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NASA NTRS2011

Spatially Resolved, In Situ Carbon Isotope Analysis of Archean Organic Matter

Spatiotemporal variability in the carbon isotope composition of sedimentary organic matter (OM) preserves information about the evolution of the biosphere and of the exogenic carbon cycle as a whole. Primary compositions, and imprints of the post-depositional processes that obscure them, exist at the scale of individual sedimentary grains (mm to micron). Secondary ion mass spectrometry (SIMS) (1) enables analysis at these scales and in petrographic context, (2) permits morphological and compositional characterization of the analyte and associated minerals prior to isotopic analysis, and (3) reveals patterns of variability homogenized by bulk techniques. Here we present new methods for in situ organic carbon isotope analysis with sub-permil precision and spatial resolution to 1 micron using SIMS, as well as new data acquired from a suite of Archean rocks. Three analytical protocols were developed for the CAMECA ims1280 at WiscSIMS to analyze domains of varying size and carbon concentration. Average reproducibility (at 2SD) using a 6 micron spot size with two Faraday cup detectors was 0.4 %, and 0.8 % for analyses using 1 micron and 3 micron spot sizes with a Faraday cup (for C-12) and an electron multiplier (for C-13). Eight coals, two ambers, a shungite, and a graphite were evaluated for micron-scale isotopic heterogeneity, and LCNN anthracite (delta C-13 = -23.56 +/- 0.1 %, 2SD) was chosen as the working standard. Correlation between instrumental bias and H/C was observed and calibrated for each analytical session using organic materials with H/C between 0.1 and 1.5 (atomic), allowing a correction based upon a C-13H/C-13 measurement included in every analysis. Matrix effects of variable C/SiO2 were evaluated by measuring mm to sub-micron graphite domains in quartzite from Bogala mine, Sri Lanka. Apparent instrumental bias and C-12 count rate are correlated in this case, but this may be related to a crystal orientation effect in graphite. Analyses of amorphous Archean OM suggest that instrumental bias is consistent for 12C count rates as low as 10% relative to anthracite. Samples from the ABDP-9 (n=3; Mount McRae Shale, approximately 2.5 Ga), RHDH2a (n=2; Carrawine Dolomite and Jeerinah Fm, approximately 2.6 Ga), WRL1 (n=3; Wittenoom Fm, Marra Mamba Iron Formation, and Jeerinah Fm, approximately 2.6 Ga), and SV1 (n=1; Tumbiana Fm, approximately 2.7 Ga) drill cores, each previously analyzed for bulk organic carbon isotope composition, yielded 100 new, in situ data from Neoarchean sedimentary OM. In these samples, delta C-13 varies between -53.1 and -28.3 % and offsets between in situ and bulk compositions range from -8.3 to 18.8%. In some cases, isotopic composition and mode of occurrence (e.g. morphology and mineral associations) are statistically correlated, enabling the identification of distinct reservoirs of OM. Our results support previous evidence for gradients of oxidation with depth in Neoarchean environments driven by photosynthesis and methane metabolism. The relevance of these findings to questions of bio- and syngenicity as well as the alteration history of previously reported Archean OM will be discussed.

Williford, Kenneth H.↗

NASA NTRS2015

Centimeter to Decimeter Size Spherical and Cylindrical Features in Gale Crater Sediments

The Curiosity rover traverse in Gale crater has explored a large series of sedimentary deposits in an ancient lake on Mars. Over the nine kilometers of traverse a recurrent observation has been southward-dipping sedimentary strata, from Shaler at the edge of Yellowknife Bay to the striated units near the Kimberley. Within the sedimentary strata cm- to decimeter- size hollow spheroidal objects and some apparent cylindrical objects have been observed. These features have not been seen by previous landed missions. The first of these were observed on sol 122 in the Gillespie Lake member at Yellowknife Bay. Additional hollow features were observed in the Point Lake outcrop in the same area. More recently a spherical and apparently hollow object, Winnipesaukee, was observed by ChemCam and Mastcam on sol 653. Here we describe the settings, morphology, and associated compositions, and we discuss possible origins of these objects.

Wiens, R. C.↗

NASA NTRS2015

Constraining the Texture and Composition of Pore-Filling Cements at Gale Crater, Mars

The Mars Science Laboratory (MSL) rover Curiosity has encountered a wide variety of sedimentary rocks deposited in fluvio-lacuestrine sequences at the base of Gale Crater. The presence of sedimentary rocks requires that initial sediments underwent diagenesis and were lithified. Lithification involves sediment compaction, cementation, and re-crystallization (or authigenic) processes. Analysis of the texture and composition of the cement can reveal the environmental conditions when the cements were deposited, enabling better understanding of early environments present within Gale Crater. The first step in lithification is sediment compaction. The Gale crater sediments do not show evidence for extensive compaction prior to cementation; the Sheepbed mudstone in Yellowknife Bay (YKB) has preserved void spaces ("hollow nodules"), indicating that sediments were cemented around the hollow prior to compaction, and conglomerates show imbrication, indicating minimal grain reorganization prior to lithification. Furthermore, assuming the maximum burial depth of these sediments is equivalent to the depth of Gale Crater, the sediments were never under more than 1 kb of pressure, and assuming a 15 C/km thermal gradient in the late Noachian, the maximum temperature of diagenesis would have been approximately 75 C. This is comparable to shallow burial diagenetic conditions on Earth. The cementation and recrystallization components of lithification are closely intertwined. Cementation describes the precipitation of minerals between grains from pore fluids, and recrystallization (or authigenesis) is when the original sedimentary mineral grains are altered into secondary minerals. The presence of authigenic smectites and magnetite in the YKB formation suggests that some recrystallization has taken place. The relatively high percentage of XRD-amorphous material (25-40%) detected by CheMin suggests that this recrystallization may be limited in scope, and therefore may not contribute significantly to the cementing material. However, relatively persistent amorphous components could exist in the Martian environment (e.g. amorphous MgSO4), so recrystallization, including loss of crystallinity, cannot yet be excluded as a method of cementation. In order to describe the rock cementation, both the rock textures and their composition must be considered. Here, we attempt to summarize the current understanding of the textural and compositional aspects of the cement across the rocks analyzed by Curiosity to this point.

Siebach, K. L.↗

NASA NTRS2016

Mineralogy of Mudstone at Gale Crater, Mars: Evidence for Dynamic Lacustrine Environments

The Mars Science Laboratory Curiosity rover landed in Gale crater in August 2012 to assess the habitability of sedimentary deposits that show orbital evidence for diverse ancient aqueous environments. Gale crater contains a 5 km high mound of layered sedimentary rocks in its center, informally named Mount Sharp. The lowermost rocks of Mount Sharp contain minerals that are consistent with a dramatic climate change during Mars' early history. During the rover's traverse across the Gale crater plains to the base of Mount Sharp, Curiosity discovered sedimentary rocks consistent with a fluviolacustrine sequence. Curiosity studied ancient lacustrine deposits at Yellowknife Bay on the plains of Gale crater and continues to study ancient lacustrine deposits in the Murray formation, the lowermost unit of Mount Sharp. These investigations include drilling into the mudstone and delivering the sieved less than 150 micrometers fraction to the CheMin XRD/XRF instrument inside the rover. Rietveld refinement of XRD patterns measured by CheMin generates mineral abundances with a detection limit of 1-2 wt.% and refined unit-cell parameters of minerals present in abundances greater than approximately 5 wt.%. FULLPAT analyses of CheMin XRD patterns provide the abundance of X-ray amorphous materials and constrain the identity of these phases (e.g., opal-A vs. opal-CT). At the time of writing, CheMin has analyzed 14 samples, seven of which were drilled from lacustrine deposits. The mineralogy from CheMin, combined with in-situ geochemical measurements and sedimentological observations, suggest an evolution in the lake waters through time, including changes in pH and salinity and transitions between oxic and anoxic conditions. In addition to a geochemically dynamic lake environment, the igneous minerals discovered in the lake sediments indicate changes in source region through time, with input from mafic and silicic igneous sources. The Murray formation is predominantly comprised of lacustrine mudstone and is 150-200 m thick, suggesting long history of lake environments in Gale crater. Curiosity has traversed through the lowermost approximately 30 m of the Murray formation, and each additional sample provides clues about the climate on early Mars.

Rampe, E. B.↗

NASA NTRS2022

Calcium Isotope Constraints on Recycled Carbonates in Subduction-related Magmas

Calcium isotope ratios are readily mass-fractionated by low-temperature depositional processes that can be recorded in sedimentary rocks and, therefore, have the potential to track distinct geochemical signatures of recycled materials in mantle-derived igneous rocks. In this study, I report calcium isotopic compositions for well-characterized lavas from the Central American volcanic arc that exhibit a range of trace element and radiogenic isotope signatures that have been used to indicate variable amounts of subducted marine carbonate and hemipelagic sedimentary rocks, fresh carbonatite lavas from Oldoinyo Lengai Volcano, Tanzania, and an intrusive carbonatite clast erupted 12.8 ka from the Laacher See Volcano, Germany. I observed no calcium isotope evidence for recycled sedimentary rocks in the Central American arc magmas or in the Oldoinyo Lengai carbonatite volcanic rocks. They all exhibit isotopic compositions similar to rocks dominated by a primitive, mantle-like, bulk silicate Earth (BSE) composition. The exception in this work is the calcium isotope composition measured in the intrusive Laacher See carbonatite that is resolvable from BSE (δ^44 Ca = 0.0). Although this calcium isotopic signature might be related to ancient carbonate recycling, the magnitude and relatively light calcium isotopic composition (δ^44 Ca = –0.4) of this carbonatite could also reflect an origin that involved partial melting of altered lithospheric mantle, from which isotopically heavy Ca-bearing fluids have been lost. The decoupled signatures between trace elements and their radiogenic isotopes and those recorded by calcium isotope data are important because they likely reflect different sources and processes, and demonstrate that sediment subduction is not a bulk mixing process.

Ca isotopes↗

NASA NTRSDate not supplied

Mineralogical Trends Over the Clay-Sulfate Transition in Gale Crater from the Mars Science Laboratory CheMin Instrument

The Mars Science Laboratory Curiosity rover landed in Gale crater in 2012 to explore a sedimentary sequence in lower Aeolis Mons (informally known as Mount Sharp)that shows changes in mineralogy from orbital visible/near-infrared reflectance spectroscopy[1]. Sedimentary layers with spectral signatures of hydrated Mg sulfate overly layers with signatures of Fe/Mg smectite, a mineralogical stratigraphy that is seen in other ancient sedimentary rocks across Mars[e.g., 2-4]. Curiosity recently completed its campaign in a valley with a strong orbital signature of smectite, named Glen Torridon. Mineralogical measurements by the CheMin X-ray diffractometer(XRD), complemented by evolved gas analyses by the Sample Analysis at Mars (SAM) instrument suite, allowed the identification of abundant Fe3+-bearing dioctahedral smectite (i.e., nontronite) in Glen Torridon [5-6]. Curiosity left Glen Torridon in February 2021 and began traversing through a “clay-sulfate transition” zone on the way to the pediment and the sulfate unit[e.g., 7]. This clay-sulfate transition is defined in orbital reflectance spectroscopy as having a weak signature of hydrated Mg sulfate. Curiosity has drilled five outcrops over the traverse through the clay-sulfate transition and delivered the rock powders to CheMin for mineralogical analysis. Here, we report on the mineral assemblages of those five targets derived from CheMin XRD patterns and discuss mineralogical trends as the rover approaches the sulfate unit.

Mars↗

NASA NTRSDate not supplied

Overview and Initial Results of DIGMARS: Digging Iceland Geology for Mars Analog Research Science

Preserved in the sedimentary rocks of Mars is a rich record of ancient surface environments and burial diagenesis. Sequences of sandstones and mudstones that indicate sedimentation in deltaic and lacustrine environments have been encountered by the Curiosity rover in Gale crater and likely will be by the Perseverance rover in Jezero crater [1-3]. The compositional variability in these sedimentary rocks points to a complex diagenetic story that bears significantly on the basin history and early martian environment. Because interaction of percolating groundwaters and with unconsolidated sediments is a process commonly observed in lacustrine environments on Earth [4], groundwater has been invoked to develop a sedimentary history for Gale crater [e.g., 5-9]. Unique conceptual models, each with their own implications for the paleoenvironment and hydrologic conditions have been put forward. However, we currently lack a terrestrial reference frame for groundwater-driven diagenesis in a basalt dominated watersheds on Earth. The Digging Iceland Geology for Mars Analog Research Science (DIGMARS) project aims to close this research gap, with the goal of exploring groundwater-sediment interaction from lakes around Iceland. Here, we present the initial results for the 2021 field campaign and the laboratory analysis of aqueous and sediment samples.

M T Thorpe↗

NASA NTRSDate not supplied

The CheMin X-ray Diffractometer on MSL Curiosity: A Decade of Mineralogical Observations from Gale Crater, Mars

For more than a decade, the CheMin X-ray Diffraction instrument on the Mars Science Laboratory rover Curiosity has been returning quantitative mineralogical data from Gale crater, Mars. CheMin receives and analyzes sieved soil and powdered rock samples from Curiosity’s Sample Acquisition / Sample Processing and Handling (SA/SPaH) system. To date, 38 samples have been analyzed over the course of a 28 km transit. These samples document more than 600 vertical meters of flat-lying lacustrine, fluvial and aeolian sediments that comprise the lower part of the central mound of Gale crater (commonly called Mt. Sharp).The principal mineralogy of the sediments is basaltic, with evidence of early and late-stage diagenetic overprinting. The rocks in many cases preserve most of their primary mineralogy and sedimentary features, suggesting that they were never strongly heated or deformed. Using aeolian soil composition as a proxy for the composition of the deposited and lithified sediment, it appears that in many cases the diagenetic changes observed are principally isochemical. Exceptions to this include secondary nodules, calcium sulfate veining and rare alteration halos. A striking hematite-rich feature in lower Mt. Sharp called Vera Rubin Ridge is interpreted to be lake sediment diagenetically altered by silica-poor fluids. A surprising and as yet poorly understood observation is that nearly all of the 3.7 Gyr old sedimentary rocks analyzed to date are comprised of 25-50% X-ray amorphous material. Overall, this 600 m vertical section of sedimentary rock explored in lower Mt. Sharp documents a perennial shallow lake environment grading upward into alternating lacustrine/fluvial and aeolian environments. The mineralogical changes observed going up-section include a transition from trioctahedral to dioctahedral clay minerals and a transition from magnetite to hematite. More recently, in the last 150 m of section, CheMin has documented an overall decrease in clay minerals and increase in Fe3+ oxides and oxyhydroxides. The mineralogical changes observed in Gale crater may document the gradual drying out and oxidation of the martian hydrosphere.

CHEMIN↗

NASA NTRSDate not supplied

Investigating Physical and Chemical Weathering of Fluvial and Aeolian Sediments in Mars-Analog Environments Using Close-Up Image Analysis

Results from the NASA Curiosity rover show that the ancient (>3 Ga) sedimentary rocks in Gale crater formed by fluvial and lacustrine processes, with aeolian processes dominating the geological record after the river-lake system ended in the Hesperian. The sedimentary system in Gale crater contains a mineralogy dominated by basaltic materials, not the quartzofeldspathic minerals that derive most sedimentary rocks on the Earth. There remains a knowledge gap for understanding how basaltic materials are physically and chemically weathered in fluvial and aeolian environments. This research aims to under-stand how the physical and chemical characteristics of basaltic sediments change as they are transported from source-to-sink in Mars-analog environments utilizing close-up images and X-Ray Diffraction (XRD) analysis. These data were collected as part of the SAND-E mission.

F D Garcia Ledezma↗

NASA NTRS2024

Past Variations of Water Level of Jezero Paleolake

The western fan of Jezero crater displays features interpreted as fluvial and deltaic sedimentary rocks from orbital data. Images obtained using the SuperCam Remote Micro-Imager (RMI) and the Mastcam-Z camera provide in-situ observations of Jezero crater’s western fan in various locations along the Perseverance traverse. In the last two years, the rover analyzed the fan front from a distance using these imaging tools and at close range using its entire payload. Then, in 2023, the Perseverance rover explored the top of the western Jezero sedimentary fan. Here we show that fluvial topsets and deltaic foresets dominate sedimentary rocks. Determining the boundary between fluvial and prodelta deposits enables us to draw the evolution of the lake level through time.

Mars 2020↗

NASA NTRSDate not supplied

Assessing Potential Geophysical and Environmental Impacts from Frequent Rocket Launch Missions at Kennedy Space Center

Kennedy Space Center (KSC) in Florida has been utilized for space missions over many years with a gradually increasing number of rocket launches. There have been multiple studies where air-coupled acoustic waves and infrasound originating from launched rockets were used for operational purposes, such as locating booster trajectories as a function of changing atmospheric conditions. However, no study has utilized the acoustoelastic waves as a signal source for subsurface seismic investigations. We conducted a dispersion analysis using the seismic energy recorded from the Artemis I rocket launch at KSC in November 2022, and from these results we generated depth-sensitivity kernels at different wave frequencies. The kernels were compared with sedimentary core data to verify boundaries of carbonate layers above the Floridan Aquifer System. Accumulative information of bedrock-sediment boundary across the sedimentary platform could especially provide geo-structural evidence that manifests the configuration of coastal features. Continuous dispersion analysis of seismic recordings from consecutive rocket launches also has potential to identify non-stationary environmental effects, such as reorientation of sedimentary structures and fluctuation of the saltwater/groundwater lens from gravitational tides, which may affect erosional susceptibility of coastal features.

Han Byul Woo↗

NASA NTRSDate not supplied

Assessing Potential Geophysical and Environmental Impacts from Frequent Rocket Launch Missions at Kennedy Space Center

Rocket Launch Seismicity↗

DOE OSTI2021

Intra-Molecular Isotope Study of Light Hydrocarbons

Light hydrocarbons (C 1 -C 10 ) are the largest fraction of petroleum hydrocarbons and some of the most ubiquitous and mobile fluids within sedimentary basins. It has been increasingly recognized that hydrocarbons of varying chain-lengths can be stable even under mantle conditions and that their fluxes may play a key role in the carbon dynamics of the Earth. Major formation mechanisms of these light hydrocarbons include microbial, thermogenic, and abiogenic origins. Despite their proven utility, conventional approaches using the bulk or global stable isotopes of light hydrocarbons are often not sufficient to distinguish their sources (particularly, biogenic vs. abiogenic), maturation stages/temperatures, and migration-degradation processes. Most natural compounds, including light hydrocarbons, are composed of a set of diverse isotopic molecules that differ in the number of isotopic substitutions and/or positions of isotopic substitution within a given molecules. Many of light hydrocarbon molecules contain hydrogen and carbon in energetically non-equivalent positions: isotopomers or position-specific (intra-molecular) isotope fractionation. Position-specific isotopic compositions can differ due either to equilibrium or to path-dependent kinetic or biological processes. Thus, the position-specific isotopic fractionation between different carbon and hydrogen positions within a single molecular compound could be used regardless of their reactants and other products. We hypothesize that the formation, transport and degradation processes of light hydrocarbons in the subsurface induce and control significant, perhaps unique position-specific 13 C/ 12 C and 2 H/ 1 H isotope fractionation. In this proposal, we propose to develop a new dimension in stable isotope geochemistry of light hydrocarbons: intra-molecular isotope study of light hydrocarbons. The specific objectives of our proposal include: (a) develop robust and routine quantitative nuclear magnetic resonance (NMR) methods for high-precision/high-accuracy isotopomer analysis of propane and other light hydrocarbons (C 3 -C 10 ), (b) gain a first clear picture on position-specific δ 2 H and δ 13 C values of select light hydrocarbons of both natural and industrial sources, including samples of natural gases (C 3 and possibly C 4 -C 5 ) collected from select sedimentary basins with conventional and unconventional reservoirs, (c) acquire information on position-specific 13 C/ 12 C and 2 H/ 1 H isotope fractionation of light hydrocarbons in key natural processes (thermogenic formation and oxidative degradation) based on well-controlled laboratory experiments, and (d) establish a general framework for interpreting/modeling position-specific 13 C/ 12 C and 2 H/ 1 H isotope compositions of light hydrocarbons. Intra-molecular isotope study of light hydrocarbons is expected to open up great potentials that the bulk and position-specific isotope fractionation of light hydrocarbons, in combination with mathematical/theoretical kinetic models, could provide unprecedented wealth of information on the sources, transport, and sinks of light hydrocarbons in sedimentary basins and deep Earth.

03 NATURAL GAS↗

DOE OSTI2026

Pore-Scale Study on the Positive Feedback Between Stress and Porosity Caused by Pressure Solution in Porous Media

Pressure solution is an important process in the evolution of sedimentary rocks, which provide storage space for most of our petroleum resources. It directly influences the generation, migration, and storage of petroleum fluids in subsurface sedimentary rocks. Here, in this paper, we develop a pore-scale, mechanochemical model to demonstrate a possible positive feedback between the local porosity and pore surface stress, in which a higher local porosity causes a higher local pore surface stress, thus enhancing pressure solution and consequently further increasing the local porosity. Pore surface stress represents stress on a solid grain adjacent to a pore. Specifically, the pore-scale, mechanochemical model directly simulates the stress distribution over solid and pore surfaces using a finite element model. The dissolution of solids at the solid-pore interfaces under a far-from-equilibrium condition is simulated using a first-order kinetics model that accounts for the local stress distribution. The updated pore geometry, caused by pore surface dissolution, is then used in the stress simulation in the next numerical iteration. Two types of porous media, the Oriskany sandstone and an artificial porous medium with spherical pores, were tested in the mechanochemical simulation. The positive stress-porosity feedback during pressure solution was observed in both samples. In addition, the model quantitatively illustrated the distribution of local mineral dissolution rates on all pore surfaces, as well as its relation to the effective mineral dissolution rate of the entire sample. Based on the comparison between the two porous media, the local mineral dissolution was regulated by pore space distribution, geometry, and coalescence during pressure solution. This work is the first that uses direct, pore-scale numerical simulation to demonstrate the positive stress-porosity feedback during pressure solution, which has the potential to advance the understanding of the mechanical-chemical (MC) coupling in many geological processes that are relevant to subsurface energy systems, such as the recovery of petroleum hydrocarbons and geothermal energy.

CT scanning↗

DOE OSTI2020

Large-Scale Molecular Dynamics Simulation of the Dehydration of a Suspension of Smectite Clay Nanoparticles

Fine-grained sediments and sedimentary rocks play important roles in a variety of modern energy technologies from petroleum geology to geological carbon sequestration and radioactive waste management. However, despite their utility and ubiquity, many of their properties remain poorly understood. In particular, the ability to predict the permeability and mechanics of these media remains a persistent fundamental challenge in the geosciences. In the present work, we show how large-scale classical molecular dynamics (MD) simulations can help interpret the properties of fine-grained sedimentary material. All-atom simulations containing 30 discrete clay particles are utilized to understand the evolution of a clay nanoparticle suspension during its progressive dehydration. Microstructural (pore size distribution, tortuosity, anisotropy), thermodynamic (enthalpy and free energy of hydration, anion exclusion), mechanical (total suction), and transport properties (diffusion coefficient tensors of water and sodium) are calculated and compared to the experiment. Overall, our results provide new insight into the coupled chemistry, mechanics, and transport properties of disordered nanoparticle assemblages and shed light upon the important role of water films in controlling these properties.

02 PETROLEUM↗

DOE OSTI2025

High-resolution analysis of clay minerals and amorphous materials in martian analog environments

Mudrocks and mud-sized sediments (i.e., silt to clay) dominate the surface of Earth and Mars. These fine-grained sediments preserve a rich history of sedimentary processes from source to sink and shed light on ancient climates. However, both the physical and chemical nature of these materials make them difficult to fully characterize with traditional laboratory techniques. Here, we explore a cross-disciplinary and high-resolution approach using synchrotron radiation for X-ray diffraction, pair distribution function analysis, and submicrometer-scale X-ray fluorescence, combined with transmission electron microscopy, to better understand the nanostructure and composition of mud-sized sediments from a glacio-fluvial watershed in southwest Iceland. Our results demonstrate that sediments in the cold and wet climate of Iceland are more altered than previously thought, as evidenced by the identification of kaolinite and mixed-layer kaolinite-smectite. Additionally, sediments are enriched in amorphous materials and nanocrystalline phases, as determined from grain morphologies and compositions consistent with allophane, hisingerite, ferrihydrite, and halloysite. These alteration products are present as intimate mixtures that vary across depositional sites, demonstrating the dynamic nature of the secondary assemblage from source to sink. This work has implications for Mars, where, for example, basalt-sourced sedimentary rocks from Gale crater are abundant in clay minerals and amorphous materials. Finally, this work underpins the importance of using high-resolution techniques, a coordinated methodology, and developing innovative approaches for future planetary sample return missions (e.g., Mars sample return).

36 MATERIALS SCIENCE↗

DOE OSTI2025

Impact of Salinity on Ground Ice Distribution Across an Arctic Coastal Polygonal Tundra Environment

The heterogeneous distribution of ground ice in the Arctic is a key driver of uneven ground subsidence as permafrost thaws, significantly impacting infrastructure and surface/subsurface hydrology. These topographic and hydrological changes contribute to major uncertainties in energy and carbon fluxes and storage in a warming Arctic. This study aims to improve our understanding of the controls on ground ice and organic matter distribution within the top 3 m of permafrost in coastal polygonal tundra near Utqiagvik, Alaska. To this end, we apply a neural network approach to bulk density distributions derived from nondestructive X-ray tomography of soil cores, trained with laboratory analyses, to improve the resolution and spatial coverage of estimates of dry bulk density, ice content, and organic matter content. In addition, we use capacitively coupled geophysical imaging to map soil electrical conductivity and salinity variations. The results show that sedimentary deposits from ocean transgressions, along with subsequent ice wedge polygon geomorphological processes, jointly influence the distribution of ice content at various scales. The impact of the latter decreases with depth, whereas the influence of salinity and sedimentary history increases. Although the controls on the distribution of soil organic matter content (g/cm 3 ) remain unclear, the pronounced heterogeneity in bulk density strongly influences its calculation from laboratory mass fraction measurements (g/g). From a methodological perspective, the interdependencies among soil components and the need for increased data coverage underscore the value of high-resolution density measurements, such as using X-ray tomography. Overall, this study emphasizes the importance of considering salinity constraints on ice content distribution in coastal permafrost regions. The results are expected to aid in the development of data products and process representations in geomorphological and ecosystem models.

Dafflon, Baptiste [Lawrence Berkeley National Labo↗

DOE OSTI2020

Shifting modes of iron sulfidization at the onset of OAE-2 drive regional shifts in pyrite δ 34 S records

We report total reduced inorganic S isotope ratios (δ 34 S CRS ) shift toward more negative values across much of the southern North Atlantic just before the onset of the Cenomanian-Turonian Ocean Anoxic Event (OAE-2). At the same time, there is no parallel isotopic change in the significantly larger pool of kerogen (organic) S, which indicates that the distribution and S-isotope composition of sulfide in the environment likely did not drive the change in δ 34 S CRS . Here, we investigate possible explanations for the negative shift in δ 34 S CRS values and their divergence from organic S by isolating iron sulfides for morphological identification and grain-specific isotopic analysis using secondary ion mass spectrometry (SIMS). In pre- and syn-OAE-2 sedimentary rocks from Demerara Rise, we find four distinct morphologies of iron sulfides: pyrite framboids (1–20 μm diameter), irregular pyrite aggregates (1–38 μm diameter), large cemented pyrite aggregates (~60 μm diameter), and irregular and cemented aggregates of the pyrite polymorph marcasite (1–45 μm diameter). These different textural groups have distinct S-isotopic compositions that are largely consistent through the onset of OAE-2. As such, the secular change in bulk δ 34 S CRS values likely reflects the changing proportions of these phases stratigraphically across OAE-2. All textural groups feature resolvable intra-grain δ 34 S variability, suggesting that the environments in which they formed were characterized by dynamic sulfide δ 34 S values and/or by partial closed-system distillation. We use grain-specific δ 34 S distributions to rule out shoaling of the chemocline within the sediments as a mechanism for the observed decrease in δ 34 S CRS . Instead, we propose that changes in the reactivity of the iron species delivered to Demerara Rise over the ~200 kyr leading up to the onset of OAE-2 impacted the relative contributions of pyrite with S-isotope signatures reflecting the water column, shallow sediments, and deeper sediments to the bulk sedimentary δ 34 S CRS value. Specifically, the change in iron reactivity at the onset of OAE-2 favored the production of 34 S-depleted large, cemented aggregates and framboids at the expense of more 34 S-enriched irregular aggregates. Our results underscore that bulk δ 34 S CRS measurements integrate multiple reduced phases that form via distinct reaction mechanisms and potentially in different parts of the depositional environment. Grain-specific SIMS analyses dramatically enrich our ability to interpret pyrite isotopic patterns in the geologic record.

58 GEOSCIENCES↗