Coupled W–Os–Pt isotope systematics in IVB iron meteorites: In situ neutron dosimetry for W isotope chronology

Tungsten isotope compositions of magmatic iron meteorites yield ages of differentiation that are within ±2 Ma of the formation of CAIs, with the exception of IVB irons that plot to systematically less radiogenic compositions yielding erroneously old ages. Secondary neutron capture due to galactic cosmic ray (GCR) irradiation is known to lower the ε182W of iron meteorites, adequate correction of which requires a measure of neutron dosage which has not been available, thus far. The W, Os and Pt isotope systematics of 12 of the 13 known IVB iron meteorites were determined by MC-ICP-MS (W, Os, Pt) and TIMS (Os). On the same dissolutions that yield precise ε182W, stable Os and Pt isotopes were determined as in situ neutron dosimeters for empirical correction of the ubiquitous cosmic-ray induced burn-out of 182W in iron meteorites. The W isotope data reveal a main cluster with ε182W of ∼−3.6, but a much larger range than observed in previous studies including irons (Weaver Mountains and Warburton Range) that show essentially no cosmogenic effect on their ε182W. The IVB data exhibits resolvable negative anomalies in ε189Os (−0.6ε) and complementary ε190Os anomalies (+0.4ε) in Tlacotepec due to neutron capture on 189Os which has approximately the same neutron capture cross section as 182W, and captures neutrons to produce 190Os. The least irradiated IVB iron, Warburton Range, has ε189Os and ε190Os identical to terrestrial values. Similarly, Pt isotopes, which are presented as ε192Pt, ε194Pt and ε196Pt range from +4.4ε to +53ε, +1.54ε to −0.32ε and +0.73ε to −0.20ε, respectively, also identify Tlacotepec and Dumont as the most GCR-damaged samples. In W–Os and W–Pt isotope space, the correlated isotope data back-project toward a 0-epsilon value of ε192Pt, ε189Os and ε190Os from which a pre-GCR irradiation ε182W of −3.42±0.09 (2σ) is derived. This pre-GCR irradiation ε182W is within uncertainty of the currently accepted CAI initial ε182W. The Pt and Os isotope correlations in the IVB irons are in good agreement with a nuclear model for spherical irons undergoing GCR spallation, although this model over-predicts the change of ε182W by ∼2×, indicating a need for better W neutron capture cross section determinations. A nucleosynthetic effect in ε184W in these irons of −0.14±0.08 is confirmed, consistent with the presence of Mo and Ru isotope anomalies in IVB irons. The lack of a non-GCR Os isotope anomaly in these irons requires more complex explanations for the production of W, Ru and Mo anomalies than nebular heterogeneity in the distribution of s-process to r-process nuclides.

Neutron capture on Pt isotopes in iron meteorites and the Hf–W chronology of core formation in planetesimals

The short-lived 182Hf–182W isotope system can provide powerful constraints on the timescales of planetary core formation, but its application to iron meteorites is hampered by neutron capture reactions on W isotopes resulting from exposure to galactic cosmic rays. Here we show that Pt isotopes in magmatic iron meteorites are also affected by capture of (epi)thermal neutrons and that the Pt isotope variations are correlated with variations in 182W/184W. This makes Pt isotopes a sensitive neutron dosimeter for correcting cosmic ray-induced W isotope shifts. The pre-exposure 182W/184W derived from the Pt–W isotope correlations of the IID, IVA and IVB iron meteorites are higher than most previous estimates and are more radiogenic than the initial 182W/184W of Ca–Al-rich inclusions (CAI). The Hf–W model ages for core formation range from +1.6±1.0 million years (Ma; for the IVA irons) to +2.7±1.3 Ma after CAI formation (for the IID irons), indicating that there was a time gap of at least ∼1 Ma between CAI formation and metal segregation in the parent bodies of some iron meteorites. From the Hf–W ages a time limit of <1.5–2 Ma after CAI formation can be inferred for the accretion of the IID, IVA and IVB iron meteorite parent bodies, consistent with earlier conclusions that the accretion of differentiated planetesimals predated that of most chondrite parent bodies.

Cosmogenic 180W variations in meteorites and re-assessment of a possible 184Os–180W decay system

We measured tungsten (W) isotopes in 23 iron meteorites and the metal phase of the CB chondrite Gujba in order to ascertain if there is evidence for a large-scale nucleosynthetic heterogeneity in the p-process isotope 180W in the solar nebula as recently suggested by Schulz et al. (2013). We observed large excesses in 180W (up to ≈ 6 ε) in some irons. However, significant within-group variations in magmatic IIAB and IVB irons are not consistent with a nucleosynthetic origin, and the collateral effects on 180W from an s-deficit in IVB irons cannot explain the total variation. We present a new model for the combined effects of spallation and neutron capture reactions on 180W in iron meteorites and show that at least some of the observed within-group variability is explained by cosmic ray effects. Neutron capture causes burnout of 180W, whereas spallation reactions lead to positive shifts in 180W. These effects depend on the target composition and cosmic-ray exposure duration; spallation effects increase with Re/W and Os/W ratios in the target and with exposure age. The correlation of 180W/184W with Os/W ratios in iron meteorites results in part from spallogenic production of 180W rather than from 184Os decay, contrary to a recent study by Peters et al. (2014). Residual ε180W excesses after correction for an s-deficit and for cosmic ray effects may be due to ingrowth of 180W from 184Os decay, but the magnitude of this ingrowth is at least a factor of ≈2 smaller than previously suggested. These much smaller effects strongly limit the applicability of the putative 184Os-180W system to investigate geological problems.

Thermal and collisional history of Tishomingo iron meteorite: More evidence for early disruption of differentiated planetesimals

Tishomingo is a chemically and structurally unique iron with 32.5 wt.% Ni that contains 20% residual taenite and 80% martensite plates, which formed on cooling to between -75 and -200 °C, probably the lowest temperature recorded by any meteorite. Our studies using transmission (TEM) and scanning electron microscopy (SEM), X-ray microanalysis (AEM) and electron backscatter diffraction (EBSD) show that martensite plates in Tishomingo formed in a single crystal of taenite and decomposed during reheating forming 10-100 nm taenite particles with ∼50 wt.% Ni, kamacite with ∼4 wt.%Ni, along with martensite or taenite with 32 wt.% Ni. EBSD data and experimental constraints show that Tishomingo was reheated to 320-400 °C for about a year transforming some martensite to kamacite and to taenite particles and some martensite directly to taenite without composition change. Fizzy-textured intergrowths of troilite, kamacite with 2.7 wt.% Ni and 2.6 wt.% Co, and taenite with 56 wt.% Ni and 0.15 wt.% Co formed by localized shock melting. A single impact probably melted the sub-mm sulfides, formed stishovite, and reheated and decomposed the martensite plates. Tishomingo and its near-twin Willow Grove, which has 28 wt.% Ni, differ from IAB-related irons like Santa Catharina and San Cristobal that contain 25-36 wt.% Ni, as they are highly depleted in moderately volatile siderophiles and enriched in Ir and other refractory elements. Tishomingo and Willow Grove therefore resemble IVB irons but are chemically distinct. The absence of cloudy taenite in these two irons shows that they cooled through 250 °C abnormally fast at >0.01 °C/yr. Thus this grouplet, like the IVA and IVB irons, suffered an early impact that disrupted their parent body when it was still hot. Our noble gas data show that Tishomingo was excavated from its parent body about 100 to 200 Myr ago and exposed to cosmic rays as a meteoroid with a radius of ∼50-85 cm.

Cosmic-ray exposure ages of pallasites

We analyzed cosmogenic nuclides in metal and/or silicate (primarily olivine) separated from the main-group pallasites Admire, Ahumada, Albin, Brahin, Brenham, Esquel, Finmarken, Glorieta Mountain, Huckitta, Imilac, Krasnojarsk, Marjalahti, Molong, Seymchan, South Bend, Springwater, and Thiel Mountains and from Eagle Station. The metal separates contained an olivine fraction which although small, <1 wt% in most cases, nonetheless contributes significantly to the budgets of some nuclides (e.g., up to 35% for Ne-21 and Al-26). A correction for olivine is therefore essential and was made using model calculations and/or empirical relations for the production rates of cosmogenic nuclides in iron meteoroids and/or measured elemental concentrations. Cosmic-ray exposure (CRE) ages for the metal phases of the main-group pallasites range from 7 to 180 Ma, but many of the ages cluster around a central peak near 100 Ma. These CRE ages suggest that the parent body of the main-group pallasites underwent a major break-up that produced most of the meteorites analyzed. The CRE age distribution for the pallasites overlaps only a small fraction of the distribution for the IIIAB iron meteorites. Most pallasites and IIIAB irons originated in different collisions, probably on different parent bodies; a few IIIABs and pallasites may have come out of the same collision but a firm conclusion requires further study. CRE ages calculated from noble gas and radionuclide data of the metal fraction are higher on average than the Ne-21 exposure ages obtained for the olivine samples. As the metal and olivine fractions were taken in most cases from different specimens, the depth-dependency of the production rate ratio Be-10/Ne-21 in metal, not accounted for in our calculations, may explain the difference.

Palladium Isotopic Evidence for Nucleosynthetic and Cosmogenic Isotope Anomalies in IVB Iron Meteorites

The origin of ubiquitous nucleosynthetic isotope anomalies in meteorites may represent spatial and/or temporal heterogeneity in the sources that supplied material to the nascent solar nebula, or enhancement by chemical processing. For elements beyond the Fe peak, deficits in s-process isotopes have been reported in some (e.g., Mo, Ru, W) but not all refractory elements studied (e.g., Os) that, among the iron meteorites, are most pronounced in IVB iron meteorites. Palladium is a non-refractory element in the same mass region as Mo and Ru. In this study, we report the first precise Pd isotopic abundances from IVB irons to test the mechanisms proposed for the origin of isotope anomalies. First, this study determined the existence of a cosmogenic neutron dosimeter from the reaction 103Rh(n, beta-)104Pd in the form of excess 104Pd, correlated with excess 192Pt, in IVB irons. Second, all IVB irons show a deficit of the s-process only isotope 104Pd (\varepsilon 104Pd = -0.48 ± 0.24), an excess of the r-only isotope 110Pd (\varepsilon 110Pd = +0.46 ± 0.12), and no resolvable anomaly in the p-process 102Pd (\varepsilon 102Pd = +1 ± 1). The magnitude of the Pd isotope anomaly is about half that predicted from a uniform depletion of the s-process yields from the correlated isotope anomalies of refractory Mo and Ru. The discrepancy is best understood as the result of nebular processing of the less refractory Pd, implying that all the observed nucleosynthetic anomalies in meteorites are likely to be isotopic relicts. The Mo-Ru-Pd isotope systematics do not support enhanced rates of the 22Ne(alpha,n)25Mg neutron source for the solar system s-process.