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1.
The Li isotopic composition of the upper continental crust is estimated from the analyses of well-characterized shales, loess, granites and upper crustal composites (51 samples in total) from North America, China, Europe, Australia and New Zealand. Correlations between Li, δ7Li, and chemical weathering (as measured by the Chemical Index of Alteration (CIA)), and δ7Li and the clay content of shales (as measured by Al2O3/SiO2), reflect uptake of heavy Li from the hydrosphere by clays. S-type granites from the Lachlan fold belt (-1.1 to -1.4‰) have δ7Li indistinguishable from their associated sedimentary rocks (-0.7 to 1.2‰), and show no variation in δ7Li throughout the differentiation sequence, suggesting that isotopic fractionation during crustal anatexis and subsequent differentiation is less than analytical uncertainty (±1‰, 2σ). The isotopically light compositions for both I- and S-type granites from the Lachlan fold belt (-2.5 to + 2.7 ‰) and loess from around the world (-3.1 to + 4.5‰) reflect the influence of weathering in their source regions. Collectively, these lithologies possess a limited range of Li isotopic compositions (δ7Li of −5‰ to + 5‰), with an average (δ7Li of 0 ± 2‰ at 1σ) that is representative of the average upper continental crust. Thus, the Li isotopic composition of the upper continental crust is lighter than the average upper mantle (δ7Li of + 4 ± 2‰), reflecting the influence of weathering on the upper crustal composition. The concentration of Li in the upper continental crust is estimated to be 35 ± 11 ppm (2σ), based on the average loess composition and correlations between insoluble elements (Ti, Nb, Ta, Ga and Al2O3, Th and HREE) and Li in shales. This value is somewhat higher than previous estimates (∼20 ppm), but is probably indistinguishable when uncertainties in the latter are accounted for.  相似文献   

2.
We present whole rock Li and Mg isotope analyses of 33 ultramafic xenoliths from the terrestrial mantle, which we compare with analyses of 30 (mostly chondritic) meteorites. The accuracy of our new Mg isotope ratio measurement protocol is substantiated by a combination of standard addition experiments, the absence of mass independent effects in terrestrial samples and our obtaining identical values for rock standards using two different separation chemistries and three different mass-spectrometric introduction systems. Carbonaceous, ordinary and enstatite chondrites have irresolvable mean stable Mg isotopic compositions (δ25Mg = −0.14 ± 0.06; δ26Mg = −0.27 ± 0.12‰, 2SD), but our enstatite chondrite samples have lighter δ7Li (by up to ∼3‰) than our mean carbonaceous and ordinary chondrites (3.0 ± 1.5‰, 2SD), possibly as a result of spallation in the early solar system. Measurements of equilibrated, fertile peridotites give mean values of δ7Li = 3.5 ± 0.5‰, δ25Mg = −0.10 ± 0.03‰ and δ26Mg = −0.21 ± 0.07‰. We believe these values provide a useful estimate of the primitive mantle and they are within error of our average of bulk carbonaceous and ordinary chondrites. A fuller range of fresh, terrestrial, ultramafic samples, covering a variety of geological histories, show a broad positive correlation between bulk δ7Li and δ26Mg, which vary from −3.7‰ to +14.5‰, and −0.36‰ to + 0.06‰, respectively. Values of δ7Li and δ26Mg lower than our estimate of primitive mantle are strongly linked to kinetic isotope fractionation, occurring during transport of the mantle xenoliths. We suggest Mg and Li diffusion into the xenoliths is coupled to H loss from nominally anhydrous minerals following degassing. Diffusion models suggest that the co-variation of Mg and Li isotopes requires comparable diffusivities of Li and Mg in olivine. The isotopically lightest samples require ∼5-10 years of diffusive ingress, which we interpret as a time since volatile loss in the host magma. Xenoliths erupted in pyroclastic flows appear to have retained their mantle isotope ratios, likely as a result of little prior degassing in these explosive events. High δ7Li, coupled with high [Li], in rapidly cooled arc peridotites may indicate that these samples represent fragments of mantle wedge that has been metasomatised by heavy, slab-derived fluids. If such material is typically stirred back into the convecting mantle, it may account for the heavy δ7Li seen in some oceanic basalts.  相似文献   

3.
Komatiites from Alexo, Canada, are well preserved and represent high-degree partial mantle melts (∼50%). They are thus well suited for investigating the Mg and Fe isotopic compositions of the Archean mantle and the conditions of magmatic differentiation in komatiitic lavas. High precision Mg and Fe isotopic analyses of 22 samples taken along a 15-m depth profile in a komatiite flow are reported. The δ25Mg and δ26Mg values of the bulk flow are −0.138 ± 0.021‰ and −0.275 ± 0.042‰, respectively. These values are indistinguishable from those measured in mantle peridotites and chondrites, and represent the best estimate of the composition of the silicate Earth from analysis of volcanic rocks. Excluding the samples affected by secondary Fe mobilization, the δ56Fe and δ57Fe values of the bulk flow are +0.044 ± 0.030‰, and +0.059 ± 0.044‰, respectively. These values are consistent with a near-chondritic Fe isotopic composition of the silicate Earth and minor fractionation during komatiite magma genesis. In order to explain the early crystallization of pigeonite relative to augite in slowly cooled spinifex lavas, it was suggested that magmas trapped in the crystal mush during spinifex growth differentiated by Soret effect, which should be associated with large and coupled variations in the isotopic compositions of Mg and Fe. The lack of variations in Mg and Fe isotopic ratios either rules out the Soret effect in the komatiite flow or the effect is effaced as the solidification front migrates downward through the flow crust. Olivine separated from a cumulate sample has light δ56Fe and slightly heavy δ26Mg values relative to the bulk flow, which modeling shows can be explained by kinetic isotope fractionation associated with Fe-Mg inter-diffusion in olivine. Such variations can be used to identify diffusive processes involved in the formation of zoned minerals.  相似文献   

4.
We present high-precision measurements of Mg and Fe isotopic compositions of olivine, orthopyroxene (opx), and clinopyroxene (cpx) for 18 lherzolite xenoliths from east central China and provide the first combined Fe and Mg isotopic study of the upper mantle. δ56Fe in olivines varies from 0.18‰ to −0.22‰ with an average of −0.01 ± 0.18‰ (2SD, n = 18), opx from 0.24‰ to −0.22‰ with an average of 0.04 ± 0.20‰, and cpx from 0.24‰ to −0.16‰ with an average of 0.10 ± 0.19‰. δ26Mg of olivines varies from −0.25‰ to −0.42‰ with an average of −0.34 ± 0.10‰ (2SD, n = 18), opx from −0.19‰ to −0.34‰ with an average of −0.25 ± 0.10‰, and cpx from −0.09‰ to −0.43‰ with an average of −0.24 ± 0.18‰. Although current precision (∼±0.06‰ for δ56Fe; ±0.10‰ for δ26Mg, 2SD) limits the ability to analytically distinguish inter-mineral isotopic fractionations, systematic behavior of inter-mineral fractionation for both Fe and Mg is statistically observed: Δ56Feol-cpx = −0.10 ± 0.12‰ (2SD, n = 18); Δ56Feol-opx = −0.05 ± 0.11‰; Δ26Mgol-opx = −0.09 ± 0.12‰; Δ26Mgol-cpx = −0.10 ± 0.15‰. Fe and Mg isotopic composition of bulk rocks were calculated based on the modes of olivine, opx, and cpx. The average δ56Fe of peridotites in this study is 0.01 ± 0.17‰ (2SD, n = 18), similar to the values of chondrites but slightly lower than mid-ocean ridge basalts (MORB) and oceanic island basalts (OIB). The average δ26Mg is −0.30 ± 0.09‰, indistinguishable from chondrites, MORB, and OIB. Our data support the conclusion that the bulk silicate Earth (BSE) has chondritic δ56Fe and δ26Mg.The origin of inter-mineral fractionations of Fe and Mg isotopic ratios remains debated. δ56Fe between the main peridotite minerals shows positive linear correlations with slopes within error of unity, strongly suggesting intra-sample mineral-mineral Fe and Mg isotopic equilibrium. Because inter-mineral isotopic equilibrium should be reached earlier than major element equilibrium via chemical diffusion at mantle temperatures, Fe and Mg isotope ratios of coexisting minerals could be useful tools for justifying mineral thermometry and barometry on the basis of chemical equilibrium between minerals. Although most peridotites in this study exhibit a narrow range in δ56Fe, the larger deviations from average δ56Fe for three samples likely indicate changes due to metasomatic processes. Two samples show heavy δ56Fe relative to the average and they also have high La/Yb and total Fe content, consistent with metasomatic reaction between peridotite and Fe-rich and isotopically heavy melt. The other sample has light δ56Fe and slightly heavy δ26Mg, which may reflect Fe-Mg inter-diffusion between peridotite and percolating melt.  相似文献   

5.
Mg isotope ratios (26Mg/24Mg) are reported in soil pore-fluids, rain and seawater, grass and smectite from a 90 kyr old soil, developed on an uplifted marine terrace from Santa Cruz, California. Rain water has an invariant 26Mg/24Mg ratio (expressed as δ26Mg) at −0.79 ± 0.05‰, identical to seawater δ26Mg. Detrital smectite (from the base of the soil profile, and therefore unweathered) has a δ26Mg value of 0.11‰, potentially enriched in 26Mg by up to 0.3‰ compared to the bulk silicate Earth Mg isotope composition (although within the range of all terrestrial silicates). The soil pore-waters show a continuous profile with depth for δ26Mg, ranging from −0.99‰ near the surface to −0.43‰ at the base of the profile. Shallow pore-waters (<1 m) have δ26Mg values that are similar to, or slightly lower than the rain waters. This implies that the degree of biological cycling of Mg in the pore-waters is relatively small and is quantified as <32%, calculated using the average Mg isotope enrichment factor between grass and rain (δ26Mggrass-δ26Mgrain) of 0.21‰. The deep pore-waters (1-15 m deep) have δ26Mg values that are intermediate between the smectite and rain, ranging from −0.76‰ to −0.43‰, and show a similar trend with depth compared to Sr isotope ratios. The similarity between Sr and Mg isotope ratios confirms that the Mg in the pore-waters can be explained by a mixture between rain and smectite derived Mg, despite the fact that Mg and Sr concentrations may be buffered by the exchangeable reservoir. However, whilst Sr isotope ratios in the pore-waters span almost the complete range between mineral and rain inputs, Mg isotopes compositions are much closer to the rain inputs. If Mg and Sr isotope ratios are controlled uniquely by a mixture, the data can be used to estimate the mineral weathering inputs to the pore-waters, by correcting for the rain inputs. This isotopic correction is compared to the commonly used chloride correction for precipitation inputs. A consistent interpretation is only possible if Mg isotope ratios are fractionated either by the precipitation of a secondary Mg bearing phase, not detected by conventional methods, or selective leaching of 24Mg from smectite. There is therefore dual control on the Mg isotopic composition of the pore-waters, mixing of two inputs with distinct isotopic compositions, modified by fractionation. The data provide (1) further evidence for Mg isotope fractionation at the surface of the Earth and (2) the first field evidence of Mg isotope fractionation during uptake by natural plants. The coherent behaviour of Mg isotope ratios in soil environments is encouraging for the development of Mg isotope ratios as a quantitative tracer of both weathering inputs of Mg to waters, and the physicochemical processes that cycle Mg, a major cation linked to the carbon cycle, during continental weathering.  相似文献   

6.
This contribution reports our preliminary work to determine Cu isotope ratios for various granite rocks and examine the Cu isotope systematics within granite suites. A chemical procedure, modified from Maréchal [Maréchal, C.N., Télouk, P. and Albarède, F., 1999. Precise analysis of copper and zinc isotopic compositions by plasma-source mass spectrometry. Chemical Geology, 156(1–4): 251–273.], was used to separate Cu from rock matrix. Quantitative recovery (100.6 ± 1.6%), with a low total procedural blank (2.65 ± 0.66 ng) for Cu, has been achieved, allowing Cu isotopic measurements on samples with as little as 10 ppm Cu. The Cu isotope ratios (δ65Cu relative to NIST SRM 976) of 32 rock samples, ranging from mafic to felsic compositions, from 3 batholiths (2 I-type, 1 S-type) from the Lachlan Fold Belt in southeastern Australia, vary from ? 0.46‰ to 1.51‰. Most of them cluster around zero, with mean values for the I-type and S-type granites of 0.03 ± 0.15‰ and ? 0.03 ± 0.42‰ (2 sigma) respectively. These data, together with Cu isotope ratios of two loess samples, provide preliminary evidence that the baseline Cu isotopic composition of the crystalline part of upper continental crust is close to zero. The tight clustering of Cu isotope ratios of rocks from the I-type suites suggests that high-temperature magmatic processes do not produce significant Cu isotope fractionation. However, two granites with abnormally heavy Cu isotope signatures (up to 1.51‰) appears to be the result of localized hydrothermal alteration. Measurable variation in Cu isotopic composition of the S-type granite may reflect isotopic heterogeneity in the sedimentary source region as a result of redox processes or may be due to hydrothermal overprinting. Thus, Cu isotope geochemistry may be a useful tracer for studying hydrothermal alteration and source heterogeneity of granitic rocks.  相似文献   

7.
The aim of this article is to examine the geochemistry and geochronology of the Cadomian Mishu granites from northwest Iran, in order to elucidate petrogenesis and their role in the evolution of the Cadomian crust of Iran. The Mishu granites mainly consist of two-mica granites associated with scarce outcrops of tonalite, amphibole granodiorite, and diorite. Leucogranitic dikes locally crosscut the Mishu granites. Two-mica granites show S-type characteristics whereas amphibole granodiorite, tonalities, and diorites have I-type signatures. The I-type granites show enrichment in large-ion lithophile elements (e.g. Rb, Ba and K) and depletion in high field strength elements (e.g. Nb, Ti and Ta). These characteristics show that these granites have been formed along an ancient, fossilized subduction zone. The S-type granites have high K, Rb, Cs (and other large ion lithophile elements) contents, resembling collision-related granites. U–Pb zircon dating of the Mishu rocks yielded 238U/206Pb crystallization ages of ca. 550 Ma. Moreover, Rb–Sr errorchron shows an early Ediacaran age (547 ± 84 Ma) for the Mishu igneous rocks. The two-mica granites (S-type granites) show high 87Sr/86Sr(i) ratios, ranging from 0.7068 to 0.7095. Their ?Nd values change between ?4.2 and ?4.6. Amphibole granitoids and diorites (I-type granites) are characterized by relatively low 87Sr/86Sr(i) ratios (0.7048–0.7079) and higher values of ?Nd (?0.8 to ?4.2). Leucogranitic dikes have quite juvenile signature, with ?Nd values ranging from +1.1 to +1.4 and Nd model ages (TDM) from 1.1 to 1.2 Ga. The isotopic data suggests interaction of juvenile, mantle-derived melts with old continental crust to be the main factor for the generation of the Mishu granites. Interaction with older continental crust is also confirmed by the presence of abundant inherited zircon cores. The liquid-line of descend in the Harker diagrams suggests fractional crystallization was also a predominant mechanism during evolution of the Mishu I-type granites. The zircon U–Pb ages, whole rock trace elements, and Sr–Nd isotope data strongly indicate the similarities between the Mishu Cadomian granites with other late Neoproterozoic–early Cambrian (600–520 Ma) granites across Iran and the surrounding areas such as Turkey and Iberia. The generation of the Mishu I-type granites could be related to the subduction of the Proto-Tethyan Ocean during Cadomian orogeny, through interaction between juvenile melts and old (Mesoproterozoic or Archaean) continental crust. The S-type granites are related to the pooling of the basaltic melts within the middle–upper parts of the thick continental crust and then partial melting of that crust.  相似文献   

8.
We measured Ca stable isotope ratios (δ44/40Ca) in an ancient (2 My), hyperarid soil where the primary source of mobile Ca is atmospheric deposition. Most of the Ca in the upper meter of this soil (3.5 kmol m−2) is present as sulfates (2.5 kmol m−2), and to a lesser extent carbonates (0.4 kmol m−2). In aqueous extracts of variably hydrated calcium sulfate minerals, δ44/40CaE values (vs. bulk Earth) increase with depth (1.4 m) from a minimum of −1.91‰ to a maximum of +0.59‰. The trend in carbonate-δ44/40Ca in the top six horizons resembles that of sulfate-δ44/40Ca, but with values 0.1-0.6‰ higher. The range of observed Ca isotope values in this soil is about half that of δ44/40Ca values observed on Earth. Linear correlation among δ44/40Ca, δ34S and δ18O values indicates either (a) a simultaneous change in atmospheric input values for all three elements over time, or (b) isotopic fractionation of all three elements during downward transport. We present evidence that the latter is the primary cause of the isotopic variation that we observe. Sulfate-δ34S values are positively correlated with sulfate-δ18O values (R2 = 0.78) and negatively correlated with sulfate δ44/40CaE values (R2 = 0.70). If constant fractionation and conservation of mass with downward transport are assumed, these relationships indicate a δ44/40Ca fractionation factor of −0.4‰ in CaSO4. The overall depth trend in Ca isotopes is reproduced by a model of isotopic fractionation during downward Ca transport that considers small and infrequent but regularly recurring rainfall events. Near surface low Ca isotope values are reproduced by a Rayleigh model derived from measured Ca concentrations and the Ca fractionation factor predicted by the relationship with S isotopes. This indicates that the primary mechanism of stable isotope fractionation in CaSO4 is incremental and effectively irreversible removal of an isotopically enriched dissolved phase by downward transport during small rainfall events.  相似文献   

9.
Magnesium and strontium isotope signatures were determined during different seasons for the main rivers of the Moselle basin, northeastern France. This small basin is remarkable for its well-constrained and varied lithology on a small distance scale, and this is reflected in river water Sr isotope compositions. Upstream, where the Moselle River drains silicate rocks of the Vosges mountains, waters are characterized by relatively high 87Sr/86Sr ratios (0.7128-0.7174). In contrast, downstream of the city of Epinal where the Moselle River flows through carbonates and evaporites of the Lorraine plateau, 87Sr/86Sr ratios are lower, down to 0.70824.Magnesium in river waters draining silicates is systematically depleted in heavy isotopes (δ26Mg values range from −1.2 to −0.7‰) relative to the value presently estimated for the continental crust and a local diorite (−0.5‰). In comparison, δ26Mg values measured in soil samples are higher (∼0.0‰). This suggests that Mg isotope fractionation occurs during mineral leaching and/or formation of secondary clay minerals. On the Lorraine plateau, tributaries draining marls, carbonates and evaporites are characterized by low Ca/Mg (1.5-3.2) and low Ca/Sr (80-400) when compared to local carbonate rocks (Ca/Mg = 29-59; Ca/Sr = 370-2200), similar to other rivers draining carbonates. The most likely cause of the Mg and Sr excesses in these rivers is early thermodynamic saturation of groundwater with calcite relative to magnesite and strontianite as groundwater chemistry progressively evolves in the aquifer. δ26Mg of the dissolved phases of tributaries draining mainly carbonates and evaporites are relatively low and constant throughout the year (from −1.4‰ to −1.6‰ and from −1.2‰ to −1.4‰, respectively), within the range defined for the underlying rocks. Downstream of Epinal, the compositions of the Moselle River samples in a δ26Mg vs. 87Sr/86Sr diagram can be explained by mixing curves between silicate, carbonate and evaporite waters, with a significant contribution from the Vosgian silicate lithologies (>70%). Temporal co-variation between δ26Mg and 87Sr/86Sr for the Moselle River throughout year is also observed, and is consistent with a higher contribution from the Vosges mountains in winter, in terms of runoff and dissolved element flux. Overall, this study shows that Mg isotopes measured in waters, rocks and soils, coupled with other tracers such as Sr isotopes, could be used to better constrain riverine Mg sources, particularly if analytical uncertainties in Mg isotope measurements can be improved in order to perform more precise quantifications.  相似文献   

10.
Boron isotope compositions (δ11B) and B concentrations of rains and snows were studied in order to characterize the sources and fractionation processes during the boron atmospheric cycle. The 11B/10B ratios of instantaneous and cumulative rains and snows from coastal and continental sites show a large range of variations, from −1.5 ± 0.4 to +26.0 ± 0.5‰ and from −10.2 ± 0.5 to +34.4 ± 0.2‰, respectively. Boron concentrations in rains and snows vary between 0.1 and 3.0 ppb. All these precipitation samples are enriched in 10B compared to the ocean value (δ11B = +39.5‰). An empirical rain-vapour isotopic fractionation of +31‰ is estimated from three largely independent methods. The deduced seawater-vapour fractionation is +25.5‰, with the difference between the rain and seawater fractionations principally reflecting changes in the speciation of boron in the liquid with ∼100% B(OH)3 present in precipitations. A boron meteoric water line, δD = 2.6δ11B − 133, is proposed which describes the relationship between δD and δ11B in many, but not all, precipitations. Boron isotopic compositions of precipitations can be related to that of the seawater reservoir by the seawater-vapour fractionation and one or more of (1) the rain-vapour isotopic fractionation, (2) evolution of the δ11B value of the atmospheric vapour reservoir via condensation-precipitation processes (Rayleigh distillation process), (3) any contribution of vapour from the evaporation of seawater aerosols, and (4) any contribution from particulate matter, principally sea salt, continental dust and, perhaps more regionally, anthropogenic sources (burning of biomass and fossil fuels). From the δ11B values of continental precipitations, a sea salt contribution cannot be more than a percent or so of the total B in precipitation over these areas.  相似文献   

11.
This paper provides the first measurements of the nitrogen (N) concentrations and isotopic compositions of high- and ultrahigh-pressure mafic eclogites, aimed at characterizing the subduction input flux of N in deeply subducting altered oceanic crust (AOC). The samples that were studied are from the Raspas Complex (Ecuador), Lago di Cignana (Italy), the Zambezi Belt (Zambia) and Cabo Ortegal (Spain), together representing subduction to 50-90 km depths. The eclogites contain 2-20 ppm N with δ15Nair values ranging from −1 to +8‰. These values overlap those of altered oceanic crust, but are distinct from values for fresh MORB (for the latter, ∼1.1 ppm N and δ15Nair ∼ −4‰). Based on N data in combination with other trace element data, the eclogite suites can be subdivided into those that are indistinguishable from their likely protolith, AOC, with or without superimposed effects of devolatilization (Lago di Cignana, Cabo Ortegal), and those that have experienced metasomatic additions during subduction-zone metamorphism (Zambezi Belt, Raspas). For the former group, the lack of a detectable loss of N in the eclogites, compared to various altered MORB compositions, suggests the retention of N in deeply subducted oceanic crust. The metasomatic effects affecting the latter group can be best explained by mixing with a (meta)sedimentary component, resulting in correlated enrichments of N and other trace elements (in particular, Ba and Pb) thought to be mobilized during HP/UHP metamorphism. Serpentinized and high-pressure metamorphosed peridotites, associated with the eclogites at Raspas and Cabo Ortegal, contain 3-15 ppm N with δ15Nair values ranging from +3 to +6‰, significantly higher than the generally accepted values for the MORB mantle (δ15Nair ∼ −5‰). Based on their relatively high N contents and their homogeneous and positive δ15N values, admixing of sedimentary N is also indicated for the serpentinized peridotites.One possible pathway for the addition of sediment-derived N into eclogites and peridotites involves mixing with fluids along the slab-mantle wedge interface. Alternatively, sedimentary N could be incorporated into peridotites during serpentinization at bending-related faults at the outer rise and, during later deserpentinization, released into fluids that then infiltrate overlying rocks. Deep retention of N in subducting oceanic crust should be considered in any attempt to balance subduction inputs with outputs in the form of arc volcanic gases. If materials such as these eclogites and serpentinized peridotites are eventually subducted to beyond sub-arc depths into the deeper mantle, containing some fraction of their forearc-subarc N inventory (documented here), they could deliver isotopically heavy N into the mantle to potentially be sampled by plume-related magmas.  相似文献   

12.
The isotopic composition of U in nature is generally assumed to be invariant. Here, we report variations of the 238U/235U isotope ratio in natural samples (basalts, granites, seawater, corals, black shales, suboxic sediments, ferromanganese crusts/nodules and BIFs) of ∼1.3‰, exceeding by far the analytical precision of our method (≈0.06‰, 2SD). U isotopes were analyzed with MC-ICP-MS using a mixed 236U-233U isotopic tracer (double spike) to correct for isotope fractionation during sample purification and instrumental mass bias. The largest isotope variations found in our survey are between oxidized and reduced depositional environments, with seawater and suboxic sediments falling in between. Light U isotope compositions (relative to SRM-950a) were observed for manganese crusts from the Atlantic and Pacific oceans, which display δ238U of −0.54‰ to −0.62‰ and for three of four analyzed Banded Iron Formations, which have δ238U of −0.89‰, −0.72‰ and −0.70‰, respectively. High δ238U values are observed for black shales from the Black Sea (unit-I and unit-II) and three Kupferschiefer samples (Germany), which display δ238U of −0.06‰ to +0.43‰. Also, suboxic sediments have slightly elevated δ238U (−0.41‰ to −0.16‰) compared to seawater, which has δ238U of −0.41 ± 0.03‰. Granites define a range of δ238U between −0.20‰ and −0.46‰, but all analyzed basalts are identical within uncertainties and slightly lighter than seawater (δ238U = −0.29‰).Our findings imply that U isotope fractionation occurs in both oxic (manganese crusts) and suboxic to euxinic environments with opposite directions. In the first case, we hypothesize that this fractionation results from adsorption of U to ferromanganese oxides, as is the case for Mo and possibly Tl isotopes. In the second case, reduction of soluble UVI to insoluble UIV probably results in fractionation toward heavy U isotope compositions relative to seawater. These findings imply that variable ocean redox conditions through geological time should result in variations of the seawater U isotope compositions, which may be recorded in sediments or fossils. Thus, U isotopes might be a promising novel geochemical tracer for paleo-redox conditions and the redox evolution on Earth. The discovery that 238U/235U varies in nature also has implications for the precision and accuracy of U-Pb dating. The total observed range in U isotope compositions would produce variations in 207Pb/206Pb ages of young U-bearing minerals of up to 3 Ma, and up to 2 Ma for minerals that are 3 billion years old.  相似文献   

13.
Silicon isotope fractionation during magmatic differentiation   总被引：3，自引：0，他引：3  
The Si isotopic composition of Earth’s mantle is thought to be homogeneous (δ30Si = −0.29 ± 0.08‰, 2 s.d.) and not greatly affected by partial melting and recycling. Previous analyses of evolved igneous material indicate that such rocks are isotopically heavy relative to the mantle. To understand this variation, it is necessary to investigate the degree of Si isotopic fractionation that takes place during magmatic differentiation. Here we report Si isotopic compositions of lavas from Hekla volcano, Iceland, which has formed in a region devoid of old, geochemically diverse crust. We show that Si isotopic composition varies linearly as a function of silica content, with more differentiated rocks possessing heavier isotopic compositions. Data for samples from the Afar Rift Zone, as well as various igneous USGS standards are collinear with the Hekla trend, providing evidence of a fundamental relationship between magmatic differentiation and Si isotopes. The effect of fractionation has been tested by studying cumulates from the Skaergaard Complex, which show that olivine and pyroxene are isotopically light, and plagioclase heavy, relative to the Si isotopic composition of the Earth’s mantle. Therefore, Si isotopes can be utilised to model the competing effects of mafic and felsic mineral fractionation in evolving silicate liquids and cumulates.At an average SiO2 content of ∼60 wt.%, the predicted δ30Si value of the continental crust that should result from magmatic fractionation alone is −0.23 ± 0.05‰ (2 s.e.), barely heavier than the mantle. This is, at most, a maximum estimate, as this does not take into account weathered material whose formation drives the products toward lighter δ30Si values. Mass balance calculations suggest that removal of continental crust of this composition from the upper mantle will not affect the Si isotopic composition of the mantle.  相似文献   

14.
This study investigates the application of sulphur isotope ratios (δ34S) in combination with carbon (δ13C) and nitrogen (δ15N) ratios to understand the influence of environmental sulphur on the isotopic composition of archaeological human and faunal remains from Roman era sites in Oxfordshire, UK. Humans (n = 83), terrestrial animals (n = 11), and freshwater fish (n = 5) were analysed for their isotope values from four locations in the Thames River Valley, and a broad range of δ34S values were found. The δ34S values from the terrestrial animals were highly variable (−13.6‰ to +0.5‰), but the δ34S values of the fish were clustered and 34S-depleted (−20.9‰ to −17.3‰). The results of the faunal remains suggest that riverine sulphur influenced the terrestrial sulphur isotopic signatures. Terrestrial animals were possibly raised on the floodplains of the River Thames, where highly 34S-depleted sulphur influenced the soil. The humans show the largest range of δ34S values (−18.8‰ to +9.6‰) from any archaeological context to date. No differences in δ34S values were found between the males (−7.8 ± 6.0‰) and females (−5.3 ± 6.8‰), but the females had a linear correlation (R2 = 0.71; p < 0.0001) between their δ15N and δ34S compositions. These δ34S results suggest a greater dietary variability for the inhabitants of Roman Oxfordshire than previously thought, with some individuals eating solely terrestrial protein resources and others showing a diet almost exclusively based on freshwater protein such as fish. Such large dietary variability was not visible by analysing only the carbon and nitrogen isotope ratios, and this research represents the largest and most detailed application of δ34S analysis to examine dietary practices (including breastfeeding and weaning patterns) during the Romano-British Period.  相似文献   

15.
Isotopic fractionation of Cu in tektites   总被引：1，自引：0，他引：1  
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 (δ66/64Zn 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   

16.
Global-scale cycling of silicon through the biosphere, atmosphere, and hydrosphere has received much attention although, silicon cycling in the Earth’s lithosphere remains poorly understood. As the products of internal heat and material exchange, igneous rocks preserve significant information of silicon migration through the lithosphere. Here we report silicon isotopic compositions of nine peraluminous granites from the Chinese Altai, which forms part of the Central Asian Orogenic Belt. These rocks are characterized by the heaviest δ30Si values (−0.13 ± 0.03‰ to +0.78 ± 0.05‰) compared to global granites, with a linear variation in the silicon isotopic values against silica content, with high silica-rich granites displaying more depleted isotopic compositions. In conjunction with the whole rock weakly negative ɛNd(t) and uniform δ26Mg values, as well as high δ18O values, we suggest that the δ30Si values of these granites were mainly inherited from the magma source, rather than produced by magmatic fractionation. In addition, the wide range of initial 87Sr/86Sr ratios and high Ba content of the samples suggest the role of aqueous fluids. The Chinese Altai is considered to have formed through accretion of volcanic arcs associated with subduction of the Paleo-Asian oceanic lithosphere. The magma derived through partial melting of metasomatic mantle scavenges the heavy 30Si isotopes derived through fluids released from oceanic sediments and transfers to the upper crust where partial melting of crustal sedimentary rocks occur. Mixing of these two melts generated the peraluminous granites. Our study offers a novel insight into a potentially important mechanism of silicon cycling in the lithosphere.  相似文献   

17.
Chondritic Mg isotope composition of the Earth   总被引：2，自引：0，他引：2  
The processes of planetary accretion and differentiation have potentially been recorded as variations in the stable isotope ratios of the major elements between planetary objects. However, the magnitude of observed isotopic variations for several elements (Mg, Fe, Si) is at the limit of what current analytical precision and accuracy are able to resolve. Here, we present a comprehensive data set of Mg isotope ratios measured in ocean island and mid-ocean ridge basalts, peridotites and chondrites. The precision and accuracy were verified by isotopic standard addition for two samples, one carbonaceous chondrite (Murchison) and one continental flood basalt (BCR-1). In contrast with some previous studies, our data from terrestrial and chondritic materials have invariant Mg isotope ratios within the uncertainty of the method (0.1‰ for the 26Mg/24Mg ratio, 2SD). Although isotopic variations of less than about 0.1‰ could still be present, the data demonstrate that, at this level of uncertainty, the bulk silicate Earth and chondritic Mg reservoir have a homogeneous δ26Mg = −0.23‰ (26Mg/24Mg ratio of the sample relative to the DSM3 standard set to zero by definition). This implies that neither planetary accretion processes nor partial mantle melting and subsequent shallow-level differentiation have fractionated Mg isotope ratios. These observations imply in particular that the formation of the Earth cannot stem from preferential sorting of chondrite constituents that would have been fractionated in their Mg isotope composition. It also implies that unlike oxygen isotopes, there was no zonation in Mg isotopes in the inner solar system.  相似文献   

18.
Magnesium isotopic composition of the Earth and chondrites   总被引：3，自引：0，他引：3  
To constrain further the Mg isotopic composition of the Earth and chondrites, and investigate the behavior of Mg isotopes during planetary formation and magmatic processes, we report high-precision (±0.06‰ on δ25Mg and ±0.07‰ on δ26Mg, 2SD) analyses of Mg isotopes for (1) 47 mid-ocean ridge basalts covering global major ridge segments and spanning a broad range in latitudes, geochemical and radiogenic isotopic compositions; (2) 63 ocean island basalts from Hawaii (Kilauea, Koolau and Loihi) and French Polynesia (Society Island and Cook-Austral chain); (3) 29 peridotite xenoliths from Australia, China, France, Tanzania and USA; and (4) 38 carbonaceous, ordinary and enstatite chondrites including 9 chondrite groups (CI, CM, CO, CV, L, LL, H, EH and EL).Oceanic basalts and peridotite xenoliths have similar Mg isotopic compositions, with average values of δ25Mg = −0.13 ± 0.05 (2SD) and δ26Mg = −0.26 ± 0.07 (2SD) for global oceanic basalts (n = 110) and δ25Mg = −0.13 ± 0.03 (2SD) and δ26Mg = −0.25 ± 0.04 (2SD) for global peridotite xenoliths (n = 29). The identical Mg isotopic compositions in oceanic basalts and peridotites suggest that equilibrium Mg isotope fractionation during partial melting of peridotite mantle and magmatic differentiation of basaltic magma is negligible. Thirty-eight chondrites have indistinguishable Mg isotopic compositions, with δ25Mg = −0.15 ± 0.04 (2SD) and δ26Mg = −0.28 ± 0.06 (2SD). The constancy of Mg isotopic compositions in all major types of chondrites suggest that primary and secondary processes that affected the chemical and oxygen isotopic compositions of chondrites did not significantly fractionate Mg isotopes.Collectively, the Mg isotopic composition of the Earth’s mantle, based on oceanic basalts and peridotites, is estimated to be −0.13 ± 0.04 for δ25Mg and −0.25 ± 0.07 for δ26Mg (2SD, n = 139). The Mg isotopic composition of the Earth, as represented by the mantle, is similar to chondrites. The chondritic composition of the Earth implies that Mg isotopes were well mixed during accretion of the inner solar system.  相似文献   

19.
The chemical and isotopic composition of speleothem calcite and particularly that of stalagmites and flowstones is increasingly exploited as an archive of past environmental change in continental settings. Despite intensive research, including modelling and novel approaches, speleothem data remain difficult to interpret. A possible way foreword is to apply a multi-proxy approach including non-conventional isotope systems. For the first time, we here present a complete analytical dataset of magnesium isotopes (δ26Mg) from a monitored cave in NW Germany (Bunker Cave). The data set includes δ26Mg values of loess-derived soil above the cave (−1.0 ± 0.5‰), soil water (−1.2 ± 0.5‰), the carbonate hostrock (−3.8 ± 0.5‰), dripwater in the cave (−1.8 ± 0.2‰), speleothem low-Mg calcite (stalactites, stalagmites; −4.3 ± 0.6‰), cave loam (−0.6 ± 0.1‰) and runoff water (−1.8 ± 0.1‰) in the cave, respectively. Magnesium-isotope fractionation processes during weathering and interaction between soil cover, hostrock and solute-bearing soil water are non-trivial and depend on a number of variables including solution residence times, dissolution rates, adsorption effects and potential neo-formation of solids in the regolith and the carbonate aquifer. Apparent Mg-isotope fractionation between dripwater and speleothem low-Mg calcite is about 1000lnαMg-cc-Mg(aq) = −2.4‰. A similar Mg-isotope fractionation (1000lnαMg-cc-Mg(aq) ≈ −2.1‰) is obtained by abiogenic precipitation experiments carried out at aqueous Mg/Ca ratios and temperatures close to cave conditions. Accordingly, 26Mg discrimination during low-Mg calcite formation in caves is highly related to inorganic fractionation effects, which may comprise dehydration of Mg2+ prior to incorporation into calcite, surface entrapment of light isotopes and reaction kinetics. Relevance of kinetics is supported by a significant negative correlation of Mg-isotope fractionation with the precipitation rate for inorganic precipitation experiments.  相似文献   

20.
Measurements are presented of the magnesium isotopic composition of chlorophyll-a, extracted from cyanobacteria, relative to the isotopic composition of the culture medium in which the cyanobacteria were grown. Yields of 50-93% chlorophyll-a were achieved from the pigment extracts of Synechococcus elongatus, a unicellular cyanobacteria. This material was then digested using concentrated nitric acid to extract magnesium. Separation was accomplished using columns of cation-exchange resin, which achieved a 103 ± 10% yield of magnesium from chlorophyll-a. This procedure ensured accurate measurement of the magnesium-isotopic ratios without isobaric interferences using a multi-collector inductively coupled plasma mass spectrometry (MC-ICP-MS). We find a slight depletion in the heavier isotopes of magnesium in chlorophyll-a relative to culture medium, early growth phase: Δ26Mg = −0.71(±0.35)‰ and Δ25Mg = −0.37(±0.18)‰; late growth phase: Δ26Mg = −0.53(±0.20)‰ and Δ25Mg = −0.26(±0.11)‰, due to an apparent mass-dependent fractionation. We suggest that the small fractionation results from chelation during intracellular processes. A likely candidate for this chelation step involves the magnesium-chelatase enzyme, which mediates the insertion of magnesium to the tetrapyrrole ring during chlorophyll-a biosynthesis. Proof of this hypothesis can be tested with biological controls whereby steps in the enzymatic pathways of chlorophyll synthesis are selectively suppressed.  相似文献   

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