ACP Atmospheric Chemistry and Physics ACP 1680-7324 Copernicus GmbH Göttingen, Germany 10.5194/acp-9-3303-2009 Effect of chemical mixing state on the hygroscopicity and cloud nucleation properties of calcium mineral dust particles Sullivan R. C. 1 4 Moore M. J. K. 1 Petters M. D. 2 Kreidenweis S. M. 2 Roberts G. C. 3 Prather K. A. 1 3 Department of Chemistry and Biochemistry, University of California, San Diego, La Jolla, CA, 92093, USA Department of Atmospheric Science, Colorado State University, Fort Collins, CO, 80523, USA Scripps Institution of Oceanography, University of California, San Diego, La Jolla, CA, 92093, USA currently at: Department of Atmospheric Science, Colorado State University, Fort Collins, CO, 80523, USA 20 05 2009 9 10 3303 3316 This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited. This article is available from http://www.atmos-chem-phys.net/9/3303/2009/acp-9-3303-2009.html The full text article is available as a PDF file from http://www.atmos-chem-phys.net/9/3303/2009/acp-9-3303-2009.pdf

Atmospheric mineral dust particles can alter cloud properties and thus climate by acting as cloud condensation nuclei (CCN) that form cloud droplets. The CCN activation properties of various calcium mineral dust particles were studied experimentally to investigate the consequences of field observations showing the segregation of sulphate from nitrate and chloride between individual aged Asian dust particles, and the enrichment of oxalic acid in Asian dust. Each mineral's observed apparent hygroscopicity was primarily controlled by its solubility, which determines the degree to which the mineral's intrinsic hygroscopicity can be expressed. The significant increase in hygroscopicity caused by mixing soluble hygroscopic material with insoluble mineral particles is also presented. Insoluble minerals including calcium carbonate, representing fresh unprocessed dust, and calcium sulphate, representing atmospherically processed dust, had similarly small apparent hygroscopicities. Their activation is accurately described by a deliquescence limit following the Kelvin effect and corresponded to an apparent single-hygroscopicity parameter, κ, of ~0.001. Soluble calcium chloride and calcium nitrate, representing atmospherically processed mineral dust particles, were much more hygroscopic, activating similar to ammonium sulphate with κ~0.5. Calcium oxalate monohydrate (κ=0.05) was significantly less CCN-active than oxalic acid (κ=0.3), but not as inactive as its low solubility would predict. These results indicate that the common assumption that all mineral dust particles become more hygroscopic and CCN-active after atmospheric processing should be revisited. Calcium sulphate and calcium oxalate are two realistic proxies for aged mineral dust that remain non-hygroscopic. The dust's apparent hygroscopicity will be controlled by its chemical mixing state, which is determined by its mineralogy and the chemical reaction pathways it experiences during transport.

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