Letter

Halogens in chondritic meteorites and terrestrial accretion

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Abstract

Volatile element delivery and retention played a fundamental part in Earth’s formation and subsequent chemical differentiation. The heavy halogens—chlorine (Cl), bromine (Br) and iodine (I)—are key tracers of accretionary processes owing to their high volatility and incompatibility, but have low abundances in most geological and planetary materials. However, noble gas proxy isotopes produced during neutron irradiation provide a high-sensitivity tool for the determination of heavy halogen abundances. Using such isotopes, here we show that Cl, Br and I abundances in carbonaceous, enstatite, Rumuruti and primitive ordinary chondrites are about 6 times, 9 times and 15–37 times lower, respectively, than previously reported and usually accepted estimates1. This is independent of the oxidation state or petrological type of the chondrites. The ratios Br/Cl and I/Cl in all studied chondrites show a limited range, indistinguishable from bulk silicate Earth estimates. Our results demonstrate that the halogen depletion of bulk silicate Earth relative to primitive meteorites is consistent with the depletion of lithophile elements of similar volatility. These results for carbonaceous chondrites reveal that late accretion, constrained to a maximum of 0.5 ± 0.2 per cent of Earth’s silicate mass2,3,4,5, cannot solely account for present-day terrestrial halogen inventories6,7. It is estimated that 80–90 per cent of heavy halogens are concentrated in Earth’s surface reservoirs7,8 and have not undergone the extreme early loss observed in atmosphere-forming elements9. Therefore, in addition to late-stage terrestrial accretion of halogens and mantle degassing, which has removed less than half of Earth’s dissolved mantle gases10, the efficient extraction of halogen-rich fluids6 from the solid Earth during the earliest stages of terrestrial differentiation is also required to explain the presence of these heavy halogens at the surface. The hydropilic nature of halogens, whereby they track with water, supports this requirement, and is consistent with volatile-rich or water-rich late-stage terrestrial accretion5,11,12,13,14.

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Acknowledgements

We acknowledge the following organisations and individuals for the provision of samples: NASA Antarctic Meteorite Working Group (MIL 07139, MIL 07028 and ALH 77295); P. Heck, Chicago Field Museum (Indarch); Izikio Museum of South Africa (St Marks); M. Boyet (SAH 97096); M. Schönbächler (GRA 06100, EET 92159, Murray, Orgueil); and A. Ruzicka (NWA 753 and NWA 755). We thank J. Cowpe for assistance with noble gas measurements, K. J. Theis for laboratory assistance and W. Akram for help with sample preparation. H.B. acknowledges support from the PlanetS National Center of Competence in Research (NCCR) of the Swiss National Science Foundation. This project was funded by the European Research Council FP7 ‘NOBLE’ grant number 267692.

Author information

Affiliations

  1. School of Earth and Environmental Sciences, University of Manchester, Manchester M13 9PL, UK

    • Patricia L. Clay
    • , Ray Burgess
    •  & Lorraine Ruzié-Hamilton
  2. Institute for Geochemistry and Petrology, ETH Zürich, Clausiusstrasse 25, 8092 Zürich, Switzerland

    • Henner Busemann
  3. Institute for Mineralogy and Petrography, University of Innsbruck, Innrain 52, A-6020 Innsbruck, Austria

    • Bastian Joachim
  4. Scripps Institution of Oceanography, University of California San Diego, La Jolla, California 92093-0244, USA

    • James M. D. Day
  5. Department of Earth Sciences, University of Oxford, South Parks Road, Oxford OX1 3AN, UK.

    • Christopher J. Ballentine

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Contributions

P.L.C., R.B. and C.J.B. designed the study. P.L.C. and H.B. acquired the samples (with material also provided by J.M.D.D.). P.L.C. analysed the samples and wrote the first draft of the manuscript. All authors contributed to the discussion of the results, interpretation of the data, and editing of the manuscript.

Competing interests

The authors declare no competing financial interests.

Corresponding author

Correspondence to Patricia L. Clay.

Reviewer Information Nature thanks H. Becker and the other anonymous reviewer(s) for their contribution to the peer review of this work.

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