Paleoarchean rocks from the Pilbara Craton of Western Australia provide a variety of clues to the existence of early life on Earth, such as stromatolites, putative microfossils and geochemical signatures of microbial activity. However, some of these features have also been explained by non-biological processes. Further lines of evidence are therefore required to convincingly argue for the presence of microbial life. Here we describe a new type of microbial mat facies from the 3.4 Ga Strelley Pool Formation, which directly overlies well known stromatolitic carbonates from the same formation. This microbial mat facies consists of laminated, very fine-grained black cherts with discontinuous white quartz layers and lenses, and contains small domical stromatolites and wind-blown crescentic ripples. Light- and cathodoluminescence microscopy, Raman spectroscopy, and time of flight—secondary ion mass spectrometry (ToF-SIMS) reveal a spatial association of carbonates, organic material, and highly abundant framboidal pyrite within the black cherts. Nano secondary ion mass spectrometry (NanoSIMS) confirmed the presence of distinct spheroidal carbonate bodies up to several tens of μm that are surrounded by organic material and pyrite. These aggregates are interpreted as biogenic. Comparison with Phanerozoic analogues indicates that the facies represents microbial mats formed in a shallow marine environment. Carbonate precipitation and silicification by hydrothermal fluids occurred during sedimentation and earliest diagenesis. The deciphered environment, as well as the δ¹³C signature of bulk organic matter (-35.3‰), are in accord with the presence of photoautotrophs. At the same time, highly abundant framboidal pyrite exhibits a sulfur isotopic signature (δ³⁴S = +3.05‰; Δ³³S = 0.268‰; and Δ³⁶S = -0.282‰) that is consistent with microbial sulfate reduction. Taken together, our results strongly support a microbial mat origin of the black chert facies, thus providing another line of evidence for life in the 3.4 Ga Strelley Pool Formation.

Archaean hydrothermal chert veins commonly contain abundant organic carbon of uncertain origin (abiotic vs. biotic). In this study, we analysed kerogen contained in a hydrothermal chert vein from the ca. 3.5 Ga Dresser Formation (Pilbara Craton, Western Australia). Catalytic hydropyrolysis (HyPy) of this kerogen yielded n-alkanes up to n-C₂₂, with a sharp decrease in abundance beyond n-C₁₈. This distribution (≤ n-C₁₈) is very similar to that observed in HyPy products of recent bacterial biomass, which was used as reference material, whereas it differs markedly from the unimodal distribution of abiotic compounds experimentally formed via Fischer–Tropsch-type synthesis. We therefore propose that the organic matter in the Archaean chert veins has a primarily microbial origin. The microbially derived organic matter accumulated in anoxic aquatic (surface and/or subsurface) environments and was then assimilated, redistributed and sequestered by the hydrothermal fluids (“hydrothermal pump hypothesis”).

It is widely hypothesised that primeval life utilised small organic molecules as sources of carbon and energy. However, the presence of such primordial ingredients in early Earth habitats has not yet been demonstrated. Here we report the existence of indigenous organic molecules and gases in primary fluid inclusions in c. 3.5-billion-year-old barites (Dresser Formation, Pilbara Craton, Western Australia). The compounds identified (e.g., H₂S, COS, CS₂, CH₄, acetic acid, organic (poly-)sulfanes, thiols) may have formed important substrates for purported ancestral sulfur and methanogenic metabolisms. They also include stable building blocks of methyl thioacetate (methanethiol, acetic acid) – a putative key agent in primordial energy metabolism and thus the emergence of life. Delivered by hydrothermal fluids, some of these compounds may have fuelled microbial communities associated with the barite deposits. Our findings demonstrate that early Archaean hydrothermal fluids contained essential primordial ingredients that provided fertile substrates for earliest life on our planet.

Lipid biomarkers have been extensively applied for tracing organisms and evolutionary processes through Earth's history. They have become especially important for the reconstruction of early life on Earth and, potentially, for the detection of life in the extraterrestrial realm. However, it is not always clear how exactly biomarkers reflect a paleoecosystem as their preservation may be influenced by increasing temperatures (T) and pressures (P) during burial. While a number of biomarker indices reflecting thermal maturity have been established, it is often less well constrained to which extent biomarker ratios used for paleoreconstruction are compromised by T and P processes. In this study we conducted hydrous pyrolysis of Green River Shale (GRS) kerogen in gold capsules for 2–2400 h at 300°C to assess the maturation behaviour of several compounds used as life tracers and for the reconstruction of paleoenvironments (n-alkanes, pristane, phytane, gammacerane, steranes, hopanes and cheilanthanes). Lignite samples were maturated in parallel with the GRS kerogen to obtain exact vitrinite reflectance data at every sampling point. Our experiment confirms the applicability of biomarker-based indices and ratios as maturity indicators (e.g. total cheilanthanes/hopanes ratio; sterane and hopane isomerization indices). However, several biomarker ratios that are commonly used for paleoreconstructions (e.g. pristane/phytane, pristane/n-C₁₇, phytane/n-C₁₈ and total steranes/hopanes) were considerably affected by differences in the thermal degradation behaviour of the respective compounds. Short-term experiments (48 h) performed at 400°C also revealed that biomarkers >C₁₅ (especially steranes and hopanes) and ‘biological’ chain length preferences for n-alkanes are vanished at a vitrinite reflectance between 1.38 and 1.83% R_O. Our data highlight that ‘thermal taphonomy’ effects have to be carefully considered in the interpretation of biomarkers in ancient rocks and, potentially, extraterrestrial materials.