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Submitted in partial fulfillment of the requirements for the degree of Doctor of Philosophy at the Massachusetts Institute of Technology and the Woods Hole Oceanographic Institution February 2023., Subduction zones are important sites of material recycling on Earth, with volatiles playing key roles in mass transfer processes and magma formation. This thesis investigates outstanding questions associated with a continuum of interrelated processes that occur as oceanic plates descend in subduction zones by integrating petrological and geochemical constraints from exhumed high-pressure rocks and erupted arc magmas, high pressure-temperature laboratory experiments, and thermodynamic calculations. Chapters 2 and 3 investigate the fluid-mediated reactions between mafic and ultramafic rocks at conditions relevant to the slab-mantle interface and show that Mg-metasomatism of mafic rocks to form chlorite-rich assemblages is favored and is likely more pervasive in subduction zones than in oceanic settings. Contrary to common belief, talc is unlikely to form in high abundance in ultramafic rocks metasomatized by Si-rich slabderived fluids. This means that talc-rich assemblages formed via Si-metasomatism along the slabmantle interface are less likely to be playing prominent roles in volatile transport, in facilitating slow-slip events, and in controlling the decoupling-coupling transition of the plate interface. Chapter 4 experimentally investigates the phase equilibria, melting, and density evolution of mélange rocks that formed by mixing and fluid-rock interactions. Results show that melting of mélanges is unlikely to occur along slab-tops at pressures ≤ 2.5 GPa. Accordingly, diapirism into the hotter mantle wedge would be required to initiate melting. The density contrast between mélanges and the overlying mantle would allow for buoyancy-driven diapirism at relatively low pressures and melting could subsequently occur in the hotter mantle wedge during ascent. However, diapir buoyancy may be limited at higher pressures due to the formation of abundant garnet especially in mélange rocks with peraluminous composition. Chapter 5 experimentally investigates the compositions, This work has been supported financially by the National Science Foundation-Office of International Science & Engineering, Petrology & Geochemistry (NSF-OISE) PIRE, Award# 1545903 to F.K. and the Geoprisms program Collaborative Research Award# 1852610 to V.L.R. Research support through the WHOI Ocean Ventures Fund, US Science Support Program E-FIRE European Training Fund, WHOI Conference Fund are awarded to E.A.C.

© The Author(s), 2022. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Shu, Y., Nielsen, S. G., Le Roux, V., Wörner, G., Blusztajn, J., & Auro, M. Sources of dehydration fluids underneath the Kamchatka arc. Nature Communications, 13(1), (2022): 4467, https://doi.org/10.1038/s41467-022-32211-5., 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., This study was financially supported by grants from the National Natural Science Foundation of China (NSFC) (Grant No. 41903008) and Chinese Postdoctoral Science Foundation (Grant No. 2019M660153) to Y.S., NSF (Grant No. EAR-1829546) to S.G.N. and NSF (Grant No. EAR-1855302) to V.L.R.

Submitted in partial fulfillment of the requirements for the degree of Doctor of Philosophy at the Massachusetts Institute of Technology and the Woods Hole Oceanographic Institution February 2021., This thesis explores the volatile content of the mantle, subducted oceanic crust, and arc magmas as well as the structure of slow spreading ocean crust and the heterogeneity of Earth’s upper mantle. In Chapter 2, I directly explore the halogen (F and Cl) content of mantle minerals in situ, then use these measurements to assess the halogen content of the upper mantle. In Chapter 3, I investigate the volatile content of Raspas eclogites (SW Ecuador), a proxy for deeply subducted oceanic crust, to evaluate volatile transfer from crustal generation at divergent plate boundaries (e.g., mid-ocean ridges) to recycling of ocean crust at subduction zones. In Chapter 4, I use the H2O content of nominally anhydrous minerals in plutonic arc cumulates to elucidate the H2O content of the melts from which the rocks crystallized. In this way, I assert that primitive arc magmas may contain 4–10 wt.% H2O and through fractional crystallization up to ~20 wt.% H2O, making them far more hydrous than traditional methods (i.e., olivine-hosted melt inclusions) surmise. In Chapter 5, I show that mantle peridotite exposed along the 16ºN region of the Mid-Atlantic Ridge originated in an arc setting and has been remixed into subridge mantle, indicating that the sub-ridge mantle is more heterogeneous and depleted than inferences made from mid-ocean ridge basalts suggest. Chapter 6 surveys the life cycle of oceanic core complexes through zircon geochronology and posits an updated framework for understanding the termination of oceanic core complexes, and more broadly oceanic detachment faults. Together, this contribution highlights the chemical heterogeneity of the mantle, and quantifies the full extent of volatiles hosted by mantle and crustal reservoirs., The Stanley Watson Fellowship (WHOI) provided financial support during my first year of graduate school. The Academic Programs Office Ocean Venture Fund (WHOI) provided seed funding which initiated Chapters 3 and 4, and ultimately led to two funded NSF proposals. These resources are vital to JP students, and I am incredibly grateful for them. Primary support was provided by the National Science Foundation grants to Veronique Le Roux (EAR P&G #1524311, #1839128, #1855302) and Henry Dick (MG&G #1637130, #1657983).

Dissociation of methane hydrates due to ocean warming releases methane, a powerful greenhouse gas, to the atmosphere. Dissociation of gas hydrates may have led to rapid and dramatic environmental changes in the past. Thus, understanding the impact of those events requires information about their timing and magnitudes. While the foraminiferal fossil record provides a powerful tool to understand past environmental conditions, seep-endemic foraminifera are unknown, which limits evaluation of seep-specific information. However, geographically widespread benthic foraminifera do inhabit seep sites, as documented widely in the literature, and may provide information useful to the understanding of past methane releases. In an effort to better understand how benthic foraminifera inhabit this chemosynthesis-based ecosystem, and if they faithfully record the methane emissions, we conducted a multipronged analysis of foraminifera associated with a gas hydrate emission site in the Arctic. Our goal was to simultaneously assess, in single representative calcareous benthic foraminiferal individuals, the cell biology, test stable carbon isotope ratio, and carbonate microstructure (e.g., wall thickness, survey for authigenic overgrowths), from samples collected south of Svalbard, or on Vestnesa Ridge, west of Svalbard). Serially, each specimen was scanned with microCT (computerized tomography) to assess test characteristics, then the test dissolved by acidification while capturing gas to measure stable carbon isotope ratio via continuous-flow mass spectrometry, and finally the remaining soft parts embedded and examined for cell ultrastructure with a Transmission Electron Microscope (TEM). TEM). Data from isotopic analyses, microCT scans and TEM imaging are presented here., This project was funded by NSF (WHOI) OCE-1634469 NSF (UFL) OCE-1634248 Norwegian Research Council 223259

The large range of H2O contents recorded in minerals from exhumed mantle rocks has been challenging to interpret, as it often records a combination of melting, metasomatism, and diffusional processes in spatially isolated samples. Here, we determine the temporal variations of H2O contents in pyroxenes from a 24-Ma time series of abyssal peridotites exposed along the Vema fracture zone (Atlantic Ocean). The H2O contents of pyroxenes correlate with both crustal ages and pyroxene chemistry and increase toward younger and more refractory peridotites. These variations are inconsistent with residual values after melting and opposite to trends often observed in mantle xenoliths. Postmelting hydrogen enrichment occurred by ionic diffusion during cryptic metasomatism of peridotite residues by low-degree, volatile-rich melts and was particularly effective in the most depleted peridotites. The presence of hydrous melts under ridges leads to widespread hydrogen incorporation in the oceanic lithosphere, likely lowering mantle viscosity compared to dry models.

Author Posting. © American Geophysical Union, 2019. This article is posted here by permission of American Geophysical Union for personal use, not for redistribution. The definitive version was published in Geochemistry, Geophysics, Geosystems 20, (2019): 6123-6139, doi: 10.1029/2019GC008711., Gravity, magnetic, and bathymetry data collected along a continuous 1,400‐km‐long spreading‐parallel flow line across the Mid‐Atlantic Ridge indicate significant tectonic and magmatic fluctuations in the formation of oceanic crust over a range of time scales. The transect spans from 28 Ma on the African Plate to 74 Ma on the North American plate, crossing the Mid‐Atlantic Ridge at 35.8°N. Gravity‐derived crustal thicknesses vary from 3–9 km with a standard deviation of 1.0 km. Spectral analysis of bathymetry and residual mantle Bouguer anomaly show a diffuse power at >1 Myr and concurrent peaks at 390, 550, and 950 kyr. Large‐scale (>10 km) mantle thermal and compositional heterogeneities, variations in upper mantle flow, and detachment faulting likely generate the >1 Myr diffuse power. The 550‐ and 950‐kyr peaks may reflect the presence of magma solitons and/or regularly spaced ~7.7 and 13.3 km short‐wavelength mantle compositional heterogeneities. The 390‐kyr spectral peak corresponds to the characteristic spacing of faults along the flow line. Fault spacing also varies over longer periods (>10 Myr), which we interpret as reflecting long‐lived changes in the fraction of tectonically versus magmatically accommodated extensional strain. A newly discovered off‐axis oceanic core complex (Kafka Dome) found at 8 Ma on the African plate further suggests extended time periods of tectonically‐dominated plate separation. Fault spacing negatively correlates with gravity‐derived crustal thickness, supporting a strong link between magma input and fault style at mid‐ocean ridges., Data and supplemental materials are available at the Woods Hole Open Access Server (doi.org/10.26025/1912/24796). We would like to thank the Woods Hole Oceanographic Institution, National Science Foundation, Naval Oceanographic Office, and the captain and crew of R/V Neil Armstrong for making the SCARF cruise possible. We would also like to thank Eboné Pierce for her help during the cruise. We thank Meghan Jones for advice using MBSystem. We also thank Maurice Tivey, John Greene, and Masako Tominaga for advice on processing the magnetic data sets. We would like to thank Peter Huybers for sharing his spectral analysis codes. We would like to thank Rob Sohn for his help on interpreting the spectral analysis. We would like to thank Del Bohnenstiel, Milena Marjanović, one anonymous reviewer, and Editor Thorsten Becker for their very helpful comments that improved this manuscript. Funding was provided for this research by NSF OCE‐14‐58201., 2020-05-19

Gravity, magnetic, and bathymetry data collected along a continuous 1,400‐km‐long spreading‐parallel flow line across the Mid‐Atlantic Ridge indicate significant tectonic and magmatic fluctuations in the formation of oceanic crust over a range of time scales. The transect spans from 28 Ma on the African Plate to 74 Ma on the North American plate, crossing the Mid‐Atlantic Ridge at 35.8°N. Gravity‐derived crustal thicknesses vary from 3–9 km with a standard deviation of 1.0 km. Spectral analysis of bathymetry and residual mantle Bouguer anomaly show a diffuse power at >1 Myr and concurrent peaks at 390, 550, and 950 kyr. Large‐scale (>10 km) mantle thermal and compositional heterogeneities, variations in upper mantle flow, and detachment faulting likely generate the >1 Myr diffuse power. The 550‐ and 950‐kyr peaks may reflect the presence of magma solitons and/or regularly spaced ~7.7 and 13.3 km short‐wavelength mantle compositional heterogeneities. The 390‐kyr spectral peak corresponds to the characteristic spacing of faults along the flow line. Fault spacing also varies over longer periods (>10 Myr), which we interpret as reflecting long‐lived changes in the fraction of tectonically versus magmatically accommodated extensional strain. A newly discovered off‐axis oceanic core complex (Kafka Dome) found at 8 Ma on the African plate further suggests extended time periods of tectonically‐dominated plate separation. Fault spacing negatively correlates with gravity‐derived crustal thickness, supporting a strong link between magma input and fault style at mid‐ocean ridges.

The peridotite section of supra-subduction zone ophiolites is often crosscut by pyroxenite veins, reflecting the variety of melts that percolate through the mantle wedge, react, and eventually crystallize in the shallow lithospheric mantle. Understanding the nature of parental melts and the timing of formation of these pyroxenites provides unique constraints on melt infiltration processes that may occur in active subduction zones. This study deciphers the processes of orthopyroxenite and clinopyroxenite formation in the Josephine ophiolite (USA), using new trace and major element analyses of pyroxenite minerals, closure temperatures, elemental profiles, diffusion modeling, and equilibrium melt calculations. We show that multiple melt percolation events are required to explain the variable chemistry of peridotite-hosted pyroxenite veins, consistent with previous observations in the xenolith record. We argue that the Josephine ophiolite evolved in conditions intermediate between back-arc and sub-arc. Clinopyroxenites formed at an early stage of ophiolite formation from percolation of high-Ca boninites. Several million years later, and shortly before exhumation, orthopyroxenites formed through remelting of the Josephine harzburgites through percolation of ultra-depleted low-Ca boninites. Thus, we support the hypothesis that multiple types of boninites can be created at different stages of arc formation and that ophiolitic pyroxenites uniquely record the timing of boninite percolation in subduction zone mantle.

© The Author(s), 2018. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Science Advances 4 (2018): eaas8675, doi: 10.1126/sciadv.aas8675., The 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., This study was supported by NSF grants EAR-1119373 and EAR-1427310 to S.G.N.

© The Author(s), 2018. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Nature Communications 9 (2018): 2864, doi:10.1038/s41467-018-05313-2., The mechanisms of transfer of crustal material from the subducting slab to the overlying mantle wedge are still debated. Mélange rocks, formed by mixing of sediments, oceanic crust, and ultramafics along the slab-mantle interface, are predicted to ascend as diapirs from the slab-top and transfer their compositional signatures to the source region of arc magmas. However, the compositions of melts that result from the interaction of mélanges with a peridotite wedge remain unknown. Here we present experimental evidence that melting of peridotite hybridized by mélanges produces melts that carry the major and trace element abundances observed in natural arc magmas. We propose that differences in nature and relative contributions of mélanges hybridizing the mantle produce a range of primary arc magmas, from tholeiitic to calc-alkaline. Thus, assimilation of mélanges into the wedge may play a key role in transferring subduction signatures from the slab to the source of arc magmas., This project was supported by the WHOI Ocean Exploration Institute (OEI) 27071178 to V.L.R.; Previous related projects were supported by NSF EAR-1348063 and WHOI OEI to H.R.M.

Observations of dunite channels in ophiolites and uranium series disequilibria in mid-ocean ridge basalt suggest that melt transport in the upper mantle beneath mid-ocean ridges is strongly channelized. We present experimental evidence that spatial variations in mineralogy can also focus melt on the grain scale. This lithologic melt partitioning, which results from differences in the interfacial energies associated with olivine-melt and orthopyroxene-melt boundaries, may complement other melt focusing mechanisms in the upper mantle such as mechanical shear and pyroxene dissolution. We document here lithologic melt partitioning in olivine-/orthopyroxene-basaltic melt samples containing nominal olivine to orthopyroxene ratio of 3 to 2 and melt fractions of 0.02 to 0.20. Experimental samples were imaged using synchrotron-based X-ray microcomputed tomography at a resolution of 700 nm per voxel. By analyzing the local melt fraction distributions associated with olivine and orthopyroxene grains in each sample, we found that the melt partitioning coefficient, i.e., the ratio of melt fraction around olivine to that around orthopyroxene grains, varies between 1.1 and 1.6. The permeability and electrical conductivity of our digital samples were estimated using numerical models and compared to those of samples containing only olivine and basaltic melt. Our results suggest that lithologic melt partitioning and preferential localization of melt around olivine grains might play a role in melt focusing, potentially enhancing average melt ascent velocities.