The oxygen‐isotopic record in enstatite meteorites

Abstract— Oxygen‐isotopic compositions were determined for a suite of enstatite chondrites and aubrites. In agreement with previous work (Clayton et al., 1984), most samples have O‐isotopic compositions close to the terrestrial fractionation line (TFL), and there appear to be no significant differences in O‐isotopic compositions between individual EH and EL chondrites and aubrites. Five enstatite meteorites have O‐isotopic compositions that are significantly different from the other samples and >0.2% away from the TFL. Two of these have petrographic evidence of brecciation and interaction between other meteorite types; for the other three, similar scenarios are suggested. There appears to be a systematic increase in δ¹⁸O from enstatite chondrites (both EH and EL) of petrologic type 3 to those of type 6. There is also good evidence that the EH meteorites do not fall along a mass fractionation line but along a line slope 0.66. At the present time, detailed understanding of the origin of these O‐isotopic systematics remain elusive but clearly point to a complex accretion history, parent‐body evolution, or both.     

Clastic matrix in EH3 chondrites

Abstract— Patches of clastic matrix (15 to 730 μm in size) constitute 4.9 vol% of EH3 Yamato (Y‐) 691 and 11.7 vol% of EH3 Allan Hills (ALH) 81189. Individual patches in Y‐691 consist of 1) ?25 vol% relatively coarse opaque grain fragments and polycrystalline assemblages of kamacite, schreibersite, perryite, troilite (some grains with daubréelite exsolution lamellae), niningerite, oldhamite, and caswellsilverite; 2) ?30 vol% relatively coarse silicate grains including enstatite, albitic plagioclase, silica and diopside; and 3) an inferred fine nebular component (?45 vol%) comprised of submicrometer‐size grains. Clastic matrix patches in ALH 81189 contain relatively coarse grains of opaques (?20 vol%; kamacite, schreibersite, perryite and troilite) and silicates (?30 vol%; enstatite, silica and forsterite) as well as an inferred fine nebular component (?50 vol%). The O‐isotopic composition of clastic matrix in Y‐691 is indistinguishable from that of olivine and pyroxene grains in adjacent chondrules; both sets of objects lie on the terrestrial mass‐fractionation line on the standard three‐isotope graph. Some patches of fine‐grained matrix in Y‐691 have distinguishable bulk concentrations of Na and K, inferred to be inherited from the solar nebula. Some patches in ALH 81189 differ in their bulk concentrations of Ca, Cr, Mn, and Ni. The average compositions of matrix material in Y‐691 and ALH 81189 are similar but not identical‐matrix in ALH 81189 is much richer in Mn (0.23 ± 0.05 versus 0.07 ± 0.02 wt%) and appreciably richer in Ni (0.36 ± 0.10 versus 0.18 ± 0.05 wt%) than matrix in Y‐691. Each of the two whole‐rocks exhibits a petrofabric, probably produced by shock processes on their parent asteroid.     

Sulfur in presolar silicon carbide grains from asymptotic giant branch stars

We studied 14 presolar SiC mainstream grains for C‐, Si‐, and S‐isotopic compositions and S elemental abundances. Ten grains have low levels of S contamination and CI chondrite‐normalized S/Si ratios between 2 × 10^?5 and 2 × 10^?4. All grains have S‐isotopic compositions compatible within 2σ of solar values. Their mean S isotope composition deviates from solar by at most a few percent, and is consistent with values observed for the carbon star IRC+10216, believed to be a representative source star of the grains, and the interstellar medium. The isotopic data are also consistent with stellar model predictions of low‐mass asymptotic giant branch (AGB) stars. In a δ³³S versus δ³⁴S plot the data fit along a line with a slope of 1.8 ± 0.7, suggesting imprints from galactic chemical evolution. The observed S abundances are lower than expected from equilibrium condensation of CaS in solid solution with SiC under pressure and temperature conditions inferred from the abundances of more refractory elements in SiC. Calcium to S abundance ratios are generally above unity, contrary to expectations for stoichiometric CaS solution in the grains, possibly due to condensation of CaC₂ into SiC. We observed a correlation between Mg and S abundances suggesting solid solution of MgS in SiC. The low abundances of S in mainstream grains support the view that the significantly higher abundances of excess ³²S found in some Type AB SiC grains are the result of in situ decay of radioactive ³²Si from born‐again AGB stars that condensed into AB grains.     

Presolar silicon carbide from the Indarch (EH4) meteorite: Comparison with silicon carbide populations from other meteorite classes

Abstract— Presolar SiC from the Indarch (EH4) meteorite was studied by scanning electron microscopy (SEM), by ion probe analysis for C and Si isotopic compositions, and by static source mass spectrometry for noble gas and C isotopic compositions. The data obtained are compared to SiC data from other meteorites, especially from Murchison (CM2), for which there is the most information available. The isotopic compositions of the major elements in SiC from Indarch and Murchison are similar. Stepped combustion data suggest a mean δ¹³C for SiC from both meteorites of ～+1430%o. Silicon isotopes in Indarch and Murchison SiC also compare well. In some other important respects, however, SiC in the two meteorites are different. Morphologically, SiC from Indarch appears finer grained than SiC from Murchison and is entirely composed of submicron grains. The finer-grained nature of Indarch SiC is confirmed by its noble gas characteristics. The mean Ne-E/Xe-S ratio for bulk Indarch SiC is significantly lower than the same ratio in Murchison (625 ± 47 vs. ～3500) but is similar to that of the finest grain-size fractions (<1 μm) in Murchison. A comparison of noble gas data from SiC from several different meteorites suggests that it might be Murchison SiC, rather than Indarch SiC, that is unusual. The grain-size disparities in SiC between meteorites are difficult to explain by residue processing differences or differing parent body processing. Instead, we speculate that a grain-size sorting mechanism for SiC may have operated in the solar nebula.     

Bo Xian (LL3.9): Oxygen‐isotopic and mineralogical characterisation of separated chondrules

Abstract— We report the results of a mineralogical and O‐isotopic study of 362 chondrules disaggregated from the Bo Xian chondrite. The range of mineral compositions (Fa = 0.8–31.2%, mean = 23.5%, mode = 27–28%) are consistent with a reclassification of this meteorite from LL4 to LL3.9. Chondrule diameters range from 0.20 to 3.40 mm (mean = 0.74 mm) in the disaggregated population. A lower mean diameter (0.64 mm) calculated from thin‐section measurements partly reflects the high proportion of chondrule fragments. The chondrule size distribution, which is approximately log‐normal, is consistent with size‐sorting mechanisms. This sorting could be linked to the fragmentation of many chondrules on the parent body. However, in detail, the variation in diameter of different chondrule types and a hiatus in the size distribution at 0.6 mm indicate that there may have been complex controls perhaps partly being determined by the chondrule formation mechanism. Seven percent of the sectioned chondrules (102) contain chemically fractionated mineral assemblages: cristobalite‐bearing and Al‐rich. This significant degree of chemical heterogeneity probably resulted from both igneous and volatility controls. Oxygen‐isotopic compositions were determined on mineral separates and 16 of the sectioned chondrules. Three separate isotopic exchange events have been identified. The dominant one is a low‐temperature hydrous gas‐solid exchange event between ¹⁶O‐rich solid and ¹⁶O‐poor gas reservoirs that lay along a slope 1.0 line on three‐isotope plots. Partial equilibration with the gas by feldspar and cristobalite, which exchanged more rapidly than olivine or pyroxene, led to formation of a slope 0.77 mixing line for Bo Xian and other LL chondrites. Mineralogy is the dominant control on the extent of this exchange; no relationship between isotopic composition and chondrule texture or size was identified. The feldspar separate and cristobalite‐rich chondrules have the most ¹⁶O‐poor compositions. Subsequently, thermal metamorphism in the parent body led to partial isotopic equilibration between the different mineral phases. A third exchange event, predating the other two events, is probably shown by one of the Al‐rich chondrules. This has an ¹⁶O‐rich composition, lying below the terrestrial fractionation line. Another Al‐rich chondrule has a normal ordinary chondrite isotopic composition. It is not clear whether the isotopic fractionation recorded in some Al‐rich chondrules can be achieved by the dominant gas‐solid exchange. Instead, the precursor O to the mineral phases may have become ¹⁶O‐rich during an earlier phase of mass‐independent fractionation.     

Krypton and xenon fractionation in North American tektites

Abstract— Elemental and isotopic compositions of the noble gases have been determined in six North American tektites (4 bediasites and 2 georgiaites) and one Ivory Coast tektite. Radiogenically produced ⁴He may explain the large ⁴He/³⁶Ar ratios measured relative to air, despite significant diffusive losses. The Ne isotopic composition is enriched in ²⁰Ne consistent with a single stage mass fractionation process. The enormous ²⁰Ne/³⁶Ar enrichments observed in all tektite samples, similar to those reported from other tektites and impact glasses, are attributed to atmospheric diffusion into the samples following solidification. The North American tektites show a systematic increase in ⁸⁴Kr/³⁶Ar and ¹³²Xe/³⁶Ar relative to air, with enrichments greater than those determined for any other tektite group or terrestrial samples other than shales. These enrichments are inconsistent with existing models of dissolving Kr and Xe in tektite glass without elemental fractionation at atmospheric pressures equivalent to ∼40 km altitude. The Kr and Xe isotopic compositions are indistinguishable from atmospheric within experimental uncertainty.     

Mass‐dependent fractionation of nickel isotopes in meteoritic metal

Abstract— We measured nickel isotopes via multicollector inductively coupled plasma mass spectrometry (MC‐ICPMS) in the bulk metal from 36 meteorites, including chondrites, pallasites, and irons (magmatic and non‐magmatic). The Ni isotopes in these meteorites are mass fractionated; the fractionation spans an overall range of ～0.4‰ amu^?1. The ranges of Ni isotopic compositions (relative to the SRM 986 Ni isotopic standard) in metal from iron meteorites (～0.0 to ～0.3‰ amu^?1) and chondrites (～0.0 to ～0.2‰ amu^?1) are similar, whereas the range in pallasite metal (～–0.1 to 0.0‰ amu^?1) appears distinct. The fractionation of Ni isotopes within a suite of fourteen IIIAB irons (～0.0 to ～0.3‰ amu^?1) spans the entire range measured in all magmatic irons. However, the degree of Ni isotopic fractionation in these samples does not correlate with their Ni content, suggesting that core crystallization did not fractionate Ni isotopes in a systematic way. We also measured the Ni and Fe isotopes in adjacent kamacite and taenite from the Toluca IAB iron meteorite. Nickel isotopes show clearly resolvable fractionation between these two phases; kamacite is heavier relative to taenite by ～0.4‰ amu^?1. In contrast, the Fe isotopes do not show a resolvable fractionation between kamacite and taenite. The observed isotopic compositions of kamacite and taenite can be understood in terms of kinetic fractionation due to diffusion of Ni during cooling of the Fe‐Ni alloy and the development of the Widmanstätten pattern.     

Oxygen isotopic and chemical composition of chromites in micrometeorites: Evidence of ordinary chondrite precursors

We identified 66 chromite grains from 42 of ~5000 micrometeorites collected from Indian Ocean deep‐sea sediments and the South Pole water well. To determine the chromite grains precursors and their contribution to the micrometeorite flux, we combined quantitative electron microprobe analyses and oxygen isotopic analyses by high‐resolution secondary ion mass spectrometry. Micrometeorite chromite grains show variable O isotopic compositions with δ¹⁸O values ranging from ?0.8 to 6.0‰, δ¹⁷O values from 0.3 to 3.6‰, and Δ¹⁷O values from ?0.9 to 1.6‰, most of them being similar to those of chromites from ordinary chondrites. The oxygen isotopic compositions of olivine, considered as a proxy of chromite in chromite‐bearing micrometeorites where chromite is too small to be measured in ion microprobe have Δ¹⁷O values suggesting a principal relationship to ordinary chondrites with some having carbonaceous chondrite precursors. Furthermore, the chemical compositions of chromites in micrometeorites are close to those reported for ordinary chondrite chromites, but some contribution from carbonaceous chondrites cannot be ruled out. Consequently, carbonaceous chondrites cannot be a major contributor of chromite‐bearing micrometeorites. Based on their oxygen isotopic and elemental compositions, we thus conclude with no ambiguity that chromite‐bearing micrometeorites are largely related to fragments of ordinary chondrites with a small fraction from carbonaceous chondrites, unlike other micrometeorites deriving largely from carbonaceous chondrites.     

A comparative study of opaque phases in Qingzhen (EH3) and MacAlpine Hills 88136 (EL3): Representatives of EH and EL parent bodies

Abstract— Opaque minerals in the Qingzhen (EH3) and MacAlpine Hills (MAC) 88136 (EL3) enstatite chondrites were studied and compared with other EH and EL chondrites. All opaque minerals usually occur in multi‐sulfide‐metal clasts and nodules in the matrix between chondrules (El Goresy et al., 1988). The higher abundance of opaque minerals, the occurrence of niningerite and various alkali‐sulfides (e.g., caswellsilverite, phases A and B, djerfisherite) are diagnostic criteria for EH chondrites, while alabandite is characteristic for EL chondrites. In addition, EH chondrites are characterized by enrichments of Si in both kamacite and perryite, and alkali elements in sphalerite and chalcopyrite. The Mn contents of daubreelite and sphalerite are lower in EH than in EL chondrites. These are consistent with lower oxygen fugacity and higher H₂S fugacity of EH than EL chondrites. In contrast, the discovery of sphalerite and Zn‐rich daubreelite in MAC 88136 indicates that their absence in EL6 chondrites is probably related to thermal metamorphism in the parent body. Schreibersite microspherules are commonly enclosed in most sulfides in Qingzhen, but are absent in MAC 88136. They were once molten, and probably predated all sulfide host phases. The petrographic setting and chemical compositions of the sulfide hosts of the schreibersite microspherules in EH3 chondrites are consistent with formation by condensation. The earliest sulfide condensates oldhamite and niningerite occupy the interiors of the clasts and nodules, whereas the rims consist of troilite and djerfisherite. In addition, in Qingzhen, some other troilite, djerfisherite and sphalerite assemblages coexist with perryite. They were produced by sulfurization of metallic Fe‐Ni in the nebula. In MAC 88136, sulfurization of Si‐bearing Fe‐Ni metal is less pronounced, and it produced troilite, schreibersite and less abundant perryite. Two kinds of normal zoning and a reverse zoning trends of niningerite, and both normal and reverse zoning of sphalerite were found in clasts and nodules in Qingzhen. The coexistence of normal and reverse zoning profiles in niningerite grains in the same meteorite strongly suggests that they formed before accretion in the parent body, because an asteroidal metamorphic or an impact event in the parent body would have erased these contrasting profiles and destroyed the textural settings. In contrast, alabandite in MAC 88136 shows only normal zoning, with the FeS content decreasing to 9.3 mol% toward troilite, indicating very slow cooling at low temperature.     

Sulfur four isotope NanoSIMS analysis of comet‐81P/Wild 2 dust in impact craters on aluminum foil C2037N from NASA’s Stardust mission

Abstract– We present NanoSIMS four‐isotope S analyses of 24 comet Wild 2 dust impact residues in craters on aluminum foil C2037N returned by NASA’s Stardust mission. Except for one sample, all impact residues have normal S isotopic compositions within 2σ uncertainties of at least two S isotope ratios. This implies that most S‐rich Wild 2 dust impactors formed in the solar system. Instrumental isotope fractionation due to sample topography is the main contribution to our analytical uncertainty. One impact crater residue shows small anomalies of δ³³S = ?57 ± 17‰, and δ³⁴S = ?41 ± 17‰ (1σ uncertainties). Although this could be simply a statistical outlier or the fingerprint of a chemical isotope fractionation it is also possible that the observed anomaly results from the mixture of a cometary FeS particle with a small (150 nm diam.) presolar FeS supernova grain. This would translate into a presolar sulfide abundance of approximately 200 ppm.     

Zinc isotopic composition of iron meteorites: Absence of isotopic anomalies and origin of the volatile element depletion

High‐precision Zn isotopic compositions measured by MC‐ICP‐MS are documented for 32 iron meteorites from various fractionally crystallized and silicate‐bearing groups. The δ⁶⁶Zn values range from ?0.59‰ up to +5.61‰ with most samples being slightly enriched in the heavier isotopes compared with carbonaceous chondrites (0 < δ⁶⁶Zn < 0.5). The δ⁶⁶Zn versus δ⁶⁸Zn plot of all samples defines a common linear fractionation line, which supports the hypothesis that Zn was derived from a single reservoir or from multiple reservoirs linked by mass‐dependent fractionation processes. Our data for Redfields fall on a mass fractionation line and therefore refute a previous claim of it having an anomalous isotopic composition due to nonmixing of nucleosynthetic products. The negative correlation between δ⁶⁶Zn and the Zn concentration of IAB and IIE is consistent with mass‐dependent isotopic fractionation due to evaporation with preferential loss of lighter isotopes in the vapor phase. Data for the Zn concentrations and isotopic compositions of two IVA samples demonstrate that volatile depletion in the IVA parent body is not likely the result of evaporation. This is important evidence that favors the incomplete condensation origin for the volatile depletion of the IVA parent body.     

Nuclear field shift effect as a possible cause of Te isotopic anomalies in the early solar system—An alternative explanation of Fehr et al. (2006 and 2009)

Abstract— We explore the possibility that Te isotopic anomalies measured in Ca‐Al‐rich inclusions (Fehr et al. 2009) and in leachates of carbonaceous chondrites (Fehr et al. 2006) may be due to mass‐independent effects controlled by nuclear field shift rather than to nucleosynthetic processes. Fehr et al.'s spectrum of mass‐independent anomalies of Te isotopes shows a smooth correlation with mass number and nuclear charge distribution. Ratios of even to odd isotopes, as the ¹²⁵Te/¹²⁶Te ratio used by these authors for normalization are particularly prone to nuclear field shift effects. We show that the alternative normalization of isotopic ratios to ¹³⁰Te/¹²⁶Te strongly reduces the trend of isotopic fractionation with mass number, leaving only ¹²⁵Te as truly anomalous. For both normalizations (¹²⁵Te/¹²⁶Te and ¹³⁰Te/¹²⁶Te), Fehr et al.'s results fit the theory of Bigeleisen (1996), which suggests that the nuclear field shift effect can potentially account for the observed Te isotope abundances, as an alternative to nucleosynthetic processes. We propose that these mass‐independent effects may be acquired during accretion of sulfides from the solar nebula.     

Partial melting of the Indarch (EH4) meteorite: A textural,chemical, and phase relations view of melting and melt migration

Abstract— To test whether aubrites can be formed by melting of enstatite chondrites and to understand igneous processes at very low O fugacities, we have conducted partial melting experiments on the Indarch (EH4) chondrite at 1000–1500 °C. Silicate melting begins at 1000 °C, and Indarch is completely melted by 1500 °C. The metal-sulfide component melts completely at 1000 °C. Substantial melt migration occurs at 1300–1400 °C, and metal migrates out of the silicate charge at 1450 °C and ～50% silicate partial melting. As a group, our experiments contain three immiscible metallic melts (Si-, P-, and C-rich), two immiscible sulfide melts (Fe- and FeMgMnCa-rich), and silicate melt. Our partial melting experiments on the Indarch (EH4) enstatite chondrite suggest that igneous processes at low fO₂ exhibit several unique features. The complete melting of sulfides at 1000 °C suggests that aubritic sulfides are not relics. Aubritic oldhamite may have crystallized from Ca and S complexed in the silicate melt. Significant metal-sulfide melt migration might occur at relatively low degrees of silicate partial melting. Substantial elemental exchange occurred between different melts (e.g., S between sulfide and silicate, Si between silicate and metal), a feature not observed during experiments at higher fO₂. This exchange may help explain the formation of aubrites from known enstatite chondrites.     

Calcium‐aluminum‐rich inclusions in enstatite chondrites (II): Oxygen isotopes

Abstract— In situ io n microprobe analyses of spinel in refractory calcium‐aluminium‐rich inclusions (CAIs) from type 3 EH chondrites yield ¹⁶O‐rich compositions (δ ¹⁸O and δ ¹⁷O about‐40‰). Spinel and feldspar in a CAI from an EL3 chondrite have significantly heavier isotopic compositions (δ ¹⁸O and δ ¹⁷O about ?5‰). A regression through the data results in a line with slope 1.0 on a three‐isotope plot, similar to isotopic results from unaltered minerals in CAIs from carbonaceous chondrites. The existence of CAIs with ¹⁶O‐rich and ¹⁶O‐poor compositions in carbonaceous as well as enstatite chondrites indicates that CAIs formed in at least two temporally or spatially distinct oxygen reservoirs. General similarities in oxygen isotopic compositions of CAIs from enstatite, carbonaceous, and ordinary chondrites indicate a common nebular mechanism or locale for the production of most CAIs.     

Raman spectroscopic properties and Raman identification of CaS‐MgS‐MnS‐FeS‐Cr2FeS4 sulfides in meteorites and reduced sulfur‐rich systems

Raman spectra were acquired on a series of natural and synthetic sulfide minerals, commonly found in enstatite meteorites: oldhamite (CaS), niningerite or keilite ((Mg,Fe)S), alabandite (MnS), troilite (FeS), and daubreelite (Cr₂FeS₄). Natural samples come from three enstatite chondrites, three aubrites, and one anomalous ungrouped enstatite meteorite. Synthetic samples range from pure endmembers (CaS, FeS, MgS) to complex solid solutions (Fe, Mg, Ca)S. The main Raman peaks are localized at 225, 285, 360, and 470 cm^?1 for the Mg‐rich sulfides; at 185, 205, and 285 cm^?1 for the Ca‐rich sulfides; at 250, 370, and 580 cm^?1 for the Mn‐rich sulfides; at 255, 290, and 365 cm^?1 for the Cr‐rich sulfides; and at 290 and 335 cm^?1 for troilite with, occasionally, an extra peak at 240 cm^?1. A peak at 160 cm^?1 is present in all Raman spectra and cannot be used to discriminate between the different sulfide compositions. According to group theory, none of the cubic monosulfides oldhamite, niningerite, or alabandite should present first‐order Raman spectra because of their ideal rocksalt structure. The occurrence of broad Raman peaks is tentatively explained by local breaking of symmetry rules. Measurements compare well with the infrared frequencies calculated from first‐principles calculations. Raman spectra arise from activation of certain vibrational modes due to clustering in the solid solutions or to coupling with electronic transitions in semiconductor sulfides.     

Solar wind and other gases in the regoliths of the Pesyanoe parent object and the moon

We report new data from Pesyanoe‐90,1 (dark lithology) on the isotopic signature of solar wind (SW) Xe as recorded in this enstatite achondrite which represents a soil‐breccia of an asteroidal regolith. The low temperature (≤800°C) steps define the Pesyanoe‐S xenon component, which is isotopically consistent with SW Xe reported for the lunar regolith. This implies that the SW Xe isotopic signature was the same at two distinct solar system locations and, importantly, also at different times of solar irradiation. Further, we compare the calculated average solar wind “SW‐Xe” signature to Chass‐S Xe, the indigenous Xe observed in SNC (Mars) meteorites. Again, a close agreement between these compositions is observed, which implies that a mass‐dependent differential fractionation of Xe between SW‐Xe and Chass‐S Xe is >1.5%_o per amu. We also observe fractionated (Pesyanoe‐F) Xe and Ar components in higher temperature steps and we document a fission component due to extinct ²⁴⁴Pu. Interestingly, the Pesyanoe‐F Xe component is revealed only at the highest temperatures (>1200°C). The Pesyanoe‐F gas reveals Xe isotopic signatures that are consistent with lunar solar energetic particles (SEP) data and may indicate a distinct solar energetic particle radiation as was inferred for the moon. However, we cannot rule out fractionation processes due to parent body processes. We note that ratios ³⁶Ar/³⁸Ar≤5 are also consistent with SEP data. Calculated abundances of the fission component correlate well with radiogenic ⁴⁰Ar concentrations, revealing rather constant ²⁴⁴Pu/K ratios in Pesyanoe, and separates thereof, and indicate that both components were retained. We identify a nitrogen component (δ¹⁵N = 44%_o) of non‐solar origin with an isotopic signature distinct from indigenous N (δ¹⁵N = ?33%^o). While large excesses at ¹²⁸Xe and ¹²⁹Xe are observed in the lunar regolith samples, these excesses in Pesyanoe are small. On the other hand, significant ¹²⁶Xe isotopic excesses, comparable to relative excesses observed in lunar soils and breccias, are prominent in the intermediate temperature steps of Pesyanoe‐90,1.     

Iron isotopic measurements in presolar silicate and oxide grains from the Acfer 094 ungrouped carbonaceous chondrite

We carried out Fe isotopic analyses on 21 O‐rich presolar grains from the Acfer 094 ungrouped carbonaceous chondrite. Presolar grains were identified on the basis of oxygen isotopic ratios, and elemental compositions were measured by Auger spectroscopy. The Fe isotopic measurements were carried out by analyzing the Fe isotopes as negative secondary oxides with the NanoSIMS to take advantage of the higher spatial resolution of the Cs⁺ primary ion beam. Our results demonstrate the effectiveness of this approach for measuring both ⁵⁴Fe/⁵⁶Fe and ⁵⁷Fe/⁵⁶Fe. The ion yield for FeO^– is significantly lower than for Fe⁺, but this is not a serious limitation for presolar silicate grains with Fe as a major element. Most of the grains analyzed are ferromagnesian silicates, but we also measured four oxide grains. Iron contents are high in all of the grains, ranging from 10 to 40 atom%. Three of the grains belong to oxygen isotope Group 4. All of them have ⁵⁴Fe/⁵⁶Fe and ⁵⁷Fe/⁵⁶Fe ratios that are solar within errors, consistent with an origin in the outer zones of a Type II supernova, as indicated by their oxygen isotopic compositions. The remaining grains belong to oxygen isotope Group 1, with origins in low‐mass AGB stars. The majority of these also have solar ⁵⁴Fe/⁵⁶Fe and ⁵⁷Fe/⁵⁶Fe ratios. However, four grains are depleted in ⁵⁷Fe; one is also slightly depleted in ⁵⁴Fe. Current AGB models predict excesses in ⁵⁷Fe with ⁵⁴Fe/⁵⁶Fe ratios that largely reflect the metallicity of the parent star. While the solar ⁵⁷Fe/⁵⁶Fe ratios are consistent with formation of the grains in early third dredge‐up episodes, these models cannot account for the grains with ⁵⁷Fe depletions. Comparison with galactic evolution models suggests formation of these grains from stars with significantly subsolar metallicity; however, these models also predict large depletions in ⁵⁴Fe, which are not observed in the grains. Thus, the isotopic compositions of these grains remain unexplained.     

Structural and isotopic microanalysis of presolar SiC from supernovae

Abstract– We report on the microstructure, crystallography, chemistry, and isotopic compositions of seven SiC X grains and two mainstream grains from the Murchison meteorite. TEM crystallographic analysis revealed that the X grains (approximately 3 μm) are composed of many small crystals (24–457 nm), while the similarly sized mainstream grains are composed of only a few crystals (0.5–1.7 μm). The difference in crystal size likely results from differences in their formation environments: the X grain crystals evidently formed under conditions of greater supersaturation and rapid growth compared to their mainstream counterparts. However, the same polytypes are observed in both mainstream and X grains. Six X grains and both mainstream grains are entirely the 3C‐SiC polytype and one X grain is an intergrowth of the 3C‐SiC and 2H‐SiC polytypes. EDXS measurements indicate relatively high Mg content in the X grains (≲5 atomic%), while Mg was undetectable in the mainstream grains. The high Mg content is probably from the decay of ²⁶Al into ²⁶Mg. Estimates of the ²⁶Al/²⁷Al ratios, which range from 0.44–0.67, were made from elemental Mg/Al ratios. This range is consistent with the ²⁶Al/²⁷Al ratios inferred from previous isotopic measurements of X grains. We also report the first direct observations of subgrains in X grains, including the first silicides [(Fe,Ni)_nSi_m]. Diffraction data do not match any previously observed presolar phases, but are a good fit to silicides, which are predicted stable SN condensates. Eight subgrains with highly variable Ni/Fe ratios (0.12–1.60) were observed in two X grains.     

Isotopic properties of silicon carbide X grains from the Murchison meteorite in the size range 0.5‐1.5 μm

Abstract— We report isotopic abundances for C, N, Mg‐Al, Si, Ca‐Ti, and Fe in 99 presolar silicon carbide (SiC) grains of type X (84 grains from this work and 15 grains from previous studies) from the Murchison CM2 meteorite, ranging in size from 0.5 to 1.5 μm. Carbon was measured in 41 X grains, n in 37 grains, Mg‐Al in 18 grains, Si in 87 grains, Ca‐Ti in 25 grains, and Fe in 8 grains. These X grains have ¹²C/¹³C ratios between 18 and 6800, ¹⁴N/¹⁵n ratios from 13 to 200, δ²⁹Si/²⁸Si between ?750 and +60%₀, δ³⁰Si/²⁸Si from ?770 to ?10%₀, and ⁵⁴Fe/⁵⁶Fe ratios that are compatible with solar within the analytical uncertainties of several tens of percent. Many X grains carry large amounts of radiogenic ²⁶Mg (from the radioactive decay of ²⁶Al, half‐life ? 7 times 10⁵ years) and radiogenic ⁴⁴Ca (from the radioactive decay of ⁴⁴Ti, half‐life = 60 years). While all X grains but one have radiogenic ²⁶Mg, only ～20% of them have detectable amounts of radiogenic ⁴⁴Ca. Initial ²⁶Al/²⁷Al ratios of up to 0.36 and initial ⁴⁴Ti/⁴⁸Ti ratios of up to 0.56 can be inferred. The isotopic data are compared with those expected from the potential stellar sources of SiC dust. Carbon stars, Wolf‐Rayet stars, and novae are ruled out as stellar sources of the X grains. The isotopic compositions of C and Fe and abundances of extinct ⁴⁴Ti are well explained both by type Ia and type II supernova (SN) models. The same holds for ²⁶Al/²⁷Al ratios, except for the highest ²⁶Al/²⁷Al ratios of >0.2 in some X grains. Silicon agrees qualitatively with SN model predictions, but the observed ²⁹Si/³⁰Si ratios in the X grains are in most cases too high, pointing to deficiencies in the current understanding of the production of Si in SN environments. The measured ¹⁴n/¹⁵n ratios are lower than those expected from SN mixing models. This problem can be overcome in a 15 M_odot; type II SN if rotational mixing, preferential trapping of N, or both from ¹⁵n‐rich regions in the ejecta are considered. The isotopic characteristics of C, N, Si, and initial ²⁶Al/²⁷Al ratios in small X grains are remarkably similar to those of large X grains (2–10 μm). Titanium‐44 concentrations are generally much higher in smaller grains, indicative of the presence of Ti‐bearing subgrains that might have served as condensation nuclei for SiC. The fraction of X grains among presolar SiC is largely independent of grain size. This implies similar grain‐size distributions for SiC from carbon stars (mainstream grains) and supernovae (X grains), a surprising conclusion in view of the different conditions for dust formation in these two types of stellar sources.     

Constraining the 13C neutron source in AGB stars through isotopic analysis of trace elements in presolar SiC

Abstract— Analyses of the isotopic compositions of multiple elements (Mo, Zr, and Ba) in individual mainstream presolar SiC grains were done by resonant ionization mass spectrometry (RIMS). While most heavy element compositions were consistent with model predictions for the slow neutron capture process (s‐process) in low‐mass (1.5–3 M_⊙) asymptotic giant branch stars of solar metallicity when viewed on single‐element three‐isotope plots, grains with compositions deviating from model predictions were identified on multi‐element plots. These grains have compositions that cannot result from any neutron capture process but can be explained by contamination in some elements with solar system material. Previous work in which only one heavy element per grain was examined has been unable to identify contaminated grains. The multi‐element analyses of this study detected contaminated grains which were subsequently eliminated from consideration. The uncontaminated grains form a data set with a greatly reduced spread on the three‐isotope plots of each element measured, corresponding to a smaller range of ¹³C pocket efficiencies in parent AGB stars. Furthermore, due to this reduced spread, the nature of the stellar starting material, previously interpreted as having solar isotopic composition, is uncertain. The constraint on ¹³C pocket efficiencies in parent stars of these grains may help uncover the mechanism responsible for formation of ¹³C, the primary neutron source for s‐process nucleosynthesis in low‐mass stars.