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Volcanic ash nucleates ice when immersed in supercooled water droplets, giving it the potential to influence weather and climate from local to global scales. This ice nucleation activity (INA) is likely derived from a subset of the crystalline mineral phases in the ash. The INA of other mineral-based dusts can change when exposed to various gaseous and aqueous chemical species, many of which also interact with volcanic ash in the eruption plume and atmosphere. However, the effects of aqueous chemical aging on the INA of volcanic ash have not been explored. We show that the INA of two mineralogically distinct ash samples from Fuego and Astroni volcanoes is variably reduced following immersion in water or aqueous sulfuric acid for minutes to days. Aging in water decreases the INA of both ash samples by up to two orders of magnitude, possibly due to a reduction in surface crystallinity and cation availability accompanying leaching. Aging in sulfuric acid leads to minimal loss of INA for Fuego ash, which is proposed to reflect a quasi-equilibrium between leaching that removes ice-active sites and dissolution that reveals or creates new sites on the pyroxene phases present. Conversely, exposure to sulfuric acid reduces the INA of Astroni ash by one to two orders of magnitude, potentially through selective dissolution of ice-active sites associated with surface microtextures on some K-feldspar phases. Analysis of dissolved element concentrations in the aged ash leachates shows supersaturation of certain mineral species which could have precipitated and altered the INA of the ash. These results highlight the key role that leaching, dissolution, and precipitation likely play in the aqueous aging of volcanic ash with respect to its INA. Finally, we discuss the implications for understanding the nature and reactivity of ice-active sites on volcanic ash and its role in influencing cloud properties in the atmosphere. 

Abstract. This study presents the first full annual cycle (2019–2020) of ambient surface aerosol particle number concentration measurements (condensationnuclei > 20 nm, N20) collected at Summit Station (Summit), in the centre of the Greenland Ice Sheet (72.58∘ N, −38.45∘ E; 3250 ma.s.l.). The mean surface concentration in 2019 was 129 cm−3, with the 6 h mean ranging between 1 and 1441 cm−3. The highest monthly mean concentrations occurred during the late spring and summer, with the minimum concentrations occurring in February (mean: 18 cm−3). High-N20 events are linked to anomalous anticyclonic circulation over Greenland and the descent of free-tropospheric aerosol down to the surface, whereas low-N20 events are linked to anomalous cyclonic circulation over south-east Greenland that drives upslope flow and enhances precipitation en route to Summit. Fog strongly affects particle number concentrations, on average reducing N20 by 20 % during the first 3 h of fog formation. Extremely-low-N20 events (< 10 cm−3) occur in all seasons, and we suggest that fog, and potentially cloud formation, can be limited by low aerosol particle concentrations over central Greenland.