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Some nuclides that were produced in supernovae are heterogeneously distributed between different meteoritic materials. In some cases these heterogeneities have been interpreted as the result of interaction between ejecta from a nearby supernova and the nascent solar system. Particularly in the case of the oldest objects that formed in the solar system – Ca–Al rich inclusions (CAIs) – this view is confirm the hypothesis that a nearby supernova event facilitated or even triggered solar system formation. We present Hf isotope data for bulk meteorites, terrestrial materials and CAIs, for the first time including the low-abundance isotope 174 Hf (∼0.16%). This rare isotope was likely produced during explosive O/Ne shell burning in massive stars (i.e., the classical “p-process”), and therefore its abundance potentially provides a sensitive tracer for putative heterogeneities within the solar system that were introduced by supernova ejecta. For CAIs and one LL chondrite, also complementary W isotope data are reported for the same sample cuts. Once corrected for small neutron capture effects, different chondrite groups, eucrites, a silicate inclusion of a IAB iron meteorite, and terrestrial materials display homogeneous Hf isotope compositions including 174 Hf. Hafnium-174 was thus uniformly distributed in the inner solar system when planetesimals formed at the <50 ppm level. This finding is in good agreement with the evidently homogeneous distributions of p-process isotopes 180 W, 184 Os and possibly 190 Pt between different iron meteorite groups. In contrast to bulk meteorite samples, CAIs show variable depletions in p-process 174 Hf with respect to the inner solar system composition, and also variable r-process (or s-process) Hf and W contributions. Based on combined Hf and W isotope compositions, we show that CAIs sampled at least one component in which the proportion of r- and s-process derived Hf and W deviates from that of supernova ejecta. The Hf and W isotope anomalies in CAIs are therefore best explained by selective processing of presolar carrier phases prior to CAI formation, and not by a late injection of supernova materials. Likewise, other isotope anomalies in additional elements in CAIs relative to the bulk solar system may reflect the same process. The isotopic heterogeneities between the first refractory condensates may have been eradicated partially during CAI formation, because W isotope anomalies in CAIs appear to decrease with increasing W concentrations as inferred from time-integrated 182 W/ 184 W. Importantly, the 176 Lu– 176 Hf and 182 Hf– 182 W chronometers are not significantly affected by nucleosynthetic heterogeneity of Hf isotopes in bulk meteorites, but may be affected in CAIs. [ABSTRACT FROM AUTHOR]

Analytical protocols for measurements of isotope ratios involving low-abundance isotopes 174 Hf (~ 0.16%), 180 W (~ 0.12%), and 190 Pt (~ 0.014%) using multi-collector inductively coupled plasma mass spectrometry (MC-ICP-MS) at ca. tenfold improved precision compared to previous studies are presented. The improvements in precision result in part from the use of Faraday amplifiers equipped with 10 12 Ω resistors for collection of the isotope beams of interest, as well as for the isotope beams used to monitor isobaric interferences. For ion currents > 5 × 10 − 13 A (> 50 mV on an amplifier with 10 11 Ω resistor), uncertainties (2 s.d.) of better than 100 ppm are typically achieved for isotope ratios involving 174 Hf, 180 W and 190 Pt. Terrestrial isotope abundances (atomic percent ± 2 s.d.) of 174 Hf (0.16106 ± 0.00006; n = 15); 180 W (0.11910 ± 0.00009; n = 10); and 190 Pt (0.01286 ± 0.00005; n = 9) were determined on reference solutions throughout multiple analytical sessions over ~ 3 years. The results, however, rely on the accuracy of the reference value chosen for the isotope ratios employed for mass bias correction and, to a lesser extent, on the accuracy of the exponential mass fractionation law used for mass bias correction. For the precise determination of isotope ratios involving 174 Hf, 180 W and 190 Pt in natural materials, efficient chromatographic separation schemes for Hf and W from silicate-rich matrices, and for Pt from iron meteorite matrices, are presented that provide effective separation of the element of interest from interfering elements. First results for Pt suggest that IAB, IIAB and IIIAB iron meteorites exhibit terrestrial 190 Pt abundances within uncertainty. Three chondrite samples exhibit indistinguishable 174 Hf from terrestrial Hf. The isotope abundance of 180 W in meteorites is more variable due to radiogenic 180 W that was produced by 184 Os-decay. [ABSTRACT FROM AUTHOR]

Abstract: The decay of the rare nuclide 184Os by alpha emission to 180W has been theoretically predicted, but was previously never observed in experiments. Variable excesses of 180W were recently observed for iron meteorites, but the contribution to these excesses by 184Os-decay was regarded as insignificant. Here, we present combined 180W and Os–W concentration data for meteorites and terrestrial rocks, now indicating that the 180W heterogeneities can be explained by α-decay of 184Os. A combined 184Os–180W isochron for iron meteorites and chondrites yields a decay constant value of of (half life yr), in good agreement with theoretical estimates. The 184Os–180W decay system may constitute a viable tracer and chronometer for important geological processes like core formation, silicate differentiation or late accretion processes. This is illustrated by a measured 180W-deficit in terrestrial basalts relative to chondrites by parts in 10 000, consistent with core formation ∼4.5 Ga ago. [Copyright &y& Elsevier]

Abstract The stepwise acid digestion of primitive chondritic meteorites allows the identification of nucleosynthetic isotope anomalies that are otherwise hidden on the bulk rock scale. Here, we present combined Hf and W isotope data for acid leachates, residues, and bulk rock aliquots of several primitive chondrites that include highly precise analyses of the heavy p-process isotopes 174Hf and 180W. Including data for these two p-process isotopes enables, for the first time, the clear-cut discrimination between s- and r-process contributions to the Hf and W isotope inventory. Our analyses reveal Hf and W isotopic homogeneity at the bulk rock scale, but significant Hf and W isotope anomalies that are complementary between acid leachates and residues. Since both r- to p-process isotope ratios are invariant in leachates and residues, the observed anomalies can unambiguously be tied to variable contributions of carrier phases enriched in s-process nuclides, as previously inferred for, i.e., Mo and Ru in leaching experiments. Hafnium and W isotope anomalies co-vary in leachate and residue fractions from CM chondrites, whereas CO and CV chondrites are characterized by distinctly larger Hf isotope anomalies compared to W. This observation is most likely explained by more efficient homogenization of s-process W carrier(s) or, alternatively, by local redistribution of anomalous W into secondary less resistant phases during parent body and/or nebular processing. This implies the presence of different s-nuclide carrier phases for Hf and W. Several carriers of s-process-material appear to have been selectively dissolved by our leaching protocol, while contributions from r- and p-process Hf and W carrier phases appear invariant, possibly due to the generally more labile nature of their carrier phases during solar nebula and/or parent body processing. [ABSTRACT FROM AUTHOR]