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The chemical and isotopic characteristics of a solidified pluton represent the integration of magmatic and sub-solidus processes operating across a range of spatial and temporal scales during pluton construction, crystallization, and cooling. Disentangling these processes and understanding where chemical and isotopic signatures were acquired requires the combination of multiple tools tracing processes at different time and length scales. We combine whole-rock oxygen and Sr-Nd isotopes, zircon oxygen isotopes and trace elements, and mineral compositions with published high-precision U-Pb zircon geochronology to evaluate differentiation within the bimodal Guadalupe Igneous Complex, Sierra Nevada, California (USA). The complex was constructed in ~300 k.y. between 149 and 150 Ma. Felsic magmas crystallized as centimeter- to meter-sized segregations in gabbros in the lower part of the complex and as granites and granophyres structurally above the gabbros. A central mingling zone separates the mafic and felsic units. Pluton-wide δ18O(whole-rock), δ18O(zircon), and Sr-Nd isotopic ranges are too large to be explained by in situ, closed-system differentiation, instead requiring open-system behavior at all scales. Low δ18O(whole-rock) and δ18O(zircon) values indicate assimilation of hydrothermally altered marine host rocks during ascent and/or emplacement. In situ differentiation processes operated on a smaller scale (meters to tens of meters) for at least ~200 k.y. via (1) percolation and segregation of chemically and isotopically diverse silicic interstitial melt from a heterogeneous gabbro mush; (2) crystal accumulation; and (3) sub-solidus, high-temperature, hydrothermal alteration at the shallow roof of the complex to modify the chemical and isotopic characteristics. Whole-rock and mineral chemistry in combination with geochronology allows deciphering open-system differentiation processes at the outcrop to pluton scale from magmatic to sub-solidus temperatures over time scales of hundreds of thousands to millions of years.

The chemical and isotopic characteristics of a solidified pluton represent the integration of magmatic and sub-solidus processes operating across a range of spatial and temporal scales during pluton construction, crystallization, and cooling. Disentangling these processes and understanding where chemical and isotopic signatures were acquired requires the combination of multiple tools tracing processes at different time and length scales. We combine whole-rock oxygen and Sr-Nd isotopes, zircon oxygen isotopes and trace elements, and mineral compositions with published high-precision U-Pb zircon geochronology to evaluate differentiation within the bimodal Guadalupe Igneous Complex, Sierra Nevada, California (USA). The complex was constructed in ~300 k.y. between 149 and 150 Ma. Felsic magmas crystallized as centimeter- to meter-sized segregations in gabbros in the lower part of the complex and as granites and granophyres structurally above the gabbros. A central mingling zone separates the mafic and felsic units. Pluton-wide δ18O(whole-rock), δ18O(zircon), and Sr-Nd isotopic ranges are too large to be explained by in situ, closed-system differentiation, instead requiring open-system behavior at all scales. Low δ18O(whole-rock) and δ18O(zircon) values indicate assimilation of hydrothermally altered marine host rocks during ascent and/or emplacement. In situ differentiation processes operated on a smaller scale (meters to tens of meters) for at least ~200 k.y. via (1) percolation and segregation of chemically and isotopically diverse silicic interstitial melt from a heterogeneous gabbro mush; (2) crystal accumulation; and (3) sub-solidus, high-temperature, hydrothermal alteration at the shallow roof of the complex to modify the chemical and isotopic characteristics. Whole-rock and mineral chemistry in combination with geochronology allows deciphering open-system differentiation processes at the outcrop to pluton scale from magmatic to sub-solidus temperatures over time scales of hundreds of thousands to millions of years. [ABSTRACT FROM AUTHOR]

The Fe3+/FeT ratios (Fe3+/[Fe2++Fe3+]) in minerals can be used to understand their crystallization and post-crystallization conditions. However, as natural minerals are often zoned and contain inclusions, bulk techniques, e.g., wet chemistry, may not provide accurate Fe3+/FeT values for a single phase of interest. We determined Fe3+/FeT ratios of amphiboles in different crystallographic orientations by single-crystal synchrotron Mossbauer spectroscopy (SMS) in energy and time domain modes from four volcanic localities (Long Valley Caldera, Mount St. Helens, Lassen Volcanic Center, U.S.A., and Mt. Pinatubo, Philippines). The high spatial resolution (as low as 12 x 12 ^m spot size) and standardfree nature of SMS allow the detection of intra-grain compositional heterogeneities in Fe3+/FeT with relatively low uncertainties. We combine SMS with major element compositions, water contents, and hydrogen isotope compositions to document the Fe3+/FeT ratios as a function of mineral composition and post-crystallization dehydrogenation. Spectra were fitted with up to five distinct sites: ferrous iron on M( 1), M(2), M(3), and ferric iron on M(2) and M(3), consistent with X-ray diffraction studies on single crystals of amphibole. The Fe3+/FeT ratios range from 0.14 ± 0.03 (Long Valley Caldera), 0.51 to 0.63 ± 0.02 (representing intra-grain heterogeneities, Mount St. Helens) to 0.86 ± 0.03 (Lassen Volcanic Center). The latter grain experienced post-crystallization dehydrogenation, shown by its low water content (0.6 ± 0.05 wt%) and its elevated hydrogen isotope composition (SD = +25 ± 3%o relative to SMOW). The Fe3+/FeT ratios of 0.62 ± 0.01 and 0.20 ± 0.01 of two Mt. Pinatubo grains correlate with high-Al2O3 cores and low-Al2O3 rims and smaller phenocrysts in the sample, respectively. This study shows that SMS is capable of distinguishing two different domains with dissimilar Fe3+/FeT values formed under different crystallization conditions, demonstrating that SMS in combination with major element, water, and hydrogen isotope compositions allows the interpretation of amphibole Fe3+/FeT ratios in the context of crystallization and post-crystallization processes. [ABSTRACT FROM AUTHOR]

Magma transfer from the mantle to the crust in arcs is an important step in the global cycling of elements and volatiles from Earth's interior to the atmosphere. Arc intrusive rocks dominate the total magma mass budget over extrusive rocks. However, their total volume and rate of addition is still poorly constrained, especially in continental arcs. We present lateral (forearc to backarc) and depth‐dependent (volcanics to deep crust) magma volume additions and arc‐wide magma addition rates (MARs) calculated from three continental arc crustal sections preserving magma flare‐up periods. We observe an increase in volume addition with depth and less magma added in the forearc (~15%) and backarc (~10% to 30%) compared to the main arc. Crustal‐wide MARs for each section are remarkably similar and around 0.7–0.9 km3/km2/Ma. MARs can be used to estimate CO2 fluxes from continental arcs. With initial magma CO2 contents of 1.5 wt.%, global continental arc lengths, and MARs, we calculate changes in C (Mt/year) released from continental arcs since 750 Ma. Calculated present‐day global C fluxes are similar to values constrained by other methods. Throughout the Phanerozoic, assuming equal durations of flare‐up and lull magmatism, calculated continental CO2 flux rates vary between 4 and 18 Mt C/year with highest values in the Mesozoic. These fluxes are considered minima since the intake of mantle and/or crustal carbon is not considered. Magmatic episodicity in continental arcs and changes in arc thickness and width are critical to consider when calculating MARs through time. Plain Language Summary: The transfer of magma from Earth's interior to the crust and surface via volcanic eruptions transports elements and volatiles, which can ultimately form economically important ore deposits and release gases to the atmosphere. However, the amount and timescales of magma addition to the crust, especially in continental settings, is poorly understood. In this study, we use exposed igneous rocks solidified at different depths in the crust and deposited during volcanic eruptions to determine the amount and timescales of magma addition. We use these newly constrained rates to calculate the total amount of CO2 gas released to the atmosphere by emplacement and crystallization of magma in the crust. Our calculations agree well with present‐day published estimates of CO2 degassing from continental arcs and allow us to extrapolate CO2 fluxes throughout Earth History to track relative changes in CO2 degassing to the atmosphere. Key Points: Depth‐dependent (volcanics to deep crust) and lateral (forearc to backarc) magma volume addition rates are calculated from exposed continental crustal sectionsVolume addition increases with depth and is lower in the forearc and backarc compared to the main arc, while crustal‐wide, long‐term rates are similar between arcsAddition rates are used to calculate global CO2 fluxes from continental arcs; calculated values are similar to global CO2 fluxes estimated by other methods [ABSTRACT FROM AUTHOR]