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1.
The absolute isotope abundance of Ti has been determined in Ca-Al-rich inclusions from the Allende and Leoville meteorites and in samples of whole meteorites. The absolute Ti isotope abundances differ by a significant mass dependent isotope fractionation transformation from the previously reported abundances, which were normalized for fractionation using 46Ti48Ti. Therefore, the absolute compositions define distinct nucleosynthetic components from those previously identified or reflect the existence of significant mass dependent isotope fractionation in nature. We provide a general formalism for determining the possible isotope compositions of the exotic Ti from the measured composition, for different values of isotope fractionation in nature and for different mixing ratios of the exotic and normal components. The absolute Ti and Ca isotopic compositions still support the correlation of 50Ti and 48Ca effects in the FUN inclusions and imply contributions from neutron-rich equilibrium or quasi-equilibrium nucleosynthesis. The present identification of endemic effects at 46Ti, for the absolute composition, implies a shortfall of an explosive-oxygen component or reflects significant isotope fractionation. Additional nucleosynthetic components are required by 47Ti and 49Ti effects. Components are also defined in which 48Ti is enhanced.Bulk samples of carbonaceous meteorites (C2 and C3 types) show distinct excesses at 50Ti but no nonlinear effects at the other Ti isotopes. Other chondrites, including Orgueil (Cl), show no nonlinear effects. Relative to terrestrial Ti, a small isotope fractionation is found for only an enstatite chondrite. The Ti absolute compositions in Ca-Al-rich inclusions show significant isotope fractionation effects corresponding to an enhancement in the heavier isotopes relative to the lighter isotopes as compared to Ti in a TiO2 standard and in chondrites. The absence of a correlation of Ti isotope fractionation effects with those for Ca and Mg is indicative of multiple processes of condensation, volatilization and recondensation; however, the mechanisms causing the isotope fractionation are not well understood.  相似文献   

2.
High-precision analyses of Ti are reported for samples from a variety of meteorite classes. The expanded data base for Allende inclusions still shows Ti isotopic anomalies in every inclusion. All the coarse-grained inclusions give quite similar patterns, but fine-grained inclusions show more variable, and sometimes larger, anomalies. One inclusion, 3675A, was analyzed because others identified it as a possible “FUN” inclusion due to its mass-fractionated Mg. This designation is supported by the significantly more complex Ti isotopic pattern for 3675A compared to all our other Allende inclusions. Available data fail to suggest that any particular Allende mineral phase, including a chromite-carbon fraction from an acid residue, is especially rich in anomalous Ti. We also find anomalous Ti in a bulk sample of a Cl chondrite and in matrix separates from C2 chondrites. The excesses of 50Ti are smaller than for Allende inclusions, and subtle differences in Ti isotopic patterns tentatively suggest that parent materials for C1-C2 matrix and Allende inclusions are not directly related. Analyses of chondrules from unequilibrated ordinary chondrites did not yield clear evidence for anomalous Ti, but some “larger than usual” deficits at 5046 give encouragement for future work in this direction. Comparing the magnitude of isotopic shifts at 50Ti and 16O for all these meteorite samples indicates that they are not correlated, but the data do not preclude a correlation between concentrations of “exotic” 50Ti and 16O atoms.Whether or not Allende “FUN” inclusions are considered, at least 4 distinct isotopic components of Ti are required to account for the observed isotopic variations. The Ti data cannot be plausibly explained in terms of an early solar-system particle irradiation; instead, neutron-rich hydrostatic burning within a star is probably responsible for the dominant 50Ti anomalies, while s-process mechanisms are viable sources for some of the more subtle Ti variations. We suggest that the Ti anomalies are linked to a diversity of nucleosynthetic sources and the highly refractory behavior of Ti. Therefore, some form of “chemical memory” from the ISM, rather than “late stage supernova injection”, is most likely responsible for the preservation of observed isotopic heterogeneities.  相似文献   

3.
Refractory inclusions, or CAIs (calcium-aluminium-rich inclusions) are a unique ingredient in chondritic meteorites. As the name suggests, they are enriched in refractory elements, essentially reflecting a condensation sequence of phases from a cooling gas of solar composition. However, the widespread preservation of diverse isotopic anomalies is not compatible with the inclusions having been in a gaseous form. Rather, the CAIs appear to represent mixtures of condensate and refractory residue materials. The condensates formed from cooling solar gas and fractionation of that gas produced variations in the abundances of refractory elements according to volatility. Solar condensate has isotopically normal Ca and Ti isotopic compositions and has 26Al/27Al of the canonical value for the solar system at 5 × 10?5. Residues of material falling in toward the Sun are probably aluminous oxides such as corundum and hibonite, and preserve diverse Ca and Ti isotopic anomalies. Meteoritic inclusions from the Murchison meteorite show the best polarization of these components. Spinel-hibonite-perovskite inclusions (SHIBs) predominantly have normal Ca and Ti isotopes, 26Al/27Al at 5 × 10?5, and ultrarefractory fractionated REE patterns. Single hibonite crystal fragments (PLACs) have diverse Ca and Ti isotopic compositions and low 26Al/27Al because of the initially high proportion of 27Al in the residue. REE patterns in PLACs are variable in terms of the ultrarefractory fractionation of their REE patterns, as indicated by Tm/Tm?, but are dominated by depletion in the less refractory REE Eu and Yb. Both PLACs and SHIBs homogenized with 16O-rich gas, enriched relative to terrestrial O by up to 7%, thus removing any isotopic heterogeneity from the PLAC precursors. CAIs formed close to the Sun where condensation and re-evaporation of REE was possible, and were then ejected back to planetary radii where they were eventually accreted onto planetesimals.  相似文献   

4.
We describe the analytical techniques developed for the precise measurement of the titanium isotope abundances using a TiO+ ion beam. Terrestrial, lunar, and bulk meteorite samples yield identical results. Using a normalization to 46Ti48Ti for mass dependent isotope fractionation, we obtain the normal Ti composition: 46Ti48Ti = 0.108548; 47Ti48Ti = 0.099315 ± 0.000005; 49Ti48Ti = 0.074463 ± 0.000004; 50Ti48Ti = 0.072418 ± 0.000004 (2σ grand mean), taking 18O16O = 0.002045 and 17O16O = 0.00037. Measurements on thirteen coarse-grained and fine-grained Ca-Al-Ti-rich inclusions from the Allende and Leoville meteorites show the presence of widespread, significant, nonlinear isotope anomalies in the Ti isotopes which were not used for normalization. The data require the addition of at least three exotic components. The distinct correlation of non-linear effects for the most neutron-rich isotopes of Ca and Ti and the absence of substantial effects at 46Ca in the FUN samples EK-1-4-1 and C-1 indicate that the effects reflect neutron-rich equilibrium or quasi-equilibrium nucleosynthetic processes in the outer layers of a supernova core. The results on Ca and Ti in conjunction with the isotopic effects on other elements (Mg, Sr, Ba, Nd, Sm) show that the samples represent mixtures of different nucleosynthetic components from distinctive processes (‘e’, ‘r’, ‘p’) which do not appear to be related to processes in the same stellar sites.  相似文献   

5.
We measured the 153Eu/151Eu ratio by MC-ICP-MS for a terrestrial basalt, two terrestrial soils, and four meteorites (whole rocks and/or chondrules of Bjurböle, Forest City, Murchison, and Allende) and found no isotopic variations. By contrast, two CAI separates from two different pieces of Allende show a 153Eu deficit of up to one per mil. Such a shortage in the heavy isotopes, which had also been identified in Allende CAIs for Sr [Patchett, P.J. 1980b. Sr isotopic fractionation in Allende chondrules: a reflection of solar nebular processes. Earth Planet. Sci. Lett.50, 181-188], cannot reflect evaporative fractionation. The lack of Sm isotope fractionation in the same samples further makes fractionation by purely kinetic processes an unlikely cause of the anomalous Eu isotopic composition. An alternative interpretation is condensation from a vapor already significantly depleted in Eu, but in such a scenario the fate of the missing material is unclear. We therefore prefer yet another interpretation, based on the low ionization potential of Eu (and Sr), in which electromagnetic separation of the ionized gas preferentially depletes the nebular gas in heavy isotopes.  相似文献   

6.
Magnesium, potassium and calcium isotope compositions in terrestrial samples and refractory phases from primitive meteorites are determined using an ion microprobe. A thorough investigation of the different instrument parameters is carried out to ensure that conditions necessary for high mass resolution and high precision isotopic studies are adequately satisfied. The instrument can be tuned to achieve mass resolution (M/ΔM) of up to 10,000 (M≤60); it has a very good dynamic stability (ΔB/B≤10 ppm over durations of ≤40 minutes) and the counting system has an effective dead-time of ≤25 nsec and a dynamic background of ≤0·01 c/s. Reproducibility and precision of isotopic measurements are checked by analyzing magnesium and titanium isotopic compositions in terrestrial standards and isotopically doped silicate glasses. A precision of 2‰ (2σ m ) was achieved during magnesium isotopic analysis in samples with low Mg content (200 ppm). Results from studies of magnesium and potassium isotopic compositions in several Ca−Al-rich refractory inclusions (CAIs) from the primitive meteorites Efremovka and Grosnaja, representing some of the early solar system objects, are presented. The well-behaved Mg−Al isotopic systematics confirm the pristine nature of the Efremovka CAIs inferred earlier from petrographic and trace element studies. The Grosnaja CAIs that have experienced secondary alterations show disturbed magnesium isotopic systematics. Observation of excess26Mg in several of the analyzed CAIs confirms the presence of the now extinct26Al (t 1/2=7×105 years) in the solar nebula at the time of CAI formation. Our data also suggest a relatively uniform distribution of26Al in the solar nebula. Several Efremovka CAIs with excess26Mg also have excess41K resulting from the decay of41Ca (t 1/2≃105 years). This observation constrains the time interval between cessation of nucleosynthetic input to the solar nebula and the formation of some of the first solar system solids (CAIs) to less than a million years.  相似文献   

7.
Stepwise dissolutions of the carbonaceous chondrites Orgueil (CI), Murchison (CM) and Allende (CV) reveal large nucleosynthetic anomalies for Zr isotopes that contrast with the uniform compositions found in bulk meteorites. Two complementary nucleosynthetic components are observed: one enriched and one depleted in s-process nuclides. The latter component, characterized by excess 96Zr, is most distinctive in the acetic acid leachate (up to ε96Zr ≈ 50). The excess decreases with increasing acid strength and the final leaching steps of the experiment are depleted in 96Zr and thus enriched in s-process nuclides. Presolar silicon carbide grains are likely host phases for part of the anomalous Zr released during these later stages. However, by mass balance they cannot account for the 96Zr excesses observed in the early leaching steps and this therefore hints at the presence of at least one additional carrier phase with significant amounts of anomalous Zr. The data provide evidence that average solar system material consists of a homogenized mixture of different nucleosynthetic components, which can be partly resolved by leaching experiments of carbonaceous chondrites.  相似文献   

8.
The ion microprobe was used to measure Ti and Mg isotopes as well as rare earth and other trace elements in ten hibonites from the CM carbonaceous chondrites Murchison, Murray, and Cold Bokkeveld and in two hibonites and Ti-rich pyroxene from the CV chondrite Allende. In hibonites from Murchison and Murray fission track densities were also measured, as were Th and U concentrations. Eight of the hibonites, from all four meteorites, exhibit large Ti isotopic anomalies, particularly in 50Ti. Two grains from Murray have 50Ti excesses of ~ 10%. At least four nucleosynthetic components are required to account for all the Ti isotopic data. Neutron-rich nuclear statistical equilibrium nucleosynthesis is the most likely process to account for a 50Ti-rich component (with 50Ti49Ti$̆20). The ion probe Ti isotopic measurements confirm that the solar nebula was isotopically heterogeneous on a small spatial scale and argue for a chemical memory origin of the Ti isotopic anomalies which were probably carried into the solar system in the form of refractory dust grains. However, there is no experimental evidence that such interstellar grains survived the formation of the hibonites. The REE and trace element patterns of the hibonites are similar to those seen in CAIs and can be interpreted in terms of fractionation effects during condensation from a gas of solar composition, thus arguing for a solar system origin of the hibonites. Additional evidence for such an origin is provided by the PuTh ratios, which are ~ 10−4, and by the Mg isotopic compositions which are normal except for 26Mg1 due to 26Al.Only three out of ten hibonites exhibit 26Mg1, consistent with previous studies which demonstrated the paucity of 26Mg1 in hibonites. Because of the refractory nature of hibonite and the presence of large Ti isotopic effects, we conclude that a heterogeneous distribution of 26Al in the early solar system is the most likely reason. In particular, our observations of δ50Ti = 15%. and of an isochron with (26Al27Al)0 = 5 × 10−8 in the FUN inclusion HAL are evidence against both late formation and Mg redistribution to explain the lack of 26Al in hibonites.There are no obvious correlations between the Ti isotopic compositions, the presence of 26Mg1, the presence of 244Pu, and the REE and trace element patterns in individual hibonites. This indicates that the anomalous 50Ti, as well as 26A1 and 244Pu, were not co-produced in a single astrophysical source, and/or that these nuclides were introduced into the solar nebula by different carriers before being incorporated into the hibonites.  相似文献   

9.
We report on a study of Al3509, a large Na- and Cl-rich, radially-zoned object from the oxidized CV carbonaceous chondrite Allende. Al3509 consists of fine-grained ferroan olivine, ferroan Al-diopside, nepheline, sodalite, and andradite, and is crosscut by numerous veins of nepheline, sodalite, and ferroan Al-diopside. Some poorly-characterized phases of fine-grained material are also present; these phases contain no significant H2O. The minerals listed above are commonly found in Allende CAIs and chondrules and are attributed to late-stage iron-alkali-halogen metasomatic alteration of primary high-temperature minerals. Textural observations indicate that Al3509 is an igneous object. However, no residual crystals that might be relicts of pre-existing CAI or chondrule minerals were identified. To establish the levels of 26Al and 36Cl originally present, 26Al-26Mg and 36Cl-36S isotopic systematics in sodalite were investigated. Al3509 shows no evidence of radiogenic 26Mg∗, establishing an upper limit of the initial 26Al/27Al ratio of 3 × 10−6. All sodalite grains measured show large but variable excesses of 36S, which, however, do not correlate with 35Cl/34S ratio. If these excesses are due to decay of 36Cl, local redistribution of radiogenic 36S∗ after 36Cl had decayed is required. The oxygen-isotope pattern in Al3509 is the same as found in secondary minerals resulting from iron-alkali-halogen metasomatic alteration of Allende CAIs and chondrules and in melilite and anorthite of most CAIs in Allende. The oxygen-isotope data suggest that the secondary minerals precipitated from or equilibrated with a fluid of similar oxygen-isotope composition. These observations suggest that the formation of Al3509 and alteration products in CAIs and chondrules in Allende requires a very similar fluid phase, greatly enriched in volatiles (e.g., Na and Cl) and with Δ17O ∼ −3‰. We infer that internal heating of planetesimals by 26Al would efficiently transfer volatiles to their outer portions and enhance the formation of volatile-enriched minerals there. We conclude that the site for the production of Na- and Cl-rich fluids responsible for the formation of Al3509 and the alteration of the Allende CAIs and chondrules must have been on a protoplanetary body prior to incorporation into the Allende meteorite. Galactic cosmic rays cannot be the source of the inferred initial 36Cl in Allende. The problem of 36Cl production by solar energetic particle (SEP) bombardment and the possibility that 36Cl and 41Ca might be the product of neutron capture resulting from SEP bombardment of protoplanetary surfaces are discussed. This hypothesis can be tested comparing inferred “initial” 36Cl with neutron fluencies measured on the same samples and on phases showing 36S∗ by Sm and Gd isotopic measurements.  相似文献   

10.
Tellurium isotope data acquired by multiple-collector inductively coupled plasma-mass spectrometry (MC-ICPMS) are presented for sequential acid leachates of the carbonaceous chondrites Orgueil, Murchison, and Allende. Tellurium isotopes are produced by a broad range of nucleosynthetic pathways and they are therefore of particular interest given the isotopic anomalies previously identified for other elements in these meteorites. In addition, the data provide new constraints on the initial solar system abundance of the r-process nuclide 126Sn, which decays to 126Te with a half-life of 234,500 years. The 126Te/128Te ratios of all leachates were found to be identical, within uncertainty, despite variations in 124Sn/128Te of between about 0.002 and 1.4. The data define a 126Sn/124Sn ratio of <7.7 × 10−5 at the time of last isotopic closure, consistent with the value of <18 × 10−5 previously reported for bulk carbonaceous chondrites. How close this is to the initial 126Sn/124Sn ratio of the solar system depends on when the investigated samples last experienced redistribution of Sn and Te. No clear evidence is found for nucleosynthetic anomalies in the abundances of p-, s-, and r-process nuclides. The largest effect detected in this study is a small excess of the r-process nuclide 130Te in a nitric acid leachate of Murchison. This fraction displays an anomalous ε130Te of +3.5 ± 2.5. Although barely resolvable given the analytical uncertainties, this is consistent with the presence of a small excess r-process component or an s-process deficit. The general absence of anomalies contrasts with previous results obtained for K, Cr, Zr, Mo, and Ba isotopes in similar leachates, which display nucleosynthetic anomalies of up to 3.8%. The reason for this discrepancy is unclear but it may reflect volatility and more efficient mixing of Te in the solar nebula.  相似文献   

11.
We report measurements of the absolute isotope abundance of Ca in Ca-Al-rich inclusions from the Allende and Leoville meteorites. Improved high precision measurements are reported also for 46Ca. We find that nonlinear isotope effects in Ca are extremely rare in these inclusions. The absence of nonlinear effects in Ca, except for the effects in FUN inclusions, is in sharp contrast to the endemic effects in Ti. One fine-grained inclusion shows an excess of 46Ca of (7 ± 1)%., which is consistent with addition of only 46Ca or of an exotic (1) component with 46Ca1 ~ 48Ca1. FUN inclusion EK-1-4-1 shows a small 46Ca excess of (3.3 ± 1.0)%.; this confirms that the exotic Ca components in EK-1-4-1 were even more deficient in 46Ca relative to 48Ca than is the case for normal Ca. The Ca in the Ca-Al-rich inclusions shows mass dependent isotope fractionation effects (as deduced from the absolute 40Ca44Ca) which have a range from ?3.8 to +6.7%. per mass unit difference. This range is a factor of 20 wider than the range previously established for bulk meteorites and for terrestrial and lunar samples. Ca and Mg isotope fractionation effects in the Ca-Al-rich inclusions are common and attributed to kinetic isotope effects which imply the production of the inclusions by complex sequences of condensation, vaporization and recondensation. A correlation was found between Ca and Mg isotope fractionation effects and inclusion type. A possible correlation between isotope fractionation and rare earth element abundance patterns is discussed.  相似文献   

12.
This paper presents a review of recent available data on the first solid condensates of the Solar System, which include refractory CAIs (Ca–Al-rich Inclusions) mostly composed of Ca, Al, Mg, and Ti minerals. A theoretical condensation sequence calculated from thermodynamic data confirmed that CAIs formed as fine-grained aggregates in the protoplanetary disk from an 16О-rich gas of solar composition at temperatures >1300° K and pressures <10–4 bar. Based on the diversity of CAI types, their mineralogical, bulk chemical, and isotopic compositions, it can be concluded that CAIs experienced melting and evaporation, possibly by shock waves, which may have occurred in the protoplanetary disk within a brief time interval. Some CAIs may have experienced multiple events such as melting, evaporation, and recycling back to the disk by means of a bipolar outflow. The CAIs having an absolute age of 4567.30 ± 0.16 Myr are the oldest objects in the Solar System. The study of CAIs revealed two distinct oxygen isotope reservoirs (16О-rich and 16О-poor) and established a chronology of the sequence of processes forming individual CAI components using Mg–Al, Cr–Mn and Pb–Pb isotopic systematics.  相似文献   

13.
The abundance and isotopic composition of Hg was determined in bulk samples of both the Murchison (CM) and Allende (CV) carbonaceous chondrites using single- and multi-collector inductively coupled plasma mass spectrometry (ICP-MS). The bulk abundances of Hg are 294 ± 15 ng/g in Murchison and 30.0 ± 1.5 ng/g in Allende. These values are within the range of previous measurements of bulk Hg abundances by neutron activation analysis (NAA). Prior studies suggested that both meteorites contain isotopically anomalous Hg, with δ196/202Hg values for the anomalous, thermal-release components from bulk samples ranging from −260 ‰ to +440 ‰ in Murchison and from −620 ‰ to +540 ‰ in Allende Jovanovic and Reed 1976a, Jovanovic and Reed 1976b, Kumar and Goel 1992. Our multi-collector ICP-MS measurements suggest that the relative abundances of all seven stable Hg isotopes in both meteorites are identical to terrestrial values within 0.2 to 0.5 ‰.On-line thermal-release experiments were performed by coupling a programmable oven with the single-collector ICP-MS. Powdered aliquots of each meteorite were linearly heated from room temperature to 900°C over twenty-five minutes under an Ar atmosphere to measure the isotopic composition of Hg released from the meteorites as a function of temperature. In separate experiments, the release profiles of S and Se were determined simultaneously with Hg to constrain the Hg distribution within the meteorites and to evaluate the possibility of Se interferences in previous NAA studies. The Hg-release patterns differ between Allende and Murchison. The Hg-release profile for Allende contains two distinct peaks, at 225° and 343°C, whereas the profile for Murchison has only one peak, at 344°C. No isotopically anomalous Hg was detected in the thermal-release experiments at a precision level of 5 to 30 ‰, depending on the isotope ratio. In both meteorites the Hg peak at ∼340°C correlates with a peak in the S-release profile. This correlation suggests that Hg is associated with S-bearing phases and, thus, that HgS is a major Hg-bearing phase in both meteorites. The Hg peak at 225°C for Allende is similar to release patterns of physically adsorbed Hg on silicate and metal grains. Prior studies suggested that the isotopic anomalies reported from NAA resulted from interference between 203Hg and 75Se. However, the amount of Se released from both meteorites, relative to Hg, is insufficient to produce all of the observed anomalies.  相似文献   

14.
The oxygen isotopic micro-distributions within and among minerals in a coarse-grained Ca, Al-rich inclusion (CAI), 7R-19-1 from the Allende meteorite, were measured by in situ using secondary ion mass spectrometry (SIMS). All values of O isotopic ratios in 7R-19-1 minerals fall along the carbonaceous chondrite anhydrous mineral mixing (CCAM) line on a δ17OSMOW vs. δ18OSMOW plot. Major refractory minerals (spinel, fassaite and melilite) in 7R-19-1 showed large negative anomalies of Δ17O in the order, spinel (−21‰) > 16O-rich melilite (∼−18‰) > fassaite (−15 to +1‰) > 16O-poor melilite (−8 to +2‰). However, the lower limit values of Δ17O are similar at about −21‰, a value commonly observed in CAIs. The similarity in the extreme values of the isotope anomaly anomalies suggests that crystallization of all CAIs started from an 16O enrichment of 21‰ (Δ17O) relative to terrestrial values. The order of the O isotopic anomalies observed for 7R-19-1, except for 16O-poor melilite, is parallel to the crystallization sequence determined by experiment from CAI liquid (Stolper, 1982), indicating that the O isotopic exchange in 7R-19-1 occurred between CAI melt and surrounding gas while 7R-19-1 was crystallizing from the 16O enriched CAI liquid (∼−21‰ in Δ17O) in the 16O-poor solar nebula. However, the a single crystallization sequence during the cooling stage cannot explain the existence of 16O-poor melilite. The presence of 16O-poor melilite suggests that multiple heating events occurred during CAI formation. The sharp contact between 16O-rich and 16O-poor melilite crystals and within 16O-rich melilite indicates that these multiple heatings occurred quickly. Based on the O isotopic and chemical compositions, fassaite crystals were aggregates of relic crystals formed from CAI melt whichthat have had various O isotopic compositions from the remelting processes. The results of intra-mineral distributions of O isotopes also support multiple heating events during CAI formation.  相似文献   

15.
Application of 182Hf-182W chronometry to constrain the duration of early solar system processes requires the precise knowledge of the initial Hf and W isotope compositions of the solar system. To determine these values, we investigated the Hf-W isotopic systematics of bulk samples and mineral separates from several Ca,Al-rich inclusions (CAIs) from the CV3 chondrites Allende and NWA 2364. Most of the investigated CAIs have relative proportions of 183W, 184W, and 186W that are indistinguishable from those of bulk chondrites and the terrestrial standard. In contrast, one of the investigated Allende CAIs has a lower 184W/183W ratio, most likely reflecting an overabundance of r-process relative to s-process isotopes of W. All other bulk CAIs have similar 180Hf/184W and 182W/184W ratios that are elevated relative to average carbonaceous chondrites, probably reflecting Hf-W fractionation in the solar nebula within the first ∼3 Myr. The limited spread in 180Hf/184W ratios among the bulk CAIs precludes determination of a CAI whole-rock isochron but the fassaites have high 180Hf/184W and radiogenic 182W/184W ratios up to ∼14 ε units higher than the bulk rock. This makes it possible to obtain precise internal Hf-W isochrons for CAIs. There is evidence of disturbed Hf-W systematics in one of the CAIs but all other investigated CAIs show no detectable effects of parent body processes such as alteration and thermal metamorphism. Except for two fractions from one Allende CAI, all fractions from the investigated CAIs plot on a single well-defined isochron, which defines the initial ε182W = −3.28 ± 0.12 and 182Hf/180Hf = (9.72 ± 0.44) × 10−5 at the time of CAI formation. The initial 182Hf/180Hf and 26Al/27Al ratios of the angrites D’Orbigny and Sahara 99555 are consistent with the decay from initial abundances of 182Hf and 26Al as measured in CAIs, suggesting that these two nuclides were homogeneously distributed throughout the solar system. However, the uncertainties on the initial 182Hf/180Hf and 26Al/27Al ratios are too large to exclude that some 26Al in CAIs was produced locally by particle irradiation close to an early active Sun. The initial 182Hf/180Hf of CAIs corresponds to an absolute age of 4568.3 ± 0.7 Ma, which may be defined as the age of the solar system. This age is 0.5-2 Myr older than the most precise 207Pb-206Pb age of Efremovka CAI 60, which does not seem to date CAI formation. Tungsten model ages for magmatic iron meteorites, calculated relative to the newly and more precisely defined initial ε182W of CAIs, indicate that core formation in their parent bodies occurred in less than ∼1 Myr after CAI formation. This confirms earlier conclusions that the accretion of the parent bodies of magmatic iron meteorites predated chondrule formation and that their differentiation was triggered by heating from decay of abundant 26Al. A more precise dating of core formation in iron meteorite parent bodies requires precise quantification of cosmic-ray effects on W isotopes but this has not been established yet.  相似文献   

16.
We report results from NanoSIMS isotopic measurements on 37 presolar silicon carbide grains of type X which are believed to have formed in the ejecta of supernova explosions. Isotopic data were obtained for Si and Ca-Ti (all grains), C and N (two grains), and Ti (one grain). All X grains exhibit large enrichments in 28Si (up to 5× solar), in agreement with previously studied X grains. On a scale of 200 nm, the Si-isotopic ratios do not vary by more than the analytical uncertainties of several percent in all but one X grain. This implies that most X grains formed from well-mixed regions in supernova ejecta. X grain M9-68-3 is characterized by two regions with distinct Si- and Ti-isotopic signatures which may either represent two distinct grains or overgrowth of matter from two different mixtures in the supernova ejecta. Most of the Ca in the X grains is most likely contamination as indicated by close to normal 42Ca/40Ca ratios. Seven X grains show enhanced 44Ca/40Ca ratios of up to 6× the solar ratio. Spatial distributions of 44Ca excesses and Ti are positively correlated, giving strong support to the view that excesses in 44Ca are due to the decay of radioactive 44Ti. Inferred initial 44Ti/48Ti ratios are between 0.01 and 0.28 and are correlated with Si-isotopic ratios. Radiogenic 44Ca is widely distributed in six X grains. X grain M9-132-4 exhibits a pronounced heterogeneity in the distribution of radiogenic 44Ca and 48Ti as well as in 44Ti/48Ti, pointing to presence of a small Ti-rich subgrain or heterogeneous loss of Ca and Ti after grain formation. This grain has a unique Si-isotopic composition with 30Si/29Si = 2.2× the solar ratio and C- and N-isotopic compositions as typically observed in X grains.  相似文献   

17.
We present the first measurements of vanadium (V) stable isotopes for six reference materials – USGS PCC‐1, BHVO‐2, BCR‐2, BIR‐1a, GSP‐2 and AGV‐2 – plus the widely available carbonaceous chondrite Allende. We present standard addition and matrix spiking tests to assess the robustness and reproducibility of our data. Standard addition utilised an enriched 50V solution designated VISSOX (Vanadium Isotope Standard Solution OXford). We further assessed the veracity of the method by spiking collected sample matrices with the same amount of a V standard solution, whose isotopic composition was defined as 0‰. Standard addition and matrix spiking tests recorded no appreciable artificial isotope fractionation. We estimate that the best currently attainable long‐term reproducibility of stable 51V/50V isotope measurements in complex matrices is 0.15‰, which is in the same order as the reproducibility achievable with standard solutions. Finally, a large range of ～ 1.2‰ in stable V isotopic composition was documented, with ～ 0.5‰ of that variation in high temperature igneous materials alone. The range and resolving power of V stable isotopes, with respect to igneous material, compared favourably with the magnitude of fractionation reported for other non‐traditional stable isotope systems, which bodes well for the utility of this new system.  相似文献   

18.
We report isotopic ratio measurements of small SiC and Si3N4 grains, with special emphasis on presolar SiC grains of type Z, and new nucleosynthesis models for 26Al/27Al and the Ti isotopic ratios in asymptotic giant branch (AGB) stars. With the NanoSIMS we analyzed 310 SiC grains from Murchison (carbonaceous CM2 chondrite) separate KJB (diameters 0.25-0.45 μm) and 153 SiC grains from KJG (diameters 1.8-3.7 μm), 154 SiC and 23 Si3N4 grains from Indarch (enstatite EH4 chondrite) separate IH6 (diameters 0.25-0.65 μm) for their C and N isotopic compositions, 549 SiC and 142 Si3N4 grains from IH6 for their C and Si isotopic compositions, 13 SiC grains from Murchison and 66 from Indarch for their Al-Mg compositions, and eight SiC grains from Murchison and 10 from Indarch for their Ti isotopic compositions. One of the original objectives of this effort was to compare isotopic analyses with the NanoSIMS with analyses previously obtained with the Cameca IMS 3f ion microprobe. Many of the Si3N4 grains from Indarch have isotopic anomalies but most of these apparently originate from adjacent SiC grains. Only one Si3N4 grain, with 13C and 14N excesses, has a likely AGB origin. The C, N, and Si isotopic data show that the percentage of SiC grains of type Y and Z increase with decreasing grain size (from ∼1% for grains >2 μm to ∼5-7% for grains of 0.5 μm), providing an opportunity for isotopic analyses in these rare grains. Our measurements expand the number of Al-Mg analyses on SiC Z grains from 4 to 23 and the number of Ti analyses on Z grains from 2 to 11. Inferred26Al/27Al ratios of Z grains are in the range found in mainstream and Y grains and do not exceed those predicted by models of AGB nucleosynthesis. Cool bottom processing (CBP) has been invoked to explain the low 12C/13C ratios of Z grains, but this process apparently does not lead to increased 26Al production in the parent stars of these grains. This finding is in contrast to presolar oxide grains where CBP is needed to explain their high 26Al/27Al ratios. The low 46,47,49Ti/48Ti ratios found in Z grains and their correlation with low 29Si/28Si ratios extend the trend seen in mainstream grains and confirm an origin in low-metallicity AGB stars. The relatively large excesses in 30Si and 50Ti in Z grains are predicted by our models to be the result of increased production of these isotopes by neutron-capture nucleosynthesis in low-metallicity AGB stars. However, the predicted excesses in 50Ti (and 49Ti) are much larger than those found. Even lowering the strength of the 13C pocket cannot solve this discrepancy in a consistent way.  相似文献   

19.
Low-density graphite spherules from the Murchison carbonaceous chondrite contain TiC grains and possess excess 28Si and 44Ca (from decay of short-lived 44Ti). These and other isotopic anomalies indicate that such grains formed by condensation from mixtures of ejecta from the interior of a core-collapse supernova with those from the exterior. Using homogenized chemical and isotopic model compositions of the eight main burning zones as end-members, Travaglio et al. (1999) attempted to find mixtures whose isotopic compositions match those observed in the graphite spherules, subject to the condition that the atomic C/O ratio = 1. They were partially successful, but this chemical condition does not guarantee condensation of TiC at a higher temperature than graphite, which is indicated by the spherule textures. In the present work, model compositions of relatively thin layers of ejecta within the main burning zones computed by Rauscher et al. (2002) for Type II supernovae of 15, 21 and 25 M? are used to construct mixtures whose chemical compositions cause equilibrium condensation of TiC at a higher temperature than graphite in an attempt to match the textures and isotopic compositions of the spherules simultaneously. The variation of pressure with temperature and the change in elemental abundances with time due to radioactive decay were taken into account in the condensation calculations. Layers were found within the main Ni, O/Ne, He/C and He/N zones that, when mixed together, simultaneously match the carbon, nitrogen and oxygen isotopic compositions, 44Ti/48Ti ratios and inferred initial 26Al/27Al ratios of the low-density graphite spherules, even at subsolar 12C/13C ratios. Due to the relatively large proportion of material from the Ni zone and the relative amounts of the two layers of the Ni zone required to meet these conditions, predicted 28Si excesses are larger than observed in the low-density graphite spherules, and large negative δ46Ti/48Ti, δ47Ti/48Ti, δ49Ti/48Ti and δ50Ti/48Ti are produced, in contrast to the observed normal δ46Ti/48Ti and δ47Ti/48Ti, large positive δ49Ti/48Ti and smaller positive δ50Ti/48Ti. Although better matches to the observed δ46Ti/48Ti, δ47Ti/48Ti and 28Si excesses can be found using much smaller amounts of Ni zone material and some Si/S zone material, it is very difficult to match simultaneously the Ti and Si isotopic compositions in any mixtures of material from these deep layers with He/C and He/N zone material, regardless of the condensation sequence. The occurrence of Fe-rich, Si-poor metal grains inside the graphite spherules does not have a satisfactory explanation.  相似文献   

20.
Acid leaching of the primitive C-chondrite Murchison and O-chondrite QUE 97008 reveal nucleosynthetic anomalies in Cr, Sr, Ba, Nd, Sm and Hf. The anomalies in all but Cr and Sm are best explained by variable additions of pure s-process nuclides to a background nebular composition slightly enriched in r-process isotopes compared to average Solar System material. Leaching leaves a residue in Murchison that is strongly enriched in s-process nuclides with depletions of over 0.1% in 135Ba and seven parts in 10,000 in 84Sr. If there are p-process anomalies in these two elements, they are lost in the variability caused by different r-, s-process contributions to the normalizing isotopes. The concentration and isotope systematics are consistent with the Ba and Sr isotopic composition in the Murchison residue being strongly influenced by s-process-rich presolar SiC. In general, the nucleosynthetic isotope anomalies are 2- to 5-fold smaller in QUE 97008 than in Murchison. The different magnitudes of isotope anomalies are similar to the difference in matrix abundance between CM and O chondrites consistent with the suggestion that the carriers of nucleosynthetically anomalous material preferentially reside in the matrix and that some of this material has been distributed throughout the O-chondrite minerals as a result of thermal metamorphism.Neodymium, Sm and Hf display variable s-, r-process nuclide abundances as in Ba and Sr, but the anomalies are much smaller (e.g. ε148Nd, ε148Sm = −5.7, 2.1, respectively, in Murchison and −0.43, 0.16, respectively in QUE 97008 residues). After correcting Nd and Sm for s-, r-process variability, Sm in whole rock chondrites shows variable relative abundances of the p-process isotope 144Sm that correlate weakly with 142Nd suggesting that the direct p-process contribution to 142Nd is small (∼7-9%). Nucleosynthetic variability in Nd explains the range in 142Nd/144Nd seen between C and O, E-chondrites, but not the difference between chondrites and all modern Earth rocks, leaving decay of 146Sm and a superchondritic Sm/Nd ratio as the likely explanation for Earth’s high 142Nd/144Nd.  相似文献   

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