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Mahan, B, Siebert J, Pringle EA, Moynier F.  2017.  Elemental partitioning and isotopic fractionation of Zn between metal and silicate and geochemical estimation of the S content of the Earth’s core. Geochimica et Cosmochimica Acta. 196:252-270.   10.1016/j.gca.2016.09.013   Abstract

Zinc metal–silicate fractionation provides experimental access to the conditions of core formation and Zn has been used to estimate the S contents of the Earth’s core and of the bulk Earth, assuming that they share similar volatility and that Zn was not partitioned into the Earth’s core. Therefore, Zn provides both direct and indirect information into the origin and eventual fate of volatile and siderophile elements on Earth. However, the partitioning of Zn between metal and silicate – as well as the associated isotopic fractionation – is not well known. We have conducted a suite of partitioning experiments to characterize Zn elemental partitioning and isotopic fractionation between metal and silicate as a function of time, temperature, and composition. Experiments were conducted at 2 GPa and temperatures from 1473 K to 2273 K in a piston cylinder apparatus, with run durations from 5 to 240 min for four distinct starting materials. Chemical and isotopic equilibrium is achieved within 10 min of experimental outset. Zinc metal–silicate isotopic fractionation displays no resolvable dependence on temperature, composition, or oxygen fugacity within the data set. Therefore, the Zn isotopic composition of silicate phases can be used as a proxy for bulk telluric bodies. Partitioning results from this study and data from literature were used to robustly parameterize Zn metal–silicate partitioning as a function of temperature, pressure, and redox state. Using this parametric characterization and viable formation conditions, we have estimated a range of Zn contents in the cores of iron meteorite parent bodies (i.e. iron meteorites) of 0.1–150 ppm, in good agreement with natural observations. We have also calculated the first geochemical estimates for the Zn contents of the Earth’s core and of the bulk Earth, at 242 ± 107 ppm and 114 ± 34 ppm (respectively), that consider the slightly siderophile behavior of Zn. These estimates of the Zn contents of the Earth’s core and bulk Earth are significantly higher than previous estimates 0–30 ppm and 24–47 ppm, respectively. Assuming similar volatility for S and Zn, a chondritic S/Zn ratio, and considering our new estimates, we have calculated a geochemical upper bound for the S content of the Earth’s core of 6.3 ± 1.9 wt%. This indicates that S may be a major contributor to the density deficit of the Earth’s core or that the S/Zn ratio for the Earth is non-chondritic.
! 2016 Elsevier Ltd. All rights reserved.

Mahan, B, Moynier F, Beck P, Pringle EA, Siebert J.  2018.  A history of violence: insights into post-accretionary heating in carbonaceous chondrites from volatile element abundances, Zn isotopes, and water contents. Geochimica et Cosmochimica Acta. 220:19-35.   10.1016/j.gca.2017.09.027   Abstract

Zinc metal–silicate fractionation provides experimental access to the conditions of core formation and Zn has been used to estimate the S contents of the Earth’s core and of the bulk Earth, assuming that they share similar volatility and that Zn was not partitioned into the Earth’s core. Therefore, Zn provides both direct and indirect information into the origin and eventual fate of volatile and siderophile elements on Earth. However, the partitioning of Zn between metal and silicate – as well as the associated isotopic fractionation – is not well known. We have conducted a suite of partitioning experiments to characterize Zn elemental partitioning and isotopic fractionation between metal and silicate as a function of time, temperature, and com- position. Experiments were conducted at 2 GPa and temperatures from 1473 K to 2273 K in a piston cylinder apparatus, with run durations from 5 to 240 min for four distinct starting materials. Chemical and isotopic equilibrium is achieved within 10 min of experimental outset. Zinc metal–silicate isotopic fractionation displays no resolvable dependence on temperature, composition, or oxygen fugacity within the data set. Therefore, the Zn isotopic composition of silicate phases can be used as a proxy for bulk telluric bodies. Partitioning results from this study and data from literature were used to robustly parameterize Zn metal–silicate partitioning as a function of temperature, pressure, and redox state. Using this parametric characterization and viable formation conditions, we have estimated a range of Zn contents in the cores of iron meteorite parent bodies (i.e. iron meteorites) of $0.1–150 ppm, in good agreement with natural observations. We have also calculated the first geochemical estimates for the Zn contents of the Earth’s core and of the bulk Earth, at 242 ± 107 ppm and 114 ± 34 ppm (respectively), that consider the slightly siderophile behavior of Zn. These estimates of the Zn contents of the Earth’s core and bulk Earth are significantly higher than previous estimates 0–30 ppm and 24–47 ppm, respectively. Assuming similar volatility for S and Zn, a chondritic S/Zn ratio, and considering our new estimates, we have calculated a geochemical upper bound for the S content of the Earth’s core of 6.3 ± 1.9 wt%. This indicates that S may be a major contributor to the density deficit of the Earth’s core or that the S/Zn ratio for the Earth is non-chondritic.

Mahan, B, Moynier F, Siebert J, Gueguen B, Agranier A, Pringle EA, Bollard J, Connelly J, Bizzarro M.  In Press.  Volatile element evolution of chondrules through time. Proceedings of the National Academy of Science USA.   10.1073/pnas.1807263115   Abstract

Chondrites and their main components, chondrules, are our guides into the evolution of the Solar System. Investigating the history of chondrules, including their volatile element history and the prevailing conditions of their formation, has implications not only for the understanding of chondrule formation and evolution but for that of larger bodies such as the terrestrial planets. Here we have determined the bulk chemical composition—rare earth, refractory, main group, and volatile element contents—of a suite of chondrules previously dated using the Pb−Pb system. The volatile element contents of chondrules increase with time from ∼1 My after Solar System formation, likely the result of mixing with a volatile-enriched component during chondrule recycling. Variations in the Mn/Na ratios signify changes in redox conditions over time, suggestive of decoupled oxygen and volatile element fugacities, and indicating a decrease in oxygen fugacity and a relative increase in the fugacities of in-fluxing volatiles with time. Within the context of terrestrial planet formation via pebble accretion, these observations corroborate the early formation of Mars under relatively oxidizing conditions and the protracted growth of Earth under more reducing conditions, and further suggest that water and volatile elements in the inner Solar System may not have arrived pairwise.

Moynier, F, Pringle EA, Bouvier A, Moureau J.  2015.  Barium stable isotope composition of the Earth, meteorites, and calcium–aluminum-rich inclusions. Chemical Geology. 413:1-6.   10.1016/j.chemgeo.2015.08.002   Abstract

High-precision stable Ba isotope ratios are reported in a variety of terrestrial samples, undifferentiated primitive meteorites, and calcium–aluminum-rich inclusions (CAIs) from the Allende chondrite. All whole-rock terrestrial and meteorite samples are isotopically indistinguishable at a 50 parts per million (ppm) level per atomic mass unit (amu). Three CAIs are isotopically light, with δ138/137Ba (permil deviation of the 138Ba/137Ba ratio from a terrestrial standard) values down to −0.6‰ compared to whole-rock meteorites, whereas the matrix is enriched in heavy isotopes (δ138/137Ba: +0.2‰). Similar light isotope enrichments in CAIs have been previously observed for Eu, Sr, and Ca, while for most other elements CAIs are enriched in the heavier isotopes (e.g. Mg, Fe). Kinetic isotopic fractionation is a possible explanation for the enrichment in the lightest isotopes, either by condensation from a vapor phase enriched in light isotopes by kinetic effects or by kinetic fractionation during non-equilibrium condensation of an undercooled gas as suggested for Ca isotopes. However, the common property of Ba, Eu, and Sr is that they all have a low first ionization potential. We suggest that electromagnetic sorting of ionized species in the early Solar System is a possible alternative mechanism to explain the depletion in heavy isotopes observed in refractory inclusions for those elements.