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Amorphous silicates in meteoritic samples are significant as potential surviving interstellar dust from the formation of the Solar System. Amorphous silicate-rich grains called GEMS, glass with embedded metal and sulfides, are abundant in anhydrous interplanetary dust particles and some ultracarbonaceous Antarctic micrometeorites that have high presolar grain abundances. Some GEMS within these objects have been confirmed to be presolar. GEMS-like material, consisting of amorphous silicate with opaque inclusions, has been identified in the matrices of some primitive meteorites. We use specialized thin specimen preparation and transmission electron microscopy methods to compare the GEMS-like material in Paris (CM) and Acfer 094 (ungrouped) chondrites with GEMS in anhydrous, chondritic interplanetary dust particles. Specifically, we compared the amorphous silicate morphology, degree of partial ordering, elemental composition and dominant iron oxidation state. We find that the amorphous silicates in the GEMS-like materials in Paris and Acfer 094 show incipient ordering and are Fe-rich and highly oxidized, while those in GEMS are fully amorphous, Fe-poor, and anhydrous. From examination of various formation routes for the amorphous silicates, we conclude that the GEMS-like material in Paris and Acfer 094 is not GEMS and that it is unlikely that GEMS-like material accreted as primary amorphous material that retained its original amorphous structure since accretion. We also conclude that the presence of GEMS-like amorphous silicates in chondrite matrix is not a reliable indicator for high degrees of primitivity or pristinity since even mild, complex alteration processes may significantly alter silicate structure. Finally, we propose searches for presolar amorphous silicates in chondrite matrix samples that have been precharacterized by transmission electron microscopy methods to enable direct comparisons of presolar amorphous silicate abundances.

Amorphous silicates containing abundant nano-inclusions have been reported in the Paris CM chondrite (Leroux et al., 2015). They have chemical and morphological similarities to glass with embedded metal and sulfides (GEMS) found in interplanetary dust particles (IDPs) and micrometeorites believed to originate from comets. We used scanning transmission electron microscopy (STEM) with energy-dispersive X-ray spectroscopy (EDS) and nanodiffraction to study the chemistry and mineralogy of these inclusions in order to understand the origin of the GEMS-like material in Paris and its possible relationships to other materials found in primitive chondritic materials including IDP GEMS. EDS and diffraction analyses indicate compositional and mineralogical differences between the nanophase inclusions in cometary GEMS and Paris GEMS-like material. Metal inclusions are notably absent within Paris amorphous silicate. Ni-rich sulfides, including pentlandite, are common in even the least altered matrix material of Paris, while they are absent in GEMS-bearing IDPs and Ultracarbonaceous Antarctic Micrometeorites (UCAMMs). From examination of the inclusions, we cannot yet confirm or refute the possibility that GEMS-like material in Paris is related to cometary GEMS. The distinct compositions and mineralogy of the Paris material may be due to aqueous alteration of cometary GEMS precursors, but they may also denote an independent origin for meteoritic GEMS-like assemblages.

We used CHILI, the Chicago Instrument for Laser Ionization, a new resonance ionization mass spectrometer developed for isotopic analysis of small samples, to analyze strontium, zirconium, and barium isotopes in 22 presolar silicon carbide grains. Twenty of the grains showed detectable strontium and barium, but none of the grains had enough zirconium to be detected with CHILI. Nine grains were excluded from further consideration since they showed very little signals ( 87 Sr/ 86 Sr

Aside from recording stellar nucleosynthesis, a few elements in presolar grains can also provide insights into the galactic chemical evolution (GCE) of nuclides. We have studied the carbon, silicon, iron, and nickel isotopic compositions of presolar silicon carbide (SiC) grains from asymptotic giant branch (AGB) stars to better understand GCE. Since only the neutron-rich nuclides in these grains have been heavily influenced by the parent star, the neutron-poor nuclides serve as GCE proxies. Using CHILI, a new resonance ionization mass spectrometry (RIMS) instrument, we measured 74 presolar SiC grains for all iron and nickel isotopes. With the CHARISMA instrument, 13 presolar SiC grains were analyzed for iron isotopes. All grains were also measured by NanoSIMS for their carbon and silicon isotopic compositions. A comparison of the measured neutron-rich isotopes with models for AGB star nucleosynthesis shows that our measurements are consistent with AGB star predictions for low-mass stars between half-solar and solar metallicity. Furthermore, our measurements give an indication on the 22 Ne ( α ,n ) 25 Mg reaction rate. In terms of GCE, we find that the GCE-dominated iron and nickel isotope ratios, 54 Fe / 56 Fe and 60 Ni / 58 Ni , correlate with their GCE-dominated counterpart in silicon, 29 Si / 28 Si . The measured GCE trends include the Solar System composition, showing that the Solar System is not a special case. However, as seen in silicon and titanium, many presolar SiC grains are more evolved for iron and nickel than the Solar System. This confirms prior findings and agrees with observations of large stellar samples that a simple age-metallicity relationship for GCE cannot explain the composition of the solar neighborhood.

We report the carbon, silicon, iron, and nickel isotope compositions of twenty-five presolar SiC grains of mostly supernova (SN) origin. The iron and nickel isotope compositions were measured with the new Chicago Instrument for Laser Ionization, CHILI, which allows the analysis of all iron and nickel isotopes without the isobaric interferences that plagued previous measurements with the NanoSIMS. Despite terrestrial iron and nickel contamination, significant isotopic anomalies in 54 Fe/ 56 Fe, 57 Fe/ 56 Fe, 60 Ni/ 58 Ni, 61 Ni/ 58 Ni, 62 Ni/ 58 Ni, and 64 Ni/ 58 Ni were detected in nine SN grains (of type X). Combined multi-isotope data of three grains with the largest nickel isotope anomalies (>100‰ or

Pyrochlore-based ceramics are considered as a potential host to immobilize high-level nuclear waste in a geological repository. For this application it is essential to investigate the fundamental mechanism of the equilibration of pyrochlore in aqueous solutions. We treated cuboids of a synthetic crystalline and a natural metamict, i.e., self-irradiation-damaged Ti-based pyrochlore in 1 ml of a 1 M HCl solution containing 43.5% 18 O at 250 °C for 72 h. After the experiments the colours of the samples turned from black to almost white and their surfaces were covered by micron-sized crystallites. Both samples were mainly transformed into rutile with subordinate anatase and the reaction can be traced several tens of micrometers into the cuboids. In the case of the natural pyrochlore an additional phase (aeschynite [(REE)(Ti, Nb) 2 (O, OH) 2 ]) appeared as crystals on the surface and within an up to 100 μm thick layer at the interface between TiO 2 and the unreacted pyrochlore. 18 O is in both cases highly enriched in the reaction products with a sharp gradient (on a micrometer scale) to the unreacted pyrochlore. The replacement reaction retains even fine-scale morphological features typical for pseudomorphs. This observation along with the enrichment of 18 O in the product phases and the textural features clearly show that the dissolution of pyrochlore is spatially coupled with the precipitation of stable (metastable) TiO 2 phases at a moving front. During such a coupled process dissolution at the proceeding front is the rate controlling step. The aeschynite phase at the interface is thought to be either an intermediate alteration product or crystallized from a fluid which is located at the interface between the TiO 2 polymorphs and the unreacted pyrochlore due to changing transport properties between the interface and the fluid with increasing thickness of the TiO 2 rim. We emphasize here that our results produced under relatively extreme batch-experimental conditions show similarities with nature as well as with results derived from experiments conducted under moderate conditions rather expected in a nuclear repository.

Fragments in the size range from 40 μm to several hundred μm in the CI chondrites Orgueil, Ivuna, Alais, and Tonk show a wide range of chemical compositions with variations in major elements such as iron (10.4–42.4 wt% FeO), silicon (12.7–42.2 wt% SiO 2 ), and sulfur (1.01–15.8 wt% SO 3 ), but also important minor elements such as phosphorous (up to 5.2 wt% P 2 O 5 ) or calcium (up to 6.6 wt% CaO). These variations are the result of the varying mineralogical compositions of these fragments. The distribution of phyllosilicates, magnetites, and possibly ferrihydrite, in particular, control the abundances of these elements. High REE contents—up to 150 times the solar abundances—were observed in phosphates, while matrix and sulfates are REE-depleted. The studied 113 fragments were subdivided into eight lithologies with similar mineralogical and thus chemical properties. The most common is the CGA lithology, consisting of a groundmass of Mg-rich, coarse-grained phyllosilicates and varying abundances of inclusions such as magnetite. The second most abundant lithology is the FGA lithology, consisting of a groundmass of fine-grained Fe-rich phyllosilicates. A rare, but important lithology consists of fragments with high contents of phosphates and other minerals. The proposed model for the evolution of these lithologies is based on a closed system alteration, where mineralogical differences in the lithologies reflect heterogeneities in the starting material. Comparison of our results with literature data indicates a general similarity of the four CI chondrites analyzed. Further comparison of bulk analyses suggests that the mass ‘threshold’ for chemical heterogeneities in CI chondrite samples is smaller than ∼1–2 g.

The results of a detailed study on mineralogy, chemistry, and the carbon and oxygen isotopes of two exotic Krymka carbonaceous xenoliths are presented in this article. The investigated xenoliths are metamorphosed and shocked and have the following characteristics, which distinguish them from the Krymka host: 1. resemblance of their SiO2/MgO ratio to that of carbonaceous chondrites; 2. higher Fe content and FeO/(FeO + MgO) ratio; 3. lower concentration of Si, Ca, Al and an enrichment of S and probably of Ag; 4. smaller sizes and lower content (10 vol%) of chondrules and their clasts, and correspondingly higher content of matrix; 5. dominance of porphyritic chondrules and lack of nonporphyritic chondrules; 6. occurrence of an amoeboid olivine grain with 16O-rich composition; 7. existence of carbon in three different forms: graphite, carbon-rich material, and organic compounds. The bulk chemistry of the xenoliths is similar, but not identical, to that of carbonaceous chondrites, suggesting that they represent a chondrite parent body that has not been previously sampled. Among any known type of meteoritic material the mineralogy of the xenoliths corresponds only to that of other Krymka graphite-containing xenoliths. It differs, however, from the latter by having a lower grade of metamorphism. We infer that metamorphism of the primary carbonaceous body of the xenoliths and/or shock of the Krymka parent body are responsible for the major metamorphic alteration of the xenoliths, including the crystallization of graphite from primary organic compounds. A comparison of the features of the Krymka xenoliths with the inferred characteristics of cometary meteorites attests that their genetic relationship to cometary material remains highly inconclusive.

This is a report on the first comparative study of the effects of experimental and natural shock on the K-Ar system. First, mineral separates from a 451 {plus minus} 1 Ma old gneiss, experimentally shocked up to 60 GPa, were investigated by stepwise heating {sup 40}Ar-{sup 39}Ar technique. Compared with an unshocked samples, the shocked samples have lower {sup 40}Ar-{sup 39}Ar ages, and the diffusion properties have changed depending on peak shock pressure and mineralogic composition. Total resetting of the K-Ar clock did not occur. Secondly, to compare these results with the effects of natural shock, samples from the {approximately}23 Ma old Haughton impact crater, Devon Island, Canada, with different shock stages were investigated. Up to shock stage 3, no total resetting of the K-Ar clock was observed, but severe argon losses, depending on shock pressure, result in {sup 40}Ar-{sup 39}Ar plateau ages which are incorrect in terms of the true crater age, yet they provide an upper limit to the time of the cratering event.