Abstract

The transport and degassing pathways of volatiles through large silicic magmatic systems are central to understanding geothermal fluid compositions, ore deposit genesis, and volcanic eruption dynamics and impacts. Here, we document sulfur (S), chlorine (Cl), and fluorine (F) concentrations in a range of host materials in eruptive deposits from Taupō volcano (New Zealand). Materials analysed are groundmass glass, silicic melt inclusions, and microphenocrystic apatite that equilibrated in shallow melt-dominant magma bodies; silicic melt and apatite inclusions within crystal cores inferred to be sourced from deeper crystal mush; and olivine-hosted basaltic melt inclusions from mafic enclaves that represent the most primitive feedstock magmas. Sulfur and halogen concentrations each follow distinct concentration pathways during magma differentiation in response to changing pressures, temperatures, oxygen fugacities, crystallising mineral phases, the effects of volatile saturation, and the presence of an aqueous fluid phase. Sulfur contents in the basaltic melt inclusions (~ 2000 ppm) are typical for arc-type magmas, but drop to near detection limits by dacitic compositions, reflecting pyrrhotite crystallisation at ~ 60 wt. % SiO2 during the onset of magnetite crystallisation. In contrast, Cl increases from ~ 500 ppm in basalts to ~ 2500 ppm in dacitic compositions, due to incompatibility in the crystallising phases. Fluorine contents are similar between mafic and silicic compositions (< 1200 ppm) and are primarily controlled by the onset of apatite and/or amphibole crystallisation and then destabilisation. Sulfur and Cl partition strongly into an aqueous fluid and/or vapour phase in the shallow silicic system. Sulfur contents in the rhyolite melts are low, yet the Oruanui supereruption is associated with a major sulfate peak in ice core records in Antarctica and Greenland, implying that excess S was derived from a pre-eruptive gas phase, mafic magma recharge, and/or disintegration of a hydrothermal system. We estimate that the 25.5 ka Oruanui eruption ejected > 130 Tg of S (390 Tg sulfate) and up to ~ 1800 Tg of Cl, with potentially global impacts on climate and stratospheric ozone.

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