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Pringle, EA, Moynier F, Savage PS, Jackson MG, Moreira M, Day JMD.  2016.  Silicon isotopes reveal recycled altered oceanic crust in the mantle sources of Ocean Island Basalts. Geochimica et Cosmochimica Acta. 189:282-295.   10.1016/j.gca.2016.06.008   AbstractWebsite

The study of silicon (Si) isotopes in Ocean Island Basalts (OIB) has the potential to discern between different models for the origins of geochemical heterogeneities in the mantle. Relatively large (∼several per mil per atomic mass unit) Si isotope fractionation occurs in low-temperature environments during biochemical and geochemical precipitation of dissolved Si, where the precipitate is preferentially enriched in the lighter isotopes relative to the dissolved Si. In contrast, only a limited range (∼tenths of a per mil) of Si isotope fractionation has been observed from high-temperature igneous processes. Therefore, Si isotopes may be useful as tracers for the presence of crustal material within OIB mantle source regions that experienced relatively low-temperature surface processes in a manner similar to other stable isotope systems, such as oxygen. Characterizing the isotopic composition of the mantle is also of central importance to the use of the Si isotope system as a basis for comparisons with other planetary bodies (e.g., Moon, Mars, asteroids).

Here we present the first comprehensive suite of high-precision Si isotope data obtained by MC-ICP-MS for a diverse suite of OIB. Samples originate from ocean islands in the Pacific, Atlantic, and Indian Ocean basins and include representative end-members for the EM-1, EM-2, and HIMU mantle components. On average, δ30Si values for OIB (−0.32 ± 0.09‰, 2 sd) are in general agreement with previous estimates for the δ30Si value of Bulk Silicate Earth (−0.29 ± 0.07‰, 2 sd; Savage et al., 2014). Nonetheless, some small systematic variations are present; specifically, most HIMU-type (Mangaia; Cape Verde; La Palma, Canary Islands) and Iceland OIB are enriched in the lighter isotopes of Si (δ30Si values lower than MORB), consistent with recycled altered oceanic crust and lithospheric mantle in their mantle sources.

Pringle, EA, Moynier F, Beck P, Paniello R, Hezel DC.  2017.  The origin of volatile element depletion in early solar system material: Clues from Zn isotopes in chondrules. Earth and Planetary Science Letters. 468:62-71.   10.1016/j.epsl.2017.04.002   Abstract

Volatile lithophile elements are depleted in the different planetary materials to various degrees, but the origin of these depletions is still debated. Stable isotopes of moderately volatile elements such as Zn can be used to understand the origin of volatile element depletions. Samples with significant volatile element depletions, including the Moon and terrestrial tektites, display heavy Zn isotope compositions (i.e. enrichment of 66Zn vs. 64Zn), consistent with kinetic Zn isotope fractionation during evaporation. However, Luck et al. (2005) found a negative correlation between δ66Zn and 1/[Zn] between CI, CM, CO, and CV chondrites, opposite to what would be expected if evaporation caused the Zn abundance variations among chondrite groups.

We have analyzed the Zn isotope composition of multiple samples of the major carbonaceous chondrite classes: CI (1), CM (4), CV (2), CO (4), CB (2), CH (2), CK (4), and CK/CR (1). The bulk chondrites define a negative correlation in a plot of δ66Zn vs 1/[Zn], confirming earlier results that Zn abundance variations among carbonaceous chondrites cannot be explained by evaporation. Exceptions are CB and CH chondrites, which display Zn systematics consistent with a collisional formation mechanism that created enrichment in heavy Zn isotopes relative to the trend defined by CI–CK.

We further report Zn isotope analyses of chondrite components, including chondrules from Allende (CV3) and Mokoia (CV3), as well as an aliquot of Allende matrix. All chondrules are enriched in light Zn isotopes (∼500 ppm on 66Zn/64Zn) relative to the bulk, contrary to what would be expected if Zn were depleted during evaporation, on the other hand the matrix has a complementary heavy isotope composition. We report sequential leaching experiments in un-equilibrated ordinary chondrites, which show sulfides are isotopically heavy compared to silicates and the bulk meteorite by ca. +0.65 per mil on 66Zn/64Zn. We suggest isotopically heavy sulfides were removed from either chondrules or their precursors, thereby producing the light Zn isotope enrichments in chondrules.

Pringle, EA, Savage PS, Badro J, Barrat J-A, Moynier F.  2013.  Redox state during core formation on asteroid 4-Vesta. Earth and Planetary Science Letters. 373:75-82.   doi:10.1016/j.epsl.2013.04.012   Abstract

Core formation is the main differentiation event in the history of a planet. However, the chemical composition of planetary cores and the physicochemical conditions prevailing during core formation remain poorly understood. The asteroid 4-Vesta is the smallest extant planetary body known to have differentiated a metallic core. Howardite, Eucrite, Diogenite (HED) meteorites, which are thought to sample 4-Vesta, provide us with an opportunity to study core formation in planetary embryos.

Partitioning of elements between the core and mantle of a planet fractionates their isotopes according to formation conditions. One such element, silicon, shows large isotopic fractionation between metal and silicate, and its partitioning into a metallic core is only possible under very distinctive conditions of pressure, oxygen fugacity and temperature. Therefore, the silicon isotope system is a powerful tracer with which to study core formation in planetary bodies. Here we show through high- precision measurement of Si stable isotopes that HED meteorites are significantly enriched in the heavier isotopes compared to chondrites. This is consistent with the core of 4-Vesta containing at least 1 wt% of Si, which in turn suggests that 4-Vesta's differentiation occurred under more reducing conditions (ΔIW∼−4) than those previously suggested from analysis of the distribution of moderately siderophile elements in HEDs.

Pringle, EA, Moynier F.  2017.  Rubidium isotopic composition of the Earth, meteorites, and the Moon: Evidence for the origin of volatile loss during planetary accretion. Earth and Planetary Science Letters. 473:62-70.   10.1016/j.epsl.2017.05.033   Abstract

Understanding the origin of volatile element variations in the inner Solar System has long been a goal of cosmochemistry, but many early studies searching for the fingerprint of volatile loss using stable isotope systems failed to find any resolvable variations.

An improved method for the chemical purification of Rb for high-precision isotope ratio measurements by multi-collector inductively-coupled-plasma mass-spectrometry. This method has been used to measure the Rb isotopic composition for a suite of planetary materials, including carbonaceous, ordinary, and enstatite chondrites, as well as achondrites (eucrite, angrite), terrestrial igneous rocks (basalt, andesite, granite), and Apollo lunar samples (mare basalts, alkali suite). Volatile depleted bodies (e.g. HED parent body, thermally metamorphosed meteorites) are enriched in the heavy isotope of Rb by up to several per mil compared to chondrites, suggesting volatile loss by evaporation at the surface of planetesimals. In addition, the Moon is isotopically distinct from the Moon in Rb. The variations in Rb isotope compositions in the volatile-poor samples are attributed to volatile loss from planetesimals during accretion. This suggests that either the Rb (and other volatile elements) were lost during or following the giant impact or by evaporation earlier during the accretion history of Theia.

Pringle, EA, Savage PS, Jackson MG, Barrat JA, Moynier F.  2013.  Si isotope homogeneity of the Solar Nebula. The Astrophysical Journal. 779:123-127.   10.1088/0004-637X/779/2/123   Abstract

The presence or absence of variations in the mass-independent abundances of Si isotopes in bulk meteorites provides important clues concerning the evolution of the early solar system. No Si isotopic anomalies have been found within the level of analytical precision of 15 ppm in 29Si/28Si across a wide range of inner solar system materials, including terrestrial basalts, chondrites, and achondrites. A possible exception is the angrites, which may exhibit small excesses of 29Si. However, the general absence of anomalies suggests that primitive meteorites and differentiated planetesimals formed in a reservoir that was isotopically homogenous with respect to Si. Furthermore, the lack of resolvable anomalies in the calcium–aluminum-rich inclusion measured here suggests that any nucleosynthetic anomalies in Si isotopes were erased through mixing in the solar nebula prior to the formation of refractory solids. The homogeneity exhibited by Si isotopes may have implications for the distribution of Mg isotopes in the solar nebula. Based on supernova nucleosynthetic yield calculations, the expected magnitude of heavy-isotope overabundance is larger for Si than for Mg, suggesting that any potential Mg heterogeneity, if present, exists below the 15 ppm level.

Pringle, EA, Moynier F, Savage PS, Badro J, Barrat JA.  2014.  Silicon isotopes in angrites and volatile loss in planetesimals. Proceedings of the National Academy of Sciences USA. 111(48):17029–17032.   10.1073/pnas.1418889111   Abstract

Inner solar system bodies, including the Earth, Moon, and asteroids, are depleted in volatile elements relative to chondrites. Hypotheses for this volatile element depletion include incomplete condensation from the solar nebula and volatile loss during energetic impacts. These processes are expected to each produce characteristic stable isotope signatures. However, processes of planetary differentiation may also modify the isotopic composition of geochemical reservoirs. Angrites are rare meteorites that crystallized only a few million years after calcium–aluminum-rich inclusions and exhibit extreme depletions in volatile elements relative to chondrites, making them ideal samples with which to study volatile element depletion in the early solar system. Here we present high-precision Si isotope data that show angrites are enriched in the heavy isotopes of Si relative to chondritic meteorites by 50–100 ppm/amu. Silicon is sufficiently volatile such that it may be isotopically fractionated during incomplete condensation or evaporative mass loss, but theoretical calculations and experimental results also predict isotope fractionation under specific conditions of metal–silicate differentiation. We show that the Si isotope composition of angrites cannot be explained by any plausible core formation scenario, but rather reflects isotope fractionation during impact-induced evaporation. Our results indicate planetesimals initially formed from volatile-rich material and were subsequently depleted in volatile elements during accretion.