[Honolulu] : [University of Hawaii at Manoa], [December 2014]
Abstract
Ph.D. University of Hawaii at Manoa 2014.Includes bibliographical references.By studying carbonaceous chondrites, we can understand the processes that occurred in the protoplanetary disk, constrain the conditions in the solar nebula, and determine the composition and evolution of organic chemicals that led up to the origin of life on Earth. The CR chondrites contain ~ 5 wt% carbon, mainly in the form of macromolecular carbon (MMC). There are examples of petrologic type 3 (primitive) and type 1 (extensively aqueously altered) CR chondrites, which makes the CRs particularly interesting for studying the stages of aqueous alteration. The MMC has been studied using in situ electron probe micro analysis (EPMA), Raman spectroscopy, and secondary ion mass spectrometry (SIMS). EPMA mapping of the carbon Kα X-rays reveals that there are three types of carbon materials in these chondrites: high carbon phases (HCPs), matrix carbon (MC), and calcite. By Raman spectroscopy, we determine that the MC is MMC, but its spectra are unchanged by aqueous alteration. EPMA X-ray mapping suggests that the morphology of the HCPs and the spatial distribution of the MMC changes with extent of aqueous alteration. SIMS measurements have revealed that there is an isotopic difference between the HCPs and the MC in the GRO 95577 and QUE 99177 samples. HCPs have δ13C ≈ −25 ‰ and δ15N ≈ 40 ‰, and the MC have δ13C ≈ −35 ‰ and δ15N ≈ 160 ‰, relative to standard terrestrial isotope ratios. In order to produce the MC isotopic values, there must be a mix of the +δ15N and +δ13C soluble organic molecules and MMC (both present in the matrix). Therefore, the 'true' values for the MMC must be more enriched in 12C and 15N than the MC values. Results from the calcite measurements show that the production of calcite fractionates the carbon due to a combination of calcite crystallization and outgassing of CO2 on the CR parent body