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ArticleSources of dehydration fluids underneath the Kamchatka arc(Nature Research, 2022-08-02) Shu, Yunchao ; Nielsen, Sune G. ; Le Roux, Véronique ; Wörner, Gerhard ; Blusztajn, Jerzy S. ; Auro, Maureen E.Fluids mediate the transport of subducted slab material and play a crucial role in the generation of arc magmas. However, the source of subduction-derived fluids remains debated. The Kamchatka arc is an ideal subduction zone to identify the source of fluids because the arc magmas are comparably mafic, their source appears to be essentially free of subducted sediment-derived components, and subducted Hawaii-Emperor Seamount Chain (HESC) is thought to contribute a substantial fluid flux to the Kamchatka magmas. Here we show that Tl isotope ratios are unique tracers of HESC contribution to Kamchatka arc magma sources. In conjunction with trace element ratios and literature data, we trace the progressive dehydration and melting of subducted HESC across the Kamchatka arc. In succession, serpentine (<100 km depth), lawsonite (100–250 km depth) and phengite (>250 km depth) break down and produce fluids that contribute to arc magmatism at the Eastern Volcanic Front (EVF), Central Kamchatka Depression (CKD), and Sredinny Ridge (SR), respectively. However, given the Tl-poor nature of serpentine and lawsonite fluids, simultaneous melting of subducted HESC is required to explain the HESC-like Tl isotope signatures observed in EVF and CKD lavas. In the absence of eclogitic crust melting processes in this region of the Kamchatka arc, we propose that progressive dehydration and melting of a HESC-dominated mélange offers the most compelling interpretation of the combined isotope and trace element data.
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ArticleThallium isotope fractionation during magma degassing: evidence from experiments and Kamchatka arc lavas(American Geophysical Union, 2021-04-19) Nielsen, Sune G. ; Shu, Yunchao ; Wood, Bernard J. ; Blusztajn, Jerzy S. ; Auro, Maureen E. ; Norris, C. Ashley ; Wörner, GerhardThallium (Tl) isotope ratios are an emerging tool that can be used to trace crustal recycling processes in arc lavas and ocean island basalts (OIBs). Thallium is a highly volatile metal that is enriched in volcanic fumaroles, but it is unknown whether degassing of Tl from subaerial lavas has a significant effect on their residual Tl isotope compositions. Here, we present Tl isotope and concentration data from degassing experiments that are best explained by Rayleigh kinetic isotope fractionation during Tl loss. Our data closely follow predicted isotope fractionation models in which TlCl is the primary degassed species and where Tl loss is controlled by diffusion and natural convection, consistent with the slow gas advection velocity utilized during our experiments. We calculate that degassing into air should be associated with a net Tl isotope fractionation factor of αnet = 0.99969 for diffusion and natural gas convection (low gas velocities) and αnet = 0.99955 for diffusion and forced gas convection (high gas velocities). We also show that lavas from three volcanoes in the Kamchatka arc exhibit Tl isotope and concentration patterns that plot in between the two different gas convection regimes, implying that degassing played an important role in controlling the observed Tl isotope compositions in these three volcanoes. Literature inspection of Tl isotope data for subaerial lavas reveals that the majority of these appear only minorly affected by degassing, although a few samples from both OIBs and arc volcanoes can be identified that likely experienced some Tl degassing.
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ArticleBarium isotope evidence for pervasive sediment recycling in the upper mantle(American Association for the Advancement of Science, 2018-07-11) Nielsen, Sune G. ; Horner, Tristan J. ; Pryer, Helena V. ; Blusztajn, Jerzy S. ; Shu, Yunchao ; Kurz, Mark D. ; Le Roux, VéroniqueThe upper mantle, as sampled by mid-ocean ridge basalts (MORBs), exhibits significant chemical variability unrelated to mechanisms of melt extraction at ridges. We show that barium isotope variations in global MORBs vary systematically with radiogenic isotopes and trace element ratios, which reflects mixing between depleted and enriched MORB melts. In addition, modern sediments and enriched MORBs share similar Ba isotope signatures. Using modeling, we show that addition of ~0.1% by weight of sediment components into the depleted mantle in subduction zones must impart a sedimentary Ba signature to the overlying mantle and induce low-degree melting that produces the enriched MORB reservoir. Subsequently, these enriched domains convect toward mid-ocean ridges and produce radiogenic isotope variation typical of enriched MORBs. This mechanism can explain the chemical and isotopic features of enriched MORBs and provide strong evidence for pervasive sediment recycling in the upper mantle.
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ArticleThallium isotopes reveal brine activity during carbonatite magmatism(American Geophysical Union, 2021-01-27) Horton, Forrest ; Nielsen, Sune G. ; Shu, Yunchao ; Gagnon, Alan R. ; Blusztajn, Jerzy S.Carbonatite volcanism remains poorly understood compared to silicic volcanism due to the scarcity of carbonatite volcanoes worldwide and because volcanic H2O and CO2—major components in carbonatite volcanic systems—are not well preserved in the rock record. To further our understanding of carbonatite genesis, we utilize the non-traditional thallium (Tl) isotope system in Khanneshin carbonatites in Afghanistan. These carbonatites contain 250–30,000 ng/g Tl and have ε205Tl values (−4.6 to +4.6) that span much of the terrestrial igneous range. We observe that δ18OVSMOW (+8.6‰ to +23.5‰) correlates positively with δ13CVPDB (−4.6‰ to +3.5‰) and ε205Tl up to δ18O = 15‰. Rayleigh fractionation of calcite from an immiscible CO2-H2O fluid with a mantle-like starting composition can explain the δ18O and δ13C—but not ε205Tl—trends. Biotite fractionates Tl isotopes in other magmatic settings, so we hypothesize that a Tl-rich hydrous brine caused potassic metasomatism (i.e., biotite fenitization) of wall rock that increased the ε205Tl of the residual magma-fluid reservoir. Our results imply that, in carbonatitic volcanic systems, simultaneous igneous differentiation and potassic metasomatism increase ε205Tl, δ18O, δ13C, and light rare earth element concentrations in residual fluids. Our fractionation models suggest that the Tl isotopic compositions of the primary magmas were among the isotopically lightest (less than or equal to ε205Tl = −4.6) material derived from the mantle for which Tl isotopic constraints exist. If so, the ultimate source of Tl in Khanneshin lavas—and perhaps carbonatites elsewhere—may be recycled ocean crust.
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PreprintThallium isotopes as tracers of recycled materials in subduction zones : review and new data for lavas from Tonga-Kermadec and Central America( 2017-04) Nielsen, Sune G. ; Prytulak, Julie ; Blusztajn, Jerzy S. ; Shu, Yunchao ; Auro, Maureen E. ; Regelous, Marcel ; Walker, James A.Sediment is actively being subducted in every convergent margin worldwide. Yet, geochemical data for arc lavas from several subduction zones, such as Northern Tonga and Costa Rica have revealed either attenuated or limited evidence for sediment in their mantle source regions. Here we use thallium (Tl) isotopes to trace slab components in lavas from the Tonga-Kermadec and Central American arcs. In general, both arcs display Tl isotope data that are most compatible with addition of sediment to the sub-arc mantle from the subducting slab. This evidence is particular strong in the Tonga-Kermadec arc where pelagic clays dominate the Tl budget along the entire arc. Contributions from altered oceanic crust as well as the Louisville Seamount chain that subducts underneath Northern Tonga are not visible in Tl isotopes, which is likely due to the very high Tl concentrations found in pelagic sediments outboard of the Tonga-Kermadec arc. Lavas from Central America reveal variable and systematic Tl isotope compositions along-strike. In particular, lavas from Nicaragua are dominated by contributions from sediments, whereas Costa Rican samples reveal a significant altered oceanic crust component with little influence from sediments on thallium isotope composition. The absence of a sediment signature in Costa Rica corresponds with the Cocos Ridge and the seamount province subduction, which results in a thinner sediment cover. Furthermore, the subducted sediment is dominated by carbonates with very low Tl concentrations and, therefore, small amounts of carbonate sediment added to the mantle wedge do not contribute significantly to the overall Tl budget. A review of Tl isotope and concentration data from the Aleutians, Marianas, Tonga-Kermadec and Central American arcs demonstrate that pelagic sediments are detectable in most arcs, whereas altered oceanic crust components only become appreciable when sediment Tl concentrations are very low (e.g. carbonate) or if sediments are no longer a significant component of the subducting slab (e.g. slab melting in Western Aleutians). As such, Tl isotopes are a promising tool to trace sediment subduction although this requires at least some pelagic sediment is present in the subducted sediment package. We suggest that thallium partitioning between the slab and mantle wedge is most likely controlled by retention in phengite or by partitioning into fluids. Residual phengite likely produces high Cs/Tl ratios because Tl should be more compatible in phengite than is Cs, however, this conclusion needs experimental verification. The stability of phengite is lower at higher fluid contents, which results in hyperbolic relationships between Cs/Tl and possible indicators of fluids such as Sr/Nd and Ba/Th. Thus, combined Tl isotopic and elemental systematics not only provide detailed information about the specific slab components that contribute to arc lavas, but also potentially shed light on the mineralogy and physical conditions of subducting slabs.