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Abstract Whole rock compositions at Buldir Volcano, western Aleutian arc, record a strong, continuous trend of iron depletion with decreasing MgO, classically interpreted as a calc-alkaline liquid line of descent. In contrast, olivine-hosted melt inclusions have higher total iron (FeO*) than whole rocks and show little change in FeO* with decreasing MgO. To investigate this discrepancy and determine the conditions required for strong iron depletion, we conducted oxygen fugacity (ƒO2) buffered, water-saturated crystallization experiments at 800 MPa and ƒO2 = QFM + 1.6 ± 0.4 (1$$\sigma$$) (where QFM refers to the quartz-fayalite-magnetite buffer) on a high-Al, basaltic starting material modeled after a Buldir lava. Experimental conditions were informed by olivine-hosted melt inclusions that record minimum entrapment pressures as high as 570 MPa, >6 wt % H2O, and ƒO2 of QFM + 1.4 (±0.2), making Buldir one of the most oxidized and wettest arc volcanoes documented globally. The experiments produce melts with Si-enrichment and Fe-depletion signatures characteristic of evolved, calc-alkaline magmas at the lowest MgO, although FeO* remains roughly constant over most of the experimental temperature range. Experiments saturate CrAl-spinel and olivine at 1160°C, followed by clinopyroxene and Al-spinel at 1085°C, hornblende at 1060°C, and, finally, plagioclase and magnetite between 1040°C and 960°C. Hornblende crystallization, not magnetite, generates the largest increase in SiO2 and largest decrease in FeO* in coexisting melts. Compositions of melt inclusions are consistent with experimental melts and reflect crystallization of a basaltic parent magma at high PH2O. In contrast, the whole rock compositional trends are influenced by magma mixing and phenocryst redistribution and accumulation. The crystallization experiments and natural liquids (melt inclusions and groundmass glass) from Buldir suggest that for an oxidized, hydrous primary basalt starting composition, significant Fe depletion from the melt will not occur until intermediate to late stages of magma crystallization (< ~4.5 wt % MgO). We conclude that the Buldir whole rock trend cannot be reproduced by crystallization at arc-relevant oxygen fugacities and is not a true liquid line of descent, warranting caution when interpreting volcanic trends globally. 

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Subduction transports volatiles between Earth’s mantle, crust, and atmosphere, ultimately creating a habitable Earth. We use isotopes to track carbon from subduction to outgassing along the Aleutian-Alaska Arc. We find substantial along-strike variations in the isotopic composition of volcanic gases, explained by different recycling efficiencies of subducting carbon to the atmosphere via arc volcanism and modulated by subduction character. Fast and cool subduction facilitates recycling of ~43 to 61% sediment-derived organic carbon to the atmosphere through degassing of central Aleutian volcanoes, while slow and warm subduction favors forearc sediment removal, leading to recycling of ~6 to 9% altered oceanic crust carbon to the atmosphere through degassing of western Aleutian volcanoes. These results indicate that less carbon is returned to the deep mantle than previously thought and that subducting organic carbon is not a reliable atmospheric carbon sink over subduction time scales.