Impact of in-cloud aqueous processes on the chemical compositions and morphology of individual atmospheric aerosols

Abstract

Abstract. The composition, morphology, and mixing structure of individual cloud residues (RES) and interstitial particles (INT) at a mountaintop site were investigated. Eight types of particles were identified, including sulfate-rich (S-rich), S-organic matter (OM), aged soot, aged mineral dust, aged fly ash, aged metal, refractory, and aged refractory mixture. A shift of dominant particle types from S-rich (29 %) and aged soot (27 %) in the INT to aged refractory mixture (23 %) and S-OM (22 %) in the RES is observed. In particular, particles with organic shells are enriched in the RES (27 %) relative to the INT (12 %). Our results highlight that the formation of more oxidized organic matter in the cloud contributes to the existence of organic shells after cloud processing. The fractal dimension (Df), a morphologic parameter to represent the branching degree of particles, for soot particles in the RES (1.82 ± 0.12) is lower than that in the INT (2.11 ± 0.09), which indicates that in-cloud processes may result in less compact soot. This research emphasizes the role of in-cloud processes in the chemistry and microphysical properties of individual particles. Given that organic coatings may determine the particle hygroscopicity, activation ability, and heterogeneous chemical reactivity, the increase of OM-shelled particles upon in-cloud processes should have considerable implications.