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Quantifying the CO2 flux sustained by low-temperature fumarolic fields in hydrothermal/volcanic environments has remained a challenge, to date. Here, we explored the potential of a commercial infrared tunable laser unit for quantifying such fumarolic volcanic/hydrothermal CO2 fluxes. Our field tests were conducted between April 2013 and March 2014 at Nea Kameni (Santorini, Greece), Hekla and Krýsuvík (Iceland) and Vulcano (Aeolian Islands, Italy). At these sites, the tunable laser was used to measure the path-integrated CO2 mixing ratios along cross sections of the fumaroles' atmospheric plumes. By using a tomographic post-processing routine, we then obtained, for each manifestation, the contour maps of CO2 mixing ratios in the plumes and, from their integration, the CO2 fluxes. The calculated CO2 fluxes range from low (5.7 ± 0.9 t d−1; Krýsuvík) to moderate (524 ± 108 t d−1; La Fossa crater, Vulcano). Overall, we suggest that the cumulative CO2 contribution from weakly degassing volcanoes in the hydrothermal stage of activity may be significant at the global scale.

The 2014–2015 Holuhraun eruption in Iceland, emitted ∼11 Tg of SO2 into the troposphere over 6 months, and caused one of the most intense and widespread volcanogenic air pollution events in centuries. This study provides a number of source terms for characterisation of plumes in large fissure eruptions, in Iceland and elsewhere. We characterised the chemistry of aerosol particle matter (PM) and gas in the Holuhraun plume, and its evolution as the plume dispersed, both via measurements and modelling. The plume was sampled at the eruptive vent, and in two populated areas in Iceland. The plume caused repeated air pollution events, exceeding hourly air quality standards (350 μg/m3) for SO2 on 88 occasions in Reykjahlíð town (100 km distance), and 34 occasions in Reykjavík capital area (250 km distance). Average daily concentration of volcanogenic PM sulphate exceeded 5 μg/m3 on 30 days in Reykjavík capital area, which is the maximum concentration measured during non-eruptive background interval. There are currently no established air quality standards for sulphate. Combining the results from direct sampling and dispersion modelling, we identified two types of plume impacting the downwind populated areas. The first type was characterised by high concentrations of both SO2 and S-bearing PM, with a high Sgas/SPM mass ratio (SO2(g)/SO4 2− (PM) > 10). The second type had a low Sgas/SPM ratio (1 and PM2.5), sulphate (on average ∼90% of the PM mass) and various trace species, including heavy metals. The fine size of the volcanic PM mass (75–80% in PM2.5), and the high environmental lability of its chemical components have potential adverse implications for environmental and health impacts. However, only the dispersion of volcanic SO2 was forecast in public warnings and operationally monitored during the eruption. We make a recommendation that sulphur gas-to-aerosol conversion processes, and a sufficiently large model domain to contain the transport of a tropospheric plume on the timescale of days be utilized for public health and environmental impact forecasting in future eruptions in Iceland and elsewhere in the world.

Volcanoes are a key natural source of CO2, but global estimates of volcanic CO2 flux are predominantly based on measurements from a fraction of world's actively degassing volcanoes. We combine high‐precision airborne measurements from 2016 and 2017 with atmospheric dispersion modeling to quantify CO2 emissions from Katla, a major subglacial volcanic caldera in Iceland that last erupted 100 years ago but has been undergoing significant unrest in recent decades. Katla's sustained CO2 flux, 12–24 kt/d, is up to an order of magnitude greater than previous estimates of total CO2 release from Iceland's natural sources. Katla is one of the largest volcanic sources of CO2 on the planet, contributing up to 4% of global emissions from nonerupting volcanoes. Further measurements on subglacial volcanoes worldwide are urgently required to establish if Katla is exceptional, or if there is a significant previously unrecognized contribution to global CO2 emissions from natural sources. We combine high‐precision airborne measurements from 2016 and 2017 with atmospheric dispersion modelling to quantify CO2 emissions from Katla, a major subglacial volcanic caldera in Iceland that last erupted 100 years ago but has been undergoing significant unrest in recent decades. Katla's sustained CO2 flux, 12‐24 kt/d, is up to an order of magnitude greater than previous estimates of total CO2 release from Iceland's natural sources. Katla is one of the largest volcanic sources of CO2 on the planet, contributing up to 4% of global emissions from non‐erupting volcanoes. Further measurements on subglacial volcanoes world‐wide are urgently required to establish if Katla is exceptional, or if there is a significant previously unrecognized contribution to global CO2 emissions from natural sources.

The Multi-component Gas Analyzer System (Multi-GAS) has recently consolidated as a standard technique for the nearly real-time in-situ observation of major volcanogenic components (H2O, CO2, SO2, H2S,H2) in volcanic gas plumes. The Multi-GAS has been initially operated at open-vent volcanoes, where it has revealed ideal for long-term continuous observations at for instance Etna and Stromboli volcanoes in Italy, therein paving the way to the acquisition of unprecedentedly long and continuous volcanic gas time-series. We here initially review the present state of the expanding network of permanent Multi-GAS instruments, now covering about 10 volcanoes worldwide. We then specifically focus on the results acquired via Multi-GAS monitoring of fumarolic activity at two quiescent, but potentially hazardous volcanoes in Europe: Santorini, in Greece, and Hekla, in Iceland. Our results overall demonstrate the potential of the Multi-GAS in the monitoring of even sluggish, weak fuming hydrothermal activity as currently observed at both Santorini and Hekla. Quantitative modeling of the results open the way to charactering magmatic-hydrothermal and gas-groundwater interactions with unprecedented detail. We show that, at both volcanoes, gas compositions range in time from H2O-rich (H2O/CO2 > 1) to CO2-dominated and S-poor (CO2/H2S > 10,000), a compositional trend which we quantitatively reproduce via model runs of gas-water-rock interactions initialized using EQ 3/6.

The effusive six months long 2014-2015 Bárðarbunga eruption (31 August-27 February) was the largest in Iceland for more than 200 years, producing 1.6 ± 0.3 km3 of lava. The total SO2 emission was 11 ± 5 Mt, more than the amount emitted from Europe in 2011. The ground level concentration of SO2 exceeded the 350 µg m−3 hourly average health limit over much of Iceland for days to weeks. Anomalously high SO2 concentrations were also measured at several locations in Europe in September. The lowest pH of fresh snowmelt at the eruption site was 3.3, and 3.2 in precipitation 105 km away from the source. Elevated dissolved H2SO4, HCl, HF, and metal concentrations were measured in snow and precipitation. Environmental pressures from the eruption and impacts on populated areas were reduced by its remoteness, timing, and the weather. The anticipated primary environmental pressure is on the surface waters, soils, and vegetation of Iceland., Funding for the research came from the Icelandic government via the Icelandic Civil Protection Agency, the EC FP7 Framework programme via the Futurevolc project, the Swedish Research Council FORMAS supported the DOAS measurements Geochemical Perspectives Letters Letter Letter Geochemical Perspectives Letters 92 Geochem. Persp. Let. (2015) 1, 84-93 | doi: 10.7185/geochemlet.1509 Geochem. Persp. Let. (2015) 1, 84-93 | doi: 10.7185/geochemlet.1509 93 and The French centre of excellence “Clervolc” programme financed the microprobe analysis. We are grateful to the Environmental Protection Agency in Ireland, the National Institute for Public Health and the Environment in the Netherlands, the Belgian Interregional Environment Agency, the Department for Environment Food & Rural Affairs in UK, and the Environment Agency of Austria for ground–level SO2 concentration data in air in the respective countries.

Using a combination of body wave and surface wave data sets to reveal the mantle plume and plume head, this study presents a tomographic image of the mantle structure beneath Iceland to 400 km depth. Data comes primarily from the PASSCAL-HOTSPOT deployment of 30 broadband instruments over a period of 2 years, and is supplemented by data from the SIL and ICEMELT networks. Three sets of relative teleseismic body wave arrival times are generated through cross correlation: S and SKS arrivals at 0.03–0.1 Hz, and P and PKIKP arrivals at 0.03–0.1 and 0.8–2.0 Hz. Prior to inversion the crustal portion of the travel time anomalies is removed using the crustal model ICECRTb. This step has a significant effect on the mantle velocity variations imaged down to a depth of ∼250 km. Inversion of relative arrival times only provides information on lateral velocity variations. Surface waves are therefore used to provide absolute velocity information for the uppermost mantle beneath Iceland. The average wave number for the Love wave fundamental mode at 0.020 and 0.024 Hz is measured and used to invert for the average S velocity. Combination of the body wave and surface wave information reveals a predominantly horizontal low-velocity anomaly extending from the Moho down to ∼250 km depth, interpreted as a plume head. Below the plume head a near-cylindrical low-velocity anomaly with a radius of ∼100 km and peak VP and VS anomalies of −2% and −4%, respectively, extends down to the maximum depth of resolution at 400 km. Within the plume head, in the uppermost mantle above the core of the plume, there is a relatively high velocity with a maximum VP and VS anomaly of +2%. This high-velocity anomaly may be the result of the extreme degree of melt extraction necessary to generate the thick (46 km) crust in central Iceland. Comparison of the plume volumetric flux implied by our images, the crustal generation rate, and the degree of melting suggested by rare earth element inversions, suggests that (1) mantle material must be flowing horizontally away from the plume core faster than the overlying lithosphere and (2) the bulk of the plume material does not participate in melting beneath Iceland.

The composition of the gases released by El Chichón (Chiapas, Mexico) and Víti (Askja volcano, Iceland) volcanic lakes is examined by Multi-GAS for the first time. Our results demonstrate that H2S and SO2 are degassed by these pH 2–3 lakes. We find higher CO2/H2S and H2/H2S ratios in the lakes' emissions (31–5,685 and 0.6–35, respectively) than in the fumarolic gases feeding the lakes (13–33 and 0.08–0.5, respectively), evidencing that only a fraction (0.2–5.4% at El Chichón) of the H2S(g) contributed by the subaquatic fumaroles ultimately reaches the atmosphere. At El Chichón, we estimate a H2S output from the crater lake of 0.02–0.06t/day. Curiously, SO2 is also detected at trace levels in the gases released from both lakes (0.003–0.3ppmv). We propose that H2S supplied into the lakes initiates a series of complex oxidation reactions, having sulfite as an intermediate product, and ultimately leading to SO2 production and degassing.

Recent geophysical evidence for large-scale regional crustal inflation and localized crustal magma intrusion has made Lastarria volcano (northern Chile) the target of numerous geological, geophysical, and geochemical studies. The chemical composition of volcanic gases sampled during discrete campaigns from Lastarria volcano indicated a well-developed hydrothermal system from direct fumarole samples in A.D. 2006, 2008, and 2009, and shallow magma degassing using measurements from in situ plume sampling techniques in 2012. It is unclear if the differences in measured gas compositions and resulting interpretations were due to artifacts of the different sampling methods employed, short-term excursions from baseline due to localized changes in stress, or a systematic change in Lastarria's magmatic-hydrothermal system between 2009 and 2012. Integrated results from a two-day volcanic gas sampling and measurement campaign during the 2014 International Association of Volcanology and Chemistry of the Earth's Interior (IAVCEI) Commission on the Chemistry of Volcanic Gases (CCVG) 12th Gas Workshop are used here to compare and evaluate current gas sampling and measurement techniques, refine the existing subsurface models for Lastarria volcano, and provide new constraints on its magmatic-hydrothermal system and total degassing budget. While compositional differences among sampling methods are present, distinct compositional changes are observed, which if representative of longterm trends, indicate a change in Lastarria's overall magmatic-hydrothermal system. The composition of volcanic gases measured in 2014 contained high proportions of relatively magma- and water-soluble gases consistent with degassing of shallow magma, and in agreement with the 2012 gas composition. When compared with gas compositions measured in 2006-2009, higher relative H2O/CO2 ratios combined with lower relative CO2/St and H2O/St and stable HCl/St ratios (where St is total S [SO2 + H2S]) are observed in 2012 and 2014. These compositional changes suggest variations in the magmatic-hydrothermal system between 2009 and 2012, with possible scenarios to explain these trends including: (1) decompression-induced degassing due to magma ascent within the shallow crust; (2) crystallization-induced degassing of a stalled magma body; (3) depletion of the hydrothermal system due to heating, changes in local stress, and/or minimal precipitation; and/or (4) acidification of the hydrothermal system. These scenarios are evaluated and compared against the geophysical observations of continuous shallow inflation at ~8 km depth between 1997 and 2016, and near-surface ( < 1 km) inflation between 2000 and 2008, to further refine the existing subsurface models. Higher relative H2O/CO2 observed in 2012 and 2014 is not consistent with the depletion or acidification of a hydrothermal system, while all other observations are consistent with the four proposed models. Based on these observations, we find that scenarios 1 or 2 are the most likely to explain the geochemical and geophysical observations, and propose that targeted shallow interferometric synthetic-aperture radar (InSAR) studies could help discriminate between these two scenarios. Lastly, we use an average SO2 flux of 604 ± 296 t/d measured on 22 November 2014, along with the average gas composition and diffuse soil CO2 flux measurements, to estimate a total volatile flux from Lastarria volcano in 2014 of ~12,400 t/d, which is similar to previous estimates from 2012.

Large volcanic eruptions on Earth commonly occur with a collapse of the roof of a crustal magma reservoir, forming a caldera. Only a few such collapses occur per century, and the lack of detailed observations has obscured insight into the mechanical interplay between collapse and eruption.We usemultiparameter geophysical and geochemical data to show that the 110-square kilometer and 65-meter-deep collapse of Bárdarbunga caldera in 2014–2015 was initiated through withdrawal of magma, and lateral migration through a 48-kilometers-long dike, from a 12-kilometers deep reservoir. Interaction between the pressure exerted by the subsiding reservoir roof and the physical properties of the subsurface flow path explain the gradual, near exponential decline of both collapse rate and the intensity of the 180-day- long eruption., Civil Protection Department of the National Commissioner of the Icelandic Police. European Community’s Seventh Framework Programme grant no. 308377 (Project FUTUREVOLC). EU Seventh Framework Marie Curie project NEMOH no. 289976 CO2Volc ERC grant no. 279802, the Research Fund of the University of Iceland, the Irish Research Council, the Helmholtz Alliance on Remote Sensing and Earth System Dynamics (EDA), Bayerisches Geoinstitut through their DFG core facility for high pressure research, and UNAM/CIC Intercambio Académico.

Gas-water-rock reactions taking place within volcano-hosted hydrothermal systems scrub reactive, water-soluble species (sulfur, halogens) from the magmatic gas phase, and as such play a major control on the composition of surface gas manifestations. A number of quantitative models of magmatic gas scrubbing have been proposed in the past, but no systematic comparison of model results with observations from natural systems has been carried out, to date. Here, we present the results of novel numerical simulations, in which we initialized models of hydrothermal gas-water-rock at conditions relevant to Icelandic volcanism. We focus on Iceland as an example of a "wet" volcanic region where scrubbing is widespread. Our simulations were performed (using the EQ3/6 software package) at shallow (temperature100°C. We find that this range of model gas compositions reproduces well the (H2O-CO2-STOT) compositional range of reservoir waters and surface gas emissions in Iceland. From this validation of the model in an extreme end-member environment of high scrubbing, we conclude that EQ3/6-based reaction path simulations offer a realistic representation of gas-water-rock interaction processes occurring underneath active magmatic-hydrothermal systems.

Hekla is a frequently active volcano with an infamously short pre-eruptive warning period. Our project contributes to the ongoing work on improving Hekla's monitoring and early warning systems. In 2012 we began monitoring gas release at Hekla. The dataset comprises semi-permanent near-real time measurements with a MultiGAS system, quantification of diffuse gas flux, and direct samples analysed for composition and isotopes (δ13C, δD and δ18O). In addition, we used reaction path modelling to derive information on the origin and reaction pathways of the gas emissions.Hekla's quiescent gas composition was CO2-dominated (0.8mol fraction) and the δ13C signature was consistent with published values for Icelandic magmas. The gas is poor in H2O and S compared to hydrothermal manifestations and syn-eruptive emissions from other active volcanic systems in Iceland. The total CO2 flux from Hekla central volcano (diffuse soil emissions) is at least 44Td-1, thereof 14Td-1 are sourced from a small area at the volcano's summit. There was no detectable gas flux at other craters, even though some of them had higher ground temperatures and had erupted more recently. Our measurements are consistent with a magma reservoir at depth coupled with a shallow dike beneath the summit. In the current quiescent state, the composition of the exsolved gas is substantially modified along its pathway to the surface through cooling and interaction with wall-rock and groundwater. The modification involves both significant H2O condensation and scrubbing of S-bearing species, leading to a CO2-dominated gas emitted at the summit. We conclude that a compositional shift towards more S- and H2O-rich gas compositions if measured in the future by the permanent MultiGAS station should be viewed as sign of imminent volcanic unrest on Hekla.