Browsing by Author "Gill, Benjamin C."

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    Aspects of Cyclic Sedimentation in the Upper Mississippian, Mauch Chunk Group, southern West Virginia and southwest Virginia
    Buller, Ty Bradford (Virginia Tech, 2014-05-27)
    Late Mississippian, Mauch Chunk Group strata constitute a westward-thinning clastic wedge of strata up to 1000m thick that developed in the Central Appalachian Basin over a ~ 7 million year time interval. Included within the Mauch Chunk Group are multiple incised-valley fills and a distinctive prodeltaic succession of laminated sandstones and mudstones. Calculated estimates of drainage basin areas for incised-valley fills in the Mauch Chunk Group range from > 1,000,000 km2 for the Stony Gap Sandstone to < 100,000 km2 for the Princeton Formation. Drainage area estimates are consistent with detrital zircon geochronology and petrographic data and suggest that the Stony Gap and Ravencliff incised-valley fills were derived from distal, northern and northwestern cratonic sources that dispersed sediment into NE-SW-oriented, longitudinal incised-valley drainages and that the Princeton Formation was derived from proximal tectonic highland sources along the eastern margin of the Appalachian Basin which dispersed sediment into a transverse incised-valley. The Pride Shale overlies the Princeton incised valley fill and records a hierarchy of tidal periodicities is preserved in the Pride Shale. Microlaminated, semi-diurnal sandstone-siltstone/shale couplets record the dominant ebb tide of the day. Up to 17 semi-diurnal couplets are stacked into neap-spring (fortnightly) tidal cycles. Neap-spring cycles are arranged in thickening and thinning that record seasonal cycles driven by the annual monsoon. Total organic carbon (TOC) values are a proxy for annual climatic cycles. TOC contents are higher within intermonsoonal and lower within monsoonal components of annual cycles reflecting, respectively, lesser and greater dilution by terrestrial flux.
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    Atmosphere-ocean oxygen and productivity dynamics during the Cambrian explosion
    Dahl, Tais W.; Connelly, James N.; Li, Da; Kouchinsky, Artem; Gill, Benjamin C.; Porter, Susannah M.; Maloof, Adam C.; Bizzarro, Martin (2019-08-21)
    Large, motile animals proliferated during the Cambrian explosion,540–515 million years ago,and this period has been associated with both rising and declining O2levels on Earth [1–3]. To explore this conundrum, we reconstructed the global extent of seafloor oxygenation at ~sub-million year resolution based on U isotope compositions in 187 marine limestone samples from China, Siberia and Morocco,and coupled this record to simulations of atmospheric O2 levels using a mass balance model constrained by carbon, sulfur and strontium isotopes in the same rocks.The studied samples were investigated petrographically and geochemically to disentangle isotope fractionation processes occurring locally during diagenesis from secular changes in open seawater. We find that Sr/Ca, Mg/Ca and G18O help discriminate carbonate samples with a larger G238U offset from contemporaneous seawater, and decipher the signal that can be ascribed to global changes in the oceanic U pool. Our data demonstrate two significant expansions of seafloor anoxia in the aftermath of an interval with declining atmospheric pO2levels.The combination of atmospheric and oceanic O2records offers a self-consistent and highly dynamic picture of atmosphere-ocean oxygenation in which the evolving animal ecosystems might have both responded and contributed to global environmental change.Animals diversified possibly by a predator-prey arms race peaking in two pulses interrupted by these dramatic fluctuations in seafloor anoxia. When O2levels again rose, it occurred in concert with predicted high rates of photosynthetic production, both of which may have fueled more energy to predators and their armored prey in the evolving marine ecosystem.
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    Atmosphere–ocean oxygen and productivity dynamics during early animal radiations
    Dahl, Tais W.; Connelly, James N.; Li, Da; Kouchinsky, Artem; Gill, Benjamin C.; Porter, Susannah M.; Maloof, Adam C.; Bizzarro, Martin (National Academy of Sciences, 2019-09-24)
    The proliferation of large, motile animals 540 to 520 Ma has been linked to both rising and declining O₂ levels on Earth. To explore this conundrum, we reconstruct the global extent of seafloor oxygenation at approximately submillion-year resolution based on uranium isotope compositions of 187 marine carbonates samples from China, Siberia, and Morocco, and simulate O₂ levels in the atmosphere and surface oceans using a mass balance model constrained by carbon, sulfur, and strontium isotopes in the same sedimentary successions. Our results point to a dynamically viable and highly variable state of atmosphere–ocean oxygenation with 2 massive expansions of seafloor anoxia in the aftermath of a prolonged interval of declining atmospheric pO₂ levels. Although animals began diversifying beforehand, there were relatively few new appearances during these dramatic fluctuations in seafloor oxygenation. When O₂ levels again rose, it occurred in concert with predicted high rates of photosynthetic production, both of which may have fueled more energy to predators and their armored prey in the evolving marine ecosystem.
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    Basin Evolution and Slope System Dynamics of the Cretaceous Magallanes Basin, Chilean Patagonia
    Auchter, Neal C. (Virginia Tech, 2016-12-20)
    Deep-marine basins linked to active continental margins by sloped ocean-floor profiles commonlyhost the final accumulation of sediment that was eroded and transported from the continents. Thedeep-marine sediment archives preserved in these settings commonly offer the most completerecord of sediment transfer from continents to ocean basins over geologic time scales. This isespecially true in basins associated with regions of active tectonism, where loss or alteration ofsediment source terrains leave submarine basin deposits as the only record of the tectonic and cli-matic forcings that govern the transfer of sediment to the deep basin. The overarching goal of thisdissertation is to evaluate controls on submarine slope and basin-floor sedimentation that considersboth large-scale system drivers and the internal complexities and autogenic processes associatedwith sediment routing systems. In pursuit of this goal, the research presented in this dissertationspans a range of spatial and temporal scales. At the largest scale, the influence of sediment recy-cling is addressed to evaluate how changes in intrabasinal sediment sources reflect phases of basinevolution and what influence recycling of previously deposited basin sediments has on the fidelityof the deep-marine sedimentary record at geologic time scales. At the smaller scale, analysis ofsedimentation units and characterization of sedimentary bodies form the foundation for linkingthe stratigraphic preservation of depositional processes to discrete submarine geomorphic condi-tions. Such a linkage can provide insight into changes in slope gradient and the transition fromsediment transport and bypass to sediment deposition along the slope profile. Thirdly, a detailedinvestigation of deformed slope deposits addresses how depositional processes and stratigraphicstacking of submarine fan deposits influences slope stability. Synthesis across these broad spatialand temporal scales required integration of various tools and data types including: (1) detailedoutcrop measurements, (2) cliff-face correlation and characterization of depositional architecture,(3) geologic mapping, (4) basin-scale correlation, (5) detrital geochronology, and (6) carbonategeochemistry.
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    Biogeochemical Cycling and Paleoenvironmental Reconstructions of the Toarcian Oceanic Anoxic Event from Western North America
    Them II, Theodore Roland (Virginia Tech, 2016-08-02)
    The Toarcian Oceanic Anoxic Event (T-OAE; ~183 million years ago) represents an interval during the Mesozoic when the emplacement of the Karoo-Ferrar Large Igneous Province (LIP) is thought to have resulted in significant environmental change. Associated with this interval was the widespread deposition of organic-rich sediments, carbon cycle and seawater chemistry changes, global warming, the development of marine anoxia, and major extinction events. The majority of studies of this event that have documented these responses have come from the Boreal and Tethyan regions of Europe, thus casting some doubt to the regional versus global significance of the event. Thus my dissertation has sought to reconstruct biogeochemical and paleoenvironmental changes across the T-OAE from a sedimentary succession that was deposited on the margins of a different ocean basin away from the well-studied European successions. Specifically, I have studied the chemostratigraphy of the Fernie Formation of the Western Canada Sedimentary Basin (WCSB), which was deposited on the eastern margin of the Panthalassa Ocean. The Toarcian carbon isotope excursions (CIEs) in the WCSB confirm that these features are global phenomena. I have suggested a new driver for small-scale CIEs observed during the event: the release of wetland-derived methane during progressive global warming. The osmium isotope record and numerical modeling of the osmium cycle suggests that continental weathering rates increased during the T-OAE by 230 – 540%. Rhenium abundance data also suggests that the increased geographic extent of marine anoxia during the T-OAE caused a global drawdown in the seawater rhenium inventory. Iron speciation data are used to reconstruct redox conditions within the WCSB, which suggest ferruginous conditions developed in the more distal locations at the onset of the T-OAE before returning to euxinic (anoxic and sulfidic) conditions. This is likely related to enhanced pyrite burial on a global scale, which caused the drawdown of the seawater sulfate inventory, thus limiting pyrite formation in the distal locations. The proximal setting remained euxinic across the T-OAE, and in all locations the iron speciation data suggest anoxic conditions persistent well after the interval that has been traditionally called the end of the T-OAE.
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    Carbon cycle changes during the end-Marjuman (Cambrian) extinction in the Southern Appalachians
    Gerhardt, Angela Mae (Virginia Tech, 2014-05-16)
    The late Cambrian-early Ordovician transition contains several trilobite extinctions. The first of these extinctions (the end-Marjuman) is thought to coincide with the Steptoean Positive Carbon Isotope Excursion or SPICE, a large and rapid excursion in the marine carbon isotope record. This excursion, which is expressed in sedimentary successions globally, is thought to represent a large perturbation to the carbon cycle during this time. Additionally, a limited amount of carbon isotope data from the Deadwood Formation in the Black Hills of South Dakota suggests the possibility of a small negative ẟ¹³C excursion near the extinction and preceding the SPICE. Previous high-resolution biostratigraphy has identified an expanded record of extinction event within the Nolichucky Formation of the Southern Appalachians making it an excellent candidate for the study of the precise relationship between the extinction and changes in the carbon cycle. This investigation confirms the onset of the SPICE occurs at the extinction boundary however no negative ẟ¹³C excursion occurs at the extinction boundary. Further there is no systematic relationship between local facies changes and ẟ¹³C or the extinction interval across the basin, which suggests that global environmental changes were responsible for both the ẟ¹³C record and the extinction event.
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    Catchment Structure Regulates Hydrodynamic Drivers of Chemical Weathering in Shallow Forest Soils
    Pennino, Amanda (Virginia Tech, 2023-06-12)
    Determining where, when, and how subsurface flow affects soil processes and the resulting arrangement of soil development along flow paths is challenging. While hydrologic regime and soil solution acidity are known to influence weathering rates and soil transformation processes, an integrated understanding of these factors together is still lacking. This dissertation explores the effects of subsurface flow on the mobility and distribution of dissolved organic carbon (DOC) and base cations to explain spatial patterns in chemical weathering in a forested headwater catchment. In the first chapter, relationships between hydrologic behavior, fluxes of weathered elements, and the extent of soil elemental loss across landscape positions are established. The second chapter investigates what specific groundwater behavior best explains spatial patterns in solution DOC concentrations during storm events. Lastly, in the third chapter, near surface saturation dynamics are examined to determine when and where DOC mobilization might be enhanced by subsurface flow. Results show that weathering extent was greatest in the upper reaches of the catchment, where O horizon saturation frequency and DOC concentrations are highest. Annual base cation fluxes, which were also greatest in these positions, could indicate where weathering is likely still enhanced. Additionally, while O horizon saturation occurred across the catchment, spatial differences in DOC concentrations suggest there are other sources of acidity to groundwater solutions other than just leaching from O horizons. Shallow organic soils, near bedrock outcrops at the top of the catchment is likely this additional C source, in which drainage water is transported downslope to nearby mineral soils when water tables are high and hydrologic connectivity between soils is increased. Spring and fall storm events were identified as times when groundwater most frequently reached O horizons during the snow-free year, providing insight into the timing of these processes throughout the year. This dissertation highlights how catchment structure mediates DOC flushing events, which in turn, influences the spatial architecture of soil development and chemical weathering processes across the landscape.
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    Cenozoic Variations in the Deep Western Boundary Current as Recorded in the Seismic Stratigraphy of Contourite Drifts, Newfoundland Ridge, Offshore Canada
    Boyle, Patrick Ryan (Virginia Tech, 2014-06-03)
    A contourite drift complex on the J-Anomaly Ridge (JAR) and Southeast Newfoundland Ridge (SENR), offshore eastern Canada, records an extensive archive of North Atlantic circulatory and sedimentary dynamics formed under the influence of the Deep Western Boundary Current (DWBC). Seismic-reflection profiles constrained by drill sites from IODP Expedition 342 are used to map the spatial and temporal distribution of contourite sedimentation and to evaluate the Cenozoic history of the DWBC within a preexisting climatic framework. This study indicates three phases of sedimentation termed here Pre-Contourite-Drift Phase (~115-50 Ma), Active-Contourite-Drift Phase (~50-2.6 Ma), and Post-Contourite-Drift Phase (~2.6-0 Ma). Bottom current controlled sedimentation began at the boundary between Pre-Contourite-Drift Phase and Active-Contourite-Drift Phase (~50 Ma), and correlates to a long-term global cooling trend that initiated at the end of the Early Eocene Climatic Optimum. Within the Active-Contourite-Drift Phase at ~30 Ma depocenters shifted deeper and current energy and focus is interpreted to have increased in association with global oceanographic change at the Eocene-Oligocene transition. The beginning of Post-Contourite-Drift Phase sedimentation (~2.6 Ma) marks a shift in bottom current path towards shallower water depths, and corresponds with the onset of Northern Hemisphere ice sheets. These events of circulatory reorganization correlate with other North Atlantic seismic stratigraphic studies, suggesting that these events occurred throughout the North Atlantic. An improved understanding of long-term (>1000000 yr) dynamics of North Atlantic circulation in response to significant reorganization of Cenozoic climate provides important context towards refining models and prediction of oceanic response to contemporary climate change.
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    Chemical Controls on the Formation of Amorphous and Crystalline Calcium Phosphates
    Hoeher, Alexandria Janson (Virginia Tech, 2020-08-26)
    Transformation of amorphous calcium phosphate (ACP) and brushite into hydroxylapatite, an important biomineral, has been documented. The relationships between synthesis conditions and the formation and transformation of these phases are not comprehensively understood. The metastable nature of ACP has made it historically challenging to investigate, and many analyses attempt to stabilize the phase through drying or including additional ions or proteins in the reaction. In situ investigations provide an incisive approach to examining the structure and transformation of ACP and brushite as a function of synthesis conditions. The first project develops a new method for in situ analyses of the structure of ACP and brushite shortly after reagent mixing, without chemical stabilization. This method was used in the second project to examine how the initial Ca/P affects ACP structure and transformation. Our results identify the first structural differences in types of ACP, controlled by the initial Ca/P. At ratio 0.2 the Ca – P bonding geometry is primarily monodentate, ratio 5.0 produces a coordination that is primarily bidentate, and there is a mix of monodentate and bidentate coordinates at intermediate ratios between the two. These results are independent of system pH between the examined range of 6-11. Further ex situ transformation experiments identified that at ratio 0.2, ACP transformed directly into hydroxylapatite, but at higher ratios the transformation product is brushite. This is a promising mechanism for direct ACP to hydroxylapatite conversion at a biologically relevant pH. In the final project, the statistically significant synthesis parameters (age, pH, temperature, supersaturation, and initial ion ratio) for ACP, brushite, and hydroxylapatite formation are evaluated. Binary logistic regression analysis and nonlinear continuous logistic regression analysis are applied to a dataset compiled from the literature. Equations were developed that predict the percentage of ACP and brushite that will form. The equations and significant variables seem to depend on the transformation pathway of brushite and ACP. The current analysis did not comprehensively describe hydroxylapatite formation when trying to concurrently evaluate the ACP to hydroxylapatite and brushite to hydroxylapatite pathways. Taken together, these studies provide new ways to study and interpret calcium phosphate phases as they form and transform. Experiments identified new relationships between the chemistry and structure of ACP. The new in situ experimental method and the equations we developed can be used to improve future experimental designs towards a comprehensive understanding of the calcium phosphate system.
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    Contributions to Exceptional Fossil Preservation
    Muscente, Anthony Drew (Virginia Tech, 2016-04-21)
    Exceptionally preserved fossils—or fossils preserved with remains of originally non-biomineralized (i.e. soft) tissues—constitute a key resource for investigating the history of the biosphere. In comparison to fossils of biomineralized skeletal elements, which represent the majority of the fossil record but only a fraction of the total diversity that existed in the past, exceptionally preserved fossils are comparatively rare because soft tissues are rapidly destroyed in typical depositional environments. Assemblages of such fossils, nonetheless, have received special attention among scientists in multiple fields of Earth and life sciences because they represent relatively 'complete' windows to past life. Through such windows, researchers are able to reconstruct original biological features (e.g. soft tissue anatomies) of extinct organisms and to describe the structures and compositions of ancient soft-bodied paleocommunities. To accomplish these goals, however, researchers must incorporate background information regarding the pre- and post-burial histories of exceptionally preserved fossils. In this context, my dissertation focuses on the environmental settings, diagenetic conditions, geomicrobiological activities, and weathering processes, which influence the conservation of original biological features within exceptionally preserved fossils and control their occurrences in time and space. An improved understanding of these critical factors involved in exceptional fossil preservation will ultimately our advance our knowledge regarding the history of the biosphere and the Earth system as a whole. Each chapter of original research in this dissertation includes an innovative and distinct approach for studying exceptional fossil preservation. The second chapter describes environmental and geologic overprints in the exceptional fossil record, as revealed by a comprehensive statistical meta-analysis of a global dataset of exceptionally preserved fossil assemblages. Moving from global to specimen-based perspectives, the second and third chapters focus on minerals (products of geomicrobioloigcal, diagenetic, and weathering processes) and carbonaceous materials replicating exceptionally preserved fossils. The third chapter examines the causes of preservational variations observed among organophosphatic tubular shelly Sphenothallus fossils in the lower Cambrian of South China using an experimental approach. (Although Sphenothallus is not an exceptionally preserved fossil sensu stricto, its conservation of original organic matrix tissues in South China provides key insights into the preservation of carbonaceous material within fossils.) Lastly, the fourth chapter presents data acquired using various in situ nanoscale analytical techniques to test the hypothesis that microstructures within exceptionally preserved microfossils of the Ediacaran Doushantuo Formation of South China are some of the oldest putative cylindrical siliceous demosponge spicules in the fossil record. Collectively, these chapters describe environmental, authigenic, diagenetic, and weathering processes that affect exceptional fossil preservation, and highlight innovative methods and approaches for testing major paleobiologic and geobiologic hypotheses regarding exceptionally preserved fossils.
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    Contributions to late Ediacaran geobiology in South China and southern Namibia
    Meyer, Michael B. (Virginia Tech, 2013-06-11)
    The Ediacaran, particularly the late Ediacaran-Cambrian (E-") boundary (551-541 Ma), has been noted as a major time of biological and biochemical transition, including: the rise of predators, the emergence of skeletons, the radiation of bioturbators, and large fluctuations in oceanic chemical conditions (e.g. anoxia/euxinia/ferruginia) with emerging data  suggesting that it is not until the late Ediacaran Period (551-542 Ma) when pervasive oxidation of the deep oceans occurred. In addition, the study of Ediacaran paleobiology involves numerous factors, including but not limited to, restricted amount of outcrops, taphonomic biases, metamorphism, enigmatic phylogenetic affinities, non-actualistic atmospheric and oceanic conditions, and unusual taphonomic windows, making it difficult to assign order to the myriad types of fossils (both body and trace) found during this time . It is with these problems in mind that my dissertation focuses on taphonomic questions in the late Ediacaran. We observe fossil through the taphonomic window and thereby colors all aspects of the study of that organism. By understanding how an organism was preserved we can learn about other factors affecting it, such as their taxonomic affinities, paleoecology, and morphology. All of these factors were examined through taphonomic investigations and this can be seen in the analytical path through my chapters. In chapter two I examined the preservation of trace fossils in the late Ediacaran. In chapter three I analyzed the taphonomy of an exceptionally preserved Ediacaran fossil to solve its affinity, tubular trace or tubular soft-bodied fossil. In chapter four, understanding the nature of exceptional preservation, I investigated the taphonomy of an Ediacara fossil in coarse grained sediments. In chapter five, I combined the findings of the previous chapters and applied that knowledge to analyze the in situ three dimensional morphology of an Ediacara fossil. Each of the projects presented pairs new technologic methodologies (SEM, BSE-Z, EDS, Raman, microCT) with traditional paleontological and petrologic investigations (field work, hand sample, and petrographic thin-section analysis). The result of this union of Old and New are findings that expand our understanding of these earliest multicellular organisms, their modes of life, and their biological affinities.
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    Deep-marine depositional systems of the western North Atlantic: Insights into climate and passive-margin evolution
    Parent, Andrew Michael (Virginia Tech, 2022-02-02)
    Stratigraphic successions of sedimentary rocks represent an important repository for signals pertaining to the history and evolution of Earth. Whereas the specific processes reflected by the stratigraphic record differ with respect to a given depositional environment, deposits in deep-marine settings, particularly passive margins, provide a unique, long-term record of paleoclimate, paleoceanography, and tectonics affecting the basin in question. Whereas deep-marine strata may be used to answer myriad of questions regarding the evolution and development of Earth systems, this dissertation narrowly targets two distinct aspects of sedimentation in deep-sea settings. The first two chapters focus on the utility of sortable silt in reconstructing bottom-current intensity linked to major shifts in climate. First, the relationship of sortable silt to flow velocity was tested under controlled conditions in a flow-through flume. This chapter investigates the correlation of sortable silt metrics across several experimental parameters, which is found here to dispute longstanding assumptions that multiple metrics must correlate to infer sediment sorting by deep currents. Additionally, the results are compared to calibrations from natural settings, where the correlation between the two datasets is remarkably similar, validating the relationship of sortable silt with current velocity in the deep ocean. Chapter two leverages sortable silt to investigate the long-term evolution of the Deep Western Boundary Current in the North Atlantic, targeting contourite drifts offshore Newfoundland to investigate the Eocene-Oligocene Transition (EOT), the most recent global greenhouse-to-icehouse transition. Results suggest that the Deep Western Boundary Current intensified gradually from 35-26 Ma, not abruptly at the EOT, and change consistent with deepening of the Greenland-Scotland Ridge and enhanced overflow of deep water into the North Atlantic. Chapter three utilizes detrital zircon U-Pb dating to characterize source-to-sink pathways and linkages during the rift-to-drift transition, in the Early Cretaceous, along the U.S. mid-Atlantic passive margin. This work shows that onshore and offshore system segments were initially disconnected, and progressively integrated over the course of ~45 Myr. Taken together, this work demonstrates a focused yet powerful example of how deep-marine sedimentary systems can be leveraged to robustly model major changes throughout Earth history.
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    Development of novel computational techniques for phase identification and thermodynamic modeling, and a case study of contact metamorphism in the Triassic Culpeper Basin of Virginia
    Prouty, Jonathan Michael (Virginia Tech, 2024-08-12)
    This dissertation develops computational techniques to aid in efficiently studying petrologic systems that would otherwise be challenging. It then focuses on a case study in which the transition from diagenesis to syn-magmatic heating led to a recrystallization and sulfur mobilization. A Markov-chain Montecarlo-based methodology is developed to allow for the assessment of uncertainty in calculated phase assemblage diagrams. Such phase equilibria are ubiquitous in modern petrology, but uncertainties are rarely considered. Methods are discussed for visualizing and quantifying emergent patterns as phase diagrams are re-calculated with input data modified within permitted uncertainty bounds, and these are implemented in a new code. Results show that uncertainty varies significantly across pressure-temperature space and that in some conditions, estimates of stable mineral assemblage are known with very little confidence. A Machine-Learning (ML) based methodology is developed for automatically identifying unknown phases using Electron-dispersion spectra (EDS) in concert with a Random Forest Classification algorithm. This methodology allows for phase identification that it is insensitive to overfitting and noisy spectra. However, this tool is limited by the amount of reference spectra available in the dataset on which the ML algorithm is trained. The approximately 250 EDS spectra in the current training database must be supplemented to make the tool more widely useful, though it currently has an excellent success rate for correctly identifying various sulfide and oxide minerals. An analysis of paragenesis associated with Central Atlantic Magmatic Province (CAMP) intrusions helps to better constrain the dynamics of magma emplacement, while also providing a method for estimating the amount of sedimentary sulfide-sequestered sulfur mobilized as a result of magnetite formation associated with igneous activity. This method demonstrates that dike emplacement can trigger liberation of sedimentary sulfur with no direct cooling impact on climate.
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    Devonian rise in atmospheric oxygen correlated to the radiations of terrestrial plants and large predatory fish
    Dahl, Tais W.; Hammarlund, Emma U.; Anbar, Ariel D.; Bond, David P. G.; Gill, Benjamin C.; Gordon, Gwyneth W.; Knoll, Andrew H.; Nielsen, Arne T.; Schovsbo, Niels H.; Canfield, Donald E. (National Academy of Sciences, 2010)
    The evolution of Earth's biota is intimately linked to the oxygenation of the oceans and atmosphere. We use the isotopic composition and concentration of molybdenum (Mo) in sedimentary rocks to explore this relationship. Our results indicate two episodes of global ocean oxygenation. The first coincides with the emergence of the Ediacaran fauna, including large, motile bilaterian animals, ca. 550-560 million year ago (Ma), reinforcing previous geochemical indications that Earth surface oxygenation facilitated this radiation. The second, perhaps larger, oxygenation took place around 400 Ma, well after the initial rise of animals and, therefore, suggesting that early metazoans evolved in a relatively low oxygen environment. This later oxygenation correlates with the diversification of vascular plants, which likely contributed to increased oxygenation through the enhanced burial of organic carbon in sediments. It also correlates with a pronounced radiation of large predatory fish, animals with high oxygen demand. We thereby couple the redox history of the atmosphere and oceans to major events in animal evolution.
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    Effects of acetate, propionate, and pH on volatile fatty acid thermodynamics in continuous cultures of ruminal contents
    Li, Meng M.; Ghimire, S.; Wenner, B. A.; Kohn, R. A.; Firkins, J. L.; Gill, Benjamin C.; Hanigan, Mark D. (American Dairy Science Association, 2022-11-01)
    To investigate the effects of acetate, propionate, and pH on thermodynamics of volatile fatty acids (VFA) in the rumen, a dual-flow continuous culture study was conducted to quantify production of major VFA, interconversions among the VFA, and H2 and CH4 emissions in a 4 × 4 Latin square design. The 4 treatments were (1) control: pH buffered to an average of 6.75; (2) control plus 20 mmol/d of infused acetate (InfAc); (3) control plus 7 mmol/d of infused propionate (InfPr); and (4) a 0.5-unit decline in pH elicited by adjustment of the buffer (LowpH). All fermentors were fed 40 g of a pelleted diet containing whole alfalfa pellets and concentrate mix pellets (50:50) once daily. After 7 d of treatment, sequential, continuous infusions of [2-13C] sodium acetate (3.5 mmol/d), [U-13C] sodium propionate (2.9 mmol/d), and [1-13C] sodium butyrate (0.22 mmol/d) were carried out from 12 h before feeding for 36 h. Filtered liquid effluent (4 mL) was sampled at 0, 2, 4, 6, 8, 12, 16, and 22 h after feeding, and assessed for VFA concentrations, with another filtered sample (20 mL) used to quantify aqueous concentrations of CH4 and H2. Headspace CH4 and H2 gases were monitored continuously. Ruminal microbes were isolated from the mixed effluent samples, and the microbial community structure was analyzed using the 16S rRNA amplicon sequencing technique. The digestibility of neutral detergent fiber, acid detergent fiber, and starch and microbial C sequestrated from VFA were not affected by treatments. The LowpH treatment increased net propionate production and decreased H2 and CH4 headspace emissions, primarily due to shifts in metabolic pathways of VFA formation, likely due to the observed changes in bacterial community structure. Significant interconversions occurred between acetate and butyrate, whereas interconversions of other VFA with propionate were relatively small. The InfAc and InfPr treatments increased net acetate and propionate production, respectively; however, interconversions among VFA were not affected by pH, acetate, or propionate treatments, suggesting that thermodynamics might not be a primary influencer of metabolic pathways used for VFA formation.
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    The Effects of Contact Metamorphism by Diabase Intrusion on the Carbon and Sulfur Bearing Phases in the Siltstones of the Culpeper Basin
    Tulsky, Emma Teresa Teeter (Virginia Tech, 2017-06-06)
    Many of the large igneous provinces during the Phanerozoic have been temporally linked to mass extinction events. The intrusion of magma into country rock has been hypothesized to facilitate the release of carbon and sulfur bearing volatiles and has been proposed as one of mechanisms that drove these mass extinctions. In this study I examine a dike of the Central Atlantic Magmatic Province and its interaction with adjacent sedimentary rocks in the Culpeper Basin of Virginia. Sampling was done at the 0.5 m scale along transects of sedimentary lithologies perpendicular to the ~170 m wide diabase intrusion. The observed mineralogical and geochemical changes in sedimentary rocks occur in a much narrower zone from the intrusion than predicted by the applied thermal model. Carbon isotopes of organic matter within the sedimentary rocks are enriched in 13C toward the intrusion indicating the generation of thermogenic methane within the first meter from the intrusion. Additionally, geochemical and petrologic textures suggest both the addition of magmatic sulfur into the country rock, shown through the isotopic signatures of sulfide minerals with mantle compositions. The possible thermal break down of sedimentary pyrite is evidenced by highly negative isotopic composition of sulfide minerals and general lack of pyrite. I suggest that sedimentary pyrite initially reacted to pyrrhotite, which was then converted to chalcopyrite through reactions with copper in fluids derived from the magma. These reactions also allowed for the formation of magnetite, which is elevated near the dike-sedimentary contact and at the end of the transect. A simple illustrative model of a hypothesis of fluid flow along the bed is used to explain the observed isotopic signatures and mineralogical changes along the transect. This study highlights how models for volatile generation through magma-country rock interaction may have overestimated the volatile fluxes from these environments and the roles that heterogeneity of sedimentary rocks and kinetic factors may have in the variance in these fluxes.
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    Environmental Divers of Decoupled Marine Sulfate Oxygen and Sulfur Isotope Trends during the Toarcian Oceanic Anoxic Event
    Gomes, Maya; Waldek, Anna; Gill, Benjamin C.; Johnston, David (2019-08-12)
    The Toarcian Oceanic Anoxic Event was a major carbon cycle perturbation associated with two pulses of extinction and widespread environmental change. Studies of the biogeochemical sulfur cycle provide insight into the evolution of bottom-water redox conditions, which influence elemental cycling and habitability in the ocean. In particular, a ~6‰ positive excursion in the sulfur isotope composition of marine sulfate (d34SSO4) has been interpreted to reflect enhanced pyrite burialdue to the expansion of anoxic and euxinic sedimentary environmentsand/or changes in sulfur isotope fractionation associated with sulfate reduction. Similarly, the T-OAE preservesa6‰ positive oxygen isotope (d18OSO4) excursion that precedesthe d34SSO4 excursionatMonte Sorgenza.Using these observations, wemodel the behaviour of marine sulfate reservoir using both classic box models and a new flux balance approach to address the question of expanding euxinia and the role ofbiology.This study highlights how coupled 34SSO4 andd18OSOapproaches can provide insight into environmental changes associated with major perturbations to the carbon cycle.
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    Evaluating Records of Environmental Change and Mass Extinctions during the Early Paleozoic
    McKenzie, N. R.; Gill, Benjamin C.; Wernette, S. J.; Chen, J.; Park, T. -Y.; Myrow, P. M.; Hughes, N. C. (2019-08-21)
    The interval between the Cambrian ‘explosion’ and the Great Ordovician Biodiversification Event (GOBE) is marred by biotic turmoil.Several mass extinction events have been recognized throughout the Cambrian,with multiple Furongian (late) Cambrian extinctions mostly seen within trilobite fauna of North America.These extinctions appear to correspond with episodic ocean anoxia and carbon cycle perturbations, all of which are set to the backdrop of an extensive greenhouse climate.Here we will present new chemostratigraphic and compiled biostratigraphic data from Cambrian successions of the NorthChina/Sino-Korean block(NCB). These data help identify newly recognized trilobite extinctions in upper Cambrian carbonate platform deposits of the NCB that may be correlative to North American events, demonstrating their global extent.These extinctions also correspond with marked G13Cexcursions. The cessation of these repeated extinctions coincides with global reductions in arc-volcanism and climatic cooling, implying a causal linkage between baseline climate conditions and this extensive interval of biospheric perturbations.Collectively, these data help further elucidate the harsh environmental conditions that hindered early animal evolution.
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    Evaluating redox cycling across the Toarcian Oceanic Anoxic Event with implications for paleo-environmental reconstructions and organic matter sulfurization
    Marroquin, Selva Mariana (Virginia Tech, 2020-12-09)
    Understanding oxygenation throughout Earth history, particularly intervals where marine deoxygenation occurred, are crucial to investigating the changes in habitability on Earth. Marine deoxygenation events, in particular, can result in changes in the carbon, sulfur, and iron cycles on our planet. Changes in these elemental cycles lead to distinctive variation in the chemical composition of seawater that is recorded in marine sediments that are preserved into the sedimentary record. Our modern ocean is experiencing rapid deoxygenation, thus understanding the duration and extent of ancient deoxygenation events is vital to predicting future climate scenarios. Here I investigated the record of environmental change during the Early Jurassic Toarcian Oceanic Anoxic Event or T-OAE (~183 Ma). The first chapter of this dissertation investigates the record of marine anoxia across the Pliensbachian to Toarcian transition. Specifically, I investigate the temporal and geographic development of anoxia across three basins from the European Epicontinental Seaway. Through utilization of iron speciation, a local redox proxy, I identify anoxia developing before and persisting well after the negative carbon isotope excursion (NCIE) conventionally used to define the T-OAE. These data indicate an increase in the occurrence of anoxia at the Pliensbachian – Toarcian boundary, coincident with the initial phase of volcanism associated with the Karoo-Ferrar Large Igneous Province and an interval of heightened marine invertebrate extinction. Ultimately, our data support a greater temporal extent of anoxic conditions around the T-OAE, which support the greater sensitivity of marine oxygen levels to climatic change outside of the NCIE interval. The second chapter of this dissertation assesses the occurrence and extent of organic matter sulfurization (OMS), a biogeochemical feedback known to enhance the preservation and burial of OM. Because this process is accelerated when euxinic conditions develop in the water column, I investigated it as a mechanism promoting OM burial across two oceanic anoxic events of the Mesozoic. Importantly, I find that sulfurization does not occur uniformly across both events and propose a conceptual model of the depositional settings most favorable for sulfurization to occur and when throughout geologic time OMS is most likely to influence the global cycles of carbon and sulfur.
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    Evidence for rapid weathering response to climatic warming during the Toarcian Oceanic Anoxic Event
    Them, Theodore R.; Gill, Benjamin C.; Selby, David; Gröcke, Darren R.; Friedman, Richard M.; Owens, Jeremy D. (Nature Publishing Group, 2017-07-10)
    Chemical weathering consumes atmospheric carbon dioxide through the breakdown of silicate minerals and is thought to stabilize Earth’s long-term climate. However, the potential influence of silicate weathering on atmospheric pCO2 levels on geologically short timescales (103–105 years) remains poorly constrained. Here we focus on the record of a transient interval of severe climatic warming across the Toarcian Oceanic Anoxic Event or T-OAE from an open ocean sedimentary succession from western North America. Paired osmium isotope data and numerical modelling results suggest that weathering rates may have increased by 215% and potentially up to 530% compared to the pre-event baseline, which would have resulted in the sequestration of significant amounts of atmospheric CO2. This process would have also led to increased delivery of nutrients to the oceans and lakes stimulating bioproductivity and leading to the subsequent development of shallow-water anoxia, the hallmark of the T-OAE. This enhanced bioproductivity and anoxia would have resulted in elevated rates of organic matter burial that would have acted as an additional negative feedback on atmospheric pCO2 levels. Therefore, the enhanced weathering modulated by initially increased pCO2 levels would have operated as both a direct and indirect negative feedback to end the T-OAE.