High precision noble gas measurements of hydrothermal quartz reveal variable loss rate of Xe from the Archean atmosphere

Determining the composition of the Archean atmosphere and oceans is vital to understanding the environmental conditions that existed on the surface of the early Earth. The analysis of atmospheric remnants in fluid inclusions trapped in Archean-aged samples has shown that the Xe isotopic signature of the Archean atmosphere progressively evolved via mass-dependent fractionation, arriving at a modern atmospheric composition around the Archean-Proterozoic transition. The mechanisms driving this evolution are however not well constrained, and it is not yet clear whether the evolution proceeded continuously or via episodic bursts. Providing further constraints on the evolution of Xe in the Archean atmosphere is hampered by the limited amounts of atmospheric gas trapped within fluid inclusions during mineral formation, which impacts the precision at which the Archean atmosphere can be determined. Here, we develop a new crush-and-accumulate extraction technique that enables the heavy noble gases (Ar, Kr and Xe) released from crushing large quantities of hydrothermal quartz to be accumulated and analysed to a higher precision than was previously possible. Using this new technique, we re-evaluate the composition of atmospheric gases trapped within fluid inclusions of 3.3 Ga quartz samples from Barberton, South Africa. We find that the Xe isotopic signature is fractionated by +10.3 ± 1.0‰u−1 (2 SE) relative to modern atmosphere, which is within uncertainty of, but slightly lower than, the previous determination of 12.9 ± 2.4‰u−1 for this sample (Avice et al. 2017). We show for the first time that the Kr/Xe ratio measured within Archean quartz samples is enriched in Xe compared to the modern atmosphere, demonstrating that the atmosphere has lost Xe since the Archean. This further reinforces the proposal of atmospheric escape as the primary mechanism for Earth's Xe loss. We further show that the atmospheric Kr/Xe and Xe isotope fractionation recorded in the Barberton quartz at 3.3 Ga is incompatible with a model describing atmospheric loss at a continuous rate under a constant fractionation factor. This gives credence to numerical models of hydrodynamic escape, which suggest that Xe was lost from the Archean atmosphere in episodic bursts rather than at a constant rate. Refining the evolution curve of atmospheric Xe isotopes using the new technique presented here has the potential to shed light on discrete atmospheric events that punctuated the evolution of the Archean Earth and accompanied the evolution of life.SCOPUS: ar.j