Mantle Geochemistry Research Articles

A possible high-temperature origin of the Moon and its geochemical consequences

The formation of the Moon is thought to be the result of a giant impact between a Mercury-to-proto-Earth-sized body and the proto-Earth. However, the initial thermal state of the Moon following its accretion is not well constrained by geochemical data. Here, we provide geochemical evidence that supports a high-temperature origin of the Moon by performing high-temperature (1973–2873 K) metal-silicate partitioning experiments, simulating core formation in the newly-formed Moon. Results indicate that the observed lunar mantle depletions of Ni and Co record extreme temperatures (>2600–3700 K depending on assumptions about the composition of the lunar core) during lunar core formation. This temperature range is within range of the modeled silicate evaporation buffer in a synestia-type environment. Our results provide independent geochemical support for a giant-impact origin of the Moon and show that lunar thermal models should start with a fully molten Moon. Our results also provide quantitative constraints on the effects of high-temperature lunar differentiation on the lunar mantle geochemistry of volatile, and potentially siderophile elements Cu, Zn, Ga, Ge, Se, Sn, Cd, In, Te and Pb. At the extreme temperatures recorded by Ni and Co, many of these elements behave insufficiently siderophile to explain their depletions by core formation only, consistent with the inferred volatility-related loss of Cr, Cu, Zn, Ga and Sn during the Moon-forming event and/or subsequent magma-ocean degassing.

Influence of the subduction of the Pacific plate on the mantle characteristics of South China: Constraints from the temporal geochemical evolution of the Mesozoic basalts in the Jitai Basin

The Pacific plate since the Mesozoic is subducting into the mantle beneath the eastern Asia, and the involved recycled crustal material has greatly affected the mantle geochemistry. However, the initial timing of the subduction remains controversial, partly due to the insufficient understanding of the geochemical evolution of the Mesozoic mantle. The present study provides new constraints on this aspect using whole-rock and olivine phenocryst compositions of Mesozoic basalts from the Jitai Basin of South China, which is part of the eastern Asian volcanic belt. Multiple OIB-type basalts outcrop in the Jitai Basin ranging in age from 168 Ma to 90 Ma. In comparison with normal mantle, these basalts exhibit higher (87Sr/86Sr)i, Ba/Th, Nb/La and lower εNd(t). Their olivine phenocrysts display high Ni contents and low Mn and Ca contents. Together, these indicators suggest that components of recycled oceanic crust were involved in the mantle source of the basalts. Moreover, combined with the observations from the Hebu basalts, from 168 Ma to 63 Ma, it shows that the component of the recycled oceanic crust was continuously supplied to the mantle source of the Jitai Basin basalts. Considering that the Jitai Basin basalts have whole-rock and olivine phenocryst compositions similar to those of the Cenozoic basalts from eastern China, which were originated from a stagnant Pacific plate in the mantle transition zone, we propose that the same origin may be the best candidate for the components of recycled oceanic crust in the mantle source of the Jitai Basin basalts. Finally, it is possible to estimate that the westward subduction of the Pacific plate probably started in an earlier stage.

Encyclopedia of Geochemistry

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Effect of silicon on activity coefficients of siderophile elements (Au, Pd, Pt, P, Ga, Cu, Zn, and Pb) in liquid Fe: Roles of core formation, late sulfide matte, and late veneer in shaping terrestrial mantle geochemistry

Earth’s core contains ∼10% of a light element that may be a combination of Si, S, C, O or H, with Si potentially being the major light element. Metal-silicate partitioning of siderophile elements can place important constraints on the P-T-fO2 and composition of the early Earth, but the effect of Si alloyed in Fe liquids is unknown for many of these elements. In particular, the effect of Si on the partitioning of highly siderophile elements (Au, Re and PGE) is virtually unknown. To address this gap in understanding, we have undertaken a systematic study of the highly siderophile elements Au, Pd, and Pt, and the volatile siderophile elements P, Ga, Cu, Zn, and Pb at variable Si content of metal, and 1600 °C and 1 GPa. From our experiments we derive epsilon interaction parameters between these elements and Si in Fe metallic liquids. The new parameters are used to update an activity model for trace siderophile elements in Fe alloys; Si causes large variation in the magnitude of activity coefficients of these elements in FeSi liquids. Because the interaction parameters are all positive, Si causes a decrease in their metal/silicate partition coefficients. We combine these new activity results with experimental studies of Au, Pd, Pt, P, Ga, Cu, Zn and Pb, to derive predictive expressions for metal/silicate partition coefficients which can then be applied to Earth. The expressions are applied to two scenarios for continuous accretion of Earth; specifically for constant and increasing fO2 during accretion. The results indicate that mantle concentrations of P, Ga, Cu, Zn, and Pb can be explained by metal-silicate equilibrium during accretion of the Earth where Earth’s early magma ocean deepens to pressures of 40–60 GPa. Au, Pd, and Pt, on the other hand become too high in the mantle in such a scenario, and require a later removal mechanism, rather than an addition as traditionally argued. A late reduction event that removes 0.5% metal from a shallow magma ocean can lower the Au, Pd, and Pt contents to values near the current day BSE. On the other hand, removal of 0.2–1.0% of a late sulfide-rich matte to the core would lower the Au, Pd, and Pt concentrations in the mantle, but not to chondritic relative concentrations observed in the BSE. If sulfide matte is called upon to remove HSEs, they must be later added via a late veneer to re-establish the high and chondritic relative PUM concentrations. These results suggest that although accretion and core formation (involving a Si, S, and C-bearing metallic liquid) were the primary processes establishing many of Earth’s mantle volatile elements and HSE, a secondary removal process is required to establish HSEs at their current and near-chondritic relative BSE levels. Mn and P - two siderophile elements that are central to biochemical processes (photosynthesis and triphosphates, respectively) - have significant and opposite interactions with FeSi liquids, and their mantle concentrations would be notably different if Earth had a Si-free core.

Insights into the mantle geochemistry of scandium from a meta-analysis of garnet data

The meta-analysis of about 13,000 analyses of scandium content in garnet grains shows that, below the spinel–garnet transition, this phase carries about three-quarters of the Sc budget of the mantle, indicating its control on Sc mobility. The Sc content of garnets in mafic rocks is low, due to a dilution effect resulting from their high modal content in garnet. Garnets from ultramafic rocks exhibit a wider range of Sc concentrations. We assess the relative influence of thermobarometry, crystal chemistry and fluid-related events on the distribution of Sc in garnet from such rocks to improve the tracking of geochemical processes in the mantle. Pressure and temperature of equilibration in the mantle are second-order factors influencing the Sc content of garnet, while crystal chemistry, in particular CrCr+Al and CaCa+Mg, is the main parameter controlling the compatibility of Sc. Scandium is incorporated in both X and Y sites of Cr-Ca-rich garnets, resulting in a behaviour intermediate between rare-earth elements, incorporated in the X site, and trivalent transition elements, occupying the Y site. This affinity for both sites results in a mild compatibility of Sc in the garnet stability field of the mantle; hence Sc concentration in garnet increases with melt extraction and can be reduced by silicate-melt metasomatism. In contrast, metasomatism by volatile-rich fluids increases the Sc concentration in garnet. The control of garnet on the compatibility of Sc in deep lithospheric rocks demonstrates the potential of using Sc to track the conditions of formation of magmas and their residual rocks, as well as the origin and nature of metasomatic fluids.

Zircon evidence for incorporation of terrigenous sediments into the magma source of continental basalts

Crustal components may be incorporated into continental basalts by either shallow contamination or deep mixing. While the former proceeds at crustal depths with common preservation of refractory minerals, the latter occurs at mantle depths with rare survival of relict minerals. Discrimination between the two mechanisms has great bearing to subcontinental mantle geochemistry. Here we report the occurrence of relict zircons in Cenozoic continental basalts from eastern China. A combined study of zircon U-Pb ages and geochemistry indicates that detrital zircons were carried by terrigenous sediments into a subcontinental subduction zone, where the zircon were transferred by fluids into the magma sources of continental basalts. The basalts were sampled from three petrotectonic units with distinct differences in their magmatic and metamorphic ages, making the crustal contamination discernible. The terrigenous sediments were carried by the subducting oceanic crust into the asthenospheric mantle, producing both soluble and insoluble materials at the slab-mantle interface. These materials were served as metasomatic agents to react with the overlying mantle wedge peridotite, generating a kind of ultramafic metasomatites that contain the relict zircons. Therefore, the occurrence of relict zircons in continental basalts indicates that this refractory mineral can survive extreme temperature-pressure conditions in the asthenospheric mantle.

Mantle geochemistry: Insights from ocean island basalts

The geochemical study of the Earth’s mantle provides important constraints on our understanding of the formation and evolution of Earth, its internal structure, and the mantle dynamics. The bulk Earth composition is inferred by comparing terrestrial mantle rocks with chondrites, which leads to the chondritic Earth model. That is, Earth has the same relative proportions of refractory elements as that in chondrites, but it is depleted in volatiles. Ocean island basalts (OIB) may be produced by mantle plumes with possible deep origins; consequently, they provide unique opportunity to study the deep Earth. Isotopic variations within OIB can be described using a limited number of mantle endmembers, such as EM1, EM2 and HIMU, and they have been used to decipher important mantle processes. Introduction of crustal material into the deep mantle via subduction and delamination is important in generating mantle heterogeneity; however, there is active debate on how they were sampled by mantle melting, i.e., the role of olivine-poor lithologies in the OIB petrogenesis. The origin and location of high 3He/4He mantle remain controversial, ranging from unprocessed (or less processed) primitive material in the lower mantle to highly processed materials with shallow origins, including ancient melting residues, mafic cumulates under arcs, and recycled hydrous minerals. Possible core-mantle interaction was hypothesized to introduce distinctive geochemical signatures such as radiogenic 186Os and Fe and Ni enrichment in the OIB. Small but important variations in some short-lived nuclides, including 142Nd, 182W and several Xe isotopes, have been reported in ancient and modern terrestrial rocks, implying that the Earth’s mantle must have been differentiated within the first 100 Myr of its formation, and the mantle is not efficiently homogenized by mantle convection.

The diffusion coefficients of noble gases (He Ar) in a synthetic basaltic liquid: One-dimensional diffusion experiments

Diffusion coefficients of noble gases in silicate liquids are poorly known, and, as a result, it is difficult to quantify the importance of kinetic fractionation of noble gas abundances and isotopic compositions during magmatic processes. Nevertheless, diffusive fractionation has been invoked to explain noble gas signatures in MORBs and OIBs, with important implications for magma degassing and noble gas mantle geochemistry. In order to investigate the diffusion of noble gases in magmas, we developed an experimental protocol based on uniaxial diffusion of He and Ar through a column of synthetic basaltic liquid in a Pt tube. At the end of the experiment, the column of silicate liquid was rapidly quenched to a glass recording the diffusion profile. The glass cylinder was cut into a series of slices, which were analyzed for noble gases by traditional noble gas mass spectrometry following total gas extraction by fusion. Using this protocol, we measured He and Ar diffusivities in CMAS glass G1 (50 mol% SiO2, 9 mol% Al2O3, 16 mol% MgO, 25 mol% CaO) at temperatures of 1673 K and 1823 K: DHe = 2.75 ± 0.25 × 10− 6 cm2·s− 1 (T = 1673 K); DHe = 4.77 ± 0.42 × 10− 6 cm2·s− 1 (T = 1823 K); and DAr = 9.3 ± 1.3 × 10− 7 cm2·s− 1 (T = 1673 K). Combining these new high temperature data with diffusion coefficients measured on the same composition just above the glass transition temperature, we determined the activation energy Ea and the pre-exponential factor D0 for He and Ar diffusion in silicate liquids: D0 = 1.72 ± 0.9 × 10− 2 cm2·s− 1 and Ea = 136.5 ± 3.2 kJ/mol for Ar; D0 = 1.8 ± 0.5 × 10− 4 cm2·s− 1 and Ea = 57.6 ± 1.5 kJ/mol for He. Because He and Ar have very different activation energies for diffusion in the liquid state, the ratio DHe/DAr is strongly sensitive to temperature, decreasing from 145 at the glass transition temperature (1005 K) to 2 at 1823 K. The implication is that the kinetic fractionation of He relative to Ar in magmas is likely to be more important during the cooling stages than during the earlier, high temperature stages of magmatic history.

Whole-mantle convection with tectonic plates preserves long-term global patterns of upper mantle geochemistry

The evolution of the planetary interior during plate tectonics is controlled by slow convection within the mantle. Global-scale geochemical differences across the upper mantle are known, but how they are preserved during convection has not been adequately explained. We demonstrate that the geographic patterns of chemical variations around the Earth’s mantle endure as a direct result of whole-mantle convection within largely isolated cells defined by subducting plates. New 3D spherical numerical models embedded with the latest geological paleo-tectonic reconstructions and ground-truthed with new Hf-Nd isotope data, suggest that uppermost mantle at one location (e.g. under Indian Ocean) circulates down to the core-mantle boundary (CMB), but returns within ≥100 Myrs via large-scale convection to its approximate starting location. Modelled tracers pool at the CMB but do not disperse ubiquitously around it. Similarly, mantle beneath the Pacific does not spread to surrounding regions of the planet. The models fit global patterns of isotope data and may explain features such as the DUPAL anomaly and long-standing differences between Indian and Pacific Ocean crust. Indeed, the geochemical data suggests this mode of convection could have influenced the evolution of mantle composition since 550 Ma and potentially since the onset of plate tectonics.

There were no large volumes of felsic continental crust in the early Earth

New model growth curves for the continental crust based upon Hf isotopes in zircon suggest that large volumes of felsic continental crust were present in the Hadean and early Archean. These models sit uncomfortably with estimates of the volume of ancient crust preserved today and imply that the large volumes of crust that were created early in Earth history are now lost. However, this paper argues that there is no evidence from modern mantle geochemistry that very large volumes of early continental crust have been recycled into the mantle. In contrast, significant volumes of Archean crust may have been reworked into younger crust, although there is no evidence that this process took place in the early Archean and Hadean.

Origin of geochemical mantle components: Role of spreading ridges and thermal evolution of mantle

AbstractWe explore the element redistribution at mid‐ocean ridges (MOR) using a numerical model to evaluate the role of decompression melting of the mantle in Earth's geochemical cycle, with focus on the formation of the depleted mantle component. Our model uses a trace element mass balance based on an internally consistent thermodynamic‐petrologic computation to explain the composition of MOR basalt (MORB) and residual peridotite. Model results for MORB‐like basalts from 3.5 to 0 Ga indicate a high mantle potential temperature (Tp) of 1650–1500°C during 3.5–1.5 Ga before decreasing gradually to ∼1300°C today. The source mantle composition changed from primitive (PM) to depleted as Tp decreased, but this source mantle is variable with an early depleted reservoir (EDR) mantle periodically present. We examine a two‐stage Sr‐Nd‐Hf‐Pb isotopic evolution of mantle residues from melting of PM or EDR at MORs. At high‐Tp (3.5–1.5 Ga), the MOR process formed extremely depleted DMM. This coincided with formation of the majority of the continental crust, the subcontinental lithospheric mantle, and the enriched mantle components formed at subduction zones and now found in OIB. During cooler mantle conditions (1.5–0 Ga), the MOR process formed most of the modern ocean basin DMM. Changes in the mode of mantle convection from vigorous deep mantle recharge before ∼1.5 Ga to less vigorous afterward is suggested to explain the thermochemical mantle evolution.

Influence of the architecture of magma-poor hyperextended rifted margins on orogens produced by the closure of narrow versus wide oceans

Orogens resulting from the closure of narrow oceans, such as the Alps or the Pyrenees, usually lack voluminous synsubduction and synorogenic magmatism. Such orogenies are essentially controlled by mechanical processes in which the initial architecture of the original rifted margins strongly controls the architecture of the orogen. In this paper we first provide a synthesis of the structure, dimensions, and lithology of hyperextended rift systems and oceans, based on recent seismic and petrologic data. We then investigate how rift-related inheritance influences crustal characteristics and mantle geochemistry of orogens related to the closure of narrow oceans, and compare them to orogens resulting from the closure of wide and/or mature oceans. Our results show that narrow oceans usually lack a mature spreading system forming Penrose-type oceanic crust (i.e., 6–7-km-thick basaltic oceanic crust typical of steady-state spreading systems; see Anonymous, 1972), in contrast to wide oceans. However, there is statistically no difference in the structural and lithological architecture of their passive continental margins. Thus, the main difference between narrow and wide oceans is whether the margins are separated by a significant amount of oceanic crust and underlying depleted mantle. In addition, due to the lack of significant magmatism during the closure of narrow oceans, the mantle wedge is likely to remain relatively fertile compared to the wedge above long-lasting subduction of wide oceans. This difference in mantle composition may dictate the magmatic budget of subsequent orogenic collapse or rifting events.

Elasticity of ferropericlase and seismic heterogeneity in the Earth's lower mantle

AbstractDeciphering the origin of seismic heterogeneity has been one of the major challenges in understanding the geochemistry and geodynamics of the deep mantle. Fully anisotropic elastic properties of constituent minerals at relevant pressure‐temperature conditions of the lower mantle can be used to calculate seismic heterogeneity parameters in order to better understand chemically and thermally induced seismic heterogeneities. In this study, the single‐crystal elastic properties of ferropericlase (Mg0.94Fe0.06)O were measured using Brillouin spectroscopy and X‐ray diffraction at conditions up to 50 GPa and 900 K. The velocity‐density results were modeled using third‐order finite‐strain theory and thermoelastic equations along a representative geotherm to investigate high pressure‐temperature and compositional effects on the seismic heterogeneity parameters. Our results demonstrate that from 660 to 2000 km, compressional wave anisotropy of ferropericlase increased from 4% to 9.7%, while shear wave anisotropy increased from 9% to as high as 22.5%. The thermally induced lateral heterogeneity ratio (RS/P = ∂lnVS/∂lnVP) of ferropericlase was calculated to be 1.48 at ambient pressure but decreased to 1.43 at 40 GPa along a representative geotherm. The RS/P of a simplified pyrolite model consisting of 80% bridgmanite and 20% ferropericlase was approximately 1.5, consistent with seismic models at depths from 670 to 1500 km, but showed an increased mismatch at lower mantle depths below ~1500 km. This discrepancy below mid‐lower mantle could be due to either a contribution from chemically induced heterogeneity or the effects of the Fe spin transition in the deeper parts of the Earth's lower mantle.

Large-scale subduction of continental crust implied by India–Asia mass-balance calculation

Continental crust is buoyant compared with its oceanic counterpart and resists subduction into the mantle. When two continents collide, the mass balance for the continental crust is therefore assumed to be maintained. Here we use estimates of pre-collisional crustal thickness and convergence history derived from plate kinematic models to calculate the crustal mass balance in the India–Asia collisional system. Using the current best estimates for the timing of the diachronous onset of collision between India and Eurasia, we find that about 50% of the pre-collisional continental crustal mass cannot be accounted for in the crustal reservoir preserved at Earth’s surface today—represented by the mass preserved in the thickened crust that makes up the Himalaya, Tibet and much of adjacent Asia, as well as southeast Asian tectonic escape and exported eroded sediments. This implies large-scale subduction of continental crust during the collision, with a mass equivalent to about 15% of the total oceanic crustal subduction flux since 56 million years ago. We suggest that similar contamination of the mantle by direct input of radiogenic continental crustal materials during past continent–continent collisions is reflected in some ocean crust and ocean island basalt geochemistry. The subduction of continental crust may therefore contribute significantly to the evolution of mantle geochemistry. Buoyant continental crust is thought to resist subduction. Calculation of the crustal mass balance during the collision between India and Eurasia indicates that about 50% of pre-collisional continental crust has been subducted into the mantle.

Origin of geochemical mantle components: Role of subduction filter

AbstractWe quantitatively explore element redistribution at subduction zones using numerical mass balance models to evaluate the roles of the subduction zone filter in the Earth's geochemical cycle. Our models of slab residues after arc magma genesis differ from previous ones by being internally consistent with geodynamic models of modern arcs that successfully explain arc magma genesis and include element fluxes from the dehydration/melting of each underlying slab component. We assume that the mantle potential temperature (Tp) was 1400–1650°C at 3.5–1.7 Ga and gradually decreased to 1300–1350°C today. Hot subduction zones with Tp ∼1650°C have a thermal structure like modern SW Japan where high‐Mg andesite is formed which is chemically like continental crust. After 2.5–1.7 Gyr of storage in the mantle, the residual igneous oceanic crust from hot subduction zones can evolve isotopically to the HIMU mantle component, the residual base of the mantle wedge to EMI, the residual sediment becomes an essential part of EMII, and the residual top of the mantle wedge can become the subcontinental lithosphere component. The Common or Focal Zone component is a stable mixture of the first three residues occasionally mixed with early depleted mantle. Slab residues that recycled earlier (∼2.5 Ga) form the DUPAL anomaly in the southern hemisphere, whereas residues of more recent recycling (∼1.7 Ga) underlie the northern hemisphere. These ages correspond to major continental crust forming events. The east‐west heterogeneity of the depleted upper mantle involves subcontinental mantle except in the Pacific.

Geochemistry and Nd isotopic characteristics of Earth's Hadean mantle and primitive crust

Abstract The Isua supracrustal belt (ISB) and the Nuvvuagittuq greenstone belt (NGB) are among the oldest suites of mafic volcanic rocks preserved on Earth and are the best candidates for representing its early crust. Despite the possible 500 Ma age difference between the belts, these mantle-derived rocks show compositional similarities, with features resembling rocks formed in subduction initiation environments. With the addition of new 142Nd data for the Garbenschiefer unit of the ISB reported here, high precision 142Nd data are now available for all the mafic lithologies from both belts. Mantle-derived rocks from both the ISB and NGB belts exhibit a range of 142Nd/144Nd ratios. The datasets for the two belts, however, are significantly different, suggesting a different origin for their 142Nd anomalies. Nearly all ISB samples have excesses in 142Nd, including the newly analyzed Garbenschiefer boninitic amphibolites (mean of + 12 ppm ). Excesses in 142Nd/144Nd compared to the Nd standard for all the ISB rocks range between +8 and + 20 ppm , with a near Gaussian distribution around + 12 ppm . This distribution could simply reflect the analytical error (±5 ppm) around a single 142Nd/144Nd ratio indicating that the samples formed after the extinction of 146Sm from a source with a nearly uniform 142Nd/144Nd ratio. In contrast, the NGB shows a range of 142Nd/144Nd ratios from +8 to − 18 ppm relative to the modern Nd standard and displays a flat distribution of 142Nd/144Nd ratios. The ISB samples show no significant correlation between their 142Nd/144Nd and Sm/Nd ratios, consistent with their formation in the Eoarchean via melting of a Hadean depleted mantle. In contrast, all NGB samples display a 142Nd/144Nd vs. Sm/Nd correlation, consistent with their crystallization in the Hadean. The mantle sources for both the ISB and NGB mantle-derived rocks have a similar 142Nd/144Nd ratio at the possible age of formation of the NGB (∼4.3 Ga) suggesting the derivation of ISB and NGB rocks from a common early-formed depleted mantle source formed between 4.47 and 4.42 Ga with a 147Sm/144Nd ratio ∼0.218. This mantle appears to have been an important source component involved in the formation of the primitive crust during most of the Hadean and Eoarchean eons.

Redox-variability and controls in subduction zones from an iron-isotope perspective

An ongoing controversy in mantle geochemistry concerns the oxidation state of the sources of island arc lavas (IAL). Three key factors control oxidation–reduction (redox) of IAL sources: (i) metasomatism of the mantle wedge by fluids and/or melts, liberated from the underlying subducted slab; (ii) the oxidation state of the wedge prior to melting and metasomatism; and (iii) the loss of melt from IAL sources. Subsequently, magmatic differentiation by fractional crystallisation, possible crustal contamination and degassing of melts en route to and at the surface can further modify the redox states of IAL. The remote nature of sub-arc processes and the complex interplay between them render direct investigations difficult. However, a possible gauge for redox-controlled, high-temperature pre-eruptive differentiation conditions is variations in stable Fe isotope compositions (expressed here as δ57Fe) in erupting IAL because Fe isotopes can preserve a record of sub-surface mass transfer reactions involving the major element Fe. Here we report Fe isotope compositions of bulk IAL along the active Banda arc, Indonesia, which is well known for a prominent subducted sediment input. In conjunction with other arc rocks, δ57Fe in erupted Banda IAL indicates that fractional crystallisation and possibly crustal contamination primarily control their Fe isotope signatures. When corrected for fractional crystallisation and filtered for contamination, arc magmas that had variable sediment melt contributions in their sources show no resolvable co-variation of δ57Fe with radiogenic isotope tracers. This indicates that crustal recycling in the form of subducted sediment does not alter the Fe isotope character of arc lavas, in agreement with mass balance estimates. Primitive sources of IAL, however, are clearly isotopically lighter than those sourced beneath mid-ocean ridges, indicating either preferential Fe3+-depletion in the mantle wedge by prior, δ57Fe-heavy melt extraction, and/or addition of an isotopically-light slab-derived agent. Based on our findings and previous models of arc redox conditions, we propose a three-stage process to explain the Fe isotope composition of IAL: (i) prior melt depletion lowers Fe3+/ΣFe (Fe3+ over total Fe) in the residues, leaving refractory, δ57Fe-light and possibly reduced mantle wedge protoliths beneath arcs. The oxygen fugacity (fO2) of these refractory protoliths may be up to −2 log10 units reduced relative to the fayalite–magnetite–quartz synthetic oxygen buffer (ΔFMQ); (ii) oxidised, slab-derived fluids, Fe-poor but possibly rich in sulphate (i.e., S6+), trigger melting of depleted protoliths with minimal effect on δ57Fe. Melts derived from this fluid-modified wedge source have high Fe3+/ΣFe, oxidised by the reduction of S6+, but importantly retain the light δ57Fe from their mantle wedge source; (iii) after melt liberation from the mantle wedge, arc magmas initially become progressively oxidised and isotopically heavier in Fe through fractional crystallisation of ferromagnesian silicates. In summary, reduction consequent to Fe3+-rich melt extraction and subsequent oxidation, likely by S6+-rich fluids, results in a “redox yo-yo” in IAL sources. Fractional crystallisation will further oxidise and elevate δ57Fe in erupting IAL. Iron isotope signatures in IAL record a complex magmatic history with no simple relation between δ57Fe and calculated fO2 in erupted lavas. Records of higher fO2 in subduction zones compared to MORB sources are inherited from the subduction component.

Escape of unradiogenic osmium during sub-aerial lava degassing: Evidence from fumarolic deposits, Piton de la Fournaise, Réunion Island

This study presents new Re–Os isotope and elemental data in gas condensates and corresponding lavas in order to examine the geochemical behavior of these two elements during magma degassing at Piton de la Fournaise, Réunion Island.Gas sublimates formed between 2007 and 2011 at temperature ranging from 400 to ca. 100°C include Na–K sulfate (aphthitalite), Na sulfate (thenardite), Ca–Cu sulfate (e.g. gypsum), Ca–Mg–Al–Fe fluoride (e.g. ralstonite) and native sulfur. The high temperature deposits show trace element typical of volcanic gas with high enrichment in Re (24 to 79ppb), almost two order of magnitude higher than the corresponding lavas but with Os abundances similar to those of the lavas (14–132 ppt). In contrast the Os contents of the low temperature fluoride deposits (13–77ppb) are higher than any of the other condensates. The fluorides are also enriched in Re, albeit to lesser extent than Os (2.9–15.3ppb). Based on high-temperature samples, the fluid/melt partition coefficients estimated for Re and Os are 100±80 and 1±2, respectively. Considering 1% of fluid loss, these partition coefficients translate into emanation coefficients of 0.50 (0.17–0.65) for Re and 0.01 (0–0.03) for Os. These results indicate that Re, unlike Os, is highly volatile at Piton de la Fournaise.Osmium isotopic compositions of samples collected at medium and low temperature (<350°C) are very uniform and unfractionated (187Os/188Os between 0.130–0.135) and plot within the range of the April 2007 lava flow and the historical lavas of Piton de la Fournaise (i.e. 0.130–0.137). However the highest temperature condensates (Na–K sulfates with T of 384–400°C) yield lower 187Os/188Os ratios (i.e. 0.124–0.129) within the field of mantle signal. Such unradiogenic compositions are best explained if old mantle sulfides occur in lavas and contribute to volcanic gases. Within the general frame of osmium mantle geochemistry, loss of unradiogenic Os during magmas degassing could help to explain osmium isotope disequilibrium between lavas and melting residues.

First-principles investigations of equilibrium calcium isotope fractionation between clinopyroxene and Ca-doped orthopyroxene

Equilibrium fractionation factors of Ca isotopes among mantle minerals are essential for using Ca isotopes as an important tracer in mantle geochemistry. Using the vibrational frequencies obtained by the first-principles calculations based on density functional theory (DFT), we calculated equilibrium fractionation factors of Ca isotopes between two major Ca-bearing minerals, clinopyroxene (cpx) and orthopyroxene (opx). Our results show that opx has much higher 44Ca/40Ca than its co-existing cpx even at high temperatures (e.g., 1273K), agreeing with the observations on mantle peridotites. In addition to the well-known temperature effect, our calculations for the first time reveal that the inter-mineral Ca isotope fractionation factor between opx and cpx also has a strong dependence on the chemical composition of opx (i.e., Ca content). Specifically, it increases substantially with decreasing Ca/Mg (atomic ratio) of opx when Ca/Mgopx is lower than 1/15. Such compositional effect on inter-mineral Ca isotope fractionation provides a convincing interpretation to the different isotope fractionations between coexisting opx and cpx observed in Kilbourne Hole and San Carlos peridotites.

Conjecture with water and rheological control for subducting slab in the mantle transition zone

Seismic observations have shown structural variation near the base of the mantle transition zone (MTZ) where subducted cold slabs, as visualized with high seismic speed anomalies (HSSAs), flatten to form stagnant slabs or sink further into the lower mantle. The different slab behaviors were also accompanied by variation of the “660 km” discontinuity depths and low viscosity layers (LVLs) beneath the MTZ that are suggested by geoid inversion studies. We address that deep water transport by subducted slabs and dehydration from hydrous slabs could affect the physical properties of mantle minerals and govern slab dynamics. A systematic series of three-dimensional numerical simulation has been conducted to examine the effects of viscosity reduction or contrast between slab materials on slab behaviors near the base of the MTZ. We found that the viscosity reduction of subducted crustal material leads to a separation of crustal material from the slab main body and its transient stagnation in the MTZ. The once trapped crustal materials in the MTZ eventually sink into the lower mantle within 20–30 My from the start of the plate subduction. The results suggest crustal material recycle in the whole mantle that is consistent with evidence from mantle geochemistry as opposed to a two-layer mantle convection model. Because of the smaller capacity of water content in lower mantle minerals than in MTZ minerals, dehydration should occur at the phase transformation depth, ∼660 km. The variation of the discontinuity depths and highly localized low seismic speed anomaly (LSSA) zones observed from seismic P waveforms in a relatively high frequency band (∼1 Hz) support the hypothesis of dehydration from hydrous slabs at the phase boundary. The LSSAs which correspond to dehydration induced fluids are likely to be very local, given very small hydrogen (H+) diffusivity associated with subducted slabs. The image of such local LSSA zones embedded in HSSAs may not be necessarily captured in tomography studies. The high electrical conductivity in the MTZ beneath the northwestern Pacific subduction zone does not necessarily require a broad range of high water content homogeneously.