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Abstract. The ice nucleation ability of volcanic ash particles collected close to the Icelandic volcano Eyjafjallajökull during its eruptions in April and May 2010 is investigated experimentally, in the immersion and deposition modes, and applied to atmospheric conditions by comparison with airborne measurements and microphysical model calculations. The number of ash particles which are active as ice nuclei (IN) is strongly temperature dependent, with a very small minority being active in the immersion mode at temperatures of 250-263 K. Average ash particles show only a moderate effect on ice nucleation, by inducing freezing at temperatures between 236 K and 240 K (i.e. approximately 3-4 K higher than temperatures required for homogeneous ice nucleation, measured with the same instrument). By scaling the results to aircraft and lidar measurements of the conditions in the ash plume days down wind of the eruption, and by applying a simple microphysical model, it was found that the IN active in the immersion mode in the range 250-263 K generally occurred in atmospheric number densities at the lower end of those required to have an impact on ice cloud formation. However, 3-4 K above the homogeneous freezing point, immersion mode IN number densities a few days down wind of the eruption were sufficiently high to have a moderate influence on ice cloud formation. The efficiency of IN in the deposition mode was found to be poor except at very cold conditions (<238 K), when they reach an efficiency similar to that of mineral dust with the onset of freezing at 10 % supersaturation with respect to ice, and with the frozen fraction nearing its maximum value at a supersaturation 20 %. In summary, these investigations suggest volcanic ash particles to have only moderate effects on atmospheric ice formation.

With a paroxysmal ash eruption on 4 September 2007 and the highly explosive activity continuing in 2008, Oldoinyo Lengai (OL) has dramatically changed its behavior, crater morphology, and magma composition after 25 years of quiet extrusion of fluid natrocarbonatite lava. This explosive activity resembles the explosive phases of 1917, 1940-1941, and 1966-1967, which were characterized by mixed ashes with dominantly nephelinitic and natrocarbonatitic components. Ash and lapilli from the 2007-2008 explosive phase were collected on the slopes of OL as well as on the active cinder cone, which now occupies the entire north crater having buried completely all earlier natrocarbonatite features. The lapilli and ash samples comprise nepheline, wollastonite, combeite, Na-åkermanite, Ti-andradite, resorbed pyroxene and Fe-Ti oxides, and a Na-Ca carbonate phase with high but varying phosphorus contents which is similar, but not identical, to the common gregoryite phenocrysts in natrocarbonatite. Lapilli from the active cone best characterize the erupted material as carbonated combeitewollastonite-melilite nephelinite. The juvenile components represent a fundamentally new magma composition for OL, containing 25-30 wt.% SiO 2 , with 7-11 wt.% CO 2 , high alkalies (Na 2 O 15-19%, K 2 O 4-5%), and trace-element signatures reminiscent of natrocarbonatite enrichments. These data define an intermediate composition between natrocarbonatite and nephelinite, with about one third natrocarbonatite and two thirds nephelinite component. The data are consistent with a model in which the carbonated silicate magma has evolved from the common combeite-wollastonite nephelinite (CWN) of OL by enrichment of CO 2 and alkalies and is close to the liquid immiscible separation of natrocarbonatite from carbonated nephelinite. Material ejected in April/May 2008 indicates reversion to a more common CWN composition.

International audienc

The more than 500 fossil Ca-carbonatite occurrences on Earth are at odds with the only active East African Rift carbonatite volcano, Oldoinyo Lengai (Tanzania), which produces Na-carbonatite magmas. The volcano's recent major explosive eruptions yielded a mix of nephelinitic and carbonatite melts, supporting the hypothesis that carbonatites and spatially associated peralkaline silicate lavas are related through liquid immiscibility. Nevertheless, previous eruption temperatures of Na-carbonatites were 490-595 °C, which is 250-450 °C lower than for any suitable conjugate silicate liquid. This study demonstrates experimentally that moderately alkaline Ca-carbonatite melts evolve to Na-carbonatites through crystal fractionation. The thermal barrier of the synthetic Na-Ca-carbonate system, held to preclude an evolution from Ca-carbonatites to Na-carbonatites, vanishes in the natural system, where continuous fractionation of calcite + apatite leads to Na-carbonatites, as observed at Oldoinyo Lengai. Furthermore, saturating the Na-carbonatite with minerals present in possible conjugate nephelinites yields a parent carbonatite with total alkali contents of 8-9 wt%, i.e., concentrations that are realistic for immiscible separation from nephelinitic liquids at 1000-1050 °C. Modeling the liquid line of descent along the calcite surface requires a total fractionation of ~48% calcite, ~12% apatite, and ~2 wt% clinopyroxene. SiO 2 solubility only increases from 0.2 to 2.9 wt% at 750-1200 °C, leaving little leeway for crystallization of silicates. The experimental results suggest a moderately alkaline parent to the Oldoinyo Lengai carbonatites and therefore a common origin for carbonatites related to alkaline magmatism. *