12 research outputs found

    Anomalous fractionation of mercury isotopes in the Late Archean atmosphere

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    This work was funded by a Natural Environment Research Council (NERC) Fellowship NE/H016805/2 and Standard Grant NE/J023485/2 (to A.L.Z.). R.Y. was funded by the Chinese Academy of Sciences through the Hundred Talent Plan. G.J.I. recognizes continued support from R. Summons under the auspices of the Simons Collaboration on the Origin of Life. We thank J. Kirschvink, J. Grotzinger, A. Knoll, and the Agouron Institute for organizing and funding the Agouron Drilling Project, and the Council for Geoscience in South Africa, specifically those at the National Core Library in Donkerhoek, for facilitating access to the core materials.Earth’s surface underwent a dramatic transition ~2.3 billion years ago when atmospheric oxygen first accumulated during the Great Oxidation Event, but the detailed composition of the reducing early atmosphere is not well known. Here we develop mercury (Hg) stable isotopes as a proxy for paleoatmospheric chemistry and use Hg isotope data from 2.5 billion-year-old sedimentary rocks to examine changes in the Late Archean atmosphere immediately prior to the Great Oxidation Event. These sediments preserve evidence of strong photochemical transformations of mercury in the absence of molecular oxygen. In addition, these geochemical records combined with previously published multi-proxy data support a vital role for methane in Earth’s early atmosphere.Publisher PDFPeer reviewe

    A copper isotope investigation of methane cycling in Late Archaean sediments

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    This research was supported by NERC award NE/L002590/1 to the IAPETUS DTP, and by NERC Standard Grant NE/J023485/2 to A.L.Z. The initiation of Cu isotope analysis at the University of St Andrews was aided significantly by a Carnegie Trust Research Incentive Grant awarded to P.S.S.The rise of oxygenic photosynthesis arguably represents the most important evolutionary step in Earth history. Recent studies, however, suggest that Earth’s pre-oxidative atmosphere was also heavily influenced by biological feedbacks. Most notably, recent geochemical records propose the existence of a hydrocarbon haze which periodically formed in response to enhanced biospheric methane fluxes. Copper isotopes provide a potential proxy for biological methane cycling; Cu is a bioessential trace metal and a key element in the aerobic oxidation of methane to carbon dioxide (methanotrophy). In addition, Cu isotopes are fractionated during biological uptake. Here, we present a high-resolution Cu isotope record measured in a suite of shales and carbonates from core GKF01, through the ~2.6–2.5 Ga Campbellrand-Malmani carbonate platform. Our data show a 0.85‰ range in Cu isotope composition and a negative excursion that predates the onset of a haze event. We interpret this excursion as representing a period of enhanced aerobic methane oxidation before the onset of the Great Oxidation Event. This places valuable time constraints on the evolution of this metabolism and firmly establishing Cu isotopes as a biomarker in Late Archaean rocks.PostprintPeer reviewe

    Nitrogen fixation sustained productivity in the wake of the Palaeoproterozoic Great Oxygenation Event

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    The marine nitrogen cycle is dominated by redox-controlled biogeochemical processes and, therefore, is likely to have been revolutionised in response to Earth-surface oxygenation. The details, timing, and trajectory of nitrogen cycle evolution, however, remain elusive. Here we couple nitrogen and carbon isotope records from multiple drillcores through the Rooihoogte–Timeball Hill Formations from across the Carletonville area of the Kaapvaal Craton where the Great Oxygenation Event (GOE) and its aftermath are recorded. Our data reveal that aerobic nitrogen cycling, featuring metabolisms involving nitrogen oxyanions, was well established prior to the GOE and that ammonium may have dominated the dissolved nitrogen inventory. Pronounced signals of diazotrophy imply a stepwise evolution, with a temporary intermediate stage where both ammonium and nitrate may have been scarce. We suggest that the emergence of the modern nitrogen cycle, with metabolic processes that approximate their contemporary balance, was retarded by low environmental oxygen availability

    Reconciling discrepant minor sulfur isotope records of the Great Oxidation Event

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    Emerging sulfur isotope data divides opinion surrounding the Great Oxidation Event. Utilising computational approaches and additional data, Uveges et al. reconcile these disparities, offering a more refined framework of atmospheric oxygenation

    Early diagenesis of sulfur in Bornholm Basin sediments: The role of upward diffusion of isotopically “heavy” sulfide

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    Sediment-hosted marine sulfur cycling has played a significant role in regulating Earth’s surface chemistry over our planet’s history. Microbially-mediated reactions involving sulfur are often accompanied by sulfur isotope fractionation that, in turn, is captured by sulfate and sulfide minerals, providing the opportunity to track changes in the microbial utilization of sulfur and thus the marine sulfur cycle. Studying sulfur diagenesis within the Bornholm Basin, Baltic Sea, we explore the interplay between carbon, sulfur and iron, focusing on the fate of sulfur and the dynamics of the sulfur and oxygen isotopic response as a function of the varying thickness of the organic carbon-rich Holocene Mud Layer (HML) across the basin. Using a one-dimensional reaction-transport model, porewater sulfate and sulfide profiles were used to calculate net sulfate reduction rates (SRR) and net sulfide production rates, respectively. These calculations suggest a positive relationship between the thickness of the HML and net rates of sulfate reduction and sulfide production. Given that ascending sulfide is enriched in 34S relative to that produced in-situ, a heightened sulfide flux promotes spatially variable precipitation of 34S-enriched pyrite (δ34S ≈ −10‰) close to the sediment–water interface. Modeling results indicate that this isotopically “heavy” sulfide is formed as a consequence of mixing between ascending sulfide (up to +6.3‰) and that produced in-situ (ca. −40‰). Further, we show that the sulfur and oxygen isotopic composition of porewater sulfate is controlled by the net SRR: when the net SRR is high (i.e., in sulfide-replete settings) the downcore increase in δ18OSO4 is dampened relative to increase in δ34SSO4, whereas when net SRR is low (i.e., in iron-rich parts of the basin) downcore δ18OSO4 values increase while δ34SSO4 values remain invariant. We conclude that sedimentation rates and open system diffusion strongly influence the distribution of sulfur species and their sulfur isotopic composition, as well as the oxygen isotopic composition of sulfate, through the interaction between iron, sulfur and methane. This work highlights the importance of considering diffusion to better understand open system diagenesis and the δ34S signatures of sulfate and sulfide in both modern settings and ancient rocks

    Recent Warming Fuels Increased Organic Carbon Export From Arctic Permafrost

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    Climate-driven thawing of Arctic permafrost renders its vast carbon reserves susceptible to microbial degradation, serving as a potentially potent positive feedback hidden within the climate system. While seemingly intuitive, the relationship between thermally driven permafrost losses and organic carbon (OC) export remains largely unexplored in natural settings. Filling this knowledge gap, we present down-core bulk and compound-specific radiocarbon records of permafrost change from a sediment core taken within the Alaskan Colville River delta spanning the last c. 2,700 years. Fingerprinted by significantly older radiocarbon ages of bulk OC and long-chain fatty acids, these data expose a thermally driven increase in permafrost OC export and/or deepening of mobilizable permafrost layers over the last c. 160 years after the Little Ice Age. Comparison of OC content and radiocarbon data between recent and Roman warming episodes likely implies that the rate of warming, alongside the prevailing boundary conditions, may dictate the ultimate fate of the Arctic's permafrost inventory. Our findings highlight the importance of leveraging geological records as archives of Arctic permafrost mobilization dynamics with temperature change