Ice-nucleating particles (INPs) have the potential to remove much of the liquid water in climatically important mid- to high-latitude shallow supercooled clouds, markedly reducing their albedo. The INP sources at these latitudes are very poorly defined, but it is known that there are substantial dust sources across the high latitudes, such as Iceland. Here, we show that Icelandic dust emissions are sporadically an important source of INPs at mid to high latitudes by combining ice-nucleating active site density measurements of aircraft-collected Icelandic dust samples with a global aerosol model. Because Iceland is only one of many high-latitude dust sources, we anticipate that the combined effect of all these sources may strongly contribute to the INP population in the mid- and high-latitude northern hemisphere. This is important because these emissions are directly relevant for the cloud-phase climate feedback and because high-latitude dust emissions are expected to increase in a warmer climate.

Abstract. Volcanic ash is known to nucleate ice when immersed in supercooled water droplets. This process may impact the properties and dynamics of the eruption plume and cloud as well as those of meteorological clouds once the ash is dispersed in the atmosphere. However, knowledge of what controls the ice-nucleating activity (INA) of ash remains limited, although it has been suggested that crystalline components in ash may play an important role. Here we adopted a novel approach using nine pairs of tephra and their remelted and quenched glass equivalents to investigate the influence of chemical composition, crystallinity, and mineralogy on ash INA in the immersion mode. For all nine pairs studied, the crystal-bearing tephra nucleated ice at warmer temperatures than the corresponding crystal-free glass, indicating that crystalline phases are key to ash INA. Similar to findings for desert dust from arid and semi-arid regions, the presence of feldspar minerals characterizes the four most ice-active tephra samples, although a high INA is observed even in the absence of alkali feldspar in samples bearing plagioclase feldspar and orthopyroxene. There is evidence of a potential indirect relationship between chemical composition and ash INA, whereby a magma of felsic to intermediate composition may generate ash containing ice-active feldspar or pyroxene minerals. This complex interplay between chemical composition, crystallinity, and mineralogy could help to explain the variability in volcanic ash INA reported in the literature. Overall, by demonstrating the importance of crystalline phases in the INA of ash, our study contributes insights essential for better appraising the role of airborne ash in ice formation. Among these is the inference that glass-dominated ash emitted by the largest explosive volcanic eruptions might be less effective at impacting ice-nucleating particle populations than crystalline ash generated by smaller, more frequent eruptions.

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The atmospheric impacts of volcanic ash from explosive eruptions are rarely considered alongside those of volcanogenic gases/aerosols. While airborne particles provide solid surfaces for chemical reactions with trace gases in the atmosphere, the reactivity of airborne ash has seldom been investigated. Here we determine the total uptake capacity (NiM) and initial uptake coefficient (γM) for sulfur dioxide (SO2) and ozone (O3) on a compositional array of volcanic ash and glass powders at ~25°C in a Knudsen flow reactor. The measured ranges of NiSO2 and γSO2 (1011–1013 molecules cm−2 and 10−3–10−2) and NiO3 and γO3 (1012–1013 molecules cm−2 and 10−3–10−2) are comparable to values reported for mineral dust. Differences in ash and glass reactivity toward SO2 and O3 may relate to varying abundances of, respectively, basic and reducing sites on these materials. The typically lower SO2 and O3 uptake on ash compared to glass likely results from prior exposure of ash surfaces to acidic and oxidizing conditions within the volcanic eruption plume/cloud. While sequential uptake experiments overall suggest that these gases do not compete for reactive surface sites, SO2 uptake forming adsorbed S(IV) species may enhance the capacity for subsequent O3 uptake via redox reaction forming adsorbed S(VI) species. Our findings imply that ash emissions may represent a hitherto neglected sink for atmospheric SO2 and O3.