The Origin and Differentiation of CO2-Rich Primary Melts in Ocean Island Volcanoes: Integrating 3D X-Ray Tomography with Chemical Microanalysis of Olivine-Hosted Melt Inclusions from Pico (Azores).

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ABSTRACT Constraining the initial differentiation of primary mantle melts is vital for understanding magmatic systems as a whole. Chemical compositions of olivine-hosted melt inclusions preserve unique information about the mantle sources, crystallisation behaviour and volatile budgets of such melts. Crucially, melt inclusion CO2 contents can be linked to mantle CO2 budgets and inform us on Earth's carbon fluxes and cycles. However, determining total inclusion CO2 contents is not straightforward, as they often need to be reconstructed from CO2 dissolved in melts and CO2 stored in a vapour bubble. Here, we improve upon existing reconstruction methods by combining 3D X-ray computed tomography (CT) with geochemical microanalyses of major, trace and volatile elements. We show that in comparison to CT data, traditional reconstruction methods using 2D photomicrographs can underestimate CO2 budgets by more than 40%. We applied our improved methods to basaltic olivine-hosted melt inclusions from Pico volcano (Azores) in order constrain the formation and differentiation of volatile-rich primary melts in the context of a mantle plume. Results for these inclusions yielded 1935 to 9275 μg/g reconstructed total CO2, some of the highest values reported for ocean island volcanoes to date. Using these CO2 concentrations, we calculate entrapment pressures of 105 to 754 MPa that indicate a magma reservoir comprising stacked sills straddling the crust–mantle boundary. In the magma reservoir, crystallisation of volatile saturated melts drives extensive degassing, leading to fractionated CO2/Ba ratios of 3.5 to 62.2 and a loss of over 79% of primary mantle-derived CO2. Variabilities in trace elements (La, Y) show that differentiation occurred by concurrent mixing and crystallisation of two endmember melts, respectively depleted and enriched in trace elements. Geochemical models show that enriched endmember melts constitute 33 wt % of all melts supplied to the crust at Pico and that primary melts underwent 60% crystallisation prior to eruption. Mantle melting models indicate that the enriched and depleted primary melt endmembers are low- and high-degree melts of carbon-poor lherzolite and carbon-rich pyroxenite, respectively. Moreover, since deep magmas at Pico island are dominantly pyroxenite derived, their CO2-enrichement is mainly controlled by mantle source carbon content. Overall, our study illustrates that by combining 3D imaging, geochemical microanalyses and numerical modelling, melt inclusions provide a unique record of differentiation and storage of deep magmas, as well as mantle melting.