13Microorganisms produce and consume methane in terrestrial surface environments, sea 14 sediments and, as indicated by recent discoveries, in fractured crystalline bedrock. These 15 processes in the crystalline bedrock remain, however, unexplored both in terms of 16 mechanisms and spatiotemporal distribution. Here we have studied these processes via a 17 multi-method approach including microscale analysis of the stable isotope compositions of

In the deep biosphere, microbial sulfate reduction (MSR) is exploited for energy. Here, we show that, in fractured continental crystalline bedrock in three areas in Sweden, this process produced sulfide that reacted with iron to form pyrite extremely enriched in S relative to S. As documented by secondary ion mass spectrometry (SIMS) microanalyses, the δ S values are up to +132‰V-CDT and with a total range of 186‰. The lightest δ S values (-54‰) suggest very large fractionation during MSR from an initial sulfate with δ S values (δ S ) of +14 to +28‰. Fractionation of this magnitude requires a slow MSR rate, a feature we attribute to nutrient and electron donor shortage as well as initial sulfate abundance. The superheavy δ S values were produced by Rayleigh fractionation effects in a diminishing sulfate pool. Large volumes of pyrite with superheavy values (+120 ± 15‰) within single fracture intercepts in the boreholes, associated heavy average values up to +75‰ and heavy minimum δ S values, suggest isolation of significant amounts of isotopically light sulfide in other parts of the fracture system. Large fracture-specific δ S variability and overall average δ S values (+11 to +16‰) lower than the anticipated δ S support this hypothesis. The superheavy pyrite found locally in the borehole intercepts thus represents a late stage in a much larger fracture system undergoing Rayleigh fractionation. Microscale Rb-Sr dating and U/Th-He dating of cogenetic minerals reveal that most pyrite formed in the early Paleozoic era, but crystal overgrowths may be significantly younger. The δ C values in cogenetic calcite suggest that the superheavy δ S values are related to organotrophic MSR, in contrast to findings from marine sediments where superheavy pyrite has been proposed to be linked to anaerobic oxidation of methane. The findings provide new insights into MSR-related S-isotope systematics, particularly regarding formation of large fractions of S-rich pyrite.

Craton cores far from plate boundaries have traditionally been viewed as stable features that experience minimal vertical motion over 100–1000 Ma time scales. Here we show that the Fennoscandian Shield in southeastern Sweden experienced several episodes of burial and exhumation from ~1800 Ma to the present. Apatite, titanite, and zircon (U‐Th)/He ages from surface samples and drill cores constrain the long‐term, low‐temperature history of the Laxemar region. Single grain titanite and zircon (U‐Th)/He ages are negatively correlated (104–838 Ma for zircon and 160–945 Ma for titanite) with effective uranium (eU = U + 0.235 × Th), a measurement proportional to radiation damage. Apatite ages are 102–258 Ma and are positively correlated with eU. These correlations are interpreted with damage‐diffusivity models, and the modeled zircon He age‐eU correlations constrain multiple episodes of heating and cooling from 1800 Ma to the present, which we interpret in the context of foreland basin systems related to the Neoproterozoic Sveconorwegian and Paleozoic Caledonian orogens. Inverse time‐temperature models constrain an average burial temperature of ~217°C during the Sveconorwegian, achieved between 944 Ma and 851 Ma, and ~154°C during the Caledonian, achieved between 366 Ma and 224 Ma. Subsequent cooling to near‐surface temperatures in both cases could be related to long‐term exhumation caused by either postorogenic collapse or mantle dynamics related to the final assembly of Rodinia and Pangaea. Our titanite He age‐eU correlations cannot currently be interpreted in the same fashion; however, this study represents one of the first examples of a damage‐diffusivity relationship in this system, which deserves further research attention.

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 finegrained 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.

Recent studies reveal that organisms from all three domains of life-Archaea, Bacteria, and even Eukarya-can thrive under energy-poor, dark, and anoxic conditions at large depths in the fractured crystalline continental crust. There is a need for an increased understanding of the processes and lifeforms in this vast realm, for example, regarding the spatiotemporal extent and variability of the different processes in the crust. Here, we present a study that set out to detect signs of ancient microbial life in the Forsmark area-the target area for deep geological nuclear waste disposal in Sweden. Stable isotope compositions were determined with high spatial resolution analyses within mineral coatings, and mineralized remains of putative microorganisms were studied in several deep water-conducting fracture zones (down to 663 m depth), from which hydrochemical and gas data exist. Large isotopic variabilities of δ 13 C calcite (−36.2 to +20.2‰ V-PDB) and δ 34 S pyrite (−11.7 to +37.8‰ V-CDT) disclose discrete periods of methanogenesis, and potentially, anaerobic oxidation of methane and related microbial sulfate reduction at several depth intervals. Dominant calcite-water disequilibrium of δ 18 O and 87 Sr/ 86 Sr precludes abundant recent precipitation. Instead, the mineral coatings largely reflect an ancient archive of episodic microbial processes in the fracture system, which, according to our microscale Rb-Sr dating of co-genetic adularia and calcite, date back to the mid-Paleozoic. Potential Quaternary precipitation exists mainly at~400 m depth in one of the boreholes, where mineral-water compositions corresponded.

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Impact-generated hydrothermal systems have been suggested as favourable environments for deep microbial ecosystems on Earth, and possibly beyond. Fossil evidence from a handful of impact craters worldwide have been used to support this notion. However, as always with mineralized remains of microorganisms in crystalline rock, certain time constraints with respect to the ecosystems and their subsequent fossilization are difficult to obtain. Here we re-evaluate previously described fungal fossils from the Lockne crater (458 Ma), Sweden. Based on in-situ Rb/Sr dating of secondary calcite-albite-feldspar (356.6 ± 6.7 Ma) we conclude that the fungal colonization took place at least 100 Myr after the impact event, thus long after the impact-induced hydrothermal activity ceased. We also present microscale stable isotope data of 13C-enriched calcite suggesting the presence of methanogens contemporary with the fungi. Thus, the Lockne fungi fossils are not, as previously thought, related to the impact event, but nevertheless have colonized fractures that may have been formed or were reactivated by the impact. Instead, the Lockne fossils show similar features as recent findings of ancient microbial remains elsewhere in the fractured Swedish Precambrian basement and may thus represent a more general feature in this scarcely explored habitat than previously known.

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