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Understanding the timing of critical changes in volcanic systems, such as the beginning and end of eruptive behaviour, is a key goal of volcanic monitoring. Traditional approaches to forecasting these changes have used models motivated by the underlying physics of eruption onset, which assume that geophysical precursors will consistently display similar patterns prior to transition in volcanic state. We present a machine learning classification approach for detecting significant changes in patterns of volcanic activity, potentially signalling transitions during the onset or end of volcanic activity, which does not require a model of the physical processes underlying critical changes. We apply novelty detection, where models are trained only on data prior to eruption, to the precursory unrest at Augustine Volcano, Alaska in 2005. This approach looks promising for geophysically-monitored volcanic systems which have been in repose for some time, as no eruptive data is required for model training. We compare novelty detection results with multi32 class classification, where models are trained on examples of both non-eruptive and eruptive data. We contextualise the results of these classification models using constraints from petrological, satellite and visual observations from the 2006 eruption of Augustine Volcano. The transition from non-eruptive to eruptive behaviour we identify in mid-November 2005 is in agreement with previous estimates of the initiation of dike intrusion prior to the 2006 eruption. We find that models which include multiple types of data (seismic, deformation and gas emissions) can better distinguish between non-eruptive and eruptive data than models formulated on single data types.

Oceanic Anoxic Event 2 (OAE 2), during the Cenomanian–Turonian transition (∼94 Ma), was the largest perturbation of the global carbon cycle in the mid-Cretaceous and can be recognized by a positive carbon-isotope excursion in sedimentary strata. Although OAE 2 has been linked to large-scale volcanism, several large igneous provinces (LIPs) were active at this time (e.g. Caribbean, High Arctic, Madagascan, Ontong-Java) and little clear evidence links OAE 2 to a specific LIP. The Mid-Cenomanian Event (MCE, ∼96 Ma), identified by a small, 1 ‰ positive carbon-isotope excursion, is often referred to as a prelude to OAE 2. However, no underlying cause has yet been demonstrated and its relationship to OAE 2 is poorly constrained. Here, we report sedimentary mercury (Hg) concentration data from four sites, three from the southern margin of the Western Interior Seaway and one from Demerara Rise, in the equatorial proto-North Atlantic Ocean. We find that, in both areas, increases in mercury concentrations and Hg/TOC ratios coincide with the MCE and the OAE 2. However, the increases found in these sites are of a lower magnitude than those found in records of many other Mesozoic events, possibly characteristic of a marine rather than atmospheric dispersal of mercury for both events. Combined, the new mercury data presented here are consistent with an initial magmatic pulse at the time of the MCE, with a second, greater pulse at the onset of OAE 2, possibly related to the emplacement of LIPs in the Pacific Ocean and/or the High Arctic.

Deep carbon emissions from historically inactive volcanoes, hydrothermal, and tectonic structures are among the greatest unknowns in the long-term (∼Myr) carbon cycle. Recent estimates of diffuse CO2 flux from the Eastern Rift of the East African Rift System (EARS) suggest this could equal emissions from the entire mid-ocean ridge system. We report new CO2 surveys from the Main Ethiopian Rift (MER, northernmost EARS), and reassess the rift-related CO2 flux. Since degassing in the MER is concentrated in discrete areas of volcanic and off-edifice activity, characterization of such areas is important for extrapolation to a rift-scale budget. Locations of hot springs and fumaroles along the rift show numerous geothermal areas away from volcanic edifices. With these new data, we estimate total CO2 emissions from the central and northern MER as 0.52–4.36 Mt yr−1. Our extrapolated flux from the Eastern Rift is 3.9–32.7 Mt yr−1 CO2, overlapping with lower end of the range presented in recent estimates. By scaling, we suggest that 6–18 Mt yr−1 CO2 flux can be accounted for by magmatic extension, which implies an important role for volatile-enriched lithosphere, crustal assimilation, and/or additional magmatic intrusion to account for the upper range of flux estimates. Our results also have implications for the nature of volcanism in the MER. Many geothermal areas are found >10 km from the nearest volcanic center, suggesting ongoing hazards associated with regional volcanism.

Restless silicic calderas present major geological hazards, and yet many also host significant untapped geothermal resources. In East Africa, this poses a major challenge, although the calderas are largely unmonitored their geothermal resources could provide substantial economic benefits to the region. Understanding what causes unrest at these volcanoes is vital for weighing up the opportunities against the potential risks. Here we bring together new field and remote sensing observations to evaluate causes of ground deformation at Aluto, a restless silicic volcano located in the Main Ethiopian Rift (MER). Interferometric Synthetic Aperture Radar (InSAR) data reveal the temporal and spatial characteristics of a ground deformation episode that took place between 2008 and 2010. Deformation time series reveal pulses of accelerating uplift that transition to gradual long-term subsidence, and analytical models support inflation source depths of ∼5 km. Gases escaping along the major fault zone of Aluto show high CO2 flux, and a clear magmatic carbon signature (CO2-δ13C of −4.2‰ to −4.5‰). This provides compelling evidence that the magmatic and hydrothermal reservoirs of the complex are physically connected. We suggest that a coupled magmatic-hydrothermal system can explain the uplift-subsidence signals. We hypothesize that magmatic fluid injection and/or intrusion in the cap of the magmatic reservoir drives edifice-wide inflation while subsequent deflation is related to magmatic degassing and depressurization of the hydrothermal system. These new constraints on the plumbing of Aluto yield important insights into the behavior of rift volcanic systems and will be crucial for interpreting future patterns of unrest.

Volcanic eruptions have been hypothesized as an iron supply mechanism for phytoplankton blooms; however, little direct evidence of stimulatory responses has been obtained in the field. Here we present the results of twenty-one 1–2 day bottle enrichment experiments from cruises in the South Atlantic and Southern Ocean which conclusively demonstrated a photophysiological and biomass stimulation of phytoplankton communities following supply of basaltic or rhyolitic volcanic ash. Furthermore, experiments in the Southern Ocean demonstrated significant phytoplankton community responses to volcanic ash supply in the absence of responses to addition of dissolved iron alone. At these sites, dissolved manganese concentrations were among the lowest ever measured in seawater, and we therefore suggest that the enhanced response to ash may have been a result of the relief of manganese (co)limitation. Our results imply that volcanic ash deposition events could trigger extensive phytoplankton blooms, potentially capable of significant impacts on regional carbon cycling.

[1] A systematic survey of 3 years of L band interferometric synthetic aperture radar (InSAR) measurements of the Central American Volcanic Arc shows a striking lack of magmatic deformation. We make measurements at 20 of the 26 historically active volcanoes and demonstrate that none were deforming magmatically (2007–2010), although we do measure shallow subsidence associated with flow deposits and edifice loading at three volcanoes. The minimum detection rates for our survey, as estimated from the variance in time series of radar path delay, are relatively high due to strong variability of tropospheric water vapor. We compare the average detection threshold (2.4 cm/yr) to published InSAR measurements and show that the majority (~78%) of deformation events would have been measurable with the same level of noise as Central America. We calculate that if magmatic volcano deformation were spread evenly across historically active volcanoes worldwide, the probability of none of Central America's 26 volcanoes deforming would be < 1%. The lack of magmatic deformation in Central America may be indicative of differences in magma storage relative to other well-studied continental arcs. The high proportion of basalts that ascend directly from depth relative to andesites stored in the shallow crust may limit the potential for high magnitude deformation. Magma stored in vertically elongated reservoirs and high parental melt volatile contents that result in bubble-rich, compressible magmas at shallow depths may also reduce surface deformation. We consider the measurement and analysis of a lack of deformation at active volcanoes to be essential for realizing the potential of regional scale InSAR surveys.

We report the first satellite-based survey of volcanic sulphur dioxide (SO2) degassing in Papua New Guinea, using Ozone Monitoring Instrument (OMI) data. OMI is sensitive to low-level passive degassing. These observations are useful for volcano monitoring, hazard assessment (particularly aviation hazard) and assessment of arc geochemical budgets and are of immense value in remote regions with little ground-based instrumentation, such as Papua New Guinea. We identify Bagana, Manam, Rabaul, Ulawun and Langila as the active sources of volcanic SO2 in Papua New Guinea, with Bagana being the largest source. We present an OMI SO2 time series for 2005–2008 and a total detected regional output of ∼1.8 × 109 kg SO2. About 40% of emissions were released by major eruption events at Manam (January 2005), Bagana (June 2006) and Rabaul (October 2006). Over the past century however, we estimate that major explosive eruptions contribute

The edifice of a volcano is a unique deformational environment, dependent not just on active volcanic processes but also on its composition, structure, and morphology. We measured the deformation of Volcan Arenal, Costa Rica, using interferograms constructed from both ALOS and RadarSat data between 2005 and 2009. The volcano's western flanks are moving downslope at an angle of ∼55° below the horizontal plane and a consistent rate of at least ∼7 cm/yr. We use the pattern, rate, and direction of motion to test several hypotheses for its origin. Our favored explanation is creep along a shallow sliding plane, most likely the interface between deposits postdating the 1968 lateral blast eruption and the older lavas and paleosoils beneath. Our measurement of slope movement adds to a small set of rate measurements for gravity-driven deformation at volcanoes and is distinctive in both its relatively high rate and shallow origin. Observation of deformation at Arenal contributes both to the assessment of particular hazards around Arenal itself and, more generally, to the study of the stability of young stratovolcanoes.

[1] Persistent, open-vent degassing of Erebus volcano, Antarctica, is a significant point source of gases and aerosol to the austral polar troposphere. We report here on the chemical composition and size distribution of the Erebus aerosol, focusing on the water-soluble fraction. The aerosol was sampled at the rim of the active crater using a cascade impactor, which collected and sized particles in 14 size bins from >10 to 0.01 μm. The soluble fraction of the Erebus aerosol is distinct from other volcanic sources in several respects. It is dominated by chloride-bearing particles (over 30% of total mass) and has an unusually high Cl−/SO42− molar ratio of 3.5. Coarse particles contribute little to the total mass of the soluble fraction. Elevated concentrations of F−, Cl−, Br−, and SO42− are found in a narrow particle size fraction of 0.1–0.25 μm. The detection of particulate Br− reinforces our understanding of the potential for quiescent volcanic emissions to deplete tropospheric ozone. The small aerosol size reflects the low atmospheric temperature and humidity, which inhibit particle growth. Halide-alkali metal salts (Na, K)(Cl, F) appear to be the most abundant species in the aerosol. The concentration of Pb is high compared to other volcanoes; its exsolution may be promoted by the high abundance of halogens in Erebus magma. Despite the previously reported high NOx content in the plume, we did not detect significant quantities of nitrate in the near-vent aerosol. Our findings emphasize the potential regional significance of emissions from Erebus for understanding the Antarctic atmospheric composition and glaciochemical records.

Measuring Hg/SO2 ratios in volcanic emissions is essential for better apportioning the volcanic contribution to the global Hg atmospheric cycle. Here, we report the first real-time simultaneous measurement of Hg and SO2 in a volcanic plume, based on Lumex and MultiGAS techniques, respectively. We demonstrate that the use of these novel techniques allows the measurements of Hg/SO2 ratios with a far better time resolution than possible with more conventional methods. The Hg/SO2 ratio in the plume of FO fumarole on La Fossa Crater, Vulcano Island spanned an order of magnitude over a 30 minute monitoring period, but was on average in qualitative agreement with the Hg/SO2 ratio directly measured in the fumarole (mean plume and fumarole ratios being 1.09 × 10-6 and 2.9 × 10-6, respectively). The factor 2 difference between plume and fumarole compositions provides evidence for fast Hg chemical processing, the plume. Copyright 2007 by the American Geophysical Union.

On 28 February 2000, a volcanic cloud from Hekla volcano, Iceland, was serendipitously sampled by a DC-8 research aircraft during the SAGE III Ozone Loss and Validation Experiment (SOLVE I). It was encountered at night at 10.4 km above sea level (in the lower stratosphere) and 33-34 hours after emission. The cloud is readily identified by abundant SO2 (≤1 ppmv), HCl (≤70 ppbv), HF (≤60 ppbv), and particles (which may have included fine silicate ash). We compare observed and modeled cloud compositions to understand its chemical evolution. Abundances of sulfur and halogen species indicate some oxidation of sulfur gases but limited scavenging and removal of halides. Chemical modeling suggests that cloud concentrations of water vapor and nitric acid promoted polar stratospheric cloud (PSC) formation at 201-203 K, yielding ice, nitric acid trihydrate (NAT), sulfuric acid tetrahydrate (SAT), and liquid ternary solution H2SO4/H2O/HNO3 (STS) particles. We show that these volcanically induced PSCs, especially the ice and NAT particles, activated volcanogenic halogens in the cloud producing >2 ppbv ClOx. This would have destroyed ozone during an earlier period of daylight, consistent with the very low levels of ozone observed. This combination of volcanogenic PSCs and chlorine destroyed ozone at much faster rates than other PSCs that Arctic winter. Elevated levels of HNO3 and NOy in the cloud can be explained by atmospheric nitrogen fixation in the eruption column due to high temperatures and/or volcanic lightning. However, observed elevated levels of HOx remain unexplained given that the cloud was sampled at night. Copyright 2006 by the American Geophysical Union.

The number concentrations and size distributions of aerosol particles >0.3 mm diameter were measured at the summit of Mount Etna and up to 10 km downwind from the degassing vents during July and August 2004. Aerosol number concentrations reached in excess of 9 106 L1 at summit vents, compared to 4–8 104 L1 in background air. Number concentrations of intermediate size particles were higher in emissions from the Northeast crater compared to other summit crater vents, and chemical composition measurements showed that Northeast crater aerosols contained a higher mineral cation content compared to those from Voragine or Bocca Nuova, attributed to Strombolian or gas puffing activity within the vent. Downwind from the summit the airborne plume was located using zenith sky ultraviolet spectroscopy. Simultaneous measurements indicated a coincidence of elevated ground level aerosol concentrations with overhead SO2, demonstrating rapid downward mixing of the plume onto the lower flanks of the volcano under certain meteorological conditions. At downwind sites the ground level particle number concentrations were elevated in all size fractions, notably in the 2.0–7.5 mm size range. These findings are relevant for assessing human health hazard and suggest that aerosol size distribution measurements may aid volcanic risk management.

Recent measurements of BrO, NOx, and near-source sulfate in volcanic plumes suggest that volcanic vents might not simply act as point sources of emissions into the troposphere, but may also act as hightemperature reaction sites where mixtures of magmatic and ambient atmospheric gases may combine, giving new and previously unexpected reaction products. The detection of such species demands that a more complex model be developed for the interaction of volcanoes and atmospheres. We show that general thermodynamic models can be applied successfully to volcanic gas equilibria by comparing the results from HSC Chemistry with those from two volcanic gas equilibrium models (Solvgas and Gasmix). Using a thermodynamic model optimized for volcanic gas chemistry (C-O-S-H-F-Cl-Br-I-N-Ar speciation), we show that the volume ratio of atmospheric gas to magmatic gas in a high-temperature mixture is an important parameter of the volcanic plume chemistry, and our results suggest that even small amounts of air (a few % for an H2O-rich magmatic gas) in the high-temperature mixture are sufficient to yield elevated levels of reactive nitrogen, halogen (Cl, Br, and I), and sulfur species within the volcanic plume. Further modifications of the plume chemistry may also occur due to low-temperature reactions, and chemical schemes for the modification of halogen (Cl, Br, I), nitrogen, and sulfur chemistry are suggested, within the constraints imposed by recent measurements. Copyright 2006 by the American Geophysical Union.

Chile, reveal that both are significant and sustained emitters of SO2 (28 and 3.7 kg s � 1 , respectively), HCl (9.6 and 1.3 kg s � 1 , respectively), HF (4.5 and 0.3 kg s � 1 , respectively) and near-source sulfate aerosol (0.5 and 0.1 kg s � 1 , respectively). Aerosol plumes are characterized by particle number fluxes (0.08–4.0 mm radius) of � 10 17 s � 1 (Lascar) and � 10 16 s � 1 (Villarrica), the majority of which will act as cloud condensation nuclei at supersaturations >0.1%. Impactor studies suggest that the majority of these particles contain soluble SO4� . Most aerosol size distributions were bimodal with maxima at radii of 0.1–0.2 mm and 0.7–1.5 mm. The mean particle effective radius (Reff) ranged from 0.1 to 1.5 mm, and particle size evolution during transport appears to be controlled by particle water uptake (Villarrica) or loss (Lascar) rather than sulfate production. INDEX TERMS: 0305 Atmospheric Composition and Structure: Aerosols and particles (0345, 4801); 0322 Atmospheric Composition and Structure: Constituent sources and sinks; 0365 Atmospheric Composition and Structure: Troposphere—composition and chemistry; 8409 Volcanology: Atmospheric effects (0370); 8494 Volcanology: Instruments and techniques; KEYWORDS: volcanoes, degassing, aerosol sulphur dioxide, sulphate, Llaima

Gruppo Nazionale per Vulcanolgia (GNV), the EC 5th Framework project ‘‘MULTIMO’’, and NERC grant GR9/04655

[1] We report here the first measurements of volcanic SO2 fluxes obtained on foot, using a miniature ultraviolet spectrometer. Our measurements, based on differential optical absorption spectroscopy (DOAS), were performed ≈1 km from the summit of Masaya volcano (Nicaragua) in December 2001, and yielded a mean SO2 emission rate of 4 kg s−1, comparable with a set of contemporaneous measurements obtained by road vehicle traverses (average 6 kg s−1). SO2 flux estimates (average 4 kg s−1) were also obtained from a fixed position by scanning the plume. This range of fluxes confirms an apparent decrease in gas output from the volcano since 2000. The portability and ease of use of the spectrometer offer considerable scope for routine measurements of SO2 emissions from volcanoes, especially where road access or opportunities for airborne campaigns are limited. These approaches can be readily extended to monitor other sources and gases.