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Volcanic plume samples taken in 2008 and 2009 from the Halemàumàu eruption at Kīlauea provide new insights into Kīlauea's degassing behaviour. The Cl, F and S gas systematics are consistent with syn-eruptive East Rift Zone measurements suggesting that the new Halemàumàu activity is fed by a convecting magma reservoir shallower than the main summit storage area. Comparison with degassing models suggests that plume halogen and S composition is controlled by very shallow (77%) as gaseous elemental mercury at the point of emission. Sulphate is an important aerosol component (modal particle diameter ∼0.44μm). Aerosol halide ion concentrations are low compared to other systems, consistent with the lower proportion of gaseous hydrogen halides. Plume concentrations of many metallic elements (Rb, Cs, Be, B, Cr, Ni, Cu, Mo, Cd, W, Re, Ge, As, In, Sn, Sb, Te, Tl, Pb, Mg, Sr, Sc, Ti, V, Mn, Fe, Co, Y, Zr, Hf, Ta, Al, P, Ga, Th, U, La, Ce, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Er, Tm) are elevated above background air. There is considerable variability in metal to SO 2 ratios but our ratios (generally at the lower end of the range previously measured at Kīlauea) support assertions that Kīlauea's emissions are metal-poor compared to other volcanic settings. Our aerosol Re and Cd measurements are complementary to degassing trends observed in Hawaiian rock suites although measured aerosol metal/S ratios are about an order of magnitude lower than those calculated from degassing trends determined from glass chemistry. Plume enrichment factors with respect to Hawaiian lavas are in broad agreement with those from previous studies allowing similar element classification schemes to be followed (i.e., lithophile elements having lower volatility and chalcophile elements having higher volatility). The proportion of metal associated with the largest particle size mode collected (>2.5μm) and that bound to silicate is significantly higher for lithophiles than chalcophiles. Many metals show higher solubility in pH 7 buffer solution than deionised water suggesting that acidity is not the sole driver in terms of solubility. Nonetheless, many metals are largely water soluble when compared with the other sequential leachates suggesting that they are delivered to the environment in a bioavailable form. Preliminary analyses of environmental samples show that concentrations of metals are elevated in rainwater affected by the volcanic plume and even more so in fog. However, metal levels in grass samples showed no clear enrichment downwind of the active vents. © 2011 Elsevier Ltd.

Despite uncertainties in our understanding of early Earth volcanism and atmospheric composition, thermodynamic modelling is able to offer estimates of the global production of reactive trace species (NO, OH, SO 3, Cl, Br and I) from early Earth volcanism, and thereby to shed light on processes which may have been different in Earth's early atmosphere. Model results show that thermal decomposition of magmatic H 2O, CO 2 and SO 2 in high-T mixtures of magmatic and atmospheric gases (at T > 1400 °C) generate high levels of reactive trace gas species. Production of these reactive trace species is insensitive to atmospheric CO 2 in mixtures where the atmospheric gas is the minor component and will hence continue during periods of low atmospheric CO 2. Fluxes of NO, OH, Cl, Br and I from early Earth volcanism are predicted to exceed those from modern Earth volcanism as the higher temperature of early Earth emissions compensates for lower levels of O 2 in the atmosphere, compared to the modern Earth. Under certain conditions, the volcanic NO flux from early Earth volcanism is found to be comparable to other sources of reactive N such as lightning NO and photochemical HCN. This is one possible source of fixed nitrogen which may alleviate any postulated Archean nitrogen crisis. Our thermodynamic model reveals that production of SO 3 (a potential precursor for near-source volcanic sulphate and hence 'primary' volcanic aerosol) is likely to be significantly lower from early Earth volcanism. Uncertainty in the pathway to near-source sulphate in modern volcanism (i.e., the reaction of SO 3 with water or direct emission) introduces a large uncertainty into the production rate of near-source volcanic sulphate on the early Earth. © 2007 Elsevier Ltd. All rights reserved.

The 2008-current summit eruption at Kīlauea Volcano, Hawai'i offers a unique opportunity to test models of degassing and magma plumbing and to improve our understanding of the volatile budget. The aim of this work was to test the hypothesis that gases emitted from a summit lava lake will be rich in carbon dioxide (CO) and similar to those measured during the persistent lava lake activity in the early 20th century at Kīlauea Volcano (Gerlach and Graeber, 1985). We measured the sulfur dioxide (SO) and CO concentrations in the gas plume from Halema'uma'u using electrochemical and non-dispersive infrared sensors during April 2009. We also analysed olivine-hosted melt inclusions from tephra erupted in 2008 and 2010 for major, trace and volatile elements. The gas and melt data are both consistent with the equilibration of a relatively evolved magma batch at depths of 1.2-2.0 km beneath Halema'uma'u prior to the current degassing activity. The differences in the volatile concentrations between the melt inclusions and matrix glasses are consistent with the observed gas composition. The degassing of sulfur and halogen gases from the melt requires low pressures and hence we invoke convection to bring the magma close to the surface to degas, before sinking back into the conduit. The fluxes of gases (900 and 80 t/d SO and CO respectively) are used to estimate magma fluxes (1.2-3.4 m/s) to the surface for April 2009. The observation of minimal loss of hydrogen from the melt inclusions implies a rapid rise rate (less than a few hours), which constrains the conduit radius to 1-2 m. The inferred conduit radius is much narrower than the lava lake at the surface, implying a flared geometry. The melt inclusion data suggest that there is a progressive decrease in melt volatile concentrations with time during 2008-2010, consistent with convection, degassing and mixing in a closed, or semi-closed magma system. The degassing regime of the current summit lava lake activity is not similar to that observed in the early 20th century; instead the gases are extensively depleted in CO. © 2013 The Authors.

Tuffisite veins are glass-filled fractures formed when magma fragments during degassing within the conduit. These veins form transient channels through which exsolved gases can escape from magma. The purpose of this study is to determine the extent to which chemical heterogeneity within the melt results from gas transport, and assess how this can be used to study magma degassing. Two tuffisite veins from contrasting rhyolitic eruptions at Torfajökull (Iceland) and Chaitén (Chile) were studied in detail. The tuffisite vein from Torfajökull is from a shallow dissected conduit (~70. ka) that fed a degassed lava flow, while the sample from Chaitén was a bomb ejected during the waning phases of Plinian activity in May 2008. The results of detailed in situ chemical analyses (synchrotron XRF, FTIR, LA-ICP-MS) show that in both veins larger vesiculated fragments are enriched in volatile elements (Torfajökull: H, Li, Cl; Chaitén: Li, Cl, Cu, Zn, As, Sn, Sb) compared to the host, while the surrounding smaller particles are depleted in the Torfajökull vein (Li, Cl, Zn, Br, Rb, Pb), but enriched in the Chaitén vein (K, Cu, Zn, As, Mo, Sb, Pb). The lifespans of both veins and the fluxes of gas and particles through them can be estimated using diffusion profiles and enrichment factors. The Torfajökull vein had a longer lifespan (~a day) and low particle velocities (~cm/s), while the Chaitén vein was shorter lived (