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Supernova graphite in the NanoSIMS: Carbon, oxygen and titanium isotopic compositions of a spherule and its TiC sub-components
Authors:FJ Stadermann  TK Croat  S Amari  RM Walker  E Zinner
Institution:a Laboratory for Space Sciences and Physics Department, Washington University, St. Louis, MO 63130-4899, USA
Abstract:Presolar graphite spherules from the Murchison low-density separate KE3 contain a large number of internal TiC crystals that range in size from 15 to 500 nm. We have studied one such graphite grain in great detail by successive analyses with SEM, ims3f SIMS, TEM and NanoSIMS. Isotopic measurements of the ‘bulk’ particle in the ims3f indicate a supernova origin for this graphite spherule. The NanoSIMS measurements of C, N, O and Ti isotopes were performed directly on TEM ultramicrotome sections of the spherule, allowing correlated studies of the isotopic and mineralogical properties of the graphite grain and its internal crystals. We found isotopic gradients in 12C/13C and 16O/18O from the core of the graphite spherule to its perimeter, with the most anomalous compositions being present in the center. These gradients may be the result of isotopic exchange with isotopically normal material, either in the laboratory or during the particle’s history. No similar isotopic gradients were found in the 16O/17O and 14N/15N ratios, which are normal within analytical uncertainty throughout the graphite spherule. Due to an unusually high O signal, internal TiC crystals were easily located during NanoSIMS imaging measurements. It was thus possible to determine isotopic compositions of several internal TiC grains independent of the surrounding graphite matrix. These TiC crystals are significantly more anomalous in their O isotopes than the graphite, with 16O/18O ratios ranging from 14 to 250 (compared to a terrestrial value of 499). Even the most centrally located TiC grains show significant variations in their O isotopic compositions from crystal to crystal. Measurement of the Ti isotopes in three TiC grains found no variations among them and no large differences between the compositions of the different crystals and the ‘bulk’ graphite spherule. However, the same three TiC crystals vary by a factor of 3 in their 16O/18O ratios. It is not clear in what form the O is associated with the TiC grains and whether it is cogenetic or the result of surface reactions on the TiC grains before they accreted onto the growing graphite spherule. The presence of 44Ca from short-lived 44Ti (t1/2 = 60y) in one of the TiC subgrains confirms the identification of this graphite spherule as a supernova condensate.
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