Gas/aerosol–ash interaction in volcanic plumes: New insights from surface analyses of fine ash particles

The reactions occurring between gases/aerosols and silicate ash particles in volcanic eruption plumes remain poorly understood, despite the fact that they are at the origin of a range of volcanic, environmental, atmospheric and health effects. In this study, we apply X-ray photoelectron spectroscopy (XPS), a surface-sensitive technique, to determine the chemical composition of the near-surface region (2–10 nm) of nine ash samples collected from eight volcanoes. In addition, atomic force microscopy (AFM) is used to image the nanometer-scale surface structure of individual ash particles isolated from three samples. We demonstrate that rapid acid dissolution of ash occurs within eruption plumes. This process is favoured by the presence of fluoride and is believed to supply the cations involved in the deposition of sulphate and halide salts onto ash. AFM imaging also has permitted the detection of extremely thin (< 10 nm) coatings on the surface of ash. This material is probably composed of soluble sulphate and halide salts mixed with sparingly soluble fluoride compounds. The surface approach developed here offers promising aspects for better appraising the role of gas/aerosol–ash interaction in dictating the ability of ash to act as sinks for various volcanic and atmospheric chemical species as well as sources for others.