Volcanic emissions are a critical pathway in Earth’s carbon cycle. Here, we show that aerial measurements of volcanic gases using unoccupied aerial systems (UAS) transform our ability to measure and monitor plumes remotely and to constrain global volatile fluxes from volcanoes. Combining multi-scale measurements from ground-based remote sensing, long-range aerial sampling, and satellites, we present comprehensive gas fluxes—3760 ± [600, 310] tons day−1 CO2 and 5150 ± [730, 340] tons day−1 SO2—for a strong yet previously uncharacterized volcanic emitter: Manam, Papua New Guinea. The CO2/ST ratio of 1.07 ± 0.06 suggests a modest slab sediment contribution to the sub-arc mantle. We find that aerial strategies reduce uncertainties associated with ground-based remote sensing of SO2 flux and enable near–real-time measurements of plume chemistry and carbon isotope composition. Our data emphasize the need to account for time averaging of temporal variability in volcanic gas emissions in global flux estimates.

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Understanding lava flow processes is important for interpreting existing lavas and for hazard assessments. Although substantial progress has been made for basaltic lavas our understanding of silicic lava flows has seen limited recent advance. In particular, the formation of lava flow breakouts, which represent a characteristic process in coolinglimited basaltic lavas, but has not been described in established models of rhyolite emplacement. Using data from the 2011-2012 rhyolite eruption of Puyehue-Cordón Caulle, Chile, we develop the first conceptual framework to classify breakout types in silicic lavas, and to describe the processes involved in their progressive growth, inflation, and morphological change. By integrating multiscale satellite, field, and textural data from Cordón Caulle, we interpret breakout formation to be driven by a combination of pressure increase (from local vesiculation in the lava flow core, as well as from continued supply via extended thermally preferential pathways) and a weakening of the surface crust through lateral spreading and fracturing. Small breakouts, potentially resulting more from local vesiculation than from continued magma supply, show a domed morphology, developing into petaloid as inflation increasingly fractures the surface crust. Continued growth and fracturing results in a rubbly morphology, with the most inflated breakouts developing into a cleft-split morphology, reminiscent of tumulus inflation structures seen in basalts. These distinct morphological classes result from the evolving relative contributions of continued breakout advance and inflation. The extended nature of some breakouts highlights the role of lava supply under a stationary crust, a process ubiquitous in inflating basalt lava flows that reflects the presence of thermally preferential pathways. Textural analyses of the Cordón Caulle breakouts also emphasize the importance of late-stage volatile exsolution and vesiculation within the lava flow. Although breakouts occur across the compositional spectrum of lava flows, the greater magma viscosity is likely to make late-stage vesiculation much more important for breakout development in silicic lavas than in basalts. Such late-stage vesiculation has direct implications for hazards previously recognized from silicic lava flows, enhancing the likelihood of flow front collapse, and explosive decompression of the lava core.

Cristobalite is a low-pressure, high-temperature SiO2 polymorph that occurs as a metastable phase in many geologic settings, including as crystals deposited from vapor within the pores of volcanic rocks. Such vapor-phase cristobalite (VPC) has been inferred to result from silica redistribution by acidic volcanic gases but a precise mechanism for its formation has not been established. We address this by investigating the composition and structure of VPC deposited on plagioclase substrates within a rhyolite lava flow, at the micrometer to nanometer scale. The VPC contains impurities of the form [AlO4/Na+]0—coupled substitution of Al3+ charge-balanced by interstitial Na+—which are typical of cristobalite. However, new electron probe microanalysis (EPMA) element maps show individual crystals to have impurity concentrations that systematically decline from crystal cores-to-rims, and atom probe tomography reveals localized segregation of impurities to dislocations. Impurity concentrations are inversely correlated with degrees of crystallinity [observed by electron backscatter diffraction (EBSD), hyperspectral cathodoluminescence, laser Raman, and transmission electron microscopy (TEM)], such that crystal cores are poorly crystalline and rims are highly ordered tetragonal α-cristobalite. The VPC-plagioclase interfaces show evidence that dissolution-reprecipitation reactions between acidic gases and plagioclase crystals yield precursory amorphous SiO2 coatings that are suitable substrates for initial deposition of impure cristobalite. Successive layers of cubic β-cristobalite are deposited with impurity concentrations that decline as Al-bearing gases rapidly become unstable in the vapor cooling within pores. Final cooling to ambient temperature causes a displacive transformation from β→α cristobalite, but with locally expanded unit cells where impurities are abundant. We interpret this mechanism of VPC deposition to be a natural proxy for dopant-modulated Chemical Vapor Deposition, where halogen-rich acidic gases uptake silica, react with plagioclase surfaces to form suitable substrates and then deposit SiO2 as impure cristobalite. Our results have implications for volcanic hazards, as it has been established that the toxicity of crystalline silica is positively correlated with its purity. Furthermore, we note that VPC commonly goes unreported, but has been observed in silicic lavas of virtually all compositions and eruptive settings. We therefore suggest that despite being metastable at Earth's surface, cristobalite may be the most widely occurring SiO2 polymorph in extrusive volcanic rocks and a useful indicator of gas-solid reaction having occurred in cooling magma bodies.

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