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Abstract. The April-May, 2010 volcanic eruptions of Eyjafjallajökull, Iceland caused significant economic and social disruption in Europe whilst state of the art measurements and ash dispersion forecasts were heavily criticized by the aviation industry. Here we demonstrate for the first time that large improvements can be made in quantitative predictions of the fate of volcanic ash emissions, by using an inversion scheme that couples a priori source information and the output of a Lagrangian dispersion model with satellite data to estimate the volcanic ash source strength as a function of altitude and time. From the inversion, we obtain a total fine ash emission of the eruption of 8.3±4.2 Tg for particles in the size range of 2.8-28 µm diameter. We evaluate the results of our model results with a posteriori ash emissions using independent ground-based, airborne and space-borne measurements both in case studies and statistically. Subsequently, we estimate the area over Europe affected by volcanic ash above certain concentration thresholds relevant for the aviation industry. We find that during three episodes in April and May, volcanic ash concentrations at some altitude in the atmosphere exceeded the limits for the "Normal" flying zone in up to 14 % (6-16 %), 2 % (1-3 %) and 7 % (4-11 %), respecCorrespondence to: A. Stohl (ast@nilu.no) tively, of the European area. For a limit of 2 mg m −3 only two episodes with fractions of 1.5 % (0.2-2.8 %) and 0.9 % (0.1-1.6 %) occurred, while the current "No-Fly" zone criterion of 4 mg m −3 was rarely exceeded. Our results have important ramifications for determining air space closures and for real-time quantitative estimations of ash concentrations. Furthermore, the general nature of our method yields better constraints on the distribution and fate of volcanic ash in the Earth system.

. (2012) 'A review of volcanic ash aggregation.', Physics and chemistry of the earth, parts A/B/C., 45-46 . pp. 65-78. Further information on publisher's website:http://dx.doi.org/10.1016/j.pce. 2011.11.001 Publisher's copyright statement:Additional information: Use policyThe full-text may be used and/or reproduced, and given to third parties in any format or medium, without prior permission or charge, for personal research or study, educational, or not-for-pro t purposes provided that:• a full bibliographic reference is made to the original source • a link is made to the metadata record in DRO • the full-text is not changed in any way The full-text must not be sold in any format or medium without the formal permission of the copyright holders.Please consult the full DRO policy for further details. AbstractMost volcanic ash particles with diameters < 63 µm settle from eruption clouds as particle aggregates that cumulatively have larger sizes, lower densities, and higher terminal fall velocities than individual constituent particles. Particle aggregation reduces the atmospheric residence time of fine ash, which results in a proportional increase in fine ash fallout within 10s km to 100s km from the volcano and a reduction in airborne fine ash mass concentrations 1000s km from the volcano. Aggregate characteristics vary with distance from the volcano: proximal aggregates are typically larger (up to cm size) with concentric structures, while distal aggregates are typically smaller (sub-millimetre size). Particles comprising ash aggregates are bound through hydro-bonds (liquid and ice water) and electrostatic forces, and the rate of particle aggregation correlates with cloud liquid water availability. Eruption source parameters (including initial particle size distribution, erupted mass, eruption column height, cloud water content and temperature) and the eruption plume temperature lapse rate, coupled with the environmental parameters, determines the type and spatiotemporal distribution of aggregates. Field studies, lab experiments and modelling investigations have already provided important insights on the process of particle aggregation. However, new integrated observations that combine remote sensing studies of 2 ash clouds with field measurement and sampling, and lab experiments are required to fill current gaps in knowledge surrounding the theory of ash aggregate formation. Abstract word count: 222

[1] Ice formation in atmospheric clouds is crucial to our understanding of precipitation and cloud radiative properties. In recent work it was shown that heterogeneous ice nucleation rates can be strongly enhanced by a form of surface crystallization (Shaw et al., 2005). Here we present new laboratory data and consider the implications for contact nucleation and its relevance to ice nucleation in atmospheric clouds. Our observations contradict three leading hypotheses for contact nucleation and suggest, instead, that the notion of contact nucleation should be generalized to include surface crystallization from particles contacting a supercooled drop from the inside out, as well as from the outside in. Our findings lead to the hypothesis that the freezing temperature of an evaporating drop will suddenly become higher once the drop surface contacts an immersed ice nucleus. This mechanism for evaporation freezing is therefore a plausible explanation for the abundant observations of high ice concentrations associated with cloud dilution and droplet evaporation. Citation: Durant, A.

[1] Water is the dominant component of volcanic gas emissions, and water phase transformations, including the formation of ice, can be significant in the dynamics of volcanic clouds. The effectiveness of volcanic ash particles as ice-forming nuclei (IN) is poorly understood and the sparse data that exist for volcanic ash IN have been interpreted in the context of meteorological, rather than volcanic clouds. In this study, single-particle freezing experiments were carried out to investigate the effect of ash particle composition and surface area on water drop freezing temperature. Measured freezing temperatures show only weak correlations with ash IN composition and surface area. Our measurements, together with a review of previous volcanic ash IN measurements, suggest that fine-ash particles (equivalent diameters between approximately 1 and 1000 mm) from the majority of volcanoes will exhibit an onset of freezing between $250-260 K. In the context of explosive eruptions where super-micron particles are plentiful, this result implies that volcanic clouds are IN-rich relative to meteorological clouds, which typically are IN-limited, and therefore should exhibit distinct microphysics. We can expect that such ''overseeded'' volcanic clouds will exhibit enhanced ice crystal concentrations and smaller average ice crystal size, relative to dynamically similar meteorological clouds, and that glaciation will tend to occur over a relatively narrow altitude range.

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[1] Uncertainty remains on the origin of distal mass deposition maxima observed in many recent tephra fall deposits. In this study the link between ash aggregation and the formation of distal mass deposition maxima is investigated through reanalysis of tephra fallout from the Mount St. Helens 18 May 1980 (MSH80) eruption. In addition, we collate all the data needed to model distal ash sedimentation from the MSH80 eruption cloud. Four particle size subpopulations were present in distal fallout with modes at 2.2 F, 4.2 F, 5.9 F, and 8.3 F. Settling rates of the coarsest subpopulation closely matched predicted single-particle terminal fall velocities. Sedimentation of particles <100 mm was greatly enhanced, predominantly through aggregation of a particle subpopulation with modal diameter 5.9 ± 0.2 F (19 ± 3 mm). Mammatus on the MSH80 cloud provided a mechanism to transport very fine ash particles, with predicted atmospheric lifetimes of days to weeks, from the upper troposphere to the surface in a matter of hours. In this mechanism, ash particles initiate ice hydrometeor formation high in the troposphere. Subsequently, the volcanic cloud rapidly subsides as mammatus develop from increased particle loading and cloud base sublimation. Rapid fallout occurs as the cloud passes through the melting level in a process analogous to snowflake aggregation. Aggregates sediment en masse and form the distal mass deposition maxima observed in many recent volcanic ash fall deposits. This work provides a data resource that will facilitate tephra sedimentation modeling and allow model intercomparisons.

[1] The occurrence of particle aggregation has a dramatic effect on the transport and sedimentation of volcanic ash. The aggregation process is complex and can occur under different conditions and in multiple regions of the plume and in the ash cloud. In the companion paper, Costa et al. develop an aggregation model based on a fractal relationship to describe the rate particles are incorporated into ash aggregates. The model includes the effects of both magmatic and atmospheric water present in the volcanic cloud and demonstrates that the rate of aggregation depends on the characteristics of the initial particle size distribution. The aggregation model includes two parameters, the fractal exponent D f , which describes the efficiency of the aggregation process, and the aggregate settling velocity correction factor y e , which influences the distance at which distal mass deposition maxima form. Both parameters are adjusted using features of the observed deposits. Here this aggregation model is implemented in the FALL3D volcanic ash transport model and applied to the 18 May 1980 Mount St. Helens and the 17-18 September 1992 Crater Peak eruptions. For both eruptions, the optimized values for D f (2.96-3.00) and y e (0.27-0.33) indicate that the ash aggregates had a bulk density of 700-800 kg m −3 . The model provides a higher degree of agreement than previous fully empirical aggregation models and successfully reproduces the depositional characteristics of the deposits investigated over a large range of scales, including the position and thickness of the secondary maxima.