Galle, Bo

Volcanic plumes are common and far-reaching manifestations of volcanic activity during and be-tween eruptions. Observations of the rate of emission and composition of volcanic plumes are essential to rec-ognize and, in some cases, predict the state of volcanic activity. Measurements of the size and location of theplumes are important to assess the impact of the emission from sporadic or localized events to persistent orwidespread processes of climatic and environmental importance. These observations provide information onvolatile budgets on Earth, chemical evolution of magmas, and atmospheric circulation and dynamics. Space-based observations during the last decades have given us a global view of Earth’s volcanic emission, particularlyof sulfur dioxide (SO2). Although none of the satellite missions were intended to be used for measurementof volcanic gas emission, specially adapted algorithms have produced time-averaged global emission budgets.These have confirmed that tropospheric plumes, produced from persistent degassing of weak sources, dominatethe total emission of volcanic SO2. Although space-based observations have provided this global insight intosome aspects of Earth’s volcanism, it still has important limitations. The magnitude and short-term variabilityof lower-atmosphere emissions, historically less accessible from space, remain largely uncertain. Operationalmonitoring of volcanic plumes, at scales relevant for adequate surveillance, has been facilitated through the useof ground-based scanning differential optical absorption spectrometer (ScanDOAS) instruments since the be-ginning of this century, largely due to the coordinated effort of the Network for Observation of Volcanic andAtmospheric Change (NOVAC). In this study, we present a compilation of results of homogenized post-analysisof measurements of SO2flux and plume parameters obtained during the period March 2005 to January 2017of 32 volcanoes in NOVAC. This inventory opens a window into the short-term emission patterns of a diverseset of volcanoes in terms of magma composition, geographical location, magnitude of emission, and style oferuptive activity. We find that passive volcanic degassing is by no means a stationary process in time and thatlarge sub-daily variability is observed in the flux of volcanic gases, which has implications for emission budgetsproduced using short-term, sporadic observations. The use of a standard evaluation method allows for intercom-parison between different volcanoes and between ground- and space-based measurements of the same volcanoes.The emission of several weakly degassing volcanoes, undetected by satellites, is presented for the first time. Wealso compare our results with those reported in the literature, providing ranges of variability in emission notaccessible in the past. The open-access data repository introduced in this article will enable further exploitationof this unique dataset, with a focus on volcanological research, risk assessment, satellite-sensor validation, andimproved quantification of the prevalent tropospheric component of global volcanic emission.

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.

Volcanoes are the main pathway to the surface for volatiles that are stored within the Earth. Carbon dioxide (CO2) is of particular interest because of its potential for climate forcing. Understanding the balance of CO2 that is transferred from the Earth's surface to the Earth's interior, hinges on accurate quantification of the long-term emissions of volcanic CO2 to the atmosphere. Here we present an updated evaluation of the world's volcanic CO2 emissions that takes advantage of recent improvements in satellite-based monitoring of sulfur dioxide, the establishment of ground-based networks for semi-continuous CO2-SO2 gas sensing and a new approach to estimate key volcanic gas parameters based on magma compositions. Our results reveal a global volcanic CO2 flux of 51.3 ± 5.7 Tg CO2/y (11.7 × 1011 mol CO2/y) for non-eruptive degassing and 1.8 ± 0.9 Tg/y for eruptive degassing during the period from 2005 to 2015. While lower than recent estimates, this global volcanic flux implies that a significant proportion of the surface-derived CO2 subducted into the Earth's mantle is either stored below the arc crust, is efficiently consumed by microbial activity before entering the deeper parts of the subduction system, or becomes recycled into the deep mantle to potentially form diamonds.

A vigorously degassing lava lake appeared inside the Santiago pit crater of Masaya volcano (Nicaragua) in December 2015, after years of degassing with no (or minor) incandescence. Here we present an unprecedented-long (3 years) and continuous volcanic gas record that instrumentally characterizes the (re)activation of the lava lake. Our results show that, before appearance of the lake, the volcanic gas plume composition became unusually CO2 rich, as testified by high CO2/SO2 ratios (mean: 12.2 ± 6.3) and low H2O/CO2 ratios (mean: 2.3 ± 1.3). The volcanic CO2 flux also peaked in November 2015 (mean: 81.3 ± 40.6 kg/s; maximum: 247 kg/s). Using results of magma degassing models and budgets, we interpret this elevated CO2 degassing as sourced by degassing of a volatile-rich fast-overturning (3.6–5.2 m3 s−1) magma, supplying CO2-rich gas bubbles from minimum equivalent depths of 0.36–1.4 km. We propose this elevated gas bubble supply destabilized the shallow (<1 km) Masaya magma reservoir, leading to upward migration of vesicular (buoyant) resident magma, and ultimately to (re)formation of the lava lake. At onset of lava lake activity on 11 December 2015 (constrained by satellite-based MODIS thermal observations), the gas emissions transitioned to more SO2-rich composition, and the SO2 flux increased by a factor ∼40% (11.4 ± 5.2 kg/s) relative to background degassing (8.0 kg/s), confirming faster than normal (4.4 versus ∼3 m3 s−1) shallow magma convection. Based on thermal energy records, we estimate that only ∼0.8 of the 4.4 m3 s−1 of magma actually reached the surface to manifest into a convecting lava lake, suggesting inefficient transport of magma in the near-surface plumbing system.

The 2014–2015 Bárðarbunga fissure eruption at Holuhraun in central Iceland was distinguished by the high emission of gases, in total 9.6 Mt SO2, with almost no tephra. This work collates all ground-based measurements of this extraordinary eruption cloud made under particularly challenging conditions: remote location, optically dense cloud with high SO2 column amounts, low UV intensity, frequent clouds and precipitation, an extensive and hot lava field, developing ramparts, and high-latitude winter conditions. Semi-continuous measurements of SO2 flux with three scanning DOAS instruments were augmented by car traverses along the ring-road and along the lava. The ratios of other gases/SO2 were measured by OP-FTIR, MultiGAS, and filter packs. Ratios of SO2/HCl = 30–110 and SO2/HF = 30–130 show a halogen-poor eruption cloud. Scientists on-site reported extremely minor tephra production during the eruption. OPC and filter packs showed low particle concentrations similar to non-eruption cloud conditions. Three weather radars detected a droplet-rich eruption cloud. Top of eruption cloud heights of 0.3–5.5 km agl were measured with ground- and aircraft-based visual observations, web camera and NicAIR II infrared images, triangulation of scanning DOAS instruments, and the location of SO2 peaks measured by DOAS traverses. Cloud height and emission rate measurements were critical for initializing gas dispersal simulations for hazard forecasting

Between 2007 and 2011 four measurement campaigns (June 2007, July 2010, June 2011, and December 2011) were carried out at the crater rim of Nyiragongo volcano, DR Congo. Nyiragongo is one of the most active volcanoes in Africa. The ground-based remote sensing technique Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS), which uses scattered sunlight, the in-situ Multi-Component Gas Analyzer System (Multi-GAS) and alkaline impregnated filter were simultaneously applied during all field trips. The bromine monoxide to sulfur dioxide (BrO/SO2) and carbon dioxide to sulfur dioxide (CO2/SO2) molar ratios were determined, among other ratios. During the different field trips variations of the level of the lava lake up to several tens of meters were observed during intervals of the order of minutes up to days and also between the years. The measured gas ratios presented covariations with the lava lake level changes. BrO/SO2 ratios and CO2/SO2 ratios showed similar behavior. Annual CO2/SO2 and BrO/SO2 average values are generally positively correlated. In June 2011 increased BrO/SO2 as well as increased CO2/SO2 ratios have been observed before a sudden decrease of the lava lake. Overall the Cl/S ratio, determined by filter-pack sampling, shows an increasing trend with time, which is accompanied by a decreasing sulfur dioxide flux, the later measured nearly continuously by automated MAX-DOAS instruments since 2004. Mean gas emission fluxes of CO2, Cl and ‘minimum-BrO’ fluxes are calculated using their ratio to SO2. The first two show an increase with time, in contrast to the SO2 fluxes. A simple conceptual model is proposed which can explain in particular the June 2011 data, but as well our entire data set. The proposed model takes up the idea of convective magma cells inside the conduit and the possible temporary interruption of part of the cycling. We propose than two alternatives to explain the observed gas emission variation: 1. It is assumed that the diffuse and fumarolic degassing could have significant influence on measured gas composition. The measured gas composition might rather represent a gas mixture of plume, diffuse and fumarolic degassing than only representing the volcanic plume. 2. It is proposed that the interruption of the convection has taken place in the upper part of the conduit and deep degassing of CO2 and bromine initially continues while mixing already with gas emissions from an ageing source, which is characterized by an already diminishing sulfur content. These complex process but as well as the gas mixing of different sources, could explain general features of our dataset, but can unfortunately neither be confirmed nor disproven by the data available today.

We use the chemical and isotopic composition of volcanic gases and steam condensate, in situ measurements of plume composition and remote measurements of SO2 flux to constrain volatile sources and characterize subvolcanic conditions at three persistently degassing and seismically active volcanoes within the Katmai Volcanic Cluster (KVC), Alaska:Mount Martin,Mount Mageik and Trident. In situ plume measurements of gas composition were collected at all three volcanoes usingMultiGAS instruments to calculate gas ratios (e.g. CO2/H2S, SO2/H2S and H2O/H2S), and remote measurements of SO2 column density were collected from Mount Martin and Mount Mageik by ultraviolet spectrometer systems to calculate SO2 fluxes. Fumaroles were directly sampled for chemical and isotopic composition from Mount Mageik and Trident. Mid Ocean Ridge Basalt (MORB)-like 3He/4He ratios (~7.2–7.6 Rc/RA) within Mount Mageik and Trident's fumarole emissions and a moderate SO2 flux (~75 t/d) from Mount Martin, combined with gas compositions dominated by H2O, CO2 and H2S from all three volcanoes, indicate magma degassing and active hydrothermal systems in the subsurface of these volcanoes. Mount Martin's gas emissions have the lowest CO2/H2S ratio (~2–4) and highest SO2 flux compared to the other KVC volcanoes, indicative of shallow magma degassing. Geothermometry techniques applied to Mount Mageik and Trident's fumarolic gas compositions suggest that their hydrothermal reservoirs are located at depths of ~0.2 and 4 km below the surface, respectively. Observations of an unusually reducing gas composition at Trident and organic material in the near-surface soils suggest that thermal decomposition of sediments may be influencing gas composition. When the measured gas compositions from Mount Mageik and Trident are compared with previous samples collected in the late 1990's, relatively stable magmatic-hydrothermal conditions are inferred forMountMageik,while gradual degassing of residual magma and contamination by shallow crustal fluids is inferred for Trident. The isotopic composition of volcanic gases emitted from Mount Mageik and Trident reflect mixing of subducted slab, mantle and crustal volatile sources, with organic sediment and carbonate being the predominant sources. Considering the close proximity of the target volcanoes in comparison with the depth to the subducted slab we speculate that Aleutian Arc volatiles are fed by a relatively homogeneous subducted fluid and that much of the apparent variability in volatile provenance can be explained by shallow crustal volatile sources and/or processes.

Very little is known about the volatile element makeup of the gaseous emissions of Nyamulagira volcano. This paper tries to fill this gap by reporting the first gas composition measurements of Nyamulagira’s volcanic plume since the onset of its lava lake activity at the end of 2014. Two field surveys were carried out on 1 November 2014, and 13–15 October 2015. We applied a broad toolbox of volcanic gas composition measurement techniques in order to geochemically characterize Nyamulagira’s plume. Nyamulagira is a significant emitter of SO2, and our measurements confirm this, as we recorded SO2 emissions of up to ~ 14 kt/d during the studied period. In contrast to neighbouring Nyiragongo volcano, however, Nyamulagira exhibits relatively low CO2/SO2 molar ratios (< 4) and a highH2O content (> 92%of total gas emissions). Strong variations in the volatile composition, in particular for the CO2/SO2 ratio, were measured between 2014 and 2015, which appear to reflect the simultaneous variations in volcanic activity.We also determined the molar ratios for Cl/S, F/S and Br/S in the plume gas, finding values of 0.13 and 0.17, 0.06 and 0.11, and 2.3·10−4 and 1·10−4, in 2014 and 2015, respectively. A total gas emission flux of 48 kt/ d was estimated for 2014. The I/S ratio in 2015 was found to be 3.6·10−6. In addition, we were able to distinguish between hydrogen halides and non-hydrogen halides in the volcanic plume. Considerable amounts of bromine (18–35% of total bromine) and iodine (8–18%of total iodine) were found in compounds other than hydrogen halides. However, only a negligible fraction of chlorine was found as compounds other than hydrogen chloride.

Basaltic magma chambers are often characterized by emptying and refilling cycles that influence their evolution in space and time, and the associated eruptive activity. During April 2007, the largest historical eruption of Piton de la Fournaise (Île de La Réunion, France) drained the shallow plumbing system () and resulted in collapse of the 1-km-wide summit crater. Following these major events, Piton de la Fournaise entered a seven-year long period of near-continuous deflation interrupted, in June 2014, by a new phase of significant inflation. By integrating multiple datasets (lava discharge rates, deformation, seismicity, gas flux, gas composition, and lava chemistry), we here show that the progressive migration of magma from a deeper (below sea level) storage zone gradually rejuvenated and pressurized the above-sea-level portion of the magmatic system consisting of a vertically-zoned network of relatively small-volume magma pockets. Continuous inflation provoked four small () eruptions from vents located close to the summit cone and culminated, during August–October 2015, with a chemically zoned eruption that erupted of lava. This two-month-long eruption evolved through (i) an initial phase of waning discharge, associated to the withdrawal of differentiated magma from the shallow system, into (ii) a month-long phase of increasing lava and SO2 fluxes at the effusive vent, coupled with CO2 enrichment of summit fumaroles, and involving emission of less differentiated lavas, to end with, (iii) three short-lived (∼2 day-long) pulses in lava and gas flux, coupled with arrival of cumulative olivine at the surface and deflation. The activity observed at Piton de la Fournaise in 2014 and 2015 points to a new model of shallow system rejuvenation and discharge, whereby continuous magma supply causes eruptions from increasingly deeper and larger magma storage zones. Downward depressurization continues until unloading of the deepest, least differentiated magma triggers pulses in lava and gas flux, accompanied by rapid contraction of the volcano edifice, that empties the main shallow reservoir and terminates the cycle. Such an unloading process may characterize the evolution of shallow magmatic systems at other persistently active effusive centers.

The STRAP (Synergie Transdisciplinaire pour Répondre aux Aléas liés aux Panaches volcaniques) campaign was conducted in 2015 to investigate the volcanic plumes of Piton de La Fournaise (La Réunion, France). For the first time, measurements at the local (near the vent) and at the regional scales around the island were conducted. The STRAP 2015 campaign has become possible thanks to a strong cross-disciplinary collaboration between volcanologists and meteorologists. The main observations during four eruptive 5 periods (85 days) are summarized. They include the estimates of SO2, CO2 and H2O emissions, the altitude of the plume at the vent and over different areas of La Réunion Island, the evolution of the SO2 concentration, the aerosol size distribution, and the aerosol extinction profile. A climatology of the volcanic plume dispersion is also reported. Simulations and measurements showed that the plume formed by weak eruption has a stronger interaction with the surface of the island. Strong SO2 and particles concentrations above 1000 ppb and 50,000 cm−3, respectively, are 10 frequently measured over 20 km of distance from the Piton de la Fournaise. The measured aerosol size distribution shows the predominance of small particles in the volcanic plume. A particular emphasis is placed on the gas-particle conversion with several cases of strong nucleation of sulfuric acid observed within the plume and at the distal site of the Maïdo observatory. The STRAP 2015 campaign gave a unique set of multi-disciplinary data that can now be used by modellers to improve the numerical paramameterizations of the physical and chemical evolution of the volcanic plumes.