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Sökning: WFRF:(Drake Henrik 1979 ) > (2020-2024)

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1.
  • Tillberg, Mikael, 1990, et al. (författare)
  • Reconstructing craton-scale tectonic events via in situ Rb-Sr geochronology of poly-phased vein mineralization
  • 2021
  • Ingår i: Terra Nova. - : Wiley. - 0954-4879 .- 1365-3121. ; 33:5, s. 502-510
  • Tidskriftsartikel (refereegranskat)abstract
    • Fault- and fracture-hosted multi-stage mineral assemblages that formed by fracture reactivation and fluid migration, constitute archives of the tectonic evolution of Precambrian cratons. Complex intergrowth patterns of these mineral records often hinder absolute dating of mineralization events for geological models. We apply LA-ICP-MS/MS in situ Rb-Sr dating of single crystal growth zones in sub-mm-wide vein mineralization assemblages including illite, K-feldspar, albite, calcite, mica, zeolites, fluorite and/or epidote at three Palaeoproterozoic crystalline bedrock sites over 300 km apart in the Fennoscandian Shield. The dating campaign reveals multiple age clusters between ca. 1757 +/- 15 and 355 +/- 12 Ma correlating with fluid flow and fracture reactivation events initiated by far-field orogens and their foreland basin evolution. This new approach for reconstructing geological histories of Precambrian cratons connects micro-scale age determinations of different mineral growth zones in fractures with regional-scale crustal dynamic responses to tectonic events.
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2.
  • Bailey, Lydia R., et al. (författare)
  • Characteristics and Consequences of Red Bed Bleaching by Hydrocarbon Migration : A Natural Example From the Entrada Sandstone, Southern Utah
  • 2022
  • Ingår i: Geochemistry Geophysics Geosystems. - : John Wiley & Sons. - 1525-2027. ; 23:8
  • Tidskriftsartikel (refereegranskat)abstract
    • Extensive regions of yellow and white ("bleached") sandstones within the terrestrial Jurassic red bed deposits of the Colorado Plateau reflect widespread interaction with subsurface reduced fluids which resulted in the dissolution of iron-oxide grain coatings. Reduced fluids such as hydrocarbons, CO2, and organic acids have been proposed as bleaching agents. In this study, we characterize an altered section of the Slick Rock member of the Jurassic Entrada Sandstone that exposes bleached sandstone with bitumen-saturated pore spaces. We observe differences in texture, porosity, mineralogy, and geochemistry between red, pink, yellow, and gray facies. In the bleached yellow facies we observe quartz overgrowths, partially dissolved K-feldspar, calcite cement, fine-grained illite, TiO2-minerals, and pyrite concretions. Clay mineral content is highest at the margins of the bleached section. Fe2O3 concentrations are reduced up to 3x from the red to gray facies but enriched up to 50x in iron-oxide concretions. Metals such as Zn, Pb, and rare-earth elements are significantly enriched in the concretions. Supported by a batch geochemical model, we conclude the interaction of red sandstones with reduced hydrocarbon-bearing fluids caused iron-oxide and K-feldspar dissolution, and precipitation of quartz, calcite, clay, and pyrite. Localized redistribution of iron into concretions can account for most of the iron removed during bleaching. Pyrite and carbonate stable isotopic data suggest the hydrocarbons were sourced from the Pennsylvanian Paradox Formation. Bitumen in pore spaces and pyrite precipitation formed a reductant trap required to produce Cu, U, and V enrichment in all altered facies by younger, oxidized saline brines.
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3.
  • Drake, Henrik, Docent, 1979-, et al. (författare)
  • Biosignatures of ancient microbial life are present across the igneous crust of the Fennoscandian shield
  • 2021
  • Ingår i: Communications Earth & Environment. - : Springer Nature. - 2662-4435. ; 2:1
  • Tidskriftsartikel (refereegranskat)abstract
    • Earth’s crust contains a substantial proportion of global biomass, hosting microbial life up to several kilometers depth. Yet, knowledge of the evolution and extent of life in this environment remains elusive and patchy. Here we present isotopic, molecular and morphological signatures for deep ancient life in vein mineral specimens from mines distributed across the Precambrian Fennoscandian shield. Stable carbon isotopic signatures of calcite indicate microbial methanogenesis. In addition, sulfur isotope variability in pyrite, supported by stable carbon isotopic signatures of methyl-branched fatty acids, suggest subsequent bacterial sulfate reduction. Carbonate geochronology constrains the timing of these processes to the Cenozoic. We suggest that signatures of an ancient deep biosphere and long-term microbial activity are present throughout this shield. We suggest that microbes may have been active in the continental igneous crust over geological timescales, and that subsurface investigations may be valuable in the search for extra-terrestrial life.
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4.
  • Drake, Henrik, Docent, 1979-, et al. (författare)
  • Fossil svamp i Siljansringens meteoritkrater
  • 2021
  • Ingår i: Geologiskt Forum. - Stockholm : Geologiska föreningen. - 1104-4721. ; 110, s. 18-21
  • Tidskriftsartikel (populärvet., debatt m.m.)
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5.
  • Drake, Henrik, Docent, 1979-, et al. (författare)
  • Fossilized anaerobic and possibly methanogenesis-fueling fungi identified deep within the Siljan impact structure, Sweden
  • 2021
  • Ingår i: Communications Earth & Environment. - : Springer Science and Business Media LLC. - 2662-4435. ; 2:1, s. 1-11
  • Tidskriftsartikel (refereegranskat)abstract
    • Recent discoveries of extant and fossilized communities indicate that eukaryotes, including fungi, inhabit energy-poor and anoxic environments deep within the fractured igneous crust. This subterranean biosphere may constitute the largest fungal habitat on our planet, but knowledge of abyssal fungi and their syntrophic interactions with prokaryotes and their concomitant metabolisms is scarce. Here we report findings of fossilized, chitin-bearing fungal hyphae at ~540 m depth in fractured bedrock of the Siljan impact structure, the largest crater in Europe. Strong 13C-enrichment of calcite precipitated with and on the fungi suggests formation following methanogenesis, and that the anaerobic fungi decomposed dispersed organic matter producing for example H2 that may have fueled autotrophic methanogens. An Eocene age determined for the calcite infers the first timing constraint of fossilized fungi in the continental igneous crust. Fungi may be widespread decomposers of organic matter and overlooked providers of H2 to autotrophs in the vast rock-hosted deep biosphere.
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6.
  • Drake, Henrik, 1979-, et al. (författare)
  • Geochronology and Stable Isotope Analysis of Fracture-Fill and Karst Mineralization Reveal Sub-Surface Paleo-Fluid Flow and Microbial Activity of the COSC-1 Borehole, Scandinavian Caledonides
  • 2020
  • Ingår i: Geosciences. - : MDPI AG. - 2076-3263.
  • Annan publikation (övrigt vetenskapligt/konstnärligt)abstract
    • The deep biosphere hosted in fractured rocks within the upper continental crust is one of the least understood and studied ecological realms on Earth. Scarce knowledge of ancient life and paleo-fluid flow within this realm is owing to the lack of deep drilling into the crust. Here we apply microscale high spatial-resolution analytical techniques to fine-grained secondary minerals in a deep borehole (COSC-1) drilled into the Silurian-Devonian Scandinavian Caledonide mountain range in central Sweden. The aim is to detect and date signs of ancient microbial activity and low-temperature fluid circulation in micro-karsts (foliation-parallel dissolution cavities in the rock) and fractures at depth in the nappe system. Vein carbonates sampled at 684 to 2210 m show a decreased C isotope variability at depths below 1050 m; likely due to decreased influence of organic-C at great depth. Micro-karsts at 122–178 m depth feature at least two generations of secondary calcite and pyrite growth in the voids as shown by secondary ion mass spectrometry analytical transects within individual grains. The younger of these two precipitation phases shows 34S-depleted δ34Spyrite values (−19.8 ± 1.6‰ vs. Vienna-Canyon Diablo Troilite (V-CDT)) suggesting microbial sulfate reduction in situ. The calcite of this late phase can be distinguished from the older calcite by higher δ18Ocalcite values that correspond to precipitation from ambient meteoric water. The late stage calcite gave two separate laser ablation inductively coupled mass spectrometry-derived U-Pb ages (9.6 ± 1.3 Ma and 2.5 ± 0.2 Ma), marking a minimum age for widespread micro-karst formation within the nappe. Several stages of fluid flow and mineral precipitation followed karst formation; with related bacterial activity as late as the Neogene-Quaternary; in structures presently water conducting. The results show that our combined high spatial-resolution stable isotope and geochronology approach is suitable for characterizing paleo-fluid flow in micro-karst; in this case, of the crystalline crust comprising orogenic nappe units.
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7.
  • Drake, Henrik, Docent, 1979-, et al. (författare)
  • In Situ Rb/Sr Geochronology and Stable Isotope Geochemistry Evidence for Neoproterozoic and Paleozoic Fracture-Hosted Fluid Flow and Microbial Activity in Paleoproterozoic Basement, SW Sweden
  • 2023
  • Ingår i: Geochemistry Geophysics Geosystems. - : American Geophysical Union (AGU). - 1525-2027. ; 24:5
  • Tidskriftsartikel (refereegranskat)abstract
    • Recent studies have shown that biosignatures of ancient microbial life exist in mineral coatings in deep bedrock fractures of Precambrian cratons, but such surveys have been few and far between. Here, we report results from southwestern Sweden in an area of 1.6-1.5 Ga Paleoproterozoic rocks heavily reworked by the 1.14-0.96 Ga Sveconorwegian orogeny, a terrane previously scarcely explored for ancient microbial biosignatures. Calcite-pyrite-adularia-illite-coated fractures were analyzed for stable isotopes via Secondary Ion Mass Spectrometry (delta C-13, delta O-18, delta S-34) and in situ Rb/Sr geochronology via Laser-ablation inductively coupled plasma mass spectrometry. The Rb/Sr ages for calcite-adularia and calcite-illite show that several fluid flow events can be discerned (797 +/- 18-769 +/- 7, 391 +/- 5-387 +/- 6, 356 +/- 5-347 +/- 4, and 301 +/- 7 Ma). The delta C-13, delta O-18 and Sr-87/Sr-86 values of different calcite growth zones further confirmed episodic fluid flow. Pyrite delta S-34 values down to -49.9% V-CDT, together with systematically increased delta S-34 from crystal core to rim, suggest formation following microbial sulfate reduction under semi-closed conditions. Assemblages involving MSR-related pyrite generally have Devonian to Permian Rb/Sr ages, indicating an association to extension-related fracturing and fluid mixing during foreland-basin formation linked to Caledonian orogeny in the northwest. An assemblage with an age of 301 +/- 7 Ma is potentially related to Oslo Rift extension, whereas the Neo-Proterozoic ages relate to post-Sveconorwegian extensional tectonics. Remnants of short-chained fatty acids in the youngest calcite coatings further indicate a biogenic origin, while the absence of organic molecules in older calcite is in line with thermal degradation, potentially related to heating during Caledonian foreland basin burial. Plain Language Summary This study investigates mineral coatings in Proterozoic basement fractures of Southwestern Sweden, within the Precambrian Fennoscandian shield, to gain insights into ancient microbial life and paleo-fluid flow. Isotopic signatures of these mineral coatings suggest that microbial sulfate reducers have been present in the system as also indicated by preserved organic molecules. Microanalytical geochronology determinations reveal that the fracture system has been activated several times in the Neoproterozoic, Devonian-Early Carboniferous, and Late Carboniferous/Early Permian. These activations are associated with extension events following the Sveconorwegian and Caledonian orogenies as well as formation of the Oslo Rift. The signs of microbial activity are related to the youngest of these events, post-dating burial in the Caledonian foreland basin, when bedrock temperatures became habitable.
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8.
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9.
  • Drake, Henrik, Docent, 1979-, et al. (författare)
  • Thermochronologic perspectives on the deep-time evolution of the deep biosphere
  • 2021
  • Ingår i: Proceedings of the National Academy of Sciences of the United States of America. - : National Academy of Sciences. - 0027-8424 .- 1091-6490. ; 118:45
  • Tidskriftsartikel (refereegranskat)abstract
    • The Earth’s deep biosphere hosts some of its most ancient chemolithotrophic lineages. The history of habitation in this environment is thus of interest for understanding the origin and evolution of life. The oldest rocks on Earth, formed about 4 billion years ago, are in continental cratons that have experienced complex histories due to burial and exhumation. Isolated fracture-hosted fluids in these cratons may have residence times older than a billion years, but understanding the history of their microbial communities requires assessing the evolution of habitable conditions. Here, we present a thermochronological perspective on the habitability of Precambrian cratons through time. We show that rocks now in the upper few kilometers of cratons have been uninhabitable (>∼122 °C) for most of their lifetime or have experienced high-temperature episodes, such that the longest record of habitability does not stretch much beyond a billion years. In several cratons, habitable conditions date back only 50 to 300 million years, in agreement with dated biosignatures. The thermochronologic approach outlined here provides context for prospecting and interpreting the little-explored geologic record of the deep biosphere of Earth’s cratons, when and where microbial communities may have thrived, and candidate areas for the oldest records of chemolithotrophic microbes.
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10.
  • Drake, Henrik, Docent, 1979-, et al. (författare)
  • Tracking the Deep Biosphere through Time
  • 2020
  • Ingår i: Geosciences. - : MDPI. - 2076-3263. ; 10:11, s. 1-6
  • Tidskriftsartikel (övrigt vetenskapligt/konstnärligt)abstract
    • The oceanic and continental lithosphere constitutes Earth’s largest microbial habitat, yet it is scarcely investigated and not well understood. The physical and chemical properties here are distinctly different from the overlaying soils and the hydrosphere, which greatly impact the microbial communities and associated geobiological and geochemical processes. Fluid–rock interactions are key processes for microbial colonization and persistence in a nutrient-poor and extreme environment. Investigations during recent years have spotted microbial processes, stable isotope variations, and species that are unique to the subsurface crust. Recent advances in geochronology have enabled the direct dating of minerals formed in response to microbial activity, which in turn have led to an increased understanding of the evolution of the deep biosphere in (deep) time. Similarly, the preservation of isotopic signatures, as well as organic compounds within fossilized micro-colonies or related mineral assemblages in voids, cements, and fractures/veins in the upper crust, provides an archive that can be tapped for knowledge about ancient microbial activity, including both prokaryotic and eukaryotic life. This knowledge sheds light on how lifeforms have evolved in the energy-poor subsurface, but also contributes to the understanding of the boundaries of life on Earth, of early life when the surface was not habitable, and of the preservation of signatures of ancient life, which may have astrobiological implications. The Special Issue “Tracking the Deep Biosphere through Time” presents a collection of scientific contributions that provide a sample of forefront research in this field. The contributions involve a range of case studies of deep ancient life in continental and oceanic settings, of microbial diversity in sub-seafloor environments, of isolation of calcifying bacteria as well as reviews of clay mineralization of fungal biofilms and of the carbon isotope records of the deep biosphere.
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11.
  • Drake, Henrik, 1979-, et al. (författare)
  • Using 87Sr/86Sr LA-MC-ICP-MS Transects within Modern and Ancient Calcite Crystals to Determine Fluid Flow Events in Deep Granite Fractures
  • 2020
  • Ingår i: Geosciences. - : MDPI AG. - 2076-3263. ; 10, s. 1-23
  • Tidskriftsartikel (refereegranskat)abstract
    • The strontium isotope signature (87Sr/86Sr) of calcite precipitated in rock fractures and faults is a frequently used tool to trace paleofluid flow. However, bedrock fracture networks, such as in Precambrian cratons, have often undergone multiple fracture reactivations resulting in complex sequences of fracture mineral infillings. This includes numerous discrete calcite crystal overgrowths. Conventional 87Sr/86Sr analysis of dissolved bulk samples of such crystals is not feasible as they will result in mixed signatures of several growth zonations. In addition, the zonations are too fine-grained for sub-sampling using micro-drilling. Here, we apply high spatial resolution 87Sr/86Sr spot analysis(80 um) in transects through zoned calcite crystals in deep Paleoproterozoic granitoid fractures using laser ablation multi-collector inductively coupled plasma mass spectrometry (LA-MC-ICP-MS) to trace discrete signs of paleofluid flow events. We compare the outermost calcite growth zone with 87Sr/86Sr values of the present-day groundwater sampled in the same boreholes to distinguish potential modern precipitates. We then connect our results to previously reported radiometric dating and C and O isotope signatures to understand the temporal history and physicochemical evolution of fluid flow within the fractures. Comparisons of modern calcite precipitated in a borehole over a period of 17 years with modern waters prove the concept of using 87Sr/86Sr as a marker for fluid origin in this environment and for how 87Sr/86Sr changed during marine water infiltration. Intermittent calcite precipitation over very long time spans is indicated in calcite of the currently open fractures, showing an evolution of 87Sr/86Sr from ~0.705–0.707—a population dated to ~1.43 billion years—to crystal overgrowth values at ~0.715–0.717 that overlap with the present-day groundwater values.This shows that high spatial resolution Sr isotope analysis of fine-scaled growth zonation within single calcite crystals is applicable for tracing episodic fluid flow in fracture networks.
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12.
  • Ferguson, Grant, et al. (författare)
  • Acceleration of Deep Subsurface Fluid Fluxes in the Anthropocene
  • 2024
  • Ingår i: Earth's Future. - : John Wiley & Sons. - 2328-4277. ; 12:4
  • Tidskriftsartikel (refereegranskat)abstract
    • The Anthropocene has been framed around humanity's impact on atmospheric, biologic, and near-surface processes, such as land use and vegetation change, greenhouse gas emissions, and the above-ground hydrologic cycle. Groundwater extraction has lowered water tables in many key aquifers but comparatively little attention has been given to the impacts in the deeper subsurface. Here, we show that fluid fluxes from the extraction and injection of fluids associated with oil and gas production and inflow of water into mines likely exceed background flow rates in deep (>500 m) groundwater systems at a global scale. Projected carbon capture and sequestration (CCS), geothermal energy production, and lithium extraction to facilitate the energy transition will require fluid production rates exceeding current oil and co-produced water extraction. Natural analogs and geochemical modeling indicate that subsurface fluid manipulation in the Anthropocene will likely appear in the rock record. The magnitude and importance of these changes are unclear, due to a lack of understanding of how deep subsurface hydrologic and geochemical cycles and associated microbial life interact with the rest of the Earth system.
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13.
  • Herlambang, Adhipa, et al. (författare)
  • Physicochemical Conditions of the Devonian-Jurassic Continental Deep Biosphere Tracked by Carbonate Clumped Isotope Temperatures of Granite-Hosted Carbonate Veins
  • 2023
  • Ingår i: Geofluids. - : Hindawi Publishing Corporation. - 1468-8115 .- 1468-8123. ; 2023
  • Tidskriftsartikel (refereegranskat)abstract
    • Previous studies have shown that microorganisms thrive in oligotrophic fracture systems, and metabolisms include consumption and production of methane. In the Laxemar, Gotemar, and Forsmark areas of Sweden, ancient microbial activity has previously been demonstrated by large delta C-13(VPDB) variability of carbonate vein infillings within granitic host rocks. Here, we apply carbonate clumped isotope thermometry to reconstruct the temperature of precipitation of the carbonate within these veins. The carbonate clumped isotope temperatures indicate that mineralization took place between 46 degrees C and 108 degrees C, in line with previously published fluid inclusion data (<50 degrees C to 113 degrees C). The new carbonate clumped isotope data more accurately narrows temperatures at the lower end of this range as fluid inclusions are not easily applicable below 80 degrees C, a temperature regime of high importance for paleobiological reconstructions. Our results demonstrate that large volumes of biogenic carbonate cement were formed from low-temperature microbial processes in low-salinity water, succeeding calcite of deep brine origin. The known burial and thermal history of the region combined with our carbonate clumped isotope data place the microbial activity at the end of the Variscan orogeny and later events (e.g., Jurassic). Thus, carbonate clumped isotope thermometry reduces uncertainties in deep biosphere studies by providing more accurate temperature constraints in the low-temperature regime, the biogenic processes, and the origin of the diagenetic fluids.
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14.
  • Ivarsson, Magnus, et al. (författare)
  • A Cryptic Alternative for the Evolution of Hyphae
  • 2020
  • Ingår i: Bioessays. - : John Wiley & Sons. - 0265-9247 .- 1521-1878. ; 42:6, s. 1-9
  • Tidskriftsartikel (refereegranskat)abstract
    • A growing awareness of a subsurface fossil record of mostly hyphal fungi organisms stretching back through the Phanerozoic to approximate to 400 megaannum (Ma) and possibly earlier, provides an alternative view on hyphal development. Parallel with the emergence of hyphal fungi during Ordovician-Devonian times when plants colonized the land, which is the traditional notion of hyphal evolution, hyphae-based fungi existed in the deep biosphere. New insights suggest that the fundamental functions of hyphae may have evolved in response to an ancient subsurface endolithic life style and might have been in place before the colonization of land. To address the gaps in the current understanding of hyphal evolution a strategy based on research prospects involving investigations of uncharted geological material, new diagnostics, and comparisons to live species is proposed.
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15.
  • Ivarsson, Magnus, et al. (författare)
  • Introducing palaeolithobiology
  • 2021
  • Ingår i: GFF. - London : Taylor & Francis. - 1103-5897 .- 2000-0863. ; 143:2-3, s. 305-319
  • Tidskriftsartikel (refereegranskat)abstract
    • A growing literature of deep but also surficial fossilized remains of lithobiological life, often associated with igneous rocks, necessitates the unfolding of a sub-discipline within paleobiology. Here, we introduce the term paleolithobiology as the new auxiliary sub-discipline under which fossilized lithobiology should be handled. We present key criteria that distinguish the paleolithobiological archive from the traditional one and discuss sample strategies as well as scientific perspectives. A majority of paleolithobiological material consists of deep biosphere fossils, and in order to highlight the relevance of these, we present new data on fungal fossils from the Lockne impact crater. Fungal fossils in the Lockne drill cores have been described previously but here we provide new insights into the presence of reproductive structures that indicate the fungi to be indigenous. We also show that these fungi frequently dissolve and penetrate secondary calcite, delineating the role lithobionts plays in geobiological cycles. We hope that the formalization of the sub-discipline paleolithobiology will not only highlight an overlooked area of paleobiology as well as simplify future studies of endo- and epilithic fossil material, but also improve our understanding of the history of the deep biosphere.
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16.
  • Ivarsson, Magnus, et al. (författare)
  • The fossil record of igneous rock
  • 2020
  • Ingår i: Earth-Science Reviews. - : Elsevier. - 0012-8252 .- 1872-6828. ; 210, s. 1-20
  • Tidskriftsartikel (refereegranskat)abstract
    • A growing awareness of life in deep igneous crust expands our appreciation for life's distribution in the upper geosphere through time and space, and extends the known inhabitable realm of Earth and possibly beyond. For most of life's history, until plants colonized land in the Ordovician, the deep biosphere was the largest reservoir of living biomass. This suggests that deep crustal habitats played an important role in the evolution and development of the biosphere. Paradoxically, the paleo-perspective of deep life has been largely neglected in the exploration of the deep biosphere as well as in paleontology as a whole. Here, we review the collective understanding of the fossil record in igneous crust with the aim to highlight a rising research field with great potential for substantial findings and progress in the near future. We include new results that emphasize the importance of direct or indirect dating of fossils and introduction of new techniques into the field. Currently, an incoherent record of morphological fossils- and chemofossils stretching from present to ~2.4 Ga implies the presence of an abundant and rich, yet largely unexplored, fossil record. Further investigations of deep paleo-environments will most certainly result in substantial insights into the distribution and development of biospheres throughout life's history, the early evolution of prokaryotes and eukaryotes, and Earth's early biogeochemical cycles. We emphasize the fossil record of igneous rock to give it the same status as the fossil record in sedimentary rocks, and to implement fossil investigations as standard procedures in future international drilling campaigns.
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17.
  • Ju, YeoJin, et al. (författare)
  • Long-term change in uranium migration processes in highly eroded granite, demonstrated by uranium series disequilibrium in fracture-filling materials
  • 2023
  • Ingår i: Applied Geochemistry. - : Elsevier. - 0883-2927 .- 1872-9134. ; 148
  • Tidskriftsartikel (refereegranskat)abstract
    • The mineralization and mobilization of uranium (U) are strongly associated with subsurface redox processes, which can affect the U inventory of deep geological repositories of nuclear waste and are to be considered in safety assessments. The Korea Atomic Energy Research Institute (KAERI) underground research tunnel (KURT) is located in an active groundwater recharge area in granitic bedrock, where oxidizing meteoric water infiltrates the subsurface through permeable zones of highly weathered granite, forming multiple redox fronts. Fracture-filling materials (FFMs) are U-enriched, with concentrations of up to ∼50 mg/kg. We examined long-lived radioactive isotopes of 230Th, 232Th, 234U, 235U, and 238U and other redox-sensitive elements and isotopes, e.g., Fe, δ56Fe, and Ce/Ce*, in the FFMs to understand fluctuations in redox conditions in the granitic fracture system. The primary focus was on U migration processes and to decipher the depths of meteoric water infiltration over geological timescales. Enrichment of uranium and other redox-sensitive elements occurred in FFMs at relatively shallow depths (∼180 m below ground level, bgl), implying that the U distribution was associated with redox interactions of the intruding groundwater that precipitated the secondary minerals. Interaction of FFMs with groundwater caused activity ratios (AR) of the FFMs to deviate moderately from secular equilibrium (AR = 1); 234U/238U AR of 0.87–1.25, and 230Th/238U AR of 0.76–1.22. A dynamic redox transition zone, witnessed by uranium series disequilibrium, shows both deposition and complex redistribution in the 120–205 Ka time frame, is confined to the upper ∼180 m bgl of the fractured rock. The results provide new insights into the long-term paleo-redox processes in the complex granitic fracture systems, which are analogs of potential deep-seated geological repositories for high-level radioactive waste.
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18.
  • Kusturica, Annemie, et al. (författare)
  • LA-ICP-MS analysis of trace and rare-earth element distribution in calcite fracture fillings from Forsmark, Simpevarp and Laxemar (Sweden)
  • 2022
  • Ingår i: Environmental Earth Sciences. - : Springer. - 1866-6280 .- 1866-6299. ; 81:14
  • Tidskriftsartikel (refereegranskat)abstract
    • Concentrations and spatial distribution of trace elements in secondary minerals provide valuable information about mobility controlling processes in natural fractures. Important examples include rare-earth element contents that act as analogues for the retention of trivalent actinides such as Am/Cm or Pu(III). The secondary phases (carbonates) investigated in this study originate from exploration drilling bore cores of the Swedish Nuclear Fuel and Waste Management Company SKB (Forsmark, Simpevarp and Laxemar, Sweden). Here, high-resolution element analysis (Micro-X-ray Fluorescence-Spectrometry (mu XRF) and Laser Ablation-Inductively Coupled Plasma-Mass Spectrometry (LA-ICP-MS)) is applied to scan for Na and the trace elements Mn, Fe, Sr, Pb, Th and U as well as the rare-earth elements Y, La, Ce and Yb associated with carbonate fracture fillings. High resolution element maps highlight growth zones and microstructures within the samples, which are not detected by the usual point and line measurements. Evidence of phase-dependent partitioning is observed. The partition coefficients, D, determined from formation water and carbonate data were compared to experimentally generated coefficients and values derived from a 17-year precipitation experiment carried out at the aspo Hard Rock Laboratory (HRL). Distribution coefficients of the light rare-earth elements La and Ce have been found to be relatively high in the studied samples, whereas the coefficients of distribution of Sr and U are remarkably low. Overall, the results of this work show that the secondary calcite formed in deep granitic fractures coprecipitated periodically with significant amounts of radionuclide analogues (i.e., rare-earth elements).
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19.
  • Kutzschbach, Martin, et al. (författare)
  • Arsenic-poor fluids promote strong As partitioning into pyrite
  • 2024
  • Ingår i: Geochimica et Cosmochimica Acta. - Amsterdam : Elsevier. - 0016-7037 .- 1872-9533. ; 376, s. 37-53
  • Tidskriftsartikel (refereegranskat)abstract
    • Pyrite is a ubiquitous sulfide mineral found in diverse geological settings and holds great significance in the formation of Au deposits as well as the safe utilization of groundwater due to its remarkable ability to incorporate substantial amounts of As. However, despite its importance, there remains a dearth of fundamental data on the partitioning of As between pyrite and fluid, which is key for accurately modeling the As distribution in these environments.Here, we present new insights into the partitioning behavior of As between pyrite and fluid at conditions that mimic natural fluid systems. Pyrite was synthesized by replacement of natural siderite in hydrothermal experiments at 200 °C and pH 5 applying a wide range of fluid As concentrations, spanning from 0.001 to 100 µg/g. The As distribution and concentration in synthetic pyrite was analyzed by quantitative LA-ICP-MS mapping providing a high spatial resolution and sensitivity at 2–3 µm image pixel size at a detection limit of ∼1 µg/g at the single pixel scale. Pyrite-fluid partitioning coefficients (DAs(py/fluid)) between synthetic pyrite and experimental fluid agree with previously published data for high fluid As concentrations of 1 µg/g to 100 µg/g (DAs < 2000). However, at low As concentrations in the experimental fluid (<1 µg/g), a steep increase in the DAs(py/fluid) values of up to ∼30,000 was detected, demonstrating even stronger As partitioning into pyrite. This is confirmed by the analyses of natural pyrite that precipitated from As-poor fluids (0.3–0.4 ng/g) within a deep anoxic aquifer in SE Sweden. The discovery holds significant implications for the mobility and scavenging of As, which in turn is important for understanding the formation and fingerprinting of mineral deposits as well as for the secure utilization of groundwater resources.
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20.
  • McIntosh, Jennifer, et al. (författare)
  • Burial and Denudation Alter Microbial Life at the Bottom of the Hypo‐Critical Zone
  • 2023
  • Ingår i: Geochemistry Geophysics Geosystems. - : American Geophysical Union (AGU). - 1525-2027. ; 24:6
  • Tidskriftsartikel (refereegranskat)abstract
    • How subsurface microbial life changed at the bottom of the kilometers-deep (hypo) Critical Zone in response to evolving surface conditions over geologic time is an open question. This study investigates the burial and exhumation, biodegradation, and fluid circulation history of hydrocarbon reservoirs across the Colorado Plateau as a window into the hypo-Critical Zone. Hydrocarbon reservoirs, in the Paradox and Uinta basins, were deeply buried starting ca. 100 to 60 Ma, reaching temperatures >80–140°C, likely sterilizing microbial communities present since the deposition of sediments. High salinities associated with evaporites may have further limited microbial activity. Upward migration of hydrocarbons from shale source rocks into shallower reservoirs during maximum burial set the stage for microbial re-introduction by creating organic-rich “hot spots.” Denudation related to the incision of the Colorado River over the past few million years brought reservoirs closer to the surface under cooler temperatures, enhanced deep meteoric water circulation and flushing of saline fluids, and likely re-inoculated more permeable sediments up to several km depth. Modern- to paleo-hydrocarbon reservoirs show molecular and isotopic evidence of anaerobic oxidation of hydrocarbons coupled to bacterial sulfate reduction in areas with relatively high SO4-fluxes. Anaerobic oil biodegradation rates are high enough to explain the removal of at least some portion of postulated “supergiant oil fields” across the Colorado Plateau by microbial activity over the past several million years. Results from this study help constrain the lower limits of the hypo-Critical Zone and how it evolved over geologic time, in response to changing geologic, hydrologic, and biologic forcings.
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21.
  • Nisson, D.M., et al. (författare)
  • Hydrogeochemical and isotopic signatures elucidate deep subsurface hypersaline brine formation through radiolysis driven water-rock interaction
  • 2023
  • Ingår i: Geochimica et Cosmochimica Acta. - : Elsevier. - 0016-7037 .- 1872-9533. ; 340, s. 65-84
  • Tidskriftsartikel (refereegranskat)abstract
    • Geochemical and isotopic fluid signatures from a 2.9–3.2 km deep, 45–55 °C temperature, hypersaline brine from Moab Khotsong gold and uranium mine in the Witwatersrand Basin of South Africa were combined with radiolytic and water–rock isotopic exchange models to delineate brine evolution over geologic time, and to explore brine conditions for habitability. The Moab Khotsong brines were hypersaline (Ca-Na-Cl) with 215–246 g/L TDS, and Cl− concentrations up to 4 mol/L suggesting their position as a hypersaline end-member significantly more saline than any previously sampled Witwatersrand Basin fluids. The brines revealed low DIC (∼0.266–∼1.07 mmol/L) with high (∼8.49–∼23.6 mmol/L) DOC pools, and several reduced gaseous species (up to 46 % by volume H2) despite microoxic conditions (Eh = 135–161 mV). Alpha particle radiolysis of water to H2, H2O2, and O2 along with anhydrous-silicate-to-clay alteration reactions predicted 4 mol/L Cl− brine concentration and deuterium enrichment in the fracture waters over a period > 1.00 Ga, consistent with previously reported 40Ar noble gas-derived residence times of 1.20 Ga for this system. In addition, radiolytic production of 7–26 nmol/(L × yr) H2, 3–11 nmol/(L × yr) O2, and 1–8 nmol/(L × yr) H2O2 was predicted for 1–100 g/g 238U dosage scenarios, supporting radiolysis as a significant source of H2 and oxidant species to deep brines over time that are available to a low biomass system (102–103 cells/mL). The host rock lithology was predominately Archaean quartzite, with minerals exposed on fracture surfaces that included calcite, pyrite, and chlorite. Signatures of 18Ocalcite, 13Ccalcite, Δ33Spyrite, 34Spyrite and 87Sr/86Sr obtained from secondary ion mass spectrometry (SIMS) microanalyses suggest several discrete fluid events as the basin cooled from peak greenschist conditions to equilibrium with present-day brine temperatures. The brine physiochemistry, geochemistry, and cellular abundances were significantly different from those of a younger, shallower, low salinity dolomitic fluid in the same mine, and both were different from the mine service water. These results indicate the discovery of one of few long-isolated systems that supports subsurface brine formation via extended water–rock interaction, and an example of a subsurface brine system where abiotic geochemistry may support a low biomass microbial community.
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22.
  • Pidchenko, Ivan, et al. (författare)
  • Deep anoxic aquifers could act as sinks for uranium through microbial-assisted mineral trapping
  • 2023
  • Ingår i: Communications Earth & Environment. - : Springer. - 2662-4435. ; 4:1
  • Tidskriftsartikel (refereegranskat)abstract
    • Uptake of uranium (U) by secondary minerals, such as carbonates and iron (Fe)-sulfides, that occur ubiquitously on Earth, may be substantial in deep anoxic environments compared to surficial settings due to different environment-specific conditions. Yet, knowledge of U reductive removal pathways and related fractionation between 238U and 235U isotopes in deep anoxic groundwater systems remain elusive. Here we show bacteria-driven degradation of organic constituents that influences formation of sulfidic species facilitating reduction of geochemically mobile U(VI) with subsequent trapping of U(IV) by calcite and Fe-sulfides. The isotopic signatures recorded for U and Ca in fracture water and calcite samples provide additional insights on U(VI) reduction behaviour and calcite growth rate. The removal efficiency of U from groundwater reaching 75% in borehole sections in fractured granite, and selective U accumulation in secondary minerals in exceedingly U-deficient groundwater shows the potential of these widespread mineralogical sinks for U in deep anoxic environments.
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23.
  • Reinhardt, Manuel, et al. (författare)
  • Aspects of the biological carbon cycle in a ca. 3.42-billion-year-old marine ecosystem
  • 2024
  • Ingår i: Precambrian Research. - : Elsevier. - 0301-9268 .- 1872-7433. ; 402, s. 107289-107289
  • Tidskriftsartikel (refereegranskat)abstract
    • Microbial life on Earth was well established in the Paleoarchean, but insight into early ecosystem diversity and thus, the complexity of the early biological carbon cycle is limited. Here we investigated four carbonaceous chert samples from the lower platform facies of the ca. 3.42-billion-year-old Buck Reef Chert, Barberton greenstone belt. The analysis on multiple scales revealed exceptionally well-preserved carbonaceous matter, even on molecular level (aliphatic and aromatic hydrocarbons), resulting from rapid silicification. Geochemical evidence from stable carbon and multiple sulfur isotopes supports the presence of different microbial metabolisms in the Paleoarchean ecosystem. The local biological carbon cycle was dominated by photoautotrophs, but autotrophic sulfate reducers and methane- or acetate-producing microbes were also present. In areas of microbial methane or acetate release, methanotrophs or acetotrophs contributed to the overall biomass. These results highlight the metabolic diversity in the lower platform environment of the Buck Reef Chert, and underline that an advanced biological carbon cycle already existed in the early Archean.
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24.
  • Roberts, Nick, et al. (författare)
  • Laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS) U–Pb carbonate geochronology : strategies, progress, and limitations
  • 2020
  • Ingår i: Geochronology. - : Copernicus Publications. - 2628-3719. ; 2, s. 33-61
  • Tidskriftsartikel (refereegranskat)abstract
    • Laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS) U–Pb geochronology of carbonate minerals, calcite in particular, is rapidly gaining popularity as an absolute dating method. The high spatial resolution of LA-ICP-MS U–Pb carbonate geochronology has benefits over traditional isotope dilution methods, particularly for diagenetic and hydrothermal calcite, because uranium and lead are heterogeneously distributed on the sub-millimetre scale. At the same time, this can provide limitations to the method, as locating zones of radiogenic lead can be time-consuming and “hit or miss”. Here, we present strategies for dating carbonates with in situ techniques, through imaging and petrographic techniques to data interpretation; our examples are drawn from the dating of fracture-filling calcite, but our discussion is relevant to all carbonate applications. We review several limitations to the method, including open-system behaviour, variable initial-lead compositions, and U–daughter disequilibrium. We also discuss two approaches to data collection: traditional spot analyses guided by petrographic and elemental imaging and image-based dating that utilises LA-ICP-MS elemental and isotopic map data.
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25.
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26.
  • Tillberg, Mikael (författare)
  • Constraining the timing of veins, faults and fractures in crystalline rocks by in situ Rb-Sr geochronology
  • 2020
  • Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
    • Precambrian cratons are continent cores archiving the oldest crustal histories on Earth. The crystalline basement of cratons is typically characterized by complex arrays of multiple fracture and fault generations hosting minerals formed by fluids flowing through fracture networks. Disentangling absolute chronologies of the various fracturing, faulting and fluid flow events have to date been difficult given the micro-scale mineral intergrowths and zonations, inhibiting conventional dating techniques. In the general lack of age constraints, deformation and mineralization mechanisms cannot be attributed to specific tectonic regimes, hampering reconstruction of local and regional events of fluid flow and mineral precipitation, and ultimately of the geological evolution of cratons. This thesis presents diverse studies utilizing the radiogenic decay of fracture, fault and shear zone mineral assemblages sampled from the crystalline basement of the Fennoscandian Shield, aiming at detecting episodic fracturing reactivation, mineralization and microbial processes throughout the craton history.The analytical procedures involve, foremost, Rb-Sr geochronology, along with U-Pb and (U-Th)/He geochronology, stable isotope and trace element geochemistry, fluid inclusion thermometry and biomarkers. The in situ age determinations enabled 1) linking of greisen and distal veins to magmatic and post-magmatic fluid circulation, 2) slickenfibre growth to distinct faulting episodes, and 3) mineral precipitation in fractures, veins and shear zones to regionally extending deformation events across the Fennoscandian Shield. In addition, dating of mineralization related to deep fracture-hosted microbial life constrained the timing of such activity at several sites. The precipitation episodes stretch from Paleoproterozoic to Jurassic times with overgrowth generations separated in time by up to one billion years in single veins and even within individual crystals. The findings of the thesis demonstrate that the methodological protocol has potential to directly date a wide range of mineral assemblages in fractures, faults, veins and shear zones given that the isochron requirements are fulfilled. Fulfillment is ensured through detailed petrological and structural characterization followed by geochronological analysis and thorough data reduction allowing validation of isotopic data down to submicrometer level. The outcomes have implications for tectonic reconstructions at various scales, for the tracing of the deep ancient biosphere and for comprehending hydrothermal ore deposition, with direct societal relevance in the detection of ancient microbial activity and fracture reactivation at the candidate site for a spent nuclear fuel repository in Sweden.
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27.
  • Tillberg, Mikael, et al. (författare)
  • In situ Rb-Sr dating of slickenfibres in deep crystalline basement faults
  • 2020
  • Ingår i: Scientific Reports. - : Nature Publishing Group. - 2045-2322. ; 10:1, s. 1-12
  • Tidskriftsartikel (refereegranskat)abstract
    • Establishing temporal constraints of faulting is of importance for tectonic and seismicity reconstructions and predictions. Conventional fault dating techniques commonly use bulk samples of syn-kinematic illite and other K-bearing minerals in fault gouges, which results in mixed ages of repeatedly reactivated faults as well as grain-size dependent age variations. Here we present a new approach to resolve fault reactivation histories by applying high-spatial resolution Rb-Sr dating to fine-grained mineral slickenfibres in faults occurring in Paleoproterozoic crystalline rocks. Slickenfibre illite and/or K-feldspar together with co-genetic calcite and/or albite were targeted with 50 µm laser ablation triple quadrupole inductively coupled plasma mass spectrometry analyses (LA-ICP-MS/MS). The ages obtained disclose slickenfibre growth at several occasions spanning over 1 billion years, from at least 1527 Ma to 349 ± 9 Ma. The timing of these growth phases and the associated structural orientation information of the kinematic indicators on the fracture surfaces are linked to far-field tectonic events, including the Caledonian orogeny. Our approach links faulting to individual regional deformation events by minimizing age mixing through micro-scale analysis of individual grains and narrow crystal zones in common fault mineral assemblages.
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28.
  • Tillberg, Mikael, et al. (författare)
  • The deep geothermal energy potential of Kalmar and Nybro municipalities
  • 2024
  • Rapport (övrigt vetenskapligt/konstnärligt)abstract
    • The potential for enhanced geothermal energy production in the Kalmar and Nybro municipalities is investigated by reviewing existing data on the regional geothermal gradient and the extent of fracture zones with depth of the crystalline crust in the research area. Existing geophysical and hydrological models along with bedrock maps and results of earlier studies in the nearby region are integrated in this report. The geothermal gradient in the Kalmar-Nybro area is currently not quantified, but proximal measurements indicate that the temperature is not likely to increase significantly more than 16-17°C/km considering local bedrock properties. Target depths would in this scenario be up to 6-7 km for production drilling. The only major deformation zone in the area stretches in a WNW direction from Kalmar and has potential for containing deep open fractures. The Boda-Örsjö area appears to host an extensive fracture network of multiple converging fracture zones. However, prediction of fracture occurrence at depths of several kilometres is highly speculative since no deep drill data has been produced in the area. Suggestions for further studies required in order to develop a deep geothermal project in the region are provided, with emphasis on locating favourable structural settings and bedrock stress conditions. Nevertheless, technical method developments regarding drilling and fluid injection are likely required for enabling deep geothermal energy production in the relatively cold depths of the exposed crystalline bedrock characterizing both the examined area in this report and the predominant parts of Scandinavia. 
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29.
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30.
  • van Dam, Femke, et al. (författare)
  • Dissolved Microbial Methane in the Deep Crystalline Crust Fluids–Current Knowledge and Future Prospects
  • 2022
  • Ingår i: Geofluids. - : Hindawi Publishing Corporation. - 1468-8115 .- 1468-8123.
  • Tidskriftsartikel (refereegranskat)abstract
    • Methane is a powerful greenhouse gas, of which most is produced by microorganisms in a process called methanogenesis. One environment where methanogenic microorganisms occur is the deep biosphere. The deep biosphere environment comprises a variety of ecosystem settings; marine habitats such as subseafloor sediments, rock pore volumes within subseafloor basalts, and terrestrial settings such as sedimentary rocks and crystalline bedrock fracture networks. Microbial methane formed in these environments influence the biological, chemical, and geological cycles of the upper crust, and may seep out of the deep into the atmosphere. This review focuses on the process of microbial methanogenesis and methane oxidation in the relatively underexplored deep crystalline-bedrock hosted subsurface, as several works in recent years have shown that microbial production and consumption occur in this energy-poor rock-fracture-hosted environment. These recent findings are summarized along with techniques to study the source and origins of methane in the terrestrial crust. Future prospects for exploration of these processes are proposed to combine geochemical and microbial techniques to determine whether microbial methanogenesis is a ubiquitous phenomenon in the crystalline crust across space and time. This will aid in determining whether microbial methane in the globally vast deep rock-hosted biosphere environment is a significant contributor to the global methane reservoir.
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31.
  • Weimann, L., et al. (författare)
  • Carbonaceous matter in ∼ 3.5 Ga black bedded barite from the Dresser Formation (Pilbara Craton, Western Australia) – Insights into organic cycling on the juvenile Earth
  • 2024
  • Ingår i: Precambrian Research. - : Elsevier. - 0301-9268 .- 1872-7433. ; 403
  • Tidskriftsartikel (refereegranskat)abstract
    • Carbonaceous matter (CM) in Archean rocks represents a valuable archive for the reconstruction of early life. Here we investigate the nature of CM preserved in ∼ 3.5 Ga old black bedded barites from the Dresser Formation (Pilbara Carton, Western Australia). Using light microscopy and high-resolution Raman mapping, three populations of CM were recognized: (i) CM at the edges of single growth bands of barite crystals (most frequent), (ii) CM within the barite matrix, and (iii) CM in 50–300 µm wide secondary quartz veins that cross-cut the black bedded barite. Raman spectra of CM inside black bedded barite indicated peak metamorphic temperatures of ∼ 350 °C, consistent with those reached during the main metamorphic event in the area ∼ 3.3 Ga ago. By contrast, CM in quartz veins yielded much lower temperatures of ∼ 220 °C, suggesting that quartz-vein associated CM entered the barite after 3.3 Ga. Near edge X-ray absorption fine structure (NEXAFS) and solid-state nuclear magnetic resonance (NMR) revealed a highly aromatic nature of the CM with a lower aliphatic content, which is in line with the relatively elevated thermal maturity. Catalytic hydropyrolysis (HyPy) did not yield any hydrocarbons detectable with gas chromatography–mass spectrometry (GC–MS). Secondary ion mass spectrometry (SIMS) based δ13C values of individual CM particles ranged from − 33.4 ± 1.2 ‰ to − 16.5 ± 0.6 ‰ and are thus in accordance with a biogenic origin, which is also consistent with stromatolitic microbialites associated with the black bedded barite. Based on these results we conclude that CM at growth bands and inside the barite matrix is syngenetic and only the CM inside quartz veins, which represents a minor portion of the total CM, is a later addition to the system. Furthermore, we discuss different pathways for the input of CM into the barite-forming environment, including the cycling of biological organic material within the hydrothermal system.
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32.
  • Weimann, Lena, et al. (författare)
  • Insights Into Carbonaceous Matter in ∼3.5 Ga Hydrothermal Barites from the Dresser Formation (Pilbara Craton, Australia)
  • 2023
  • Ingår i: IMOG 2023.
  • Konferensbidrag (refereegranskat)abstract
    • The emergence of life on the juvenile Earth is still poorly understood and remains one of the major questions in geobiological research. Some of our planet´s most ancient rocks contain carbonaceous matter (CM) that may represent a valuable archive to trace earliest life.However, it is often difficult to prove the origin and syngeneity of such CM. Here we report on CM preserved in ∼3.5 Ga old barites from the Dresser Formation (Pilbara Carton, Western Australia). On outcrop scale, spatial associations between bedded and vein-hosted barites suggest that the bedded barite may have formed from hydrothermal fluids discharging into subaquatic caldera environments [1]. Bedded barites associated with stromatolites contain abundant CM (total organic carbon = 0.3 wt% [2]) whose nature has been investigated further. Three populations of CM were recognized by means of light microscopy and high-resolution Raman mapping: (i) CM flakes at the edges of single growth bands of barite crystals, (ii) CM dispersed within barite crystals, and (iii) CM in 50–300 µm wide secondary quartz veins that cross-cut barite crystals. Raman spectra of the CM indicate peak metamorphic temperatures of approximately 300 ± 50 °C, corresponding to lower greenschist-facies conditions which are consistent with the metamorphic overprint by granitic intrusions in the area ∼3.3 Ga ago [3]. Near edge X-ray absorption fine structure (NEXAFS) and solid-state nuclear magnetic resonance (NMR) measurements revealed a highly aromatic nature of the CM which is in line with relatively high thermal maturity. As all three CM populations experienced the major metamorphic overprint ∼3.3 Ga ago, a syngenetic formation of the CM with the host barite can be assumed or, in case of the vein-hosted secondary CM, an emplacement soon after barite growth.
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33.
  • Yu, Changxun, 1983-, et al. (författare)
  • A Combined X-ray Absorption and Mössbauer Spectroscopy Study on Fe Valence and Secondary Mineralogy in Granitoid Fracture Networks : Implications for Geological Disposal of Spent Nuclear Fuels
  • 2020
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 54:5, s. 2832-2842
  • Tidskriftsartikel (refereegranskat)abstract
    • Underground repository in crystalline bedrock is a widely accepted solution for long-term disposal of spent nuclear fuels. During future deglaciations, meltwater will intrude via bedrock fractures to the depths of future repositories where O2 left in the meltwater could corrode metal canisters and enhance the migration of redox-sensitive radionuclides. Since glacial meltwater is poor in reduced phases, the quantity and (bio)accessibility of minerogenic Fe(II) in bedrock fractures determine to what extent O2 in future meltwater can be consumed. Here, we determined Fe valence and mineralogy in secondary mineral assemblages sampled throughout the upper kilometer of fractured crystalline bedrock at two sites on the Baltic Shield, using X-ray absorption and Mössbauer spectroscopic techniques that were found to deliver matching results. The data point to extensive O2-consuming capacity of the bedrock fractures, because Fe(II)-rich phyllosilicates were abundant and secondary pyrite was dispersed deep into the bedrock with no overall increase in Fe(II) concentrations and Fe(II)/Fe(III) proportions with depth. The results imply that repeated Pleistocene deglaciations did not cause a measurable decrease in the Fe(II) pool. In surficial fractures, largely opened during glacial unloading, ferrihydrite and illite have formed abundantly via oxidative transformation of Fe(II)-rich phyllosilicates and recently exposed primary biotite/hornblende.
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