Implications for behavior of volatile elements during impacts—Zinc and copper systematics in sediments from the Ries impact structure and central European tektites          下载免费PDF全文

Zuzana Rodovská  Tomáš Magna  Karel Žák  Chizu Kato  Paul S. Savage  Frédéric Moynier  Roman Skála  Josef Ježek 《Meteoritics & planetary science》2017,52(10):2178-2192

Moldavites are tektites genetically related to the Ries impact structure, located in Central Europe, but the source materials and the processes related to the chemical fractionation of moldavites are not fully constrained. To further understand moldavite genesis, the Cu and Zn abundances and isotope compositions were measured in a suite of tektites from four different substrewn fields (South Bohemia, Moravia, Cheb Basin, Lusatia) and chemically diverse sediments from the surroundings of the Ries impact structure. Moldavites are slightly depleted in Zn (~10–20%) and distinctly depleted in Cu (>90%) relative to supposed sedimentary precursors. Moreover, the moldavites show a wide range in δ⁶⁶Zn values between 1.7 and 3.7‰ (relative to JMC 3‐0749 Lyon) and δ⁶⁵Cu values between 1.6 and 12.5‰ (relative to NIST SRM 976) and are thus enriched in heavy isotopes relative to their possible parent sedimentary sources (δ⁶⁶Zn = ?0.07 to +0.64‰; δ⁶⁵Cu = ?0.4 to +0.7‰). In particular, the Cheb Basin moldavites show some of the highest δ⁶⁵Cu values (up to 12.5‰) ever observed in natural samples. The relative magnitude of isotope fractionation for Cu and Zn seen here is opposite to oxygen‐poor environments such as the Moon where Zn is significantly more isotopically fractionated than Cu. One possibility is that monovalent Cu diffuses faster than divalent Zn in the reduced melt and diffusion will not affect the extent of Zn isotope fractionation. These observations imply that the capability of forming a redox environment may aid in volatilizing some elements, accompanied by isotope fractionation, during the impact process. The greater extent of elemental depletion, coupled with isotope fractionation of more refractory Cu relative to Zn, may also hinge on the presence of carbonyl species of transition metals and electromagnetic charge, which could exist in the impact‐induced high‐velocity jet of vapor and melts.  相似文献   

Isotopic fractionation of Cu in tektites   总被引：1，自引：0，他引：1  

Frederic Moynier  Christian Koeberl  Fred Jourdan 《Geochimica et cosmochimica acta》2010,74(2):799-271

Tektites are terrestrial natural glasses of up to a few centimeters in size that were produced during hypervelocity impacts on the Earth’s surface. It is well established that the chemical and isotopic composition of tektites is generally identical to that of the upper terrestrial continental crust. Tektites typically have very low water content, which has generally been explained by volatilization at high temperature; however, the exact mechanism is still debated. Because volatilization can fractionate isotopes, comparing the isotopic composition of volatile elements in tektites with those of their source rocks may help to understand the physical conditions during tektite formation.Interestingly, volatile chalcophile elements (e.g., Cd and Zn) seem to be the only elements for which isotopic fractionation is known so far in tektites. Here, we extend this study to Cu, another volatile chalcophile element. We have measured the Cu isotopic composition for 20 tektite samples from the four known different strewn fields. All of the tektites (except the Muong Nong-types) are enriched in the heavy isotopes of Cu (1.98 < δ⁶⁵Cu < 6.99) in comparison to the terrestrial crust (δ⁶⁵Cu ≈ 0) with no clear distinction between the different groups. The Muong Nong-type tektites and a Libyan Desert Glass sample are not fractionated (δ⁶⁵Cu ≈ 0) in comparison to the terrestrial crust. To refine the Cu isotopic composition of the terrestrial crust, we also present data for three geological reference materials (δ⁶⁵Cu ≈ 0).An increase of δ⁶⁵Cu with decreasing Cu abundance probably reflects that the isotopic fractionation occurred by evaporation during heating. A simple Rayleigh distillation cannot explain the Cu isotopic data and we suggest that the isotopic fractionation is governed by a diffusion-limited regime. Copper is isotopically more fractionated than the more volatile element Zn (δ^66/64Zn up to 2.49‰). This difference of behavior between Cu and Zn is predicted in a diffusion-limited regime, where the magnitude of the isotopic fractionation is regulated by the competition between the evaporative flux and the diffusive flux at the diffusion boundary layer. Due to the difference of ionic charge in silicates (Zn²⁺ vs. Cu⁺), Cu has a diffusion coefficient that is larger than that of Zn by at least two orders of magnitude. Therefore, the larger isotopic fractionation in Cu than in Zn in tektites is due to the significant difference in their respective chemical diffusivity.  相似文献   

2015 Nier Prize for Pierre Beck          下载免费PDF全文

Frédéric Moynier 《Meteoritics & planetary science》2015,50(8):1493-1494

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Theoretical and experimental investigation of nickel isotopic fractionation in species relevant to modern and ancient oceans     

Toshiyuki Fujii  Frédéric Moynier  Minori Abe 《Geochimica et cosmochimica acta》2011,75(2):469-7643

Nickel plays a central role as an enzyme co-factor in the metabolism of methanogenic Archaea. Methanogens can fractionate Ni isotopes during assimilation, opening the possibility of using the stable isotopic composition of Ni as a biomarker. However, other sources of Ni isotopic variations need to be evaluated before one can establish Ni isotopes as an unambiguous tracer of methanogenesis in the rock record. Equilibrium exchange of Ni between the different species present in the ocean is a potential source of isotopic fractionation. Through controlled laboratory experiments and theoretical calculations, we quantify equilibrium Ni isotope fractionation between different species relevant to the modern and ancient ocean: Ni(H₂O)₆²⁺, Ni(H₂O)₁₈²⁺, NiOH(H₂O)₅⁺, Ni(OH)₂(H₂O)₄, NiCl(H₂O)₅⁺, cis-NiCl₂(H₂O)₄, trans-NiCl₂(H₂O)₄, NiHS(H₂O)₅⁺, Ni(HS)₂(H₂O)₄, NiSO₄(H₂O)₄, NiHCO₃(H₂O)₄⁺, NiCO₃(H₂O)₄, and organic ligands (crown ether and oxalic acid). The magnitude of ligand-controlled Ni isotopic fractionation, approximately 1.25‰/amu (2.5‰ for the ⁶⁰Ni/⁵⁸Ni ratio), is similar to that previously measured in cultures of methanogenic Archaea.  相似文献   

Ab initio calculations of the Fe(II) and Fe(III) isotopic effects in citrates,nicotianamine, and phytosiderophore,and new Fe isotopic measurements in higher plants     

Frédéric Moynier  Toshiyuki Fujii  Kun Wang  Julien Foriel 《Comptes Rendus Geoscience》2013,345(5-6):230-240

Iron is one of the most abundant transition metal in higher plants and variations in its isotopic compositions can be used to trace its utilization. In order to better understand the effect of plant-induced isotopic fractionation on the global Fe cycling, we have estimated by quantum chemical calculations the magnitude of the isotopic fractionation between different Fe species relevant to the transport and storage of Fe in higher plants: Fe(II)-citrate, Fe(III)-citrate, Fe(II)-nicotianamine, and Fe(III)-phytosiderophore. The ab initio calculations show firstly, that Fe(II)-nicotianamine is ～3‰ (⁵⁶Fe/⁵⁴Fe) isotopically lighter than Fe(III)-phytosiderophore; secondly, even in the absence of redox changes of Fe, change in the speciation alone can create up to ～1.5‰ isotopic fractionation. For example, Fe(III)-phytosiderophore is up to 1.5‰ heavier than Fe(III)-citrate₂ and Fe(II)-nicotianamine is up to 1‰ heavier than Fe(II)-citrate. In addition, in order to better understand the Fe isotopic fractionation between different plant components, we have analyzed the iron isotopic composition of different organs (roots, seeds, germinated seeds, leaves and stems) from six species of higher plants: the dicot lentil (Lens culinaris), and the graminaceous monocots Virginia wild rye (Elymus virginicus), Johnsongrass (Sorghum halepense), Kentucky bluegrass (Poa pratensis), river oat (Uniola latifolia), and Indian goosegrass (Eleusine indica). The calculations may explain that the roots of strategy-II plants (Fe(III)-phytosiderophore) are isotopically heavier (by about 1‰ for the δ⁵⁶Fe) than the upper parts of the plants (Fe transported as Fe(III)-citrate in the xylem or Fe(II)-nicotianamine in the phloem). In addition, we suggest that the isotopic variations observed between younger and older leaves could be explained by mixing of Fe received from the xylem and the phloem.  相似文献   

Nuclear field shift in natural environments     

Frédéric Moynier  Toshiyuki Fujii  Gregory A. Brennecka  Sune G. Nielsen 《Comptes Rendus Geoscience》2013,345(3):150-159

The nuclear field shift (NFS) is an isotope shift in atomic energy levels caused by a combination of differences in nuclear size and shape and electron densities at the nucleus. The effect of NFS in isotope fractionation was theoretically established by Bigeleisen in 1996 [Bigeleisen J. (1996) J. Am. Chem. Soc. 118:3676–3680] and has been analytically measured in laboratory chemical exchange reactions. More recently, some isotopic variations of heavy elements (Hg, Tl, U) measured in natural systems as well as isotopic anomalies measured for lower-mass elements in meteorites have been attributed to the NFS effect. These isotopic variations open up new and exciting fields of investigations in Earth sciences. In this paper, we review the different natural systems in which NFS has been proposed to be the origin of isotopic variations.  相似文献   

Pb,Hf and Nd isotope compositions of the two Réunion volcanoes (Indian Ocean): A tale of two small-scale mantle “blobs”?     

Delphine Bosch  Janne Blichert-Toft  Frédéric Moynier  Bruce K. Nelson  Philippe Telouk  Pierre-Yves Gillot  Francis Albarède 《Earth and Planetary Science Letters》2008,265(3-4):748-765

Pb, Hf, Nd and Sr isotopes of basaltic lavas from the two Réunion Island volcanoes are reported in order to examine the origin of the sources feeding these volcanoes and to detect possible changes through time. Samples, chosen to cover the whole lifetime of the two volcanoes (from 2 Ma to present), yield a chemically restricted (compared to OIB lavas) but complex distribution. Réunion plume isotopic characteristics have been defined on the basis of the composition of uncontaminated shield-building lavas from the Piton de la Fournaise volcano. The average ?_Nd, ?_Hf, ⁸⁷Sr/⁸⁶Sr and ²⁰⁶Pb/²⁰⁴Pb, ²⁰⁷Pb/²⁰⁴Pb, and ²⁰⁸Pb/²⁰⁴Pb isotope ratios calculated for this component are + 4.4, + 9.1, 0.70411, 18.97, 15.59 and 39.03, respectively. In Pb–Pb isotope space, each volcano defines a distinct linear trend but slight variations are also detected within the various volcanic sequences. The Piton des Neiges volcano yields a distinct and significantly more scattered isotopic distribution than Piton de la Fournaise for both Pb, Hf and Nd isotope tracers. A principal component analysis of the Pb isotope data from Piton de la Fournaise reveals a major contribution of the C and EM-1 components (with a clear Dupal flavor) as main components for the modern Réunion plume. The same components have been identified for Piton des Neiges but with a stronger participation of a depleted mantle component and a weaker EM-1 contribution. The compositional change of the lavas erupted by the Piton des Neiges and Piton de la Fournaise volcanoes is attributed to the impingement of two small-scale blobs of plume material at the base of the Réunion lithosphere. Compared to other hot-spots worldwide, in particular Hawaii and Kerguelen, magmas beneath Réunion are generated from a considerably more homogeneous, compositionally more primitive plume higher in ²⁰⁶Pb. Although shallow-level contamination processes have been locally detected they did not alter significantly the composition of the plume magmas. This is tentatively attributed to mantle dynamics producing small, high-velocity blobs that ascend rapidly through the lithosphere, and to the lack of a well-developed magma chamber at depth in the lithosphere.  相似文献   

Identification of a meteoritic component using chromium isotopic composition of impact rocks from the Lonar impact structure,India     

Berengere Mougel  Frederic Moynier  Christian Koeberl  Daniel Wielandt  Martin Bizzarro 《Meteoritics & planetary science》2019,54(10):2592-2599

The existence of mass‐independent chromium isotope variability of nucleosynthetic origin in meteorites and their components provides a means to investigate potential genetic relationship between meteorites and planetary bodies. Moreover, chromium abundances are depleted in most surficial terrestrial rocks relative to chondrites such that Cr isotopes are a powerful tool to detect the contribution of various types of extra‐terrestrial material in terrestrial impactites. This approach can thus be used to constrain the nature of the bolide resulting in breccia and melt rocks in terrestrial impact structures. Here, we report the Cr isotope composition of impact rocks from the ~0.57 Ma Lonar crater (India), which is the best‐preserved impact structure excavated in basaltic target rocks. Results confirm the presence of a chondritic component in several bulk rock samples of up to 3%. The impactor that created the Lonar crater had a composition that was most likely similar to that of carbonaceous chondrites, possibly a CM‐type chondrite.  相似文献   

Europium isotopic variations in Allende CAIs and the nature of mass-dependent fractionation in the solar nebula     

Frédéric Moynier  Audrey Bouvier  Philippe Telouk  Francis Albarède 《Geochimica et cosmochimica acta》2006,70(16):4287-4294

We measured the ¹⁵³Eu/¹⁵¹Eu ratio by MC-ICP-MS for a terrestrial basalt, two terrestrial soils, and four meteorites (whole rocks and/or chondrules of Bjurböle, Forest City, Murchison, and Allende) and found no isotopic variations. By contrast, two CAI separates from two different pieces of Allende show a ¹⁵³Eu deficit of up to one per mil. Such a shortage in the heavy isotopes, which had also been identified in Allende CAIs for Sr [Patchett, P.J. 1980b. Sr isotopic fractionation in Allende chondrules: a reflection of solar nebular processes. Earth Planet. Sci. Lett.50, 181-188], cannot reflect evaporative fractionation. The lack of Sm isotope fractionation in the same samples further makes fractionation by purely kinetic processes an unlikely cause of the anomalous Eu isotopic composition. An alternative interpretation is condensation from a vapor already significantly depleted in Eu, but in such a scenario the fate of the missing material is unclear. We therefore prefer yet another interpretation, based on the low ionization potential of Eu (and Sr), in which electromagnetic separation of the ionized gas preferentially depletes the nebular gas in heavy isotopes.  相似文献   

Nuclear field shift effect as a possible cause of Te isotopic anomalies in the early solar system—An alternative explanation of Fehr et al. (2006 and 2009)     

Frédéric Moynier  Toshiyuki Fujii  Francis Albarède 《Meteoritics & planetary science》2009,44(11):1735-1742

Abstract— We explore the possibility that Te isotopic anomalies measured in Ca‐Al‐rich inclusions (Fehr et al. 2009) and in leachates of carbonaceous chondrites (Fehr et al. 2006) may be due to mass‐independent effects controlled by nuclear field shift rather than to nucleosynthetic processes. Fehr et al.'s spectrum of mass‐independent anomalies of Te isotopes shows a smooth correlation with mass number and nuclear charge distribution. Ratios of even to odd isotopes, as the ¹²⁵Te/¹²⁶Te ratio used by these authors for normalization are particularly prone to nuclear field shift effects. We show that the alternative normalization of isotopic ratios to ¹³⁰Te/¹²⁶Te strongly reduces the trend of isotopic fractionation with mass number, leaving only ¹²⁵Te as truly anomalous. For both normalizations (¹²⁵Te/¹²⁶Te and ¹³⁰Te/¹²⁶Te), Fehr et al.'s results fit the theory of Bigeleisen (1996), which suggests that the nuclear field shift effect can potentially account for the observed Te isotope abundances, as an alternative to nucleosynthetic processes. We propose that these mass‐independent effects may be acquired during accretion of sulfides from the solar nebula.  相似文献