We have conducted laboratory experiments with analog crystalline silicon carbide (SiC) grains using transmission electron microscopy (TEM) and electron energy-loss spectroscopy (EELS). The 3C polytype of SiC was used—the type commonly produced in the envelopes of asymptotic giant branch (AGB) stars. We rapidly heated small (∼50 nm) synthetic SiC crystals under vacuum to ∼1300 K and bombarded them with 150 keV Xe ions. TEM imaging and EELS spectroscopic mapping show that such heating and bombardment leaches silicon from the SiC surface, creating layered graphitic sheets. Surface defects in the crystals were found to distort the six-membered rings characteristic of graphite, creating hemispherical structures with diameters matching that of C60. Such
nonplanar features require the formation of five-membered rings. We also identified a circumstellar grain, preserved inside the Murchison meteorite, that contains the remnant of an SiC core almost fully encased by graphite, contradicting long-standing thermodynamic predictions of material condensation. Our combined laboratory data suggest that C60 can undergo facile formation from shock heating and ion bombardment of circumstellar SiC grains. Such heating/bombardment could occur in the protoplanetary nebula phase, accounting for the observation of C60 in these objects, in planetary nebulae (PNs) and other interstellar sources receiving PN ejecta. The synthesis of C60 in astronomical sources poses challenges, as the assembly of 60 pure carbon atoms in an H-rich environment is difficult. The formation of C60 from the surface decomposition of SiC grains is a viable mechanism that could readily occur in the heterogeneous, hydrogen-dominated gas of evolved circumstellar shells.
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Destructive Processing of Silicon Carbide Grains: Experimental Insights into the Formation of Interstellar Fullerenes and Carbon Nanotubes
The detection of the fullerenes C60 and C70 in the interstellar medium (ISM) has transformed our understanding of chemical complexity in space. These discoveries also raise the possibility for the presence of even larger molecules in astrophysical environments. Here we report in situ heating of analog silicon carbide (SiC) presolar grains using transmission electron microscopy (TEM). These heating experiments are designed to simulate the temperature conditions occurring in post-AGB stellar envelopes. Our experimental findings reveal that heating the analog SiC grains to the point of decomposition initially yields hemispherical C60-sized nanostructures, with five- and six-membered rings, which transform into multiwalled carbon nanotubes (MWCNTs) if held isothermally >2 min. These MWCNTs are certainly larger than any of the currently observed interstellar fullerene species, both in overall size and number of C atoms. These experimental simulations suggest that such MWCNTs are likely to form in post-AGB circumstellar material, where the structures, along with the smaller fullerenes, are subsequently injected into the ISM.
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- NSF-PAR ID:
- 10349998
- Date Published:
- Journal Name:
- The Journal of Physical Chemistry A
- ISSN:
- 1089-5639
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract Our detailed mineralogical, elemental, and isotopic study of the Miller Range (MIL) 07687 meteorite showed that, although this meteorite has affinities to CO chondrites, it also exhibits sufficient differences to warrant classification as an ungrouped carbonaceous chondrite. The most notable feature of MIL 07687 is the presence of two distinct matrix lithologies that result from highly localized aqueous alteration. One of these lithologies is Fe‐rich and exhibits evidence for interaction with water, including the presence of fibrous (dendritic) ferrihydrite. The other lithology, which is Fe‐poor, appears to represent relatively unaltered protolith material. MIL 07687 has presolar grain abundances consistent with those observed in other modestly altered carbonaceous chondrites: the overall abundance of O‐rich presolar grains is 137 ± 3 ppm and the overall abundance of SiC grains is 71 ± 11 ppm. However, there is a large difference in the observed O‐rich and SiC grain number densities between altered and unaltered areas, reflecting partial destruction of presolar grains (both O‐ and C‐rich grains) due to the aqueous alteration experienced by MIL 07687 under highly oxidizing conditions. Detailed coordinated NanoSIMS‐TEM analysis of a large hotspot composed of an isotopically normal core surrounded by a rim composed of17O‐rich grains is consistent with either original condensation of the core and surrounding grains in the same parent AGB star, or with grain accretion in the ISM or solar nebula.
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ABSTRACT The detection of the 11.3$\, {\rm \mu m}$ emission feature characteristic of the Si–C stretch in carbon-rich evolved stars reveals that silicon carbide (SiC) dust grains are condensed in the outflows of carbon stars. SiC dust could be a significant constituent of interstellar dust since it is generally believed that carbon stars inject a considerable amount of dust into the interstellar medium (ISM). The presence of SiC dust in the ISM is also supported by the identification of pre-solar SiC grains of stellar origin in primitive meteorites. However, the 11.3$\,\mu {\rm m}$ absorption feature of SiC has never been seen in the ISM, and oxidative destruction of SiC is often invoked. In this work, we quantitatively explore the destruction of interstellar SiC dust through oxidation based on molecular dynamics simulations and density functional theory calculations. We find that the reaction of an oxygen atom with SiC molecules and clusters is exothermic and could cause CO-loss. Nevertheless, even if this is extrapolable to bulk SiC dust, the destruction rate of SiC dust through oxidation could still be considerably smaller than the (currently believed) injection rate from carbon stars. Therefore, the lack of the 11.3$\,\mu{\rm m}$ absorption feature of SiC dust in the ISM remains a mystery. A possible solution may lie in the currently believed stellar injection rate of SiC (which may have been overestimated) and/or the size of SiC dust (which may actually be considerably smaller than submicron in size).more » « less
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1021/acs.jpca.2c01441
