Single particle analysis of ice crystal residuals observed in orographic wave clouds over Scandinavia during INTACC experiment

Abstract. Individual ice crystal residual particles collected over Scandinavia during the INTACC (INTeraction of Aerosol and Cold Clouds) experiment in October 1999 were analyzed by Scanning Electron Microscopy (SEM) equipped with Energy-Dispersive X-ray Analysis (EDX). Samples were collected onboard the British Met Office Hercules C-130 aircraft using a Counterflow Virtual Impactor (CVI). This study is based on six samples collected in orographic clouds. The main aim of this study is to characterize cloud residual elemental composition in conditions affected by different airmasses. In total 609 particles larger than 0.1 μm diameter were analyzed and their elemental composition and morphology were determined. Thereafter a hierarchical cluster analysis was performed on the signal detected with SEM-EDX in order to identify the major particle classes and their abundance. A cluster containing mineral dust, represented by aluminosilicates, Fe-rich and Si-rich particles, was the dominating class of particles, accounting for about 57.5% of the particles analyzed, followed by low-Z particles, 23.3% (presumably organic material) and sea salt (6.7%). Sulfur was detected often across all groups, indicating ageing and in-cloud processing of particles. A detailed inspection of samples individually unveiled a relationship between ice crystal residual composition and airmass origin. Cloud residual samples from clean airmasses (that is, trajectories confined to the Atlantic and Arctic Oceans and/or with source altitude in the free troposphere) were dominated primarily by low-Z and sea salt particles, while continentally-influenced airmasses (with trajectories that originated or traveled over continental areas and with source altitude in the continental boundary layer) contained mainly mineral dust residuals. Comparison of residual composition for similar cloud ambient temperatures around –27°C revealed that supercooled clouds are more likely to persist in conditions where low-Z particles represent significant part of the analyzed cloud residual particles. This indicates that organic material may be poor ice nuclei, in contrast to polluted cases when ice crystal formation was observed at the same environmental conditions and when the cloud residual composition was dominated by mineral dust. The presented results suggest that the chemical composition of cloud nuclei and airmass origin have a strong impact on the ice formation through heterogeneous nucleation in supercooled clouds.