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The shallow marine and subaerial sedimentary and hydrothermal rocks of the ~3.48 billion‐year‐old Dresser Formation are host to some of Earth's oldest stromatolites and microbial remains. This study reports on texturally distinctive, spherulitic barite micro‐mineralization that occur in association with primary, autochthonous organic matter within exceptionally preserved, strongly sulfidized stromatolite samples obtained from drill cores. Spherulitic barite micro‐mineralization within the sulfidized stromatolites generally forms submicron‐scale aggregates that show gradations from hollow to densely crystallized, irregular to partially radiating crystalline interiors. Several barite micro‐spherulites show thin outer shells. Within stromatolites, barite micro‐spherulites are intimately associated with petrographically earliest dolomite and nano‐porous pyrite enriched in organic matter, the latter of which is a possible biosignature assemblage that hosts microbial remains. Barite spherulites are also observed within layered barite in proximity to stromatolite layers, where they are overgrown by compositionally distinct (Sr‐rich), coarsely crystalline barite that may have been sourced from hydrothermal veins at depth. Micro‐spherulitic barite, such as reported here, is not known from hydrothermal systems that exceed the upper temperature limit for life. Rather, barite with near‐identical morphology and micro‐texture is known from zones of high bio‐productivity under low‐temperature conditions in the modern oceans, where microbial activity and/or organic matter of degrading biomass controls the formation of spherulitic aggregates. Hence, the presence of micro‐spherulitic barite in the organic matter‐bearing Dresser Formation sulfidized stromatolites lend further support for a biogenic origin of these unusual, exceptionally well‐preserved, and very ancient microbialites. [ABSTRACT FROM AUTHOR]

Fossil organic matter (OM) in Paleoarchean rocks is an invaluable tracer of ancient life, yet it is often contentious due to low preservation potentials of its original organic molecular characteristics under generally high metamorphic grades. This study reports on exceptionally preserved OM within black smoker-type sulfide mineralizations from the 3.24 billion-years-old Sulphur Springs volcanic-hosted massive sulfide deposit, East Pilbara Terrane, northwestern Australia. Fine scale mineralogical and organic molecular variations – documented by SEM and TEM techniques, Raman and FTIR Spectroscopy, as well as ToF-SIMS analysis – trace the formation of millimetre-scale pyritic hydrothermal orifices. Overmature OM (≳200–250 °C) enriched in aromatic hydrocarbons occurs within earliest formed colloform-banded pyrite that could have precipitated at high temperature upon mixing of hot hydrothermal fluids with cold seawater. In contrast, mature OM (within the catagenesis window; ∼100–150 °C) with lower proportions of aromatic hydrocarbons occasionally occurs alongside pyrite within barite near the inner paleofluid conduits of the hydrothermal orifices. A deposition of this OM generation from cooler fluids enriched in sulfate during waning hydrothermal activity is corroborated by its association with original mineralogy, particularly the occurrence of isolated nanoinclusions of OM within hydrothermal barite away from grain boundaries or fissures and cracks, which renders impossible an origin from post-depositional hydrocarbon migration. When compared to the overmature OM within colloform-banded pyrite, the better-preserved inner OM not only contains less abundant, smaller, and less ordered aromatic hydrocarbons, but also higher amounts of aliphatic molecules with longer chain lengths and higher proportions of carbonyl and amide functional groups. Although the latter characteristics are consistent with contributions by microbial biomass, abiotic origins are equally plausible because hydrothermal processes can produce OM with similar organic molecular attributes. Irrespective of these uncertainties on the ultimate sourcing of OM, common intergrowths of the cooler OM with nanoscopic iron oxides – hematite and lesser magnetite – hint at its hydrothermal deposition from colloidal particles that have been stabilized by iron-organic complexation. Further research is required to ascertain the significance of this process for the hydrothermal cycling and release of organic carbons and bound iron into the Paleoarchean oceans. Collectively, our results show that ancient marine hydrothermal systems can preserve OM with differing degrees of thermal degradation, which allows for insights into its sourcing, cycling, and deposition. • Exceptional preservation of mature organic matter in Paleoarchean black smoker-type sulfide mineralization. • Mineralogical and organic molecular variations trace the hydrothermal formation of pyritic fluid orifices. • Evidence for hydrothermal cycling of abiotic and/or microbial-derived organic matter. • Evidence for hydrothermal cycling and deposition of organic matter as iron-organic colloidal particles. [ABSTRACT FROM AUTHOR]

• Primary accumulations of transition metals and metalloids in Archean stromatolites. • Element distributions and concentrations correlate with microbial growth fabrics. • Accumulation owing to binding to organic matter of microbial communities. • Accumulation driven by microbial utilization. Stromatolites of the ~3.48 billion–year–old Dresser Formation (Pilbara Craton, Western Australia) provide some of the oldest convincing evidence of life on Earth. Here, we augment previous evidence with a detailed investigation of the concentrations and distributions of various transition metals (Cr, Mn, Co, Ni, Cu, Zn, Mo, Se, Ag, Sn, Au, Hg, and Pb) and metalloids (As, Sb, and Te) in unweathered samples of strongly sulfidized stromatolites from drill cores. High–resolution elemental mapping and in situ compositional analysis of sulfides (pyrite and sphalerite) show that these sedimentary and hydrothermally sourced elements are strongly concentrated in texturally distinctive, nano-porous pyrite enriched in autochthonous organic matter, which forms the major, petrogenetically earliest component of wrinkly laminated and digitate growth fabrics within the stromatolites. Repeated cyclic alternations of various transition metals and metalloids (most importantly Ni and Zn), plus the presence of disconformities and overgrowth relationships between wrinkly stromatolite laminae, suggest that these element accumulations were primarily established by depositional processes during continuous stromatolite formation. Because transition metals and metalloids generally have strong affinities for organic matter, and can play active roles in biochemical processes, we interpret these element accumulations in the Dresser Formation stromatolites to be the result of binding to organic matter of living microbial communities and/or dead biomass, and perhaps also microbial utilization. Collectively, our results show that the precise characterization of transition metal–metalloid concentrations and distributions can unveil element enrichment patterns suggestive of biological activity, even in some of Earth's oldest stromatolites. [ABSTRACT FROM AUTHOR]