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Discussion of laboratory simulations that are important to organic geochemistry in that they provide direct evidence relating to geochemical cycles involving carbon. Reviewed processes and experiments include reactions occurring in the geosphere, particularly, short-term diagenesis of biolipids and organochlorine pesticides in estuarine muds, as well as maturation of organic matter in ancient sediments.
This was a major equipment grant that provided funds ($72K) for purchase of a benchtop gas chromatograph-mass spectrometer (GC-MS) for use in experimental studies of prebiotic organic compounds. An Agilent model 689015973 GC-MS was purchased and installed in the PI's lab in August of 2003. The instrument is now being used for a variety of research projects. The primary use of the instrument is to analyze and quantify organic products of laboratory experiments conducted by the PI. One example is shown, which shows organic products (predominantly n-alkanes) formed during Fischer-Tropsch-type abiotic synthesis under hydrothermal conditions. The analytical capabilities of the GC- MS allowed identification of the numerous organic products of this as well as other laboratory experiments. A key use of the instrument in this research is that the mass spectrometer capabilities allow use of isotopically labeled reactants to trace the progress of reactions and evaluate background contaminants. collaborative projects with other scientists involved in exobiology & astrobiology research (e.g., Mitch Schulte, NASA Ames; Katrina Edwards, Woods Hole Oceanographic Institution). For instance, an analysis of membrane lipids of an lithoautotrophic iron-oxidizing bacteria being grown on basalt as a source of metabolic energy, a project where the instrument is being used to evaluate possible biomarker compounds from these organisms is shown. These iron oxidizers are thought to be similar to those living within the ocean crust, and are being investigated as possible analog organisms to those on the early Earth or crust of Mars. The instrument has also been used by an outside investigator (graduate student Brandon Canfeld, Arizona State University) for identification and isotopic characterization of experimental products of abiotic organic synthesis experiments he is conducting with Dr. John Holloway. analysis of quality control samples for other NASA-funded projects. For instance, an analysis of residual hydrocarbon contaminants on the internal surface of the shell of an atmospheric sounding rocket is shown. This analysis was used to help determine the source of the contaminating compounds. In the future, the instrument will continue to be used for quality control analysis in clean rooms and instrument construction facilities within the Laboratory for Atmospheric and Space Physics, where the GC-MS is housed.
To better understand geochemical processes occurring on Europa's seafloor, we investigated the effects of varying Fe?content in the seafloor rock and varying temperature. Iron is important in such geochemical processes as the production of methane through serpentinization (e.g. Allen and Seyfried, 2003) and can be a nutrient for microbes (Russell and Hall, 2006; Park and Kim, 2001). It can also offer clues as to the state of differentiation of Europa's core/mantle. If Europa is fully differentiated and contains an iron core, we would expect there to be little iron in the mantle and ocean floor whereas a homogeneous Europa would have iron evenly dispersed throughout the ocean floor. Furthermore, the composition of the ocean is a result of water?rock interactions at the seafloor. This project investigated the effects of temperature on geochemical processes, comparing high temperature (> 250oC) hydrothermal vents (Kelley et al., 2001) to lower temperature (~20oC) cold seeps (e.g. Orphan et al., 2002).
The fundamental goal of our research is to understand the origin and evolution of the solar system, particularly the terrestrial, "rocky" bodies. Our research involves analysis of, and experiments on, astromaterials in order to understand their nature, sources, and processes of formation. Our state-of-the-art analytical laboratories include four electron microbeam laboratories for mineral analysis, four spectroscopy laboratories for chemical and mineralogical analysis, and four mass spectrometry laboratories for isotopic analysis. Other facilities include the experimental impact laboratory and both 1-atm gas mixing and high-pressure experimental petrology laboratories. Recent research has emphasized a diverse range of topics, including: Study of the solar system's primitive materials, such as carbonaceous chondrites and interplanetary dust; Study of early solar system chronology using short-lived radioisotopes and early nebular processes through detailed geochemical and isotopic characterizations; Study of large-scale planetary differentiation and evolution via siderophile and incompatible trace element partitioning, magma ocean crystallization simulations, and isotopic systematics; Study of the petrogenesis of Martian meteorites through petrographic, isotopic, chemical, and experimental melting and crystallization studies; Interpretation of remote sensing data, especially from current robotic lunar and Mars missions, and study of terrestrial analog materials; Study of the role of organic geochemical processes in the evolution of astromaterials and the extent to which they constrain the potential for habitability and the origin of life.
We have experimentally investigated metal segregation at slow strain rates. Liquid metal pore pressure remains high during deformation and migration is by fracture. Within a crystalline mush silicate melt may migrate preferentially to metallic liquid. Additional information is contained in the original extended abstract.
We have experimentally investigated liquid metal segregation from a solid silicate matrix under conditions of applied stress. Liquid moves in fractures and formation of fayalitic olivine from orthopyroxene by migrating Fe-Ni-S-O liquids is observed. Additional information is contained in the original extended abstract.
The salt fraction in permafrost soils/sediments of the McMurdo Dry Valleys (MDV) of Antarctica can be used as a proxy for cold desert geochemical processes and paleoclimate reconstruction. Previous analyses of the salt fraction in MDV permafrost soils have largely been conducted in coastal regions where permafrost soils are variably affected by aqueous processes and mixed inputs from marine and stratospheric sources. We expand upon this work by evaluating permafrost soil/sediments in University Valley, located in the ultraxerous zone where both liquid water transport and marine influences are minimal. We determined the abundances of Cl(-), NO3(-, ClO4(-)and ClO3(-)in dry and ice-cemented soil/sediments, snow and glacier ice, and also characterized Cl(-) and NO3(-) isotopically. The data are not consistent with salt deposition in a sublimation till, nor with nuclear weapon testing fall-out, and instead point to a dominantly stratospheric source and to varying degrees of post depositional transformation depending on the substrate, from minimal alteration in bare soils to significant alteration (photodegradation and/or volatilization) in snow and glacier ice. Ionic abundances in the dry permafrost layer indicate limited vertical transport under the current climate conditions, likely due to percolation of snowmelt. Subtle changes in ClO4(-)/NO3(-) ratios and NO3(-) isotopic composition with depth and location may reflect both transport related fractionation and depositional history. Low molar ratios of ClO3(-)/ClO4(-) in surface soils compared to deposition and other arid systems suggest significant post depositional loss of ClO3(-), possibly due to reduction by iron minerals, which may have important implications for oxy-chlorine species on Mars. Salt accumulation varies with distance along the valley and apparent accumulation times based on multiple methods range from approximately 10 to 30 kyr near the glacier to 70-200 kyr near the valley mouth. The relatively young age of the salts and relatively low and homogeneous anion concentrations in the ice-cemented sediments point to either a mechanism of recent salt removal, or to relatively modern permafrost soils (less than 1 million years). Together, our results show that near surface salts in University Valley serve as an end-member of stratospheric sources not subject to biological processes or extensive remobilization.
The Joint Global Ocean Flux Study (JGOFS), currently being organized under the auspices of the Scientific Committee for Ocean Research (SCOR), is intended to be a decade long internationally coordinated program. The main goal of JGOFS is to determine and understand on a global scale the processes controlling the time-varying fluxes of carbon and associated biogenic elements in the ocean and to evaluate the related exchanges with the atmosphere, sea floor and continental boundaries. 'A long-term goal of JGOFS will be to establish strategies for observing, on long time scales, changes in ocean biogeochemical cycles in relation to climate change'. Participation from a large number of U.S. and foreign institutions is expected. JGOFS investigators have begun a set of time-series measurements and global surveys of a wide variety of biological, chemical and physical quantities, detailed process-oriented studies, satellite observations of ocean color and wind stress and modeling of the bio-geochemical processes. These experiments will generate data in amounts unprecedented in the biological and chemical communities; rapid and effortless exchange of these data will be important to the success of JGOFS.
Ophiolite sequences, sections of lower oceanic crust and upper mantle that have been thrust onto continental craton, are located in northern and central California and provide easily accessible areas that serve as good analogs for similar, more extensive areas of the early Earth. We have begun investigating and characterizing these sites in order to understand better the processes that may be responsible for the water chemistry, mineralogy and biology of similar environments on the early Earth. The geophysical and geochemical processes in these terranes provide niches for unique communities of extremeophiles and likely provide a good analog to the location that first gave rise to life on Earth. The ophiolites found in northern and central California include the Trinity, Josephine, Coast Range and Point Sal, all of which are approximately 160 million years old. Fluids from serpentinizing springs are generally alkaline with high pH and H2 contents, indicating that the mafic rock compositions control the fluid composition through water-rock reactions during relatively low-grade hydrothermal processes. There are significant amounts of primary mineralogy remaining in the rocks, meaning that substantial alteration processes are still occurring in these terranes. The general reaction for serpentinization of olivine is given by one of the authors. olivine + H2O = serpentine + brucite + magnetite + H2. We have analyzed the mineralogical composition of several rock samples collected from the Coast Range Ophiolite near Clear Lake, CA by electron microprobe. The remnant primary mineralogy is fairly urnform in composition, with an olivine composition of Fo(sub 90), and with pyroxene compositions of En(sub 90) for orthopyroxene and En(sub 49)Wo(sub 48)Fs(sub 03) for the clinopyroxene. Other primary phases observed include chromites and other spinels. Examination of petrographic thin sections reveals that serpentinization reactions have occurred in these locations. The serpentine resulting from aqueous alteration of olivine resides in veins that are see to cross cut the primary mineral grains. There are several generations of alteration products, comprised mostly of serpentines that are magnesium rich, with magnetite, brucite and carbonates observed as accessory minerals. The formation of carbonates can be taken to indicate the presence of CO2 in the altering fluids. We collected samples from a spring in the Coast Range Ophiolite in order to determine whether the geochemical environment serves as a habitat for chemotrophic microorganisms. DNA was extracted from the sediment samples and the 16s rRNA gene was PCR amplified using universal Archaeal primers. Denaturing gradient gel electrophoresis (DGGE) was used to determine the community of Archaea thriving in these samples. Our results indicate that there were 8 different genera of Archaea from a single sample. A sequence was obtained from one of these eight. The sequence is of an organism similar to Halorubrum tibetense, and alkalophilic Archaeon. This result suggests that these environments are likely hosts for communities of organisms that are adapted for the unique chemistry provided by the alkaline spring.
Hydrothermal systems on Earth are active centers in the crust where organic molecules can be synthesized biotically or abiotically under a wide range of physical and chemical conditions [1-3]. Not only are volatile species (CO, CO2, H2, and hydrocarbons) a reflection of deep-seated hydrothermal alteration processes, but they also form an important component of biological systems. Studying carbon-bearing fluids from hydrothermal systems is of specific importance to understanding (bio-)geochemical processes within these systems. With recent detection of methane in the martian atmosphere [4-7] and the possibility of its hydrothermal origin [8, 9], understanding the formation mechanisms of methane may provide constraints on the history of the martian aqueous environments and climate.
Earth, Mars, and Venus, irradiated by an evolving Sun, have had fascinating but diverging histories of habitability. Although only Earth’s surface is considered to be habitable today, all three planets might have simultaneously been habitable early in their histories to microbial life. We consider how physical processes that have operated similarly or differently on these planets determined the creation and evolution of their atmospheres and surfaces over time. These include the geophysical and geochemical processes that determined the style of their interior dynamics and the presence or absence of a magnetic field; the surface-atmosphere exchange processes that acted as a source or sink for atmospheric mass and composition; the Sun-planet interactions that controlled escape of gases to space; and the atmospheric processes that interacted with these to determine climate and habitability. The divergent evolutions of the three planets provide an invaluable context for thinking about the search for life outside the Solar System.
This research developed and applied high-precision analytical methods (electron microprobe) to determine the major- and minor-element abundances (Si, Ti, A], Cr, Fe, Mn, Mg, Ca, Na, K) in three suites of Apollo 14 volcanic green glasses. Since the precision of these data was a factor of 5-10 better than previously published results, the data provided the strongest constraints yet achieved on the geochemical processes that operated at depths less than 400 kilometers inside the Moon. The results of this work were submitted to the 29th Lunar and Planetary Science Conference, formed the basis for a Master's Thesis, and were published in the top-tier geochemical journal. Additional high-precision data on the trace abundances of sodium (Na), sulfur (S), and potassium (K) in the Apollo 17 volcanic orange glasses (74220) were also acquired during this grant-period. These data show diffusion profiles within individual 200-micron diameter, glass spherules that were apparently generated during the fire-fountain eruption of this magma in the presence of a transient vapor phase. Although these results have not yet been published, publication is planned in 2001 after additional numerical modeling has been completed. This work has also catalyzed on-going collaborative work with Professor Timothy Grove (MIT) to analyze and understand the origin of the Apollo 15 volcanic green glasses. That work will be completed for publication in 2001.
The presence of dark lithic clasts within meteorites can provide information concerning asteroidal regolith processes, the extent of interactions between asteroids, and the relationship between meteorite types, micrometeorites, and interplanetary dust particles. Accordingly, we have been seeking and characterizing dark clasts found within carbonaceous chondrites, unequilibrated ordinary chondrites, howardites, and eucrites. We find that unequilibrated chondrites in this study contain fine-grained, anhydrous unequilibrated inclusions, while the howardites often contain inclusions from geochemically processed, hydrous asteroids (type 1 and 2 carbonaceous chondrites). Eucrites and howardities contain unusual clasts, not easily classified.
Diffusion results from random motion of particles and entities. Diffusion in melts and magmas is due to thermally excited random motion of atoms, ions, and clusters, and plays a critical role in magmatic and volcanic processes. In melts and magmas, diffusion is one of the two mechanisms of mass transfer; the other being bulk flow (referred to as convection or advection). When both are present, diffusion refers to the dispersive motion relative to the mean bulk flow in a given reference frame (Richter et al. 1998). Diffusion plays critical roles in controlling magma mixing (Watson 1982; Koyaguchi 1985, 1989; Lesher 1994; Huber et al. 2009; Guo and Zhang 2020), mineral growth and dissolution rates in magmas (e.g., Watson 1982; Harrison and Watson 1983; Zhang et al. 1989; Newcombe et al. 2014; Macris et al. 2018), bubble growth and dissolution rate in magmas (Sparks 1978; Proussevitch and Sahagian 1998; Liu and Zhang 2000; Zhang 2013), and elemental and isotope fractionation during mineral 2 growth and dissolution (Jambon 1980; Richter et al. 1999, 2003; Watson and Muller 2009; Chopra et al. 2012; Watkins et al. 2014, 2017; Holycross et al. 2016, 2018). As a result, diffusion also plays an essential role in explosive volcanic eruptions and magma crystallization. Furthermore, diffusion has important applications in geospeedometry (Lasaga 1983, 1998; Zhang 1994, 2008; Trail et al. 2016; Zhang and Xu 2016). Experimental investigation of diffusion in geologically relevant silicate melts began to flourish in the 1970’s when micro-analytical measurements of diffusion profiles became available. In addition to the vast number of papers published since then, numerous books and reviews are available for diffusion in silicate melts. Hofmann et al. (1974) edited a book titled “Geochemical Transport and Kinetics” published by Carnegie Institution of Washington. This was the first landmark book summarizing the field. Lasaga and Kirkpatrick (1981) edited a book “Kinetics of Geochemical Processes” as volume 8 of the Reviews in Mineralogy (later becoming Reviews in Mineralogy and Geochemistry) series. Zhang and Cherniak (2010) edited “Diffusion in Minerals and Melts” as volume 72 of Reviews of Mineralogy and Geochemistry series, in which one chapter focused on diffusion theory, five chapters on diffusion in silicate melts (Behrens 2010; Lesher 2010; Liang 2010; Zhang and Ni 2010; Zhang et al. 2010), and other chapters were on experimental, analytical, and computational methods, and diffusion in minerals. Several textbooks covered the principles and applications of diffusion theories (Kirkaldy and Young 1987; Shewmon 1989; Cussler 1997; Lasaga 1998; Zhang 2008; Vrentas and Vrentas 2016), and two classic books covered the mathematics of diffusion (Carslaw and Jaeger 1959; Crank 1975). In preparing for this review chapter, we thought carefully about what to cover for this vast field, and decided to briefly go through the fundamentals of diffusion (more complete review can be found in Chakraborty 1995; Zhang 2008, 2010) and solutions to often-encountered 3 diffusion problems, and then focus on post-2010 diffusion studies on silicate melts and magmas. Here, melts refer to (mostly natural) silicate liquid, and magmas refer to crystal-bearing and/or bubble-bearing melts in which the continuous phase is the melt. There is a large body of work on diffusion in glasses, especially in the materials science literature, which is not covered in this review.
Biospheric, hydrospheric, lithospheric and atmospheric evolution on primitive earth, discussing secular accretion and biological and geochemical processes effect on volatile envelope
Apollo 11 lunar rock and soil elemental abundances, discussing composition, volatile element depletion, rare earths, basalt and geochemical processes
A technique has been developed to artificially fossilize microscopic algae in crystalline silica under conditions of moderately elevated temperature and pressure. The technique is designed to simulate geochemical processes thought to have resulted in the preservation of organic microfossils in Precambrian bedded cherts. In degree of preservation and mineralogic setting, the artificially permineralized microorganisms are comparable to naturally occurring fossil algae.
Computer simulations of the evolution of the earth's atmospheric composition and surface temperature have been carried out. The program took into account changes in the solar luminosity, variations in the earth's albedo, the greenhouse effect, variation in the biomass, and a variety of geochemical processes. Results indicate that prior to two billion years ago the earth had a partially reduced atmosphere, which included N2, CO2, reduced carbon compounds, some NH3, but no free H2. Surface temperatures were higher than now, due to a large greenhouse effect. When free O2 appeared the temperature fell sharply. Had earth been only slightly further from the sun, runaway glaciation would have occurred at that time. Simulations also indicate that a runaway greenhouse would have occurred early in earth's history had earth been only a few percent closer to the sun. It therefore appears that, taking into account the possibilities of either runaway glaciation or a runaway greenhouse effect, the continuously habitable zone about a solar-type star is rather narrow, extending only from roughly 0.95 to 1.01 AU.