Volcanic ash ice-nucleating activity can be enhanced or depressed by ash-gas interaction in the eruption plume

Volcanic ash can trigger ice nucleation when immersed in supercooled water. This will impact several processes (e.g., electrification, aggregation, precipitation) in the eruption plume and cloud and in the wider atmosphere upon ash dispersal. Previous studies show that ash bulk properties, reflecting the chemistry and phase state of the source magma, likely contribute to the ice-nucleating activity (INA) of ash. However, it remains unexplored how interaction with magmatic gases in the hot eruption plume, which inevitably leads to altered ash surface properties, affects the ash INA. Here we demonstrate that the INA of tephra is raised by exposure to H2O(g) mixed with SO2(g) at both 800 and 400 °C, but is substantially reduced by exposure to H2O(g) alone or mixed with HCl(g) at the same temperatures. In contrast, the INA of K-feldspar and quartz is reduced by all three eruption plume processing treatments. The decrease in INA of all silicates after heating with H2O(g) might relate to a loss of ice-active sites by surface dehydroxylation and/or oxidation. In the presence of HCl(g) or SO2(g), respectively, metal chloride or sulphate salts form on the tephra surfaces only. While NaCl and CaCl2 seem to have no effect on the tephra INA, CaSO4 is inferred to create ice-active sites, potentially through a particular combination of surface chemistry and topography. Overall, our findings suggest a complex interplay of bulk mineralogy and surface alteration in influencing ice nucleation by volcanic ash, and highlight the general sensitivity (enhancement or depression) of ash INA to interaction with magmatic gases in the eruption plume.