Archaean atmospheric evolution: evidence from the Witwatersrand gold fields, South Africa

The Witwatersrand gold fields in South Africa, the worldʹs largest gold-producing province, play a pivotal role in the reconstruction of the Archaean atmosphere and hydrosphere. Past uncertainties on the genetic model for the gold caused confusion in the debate on Archaean palaeoenvironmental conditions. The majority of Witwatersrand gold occurs together with pyrite, uraninite and locally bitumen, on degradational surfaces of fluvial conglomerates that were laid down between 2.90 and 2.84 Ga in the Central Rand Basin. Although most of the gold appears as a precipitate within, or associated with, post-depositional hydrothermal phases and along microfractures, available microtextural, mineralogical, geochemical and isotopic data all indicate that this hydrothermal gold, analogous to some pyrite and uraninite, was derived from the local mobilisation of detrital particles. Some of the key pieces of evidence are a significant correlation of the gold, pyrite and uraninite with other heavy minerals as well as sedimentary lithofacies, local preservation of in-situ gold micronuggets and abundant rounded forms of pyrite and uraninite, compositional heterogeneity on a microscale of the gold as well as the rounded pyrite and uraninte, and radiometric age data that indicate an age of the gold, pyrite and uraninite that is older than the maximum age of deposition for the host sediment. None of these observations/data is compatible with any of the suggested hydrothermal models, in which auriferous fluids were introduced from an external source into the host rock succession after sediment deposition. In contrast, those arguments, used in favour of hydrothermal models, emphasise the microtextural position of most of the gold, which highlights the undisputed hydrothermal nature of that gold in its present position, but does not explain its ultimate source. Furthermore, the macro-scale setting of the stratiform ore deposits is in stark contrast to any known type of epigenetic, hydrothermal gold deposit. Consequently, the best-fit genetic model involves post-depositional textural and mineralogical modification of original fluvial placer deposits. Kaapvaal Craton, Witwatersrand-type mineralisation is recorded over an extended period of time from 3074 to 2642 Ma. Rounded pyrite is common in the coarser grained fractions of the siliciclastic basin fill. A lack of sulphur isotope fractionation and typical magmatic δ34S values support its detrital origin. Together with rounded uraninite, which is particularly abundant in the older beds, it provides important constraints on the redox potential of the Meso- to Neoarchaean (3.1–2.6 Ga) atmosphere and hydrosphere. In combination with eukaryotic steroids documented from the Pilbara Craton, Australia, the ambient Neoarchaean oxygen fugacity is calculated as having been approximately 10−3, in equilibrium with a relatively acidic hydrosphere (pH=6). This is in agreement with the preservation of mass-independent S isotope fractionation, which provides independent support for an anoxic atmosphere and which has so far been recorded predominantly from sediments older than 2.3 Ga. An acidic meteoric palaeoenvironment is supported by intense chemical weathering below erosional unconformity surfaces in the Witwatersrand Basin. In contrast to the pyrite-bearing fluvial and near-shore shallow marine deposits, marine shale deposits contain magnetite. This supports the postulated reducing environment but also highlights total sulphur concentrations in the ancient ocean that were orders of magnitude lower than in modern ocean water.