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Magmatic outgassing of volatiles from Earth's interior probably played a critical part in determining the composition of the earliest atmosphere, more than 4,000 million years (Myr) ago. Given an elemental inventory of hydrogen, carbon, nitrogen, oxygen and sulphur, the identity of molecular species in gaseous volcanic emanations depends critically on the pressure (fugacity) of oxygen. Reduced melts having oxygen fugacities close to that defined by the iron-wüstite buffer would yield volatile species such as CH(4), H(2), H(2)S, NH(3) and CO, whereas melts close to the fayalite-magnetite-quartz buffer would be similar to present-day conditions and would be dominated by H(2)O, CO(2), SO(2) and N(2) (refs 1-4). Direct constraints on the oxidation state of terrestrial magmas before 3,850 Myr before present (that is, the Hadean eon) are tenuous because the rock record is sparse or absent. Samples from this earliest period of Earth's history are limited to igneous detrital zircons that pre-date the known rock record, with ages approaching ∼4,400 Myr (refs 5-8). Here we report a redox-sensitive calibration to determine the oxidation state of Hadean magmatic melts that is based on the incorporation of cerium into zircon crystals. We find that the melts have average oxygen fugacities that are consistent with an oxidation state defined by the fayalite-magnetite-quartz buffer, similar to present-day conditions. Moreover, selected Hadean zircons (having chemical characteristics consistent with crystallization specifically from mantle-derived melts) suggest oxygen fugacities similar to those of Archaean and present-day mantle-derived lavas as early as ∼4,350 Myr before present. These results suggest that outgassing of Earth's interior later than ∼200 Myr into the history of Solar System formation would not have resulted in a reducing atmosphere.

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The widespread presence of ribonucleic acid (RNA) catalysts and cofactors in the Earth′s biosphere today suggests that RNA was the first biopolymer to support Darwinian evolution. However, most “path‐hypotheses” to generate building blocks for RNA require reduced nitrogen‐containing compounds not made in useful amounts in the CO2−N2−H2O atmospheres of the Hadean. We review models for Earth′s impact history that invoke a single ∼1023 kg impactor (Moneta) to account for measured amounts of platinum, gold, and other siderophilic (“iron‐loving”) elements on the Earth and Moon. If it were the last sterilizing impactor, by reducing the atmosphere but not the mantle Moneta, would have opened a “window of opportunity” for RNA synthesis, a period when RNA precursors rained from the atmosphere onto land holding oxidized minerals that stabilize advanced RNA precursors and RNA. Surprisingly, this combination of physics, geology, and chemistry suggests a time when RNA formation was most probable, ∼120±100 million years after Moneta′s impact, or ∼4.36±0.1 billion years ago. Uncertainties in this time are driven by uncertainties in rates of productive atmosphere loss and amounts of sub‐aerial land.

[1] We report zircon oxygen isotope ratios and reconnaissance Ti-in-zircon concentrations, guided by cathodoluminescence image studies, for detrital zircons up to 4.34 Ga from the Narryer Gneiss Complex of Western Australia. Zircon oxygen isotope results bolster the view that some Hadean (>3.85 Ga) zircon source melts were enriched in heavy oxygen, a sensitive proxy for melt contamination by sediments altered in liquid water. Zircon crystallization temperatures calculated from Ti concentration in pre-3.8 Ga zircons yield values around 680°C in all cases except for one lower value in a 4.0 Ga grain. Elevated zircon d 18O values reported here and elsewhere, combined with low minimum-melt crystallization temperatures, and analysis of zircon/melt partitioning of rare earth elements (REEs) provide mutually consistent lines of evidence that the Hadean Earth supported an evolved rock cycle which included formation of granitic water-saturated melts, extensive continental crust, hydrosphere-lithosphere interactions, and sediment recycling within the first 150 million years of planet formation.

Hydrosphere interactions and alteration of the terrestrial crust likely played a critical role in shaping Earth’s surface, and in promoting prebiotic reactions leading to life, before 4.03 Ga (the Hadean Eon). The identity of aqueously altered material strongly depends on lithospheric cycling of abundant and water-soluble elements such as Si and O. However, direct constraints that define the character of Hadean sedimentary material are absent because samples from this earliest eon are limited to detrital zircons (ZrSiO4). Here we show that concurrent measurements of Si and O isotope ratios in Phanerozoic and detrital pre-3.0 Ga zircon constrain the composition of aqueously altered precursors incorporated into their source melts. Phanerozoic zircon from (S)edimentary-type rocks contain heterogeneous δ18O and δ30Si values consistent with assimilation of metapelitic material, distinct from the isotopic character of zircon from (I)gneous- and (A)norogenic-type rocks. The δ18O values of detrital Archean zircons are heterogeneous, although yield Si isotope compositions like mantle-derived zircon. Hadean crystals yield elevated δ18O values (vs. mantle zircon) and δ30Si values span almost the entire range observed for Phanerozoic samples. Coupled Si and O isotope data represent a constraint on Hadean weathering and sedimentary input into felsic melts including remelting of amphibolites possibly of basaltic origin, and fractional addition of chemical sediments, such as cherts and/or banded iron formations (BIFs) into source melts. That such sedimentary deposits were extensive enough to change the chemical signature of intracrustal melts suggests they may have been a suitable niche for (pre)biotic chemistry as early as 4.1 Ga.

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