238U/235U measurement in single-zircon crystals: Implications for the Hadean environment, magmatic differentiation and geochronology

François L.H. Tissot, Mauricio Ibanez-Mejia, Patrick Boehnke, Nicolas Dauphas, David McGee, Timothy L. Grove, T. Mark Harrison

Research output: Contribution to journalArticlepeer-review

10 Scopus citations

Abstract

Owing to the challengingly small amounts of uranium (U) they contain, the isotopic composition (238U/235U) of single zircon grains has never been measured. Leveraging methods we designed for analysis of small sample amounts and modern MC-ICPMS instruments, we show that precise (±0.04 to ±0.25‰) single-zircon 238U/235U measurements are now possible. We report data for 31 single grains from the Jack Hills conglomerate, and 3 reference zircon localities (FC-1, R33 and Temora). Consistent with the reducing conditions implied by the small Ce anomalies of many Hadean zircon, Jack Hills grains display only small δ238U variations (from -0.60 to -0.12‰). The distribution is centered on the average chondritic and bulk continental crust value, arguing against the widespread existence of Oklo-type reactors in the early Earth. The subtle δ238U variations in Jack Hills zircons are more plausibly explained by a small (∼0.10%) mass-dependent equilibrium isotope fractionation between at least one U-bearing accessory mineral and silicate melts, during magmatic differentiation under reducing conditions. In contrast, the large δ238U difference between pooled titanite and pooled zircon fractions from the Fish Canyon Tuff sample suggests larger isotope effects during igneous fractional crystallization under oxidizing conditions (∼QFM+2), with preferential removal of 235U from the melt and into zircon, and/or other accessory phases. We estimate that ∼50% of zircon dated by the CA-ID-TIMS method would be amenable to single-grain U isotope measurements, making this method widely applicable to future studies. This would enable (i) improvements in precision and accuracy of U-Pb and Pb-Pb dates, (ii) accurate investigation of U-series disequilibrium contribution to U-Pb discordance, and (iii) accurate re-evaluation of U decay constants.

Original languageEnglish (US)
Pages (from-to)2035-2052
Number of pages18
JournalJournal of Analytical Atomic Spectrometry
Volume34
Issue number10
DOIs
StatePublished - Oct 2019
Externally publishedYes

ASJC Scopus subject areas

  • Analytical Chemistry
  • Spectroscopy

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