abstract: The search for life on Mars is a major NASA priority. A Mars Sample Return (MSR) mission, Mars 2020, will be NASA's next step towards this goal, carrying an instrument suite that can identify samples containing potential biosignatures. Those samples will be later returned to Earth for detailed analysis. This dissertation is intended to inform strategies for fossil biosignature detection in Mars analog samples targeted for their high biosignature preservation potential (BPP) using in situ rover-based instruments. In chapter 2, I assessed the diagenesis and BPP of one relevant analog habitable Martian environment: a playa evaporite sequence within the Verde Formation, Arizona. Coupling outcrop-scale observations with laboratory analyses, results revealed four diagenetic pathways, each with distinct impacts on BPP. When MSR occurs, the sample mass returned will be restricted, highlighting the importance of developing instruments that can select the most promising samples for MSR. Raman spectroscopy is one favored technique for this purpose. Three Raman instruments will be sent onboard two upcoming Mars rover missions for the first time. In chapters 3-4, I investigated the challenges of Raman to identify samples for MSR. I examined two Raman systems, each optimized in a different way to mitigate a major problem commonly suffered by Raman instruments: background fluorescence. In Chapter 3, I focused on visible laser excitation wavelength (532 nm) gated (or time-resolved Raman, TRR) spectroscopy. Results showed occasional improvement over conventional Raman for mitigating fluorescence in samples. It was hypothesized that results were wavelength-dependent and that greater fluorescence reduction was possible with UV laser excitation. In Chapter 4, I tested this hypothesis with a time-resolved UV (266 nm) gated Raman and UV fluorescence spectroscopy capability. I acquired Raman and fluorescence data sets on samples and showed that the UV system enabled identifications of minerals and biosignatures in samples with high confidence. The results obtained in this dissertation may inform approaches for MSR by: (1) refining models for biosignature preservation in habitable Mars environments; (2) improving sample selection and caching strategies, which may increase the success of Earth-based biogenicity studies; and (3) informing the development of Raman instruments for upcoming rover-based missions. / Dissertation/Thesis / Doctoral Dissertation Geological Sciences 2016

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This Ph.D. thesis was focused on the application of Raman spectroscopy as the main analytical method for the characterization of neo-formed minerals, notably sulfates, from burning coal waste dumps. This environment associated with subsurface fires gives rise to a variety of uncommon and rare minerals. The specific features of these minerals (metastability, hygroscopy, mixed aggregates) causes that the mineralogical investigation is a challenging task using traditional laboratory-based techniques. Advantages such as the non-destructive nature, the sensitivity to the changes in the hydration degree of sulfates, little or none pretreatment, and the option of measurements directly in the field were the main reasons for applying this spectroscopy method. The scarce availability of spectroscopic data of most gas-vent minerals can be considered as the disadvantage. Therefore, artificial prepared samples of six anhydrous sulfates, which are rarely found in nature, were analyzed by Raman laboratory spectroscopy and a miniature a Raman spectrometer, and specific Raman features as well the differences with hydrated counterparts are shown. Laboratory investigation of two natural hydrated aluminum sulfates, alunogen and khademite, were carried out using Raman spectroscopy and other methods in order to obtain...

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