including EH and EL enstatite chondrites and their chondrules and different phases (by acid leaching). We observed that chondrites have heterogeneous δ 53Cr values (per mil deviation of the 53Cr/52Cr from the NIST SRM 979 standard), which we suggest reflect different physical conditions in the different chondrite accretion regions. Chondrules from a primitive EH3 chondrite (SAH 97096) possess isotopically heavier Cr relative to their host bulk chondrite, which may be caused by Cr evaporation in a reduced chondrule-forming region of the protoplanetary disk. Enstatite chondrites show a range of bulk δ 53Cr values that likely result from variable mixing of isotopically different sulfide-silicate-metal phases. The bulk silicate Earth (δ 53Cr = –0.12 ± 0.02‰, 2SE) has a lighter Cr stable isotope composition compared to the average δ 53Cr value of enstatite chondrites (–0.05 ± 0.02‰, 2SE, when two samples out of 19 are excluded). If the bulk Earth originally had a Cr isotopic composition that was similar to the average enstatite chondrites, this Cr isotope difference may be caused by evaporation under equilibrium conditions from magma oceans on Earth or its planetesimal building blocks, as previously suggested to explain the magnesium and silicon isotope differences between Earth and enstatite chondrites. Alternatively, chemical differences between Earth and enstatite chondrite can result from thermal processes in the solar nebula and the enstatite chondrite-Earth, which would also have changed the Cr isotopic composition of Earth and enstatite chondrite parent body precursors.

Tellurium isotope cosmochemistry: Implications for volatile fractionation in chondrite parent bodies and origin of the late veneer

Tellurium stable isotope compositions and abundances (δ128/126Te relative to SRM 3156) are reported for 43 ordinary, enstatite, and Rumuruti chondrites, which together with results from a companion study on carbonaceous chondrites are used to assess the origin of volatile element fractionations in chondrites. Whereas Te isotope variations among carbonaceous chondrites predominantly reflect mixing between isotopically light chondrules/chondrule precursors and CI-like matrix, Te isotope variations among non-carbonaceous chondrites mainly result from Te redistribution during parent body thermal metamorphism. The enstatite chondrites in particular display increasingly heavy Te isotopic compositions and decreasing Te concentrations with increasing degree of metamorphism, indicating migration of isotopically light Te from the strongly metamorphosed inner parts towards the cooler outer regions of the parent bodies. By contrast, ordinary and Rumuruti chondrites display less systematic Te isotope variations, implying more localized redistribution of Te during parent body thermal metamorphism.We also report Te stable isotope data for 19 terrestrial mantle-derived rocks. Peridotites with Al2O3 contents close to those inferred for the bulk silicate Earth (BSE) exhibit uniform δ128/126Te values, which we interpret to represent the Te isotopic composition of the BSE. This composition overlaps with the Te isotope composition of some volatile-rich carbonaceous chondrites (most notably CM chondrites), but also with that of enstatite chondrites. Comparison of the Te results to Se isotopes and Se/Te ratios shows that due to uncertainties in the composition of the BSE and the isotopic composition of bulk chondrite parent bodies, neither Te isotopes alone nor the combined Se-Te elemental and isotopic systematics can distinguish between a carbonaceous and enstatite chondrite-like late veneer, which is the presumed source of Se and Te in the BSE. Together, the results of this study illustrate that the relative abundances and mass-dependent isotope compositions of volatile elements like Se and Te are modified by physical and chemical processes occurring after planetary accretion, which severely complicates their use as genetic tracers. A corollary of this is that contrary to prior proposals the Se-Te systematics are not contradicting an inner solar system origin of the late veneer, as it has been inferred using nucleosynthetic isotope anomalies of other elements.

Origin of hydrogen isotopic variations in chondritic water and organics

Chondrites are rocky fragments of asteroids that formed at different times and heliocentric distances in the early solar system. Most chondrite groups contain water-bearing minerals, attesting that both water-ice and dust were accreted on their parent asteroids. Nonetheless, the hydrogen isotopic composition (D/H) of water in the different chondrite groups remains poorly constrained, due to the intimate mixture of hydrated minerals and organic compounds, the other main H-bearing phase in chondrites. Building on our recent works using in situ secondary ion mass spectrometry analyses, we determined the H isotopic composition of water in a large set of chondritic samples (CI, CM, CO, CR, and C-ungrouped carbonaceous chondrites) and report that water in each group shows a distinct and unique D/H signature. Based on a comparison with literature data on bulk chondrites and their water and organics, our data do not support a preponderant role of parent-body processes in controlling the D/H variations among chondrites. Instead, we propose that the water and organic D/H signatures were mostly shaped by interactions between the protoplanetary disk and the molecular cloud that episodically fed the disk over several million years. Because the preservation of D-rich interstellar water and/or organics in chondritic materials is only possible below their respective sublimation temperatures (160 and 350–450 K), the H isotopic signatures of chondritic materials depend on both the timing and location at which their parent body formed.

The effects of Antarctic alteration and sample heterogeneity on Sm-Nd and Lu-Hf systematics in H chondrites

Long-lived radioactive isotope systematics, such as Sm-Nd and Lu-Hf, are useful tools as important chronometers and tracers for chemical differentiation processes. Even though Antarctic meteorites include rare meteorites such as ungrouped meteorites, the effects of Antarctic alteration on the Sm-Nd and Lu-Hf systems in chondrites have not yet been evaluated in detail. Moreover, the heterogeneity of Sm-Nd and Lu-Hf data in bulk chondrites prevents the determination of precise average Sm-Nd and Lu-Hf values (e.g., for individual chondrite groups). To examine the effects of Antarctic alteration and sample heterogeneity on the Sm-Nd and Lu-Hf isotope systematics, ten Antarctic H chondrites (HCs) and three HCs from hot deserts were characterized for their modal abundances, elemental abundances, and Sm-Nd and Lu-Hf isotopic compositions. Regardless of the classical weathering index for Antarctic meteorites and the normalized Rb abundance used as a chemical alteration indicator in this study, the modal and elemental abundances in Antarctic HCs appear to be in good agreement with those in non-Antarctic HCs. The Sm-Nd and Lu-Hf isotopic compositions of the characterized H chondrites fall within the range measured for both HC falls and for falls of other chondrite groups, except in the case of the most heavily altered sample. Consequently, the effects of Antarctic alteration processes on the Sm-Nd and Lu-Hf systematics in HCs appear to be limited, except in the case of Asuka 09516. The latter meteorite exhibits severe mineralogical and chemical alteration, with considerable losses of even the rare earth elements (REEs), which are considered relatively immobile. The 147Sm/144Nd, 143Nd/144Nd, 176Lu/177Hf, and 176Hf/177Hf of bulk HCs correlate with their P/Mg and Y/Mg. Furthermore, the Lu-Hf ratios correlate strongly with their P/Ca and Y/Ca as well as their P/Mg and Y/Mg. Thus, the distribution of the elements between constituent minerals in ordinary chondrites (OCs) may control the heterogeneity observed for the bulk Sm-Nd and Lu-Hf data. In this context, the weight ratio of Ca-phosphates to Ca-pyroxene, or at least that of Ca-phosphates to silicates, may be a key factor leading to the observed elemental and isotopic variations. This observation indicates that the nugget effect of Ca-phosphates in OCs as the result of insufficient homogenization or terrestrial alteration leads to the heterogeneities displayed by the Sm-Nd and Lu-Hf data. Moreover, it also indicates that the use of equilibrated OCs for the determination of Sm-Nd and Lu-Hf data is affected more by sample heterogeneity, especially with respect to Ca-phosphates, than is the case for unequilibrated OCs, based on the re-distribution of REEs during thermal metamorphism on their parent bodies. This study demonstrates that Antarctic meteorites commonly preserve their original Sm-Nd and Lu-Hf isotopic compositions as much as chondrite falls, although exceptions are possible in the case of severe alteration. Similar to previous studies, we recommend the use of unequilibrated chondrites, for which the re-distribution of REEs is less extensive, for the determination of well-constrained average Sm-Nd and Lu-Hf isotopic compositions for individual chondrite groups as well as their robust Chondritic Uniform Reservoir values.

Bubbles to Chondrites-II. Chemical fractionations in chondrites

We attempt to develop a possible theory of chemical fractionations in chondrites, that is consistent with various features of chondritic components and current observation of protoplanetary disks (PPD). Combining the 3+2 component fitting calculation that simulates chondrule formation process proposed in paper (I) with additional mixing procedures, we investigate essential causes that made various types of chondrites evolve from the uniform solar system composition, the CI-chondritic composition. Seven chemical types of chondrites (CM, CV, CO, E, LL, L and H) are examined, for which reliable chemical compositions for both bulk chondrites and chondrules therein are known. High vaporization degree of the primordial dust aggregates (dustons) required by the calculation vindicates that the chondrule formation was the driving force for the chemical fractionations in all chondrites examined. Various initial redox states in dustons and different timings of CAIs’ invasion to the chondrule formation zone are identified for different chondrite types. These results, together with a good correlation with the D/H ratios of chondrites measured previously, lead us to the notion that PPD evolved from reducing to oxidizing. We explore the heating mechanism for the chondrule formation and the place it occurred. Only heat source being consistent with our chondrule formation model is lightning discharge. We postulate that large vortices encompassing the snow-line are ideal places for large charge separation to occur between dustons and small ice particles, and that direct strikes on dustons should make them boil for ten seconds and longer and allow a swarm of chondrules released from their surfaces. Chemical fractionations are completed by an aerodynamic separation of dustons from chondrules inside the vortex, in such a way that the dustons fall fast into the vortex center and form a planetesimal immediately, while chondrules with dust mantles fall slow and form a thin veneer on the planetesimal surface. During collisional episodes, the veneers are preferentially fragmented and reassemble themselves by a weak self-gravity to form a rubble-piled chondritic asteroid, i.e. chondrite.

Correlated isotopic and chemical evidence for condensation origins of olivine in comet 81P/Wild 2 and in AOAs from CV and CO chondrites

Magnesium stable isotope ratios and minor element abundances of five olivine particles from comet 81P/Wild 2 were examined by secondary ion mass spectrometry (SIMS). Wild 2 olivine particles exhibit only small variations in δ25Mg values from –1.0 +0.4/–0.5‰ to 0.6 +0.5/–0.6‰ (2σ). This variation can be simply explained by mass-dependent fractionation from Mg isotopic compositions of the Earth and bulk meteorites, suggesting that Wild 2 olivine particles formed in the chondritic reservoir with respect to Mg isotope compositions. We also determined minor element abundances, and O and Mg isotope ratios of olivine grains in amoeboid olivine aggregates (AOAs) from Kaba (CV3.1) and DOM 08006 (CO3.01) carbonaceous chondrites. Our new SIMS minor element data reveal uniform, low FeO contents of ∼0.05 wt% among AOA olivines from DOM 08006, suggesting that AOAs formed at more reducing environments in the solar nebula than previously thought. Furthermore, the SIMS-derived FeO contents of the AOA olivines are consistently lower than those obtained by electron microprobe analyses (∼1 wt% FeO), indicating possible fluorescence from surrounding matrix materials and/or Fe,Ni-metals in AOAs during electron microprobe analyses. For Mg isotopes, AOA olivines show more negative mass-dependent fractionation (–3.8 ± 0.5‰ ≤ δ25Mg ≤ –0.2 ± 0.3‰; 2σ) relative to Wild 2 olivines. Further, these Mg isotope variations are correlated with their host AOA textures. Large negative Mg isotope fractionations in olivine are often observed in pore-rich AOAs, while those in compact AOAs tend to have near-chondritic Mg isotopic compositions. These observations indicate that pore-rich AOAs preserved their gas–solid condensation histories, while compact AOAs experienced thermal processing in the solar nebula after their condensation and aggregation. Importantly, one 16O-rich Wild 2 LIME olivine particle (T77/F50) shows negative Mg isotope fractionation (δ25Mg = –0.8 ± 0.4‰, δ26Mg = –1.4 ± 0.9‰; 2σ) relative to bulk chondrites. Minor element abundances of T77/F50 are in excellent agreement with those of olivines from pore-rich AOAs in DOM 08006. The observed similarity in O and Mg isotopes, and minor element abundances suggest that T77/F50 formed in an environment similar to AOAs, probably near the proto-Sun, and then was transported to the Kuiper belt, where comet 81P/Wild 2 likely accreted.

Solar system Nd isotope heterogeneity: Insights into nucleosynthetic components and protoplanetary disk evolution

High-precision Nd isotope measurements of a diverse set of solar system materials including bulk chondrites and achondrites reveal that their Nd isotope composition is governed by several distinct nucleosynthetic components. The full spectrum of non-radiogenic, mass-independent Nd isotope compositions of solar system materials is best explained by heterogeneous distribution of at least three nucleosynthetic components - the classical s-process component, pure p-process component and an anomalous, previously unidentified s-/r-process component. The 142Nd/144Nd variations in solar system reservoirs specifically fall into three distinct trends - those that result from variations in the s-process component, those resulting from variations in the pure p-process component, and those resulting from coupled s-process and p-process variations. The μ148Nd value, a proxy for s-process variations, as well as μ142Nd that has been corrected for s-process heterogeneity to reflect p-process variations, broadly show an inverse correlation with ε54Cr. The linearity in μ148Nd - ε54Cr space for inner solar system bodies, CI chondrite and Allende-type CAIs possibly suggests the thermally labile nature of some s-process carrier grains unlike the mainstream refractory s-process SiC grains. The p-process carrier for Nd is inferred to be a refractory phase enriched in inner solar system materials through thermal processing. The bulk meteorite regression lines that specifically correspond to s- and p-process heterogeneity, largely define μ142Nd intercepts indistinguishable from terrestrial composition within analytical uncertainty, ruling out resolvable radiogenic μ142Nd excess on Earth that cannot otherwise be accounted for by nucleosynthetic heterogeneity.

Cadmium isotopes in chondrites and acid leachates: Nucleosynthetic homogeneity and a monitor for thermal neutron capture effects

Nucleosynthetic isotope variations are well documented for refractory elements in meteorites and the Earth, while moderately volatile elements generally display homogeneous compositions. Cadmium is a moderately volatile element with eight stable isotopes generated by a variety of nucleosynthetic processes. To address the extent of the nucleosynthetic variability in moderately volatile elements, new high precision Cd isotope data are presented for bulk samples of six carbonaceous and one enstatite chondrite. In addition, we report the first Cd isotope results of sequential acid leachates for the CM2 chondrite Jbilet Winselwan. Our new Cd data displays nucleosynthetic homogeneity for bulk chondrites and acid leachates within analytical uncertainties, in agreement with results for other moderately volatile elements. This implies that Cd isotopes were efficiently homogenised prior to incorporation into planetary bodies. We propose that Cd never significantly condensed into dust in stellar environments, or alternatively that such Cd-bearing dust was efficiently destroyed and recycled in the interstellar medium. Our leachate data provides evidence for further homogenisation during thermal processing in the protoplanetary disk including parent body processing. The data shows that Cd in carbonaceous chondrites mainly resides in the more easily dissolved phases, most likely sulphides that were affected by aqueous alteration. Less than 1% of the total Cd was recovered in the final leach fractions that employed HF and mainly dissolve silicates and refractory oxides.Cadmium is susceptible to thermal neutron-capture effects due to the large neutron capture cross-section of 113Cd (∼20,000 barns). We report variations of up to −0.6 ± 0.3 for ε113Cd (internally normalised to 116Cd/111Cd) in bulk chondrites, which renders Cd a potential thermal neutron-capture monitor. Most neutron dosimeters, such as Pt, Os and Hf, are sensitive to neutron capture in the epithermal energy range and have applications mainly limited to lunar samples or iron and stony-iron meteorites. The additional use of Cd, susceptible to neutron capture in the thermal energy range, therefore provides a new tool to determine the exposure histories of stony meteorites in more detail. Our study demonstrates that thermal neutron-capture effects in carbonaceous and enstatite chondrites can produce resolvable effects and require attention when assessing nucleosynthetic isotope variations.

A carbonaceous chondrite and cometary origin for icy moons of Jupiter and Saturn

The inner structure of icy moons comprises ices, liquid water, a silicate rocky core and sometimes an inner metallic core depending on thermal evolution and differentiation. Mineralogy and density models for the silicate part of the icy satellites cores were assessed assuming a carbonaceous chondritic (CI) bulk composition and using a free-energy minimization code and experiments. Densities of other components, solid and liquid sulfides, carbonaceous matter, were evaluated from available equations of state. Model densities for silicates are larger than assessed from magnesian terrestrial minerals, by 200 to 600 kg.m−3 for the hydrated silicates, and 300 to 500 kg.m−3 for the dry silicates, due to the high iron bulk concentration in CI. The stability of Na-phlogopite in the silicate fraction up to 1300 K favors the trapping of most 40K in the rocky/carbonaceous cores with important consequences for modeling of the thermal evolution of icy satellites. We find that CI density models of icy satellite cores taking into account only the silicate and metal/sulfide fraction cannot account for the observed densities and reduced moment of inertia of Titan and Ganymede without adding a lower density component. We propose that this low-density component is carbonaceous matter derived from insoluble organic matter, in proportion of ∼30-40% in volume and 15-20% in mass. This proportion is compatible with contributions from CI and comets, making these primitive bodies including their carbonaceous matter component likely precursors of icy moons, and potentially of most of the objects formed behind the snow line of the solar system.

An experimental assessment of the potential of sulfide saturation of the source regions of eucrites and angrites: Implications for asteroidal models of core formation, late accretion and volatile element depletions

The geochemistry of asteroidal magmas provides fundamental clues to the processes involved in the origin and early evolution of planetary bodies. Although sulfides are important reservoirs for a diverse suite of major and trace elements, it is currently unclear whether the interiors of asteroid Vesta and the Angrite Parent Body were sulfide liquid saturated during petrogenesis of non-cumulate eucrites and volcanic angrites. To assess the potential of sulfide liquid saturation in the interiors of these bodies, high pressure (P) – temperature (T) experiments were used to quantify the sulfur concentrations at sulfide saturation (SCSS) for volcanic angrites and non-cumulate eucrites. The sulfide-silicate partitioning behavior of various trace elements was simultaneously quantified to study their geochemical behavior at sulfide liquid saturation.It was found that the measured SCSS values agree well with the SCSS values predicted from a previous thermodynamic model for high-FeO* melts. To assess the possibility of sulfide liquid saturation of the source regions of non-cumulate eucrites and angrites, their S abundances were compared with the calculated SCSS values for their source regions. Results show that if eucritic and angritic source regions were saturated with FeS liquid, significant degassing (>50–80%) of S must have occurred during or following their magmatic emplacement. Such loss is inconsistent with the S, Cl, Zn and Rb isotopic compositions of non-cumulate eucrites. Sulfide liquid saturation of eucrite and angrite source regions is also excluded from the strongly incompatible behavior of Cu and HSE in non-cumulate eucrites and angrites (Riches et al., 2012).Additional calculations were performed to further explore the timing and extent of S loss during crystallization of the Vestan magma ocean. The assumption of chondritic bulk S abundances of bulk Vesta would correspond with extremely high S contents of the eucrite source region(s), even after consideration of depletion of S due to core formation. In light of the S, Cl, Zn and Rb stable isotopic compositions of eucrites, the S abundances in eucrites are most consistent with the hypothesis that the Vestan mantle was already strongly depleted in S (>70–80%) by the time of Vestan magma ocean crystallization, resulting in more realistic S contents of the eucrite source region(s). The depletion of S could have been established during initial accretion of Vesta or it could simply reflect accretion of volatile depleted components that experienced incomplete condensation (Wu et al., 2018). Modeling of the new experimentally determined sulfide-silicate partition coefficients and previously reported Vestan mantle depletions of the various chalcophile and siderophile elements suggests that sulfide liquid segregation during early Vestan magma ocean crystallization is also unlikely. The lack of sulfide liquid saturation in the source regions of non-cumulate eucrites and angrites, as well as during early Vestan magma ocean solidification, shows that current geochemical models of core formation and late accretion remain valid for these bodies.

Combined mass-dependent and nucleosynthetic isotope variations in refractory inclusions and their mineral separates to determine their original Fe isotope compositions.

Calcium-aluminum-rich inclusions (CAIs) are the oldest dated materials that provide crucial information about the isotopic reservoirs present in the early Solar System. For a variety of elements, CAIs have isotope compositions that are uniform yet distinct from later formed solid material. However, despite being the most abundant metal in the Solar System, the isotopic composition of Fe in CAIs is not well constrained. In an attempt to determine the Fe isotopic compositions of CAIs, we combine extensive work from a previously studied CAI sample set with new isotopic work characterizing mass-dependent and mass-independent (nucleosynthetic) signatures in Mg, Ca, and Fe. This investigation includes work on three mineral separates of the Allende CAI Egg 2. For all isotope systems investigated, we find that in general, fine-grained CAIs exhibit light mass-dependent isotopic signatures relative to terrestrial standards, whereas igneous CAIs have heavier isotopic compositions relative to the fine-grained CAIs. Importantly, the mass-dependent Fe isotope signatures of bulk CAIs show a range of both light (fine-grained CAIs) and heavy (igneous CAIs) isotopic signatures relative to bulk chondrites, suggesting that Fe isotope signatures in CAIs largely derive from mass fractionation events such as condensation and evaporation occurring in the nebula. Such signatures show that a significant portion of the secondary alteration experienced by CAIs, particularly prevalent in fine-grained inclusions, occurred in the nebula prior to accretion into their respective parent bodies. Regarding nucleosynthetic Fe isotope signatures, we do not observe any variation outside of analytical uncertainty in bulk CAIs compared to terrestrial standards. In contrast, all three Egg 2 mineral separates display resolved mass-independent excesses in 56Fe compared to terrestrial standards. Furthermore, we find that the combined mass-dependent and nucleosynthetic Fe isotopic compositions of the Egg 2 mineral separates are well correlated, likely indicating that Fe indigenous to the CAI is mixed with less anomalous Fe, presumably from the solar nebula. Thus, these reported nucleosynthetic anomalies may point in the direction of the original Fe isotope composition of the CAI-forming region, but they likely only provide a minimum isotopic difference between the original mass-independent Fe isotopic composition of CAIs and that of later formed solids.

Bulk chondrite variability in mass independent magnesium isotope compositions – Implications for initial solar system 26Al/27Al and the timing of terrestrial accretion

We have determined Δ′26MgDSM-3, the mass-independent variations in 26Mg/24Mg, of primitive, bulk meteorites to precisions better than ±3 ppm (2se). Our measurements of samples from 10 different chondrite groups show Δ′26MgDSM-3 that vary from −5 to 22 ppm. Our data define an array with a positive slope in a plot of Δ′26MgDSM-3 against 27Al/24Mg, which can be used to determine (26Al/27Al)0, i.e. initial 26Al/27Al, and (Δ′26MgDSM-3)0, i.e. initial Δ′26MgDSM-3. On such an isochron plot, the best fit of our new measurements combined with literature data implies (26Al/27Al)0 of (4.67±0.78)×10−5 and (Δ′26MgDSM-3)0 of −31.6 ± 5.7 ppm (2se) for ordinary and carbonaceous chondrites, other than CR chondrites, which have anomalously low Δ′26MgDSM-3. These parameters are within uncertainty of those defined by previous measurements of bulk calcium-, aluminium-rich inclusions (CAIs) that set canonical (26Al/27Al)∼05×10−5. The most straightforward interpretation of all these observations is that differences in the Al/Mg of bulk ordinary and carbonaceous chondrites are dominantly controlled by variable contributions of early-formed refractory and major silicate components derived from a common, canonical reservoir. The Δ′26MgDSM-3 of enstatite chondrites are slightly more radiogenic (∼3 ppm) at similar Al/Mg to the ordinary chondrites. We speculate that this is related to the timing of removal of a refractory component from the source reservoirs of these different meteorite groups; the higher Δ′26MgDSM-3 of the enstatite chondrites suggests later (∼0.5 Ma post CAIs) condensation and loss of this refractory component. Despite inferred consistency of (26Al/27Al)0 and (Δ′26MgDSM-3)0 across most chondrite groups, some nebular heterogeneity is required to account for the compositions of CR chondrites. Our preferred interpretation is that the CR source region has lower (Δ′26MgDSM-3)0. As the most appropriate isotopic reference for the Earth, our new mean enstatite chondrite composition allows us to assess possible ingrowth of 26Mg from live 26Al during accretion of the Earth. The Earth has Δ′26MgDSM-3 within uncertainty of enstatite chondrites, despite its higher Al/Mg. This requires that the terrestrial increase in Al/Mg, which we attribute to vapour loss during accretion, must have happened >1.5 Ma post CAI formation, in an instantaneous fractionation model.

Elemental and isotopic variability in solar system materials by mixing and processing of primordial disk reservoirs

Isotope anomalies among planetary bodies provide key constraints on planetary genetics and the Solar System's dynamical evolution. However, to unlock the full potential of these anomalies for constraining the processing, mixing, and transport of material in the disk it is essential to identify the main components responsible for producing planetary-scale isotope variations, and to investigate how they relate to the isotopic heterogeneity inherited from the Solar System's parental molecular cloud. To address these issues we measured the Ti and Sr isotopic compositions of Ca,Al-rich inclusions (CAIs) from the Allende CV3 chondrite, as well as acid leachates and an insoluble residue from the Murchison CM2 chondrite, and combine these results with literature data for presolar grains, hibonites, chondrules, and bulk meteorites. Our analysis reveals that the mineral-scale nebular isotopic heterogeneity as sampled by leachates and presolar grains is largely decoupled from the planetary-scale isotope anomalies. Combining isotope anomaly data for a large number of elements reveals that the difference between non-carbonaceous (NC) and carbonaceous (CC) meteorites is the product of mixing between NC material and a nebular reservoir (termed IC) whose isotopic composition is similar to that of CAIs, but whose chemical composition is similar to bulk chondrites. In our preferred model, the distinct isotopic compositions of these two nebular reservoirs reflect an inherited heterogeneity of the solar system's parental molecular cloud core, which therefore has never been fully homogenized during collapse. Planetary-scale isotopic anomalies are thus caused by variable mixing of isotopically distinct primordial disk reservoirs, the selective processing of these reservoirs in different nebular environments, and the heterogeneous distribution of the thereby forming nebular products.