Generation of Internally Mixed Insoluble and Soluble Aerosol Particles to Investigate the Impact of Atmospheric Aging and Heterogeneous Processing on the CCN Activity of Mineral Dust Aerosol

Abstract

Heterogeneous reactions of trace gases with mineral dust aerosol not only impact the chemical balance of the atmosphere but also the physicochemical properties of the dust particle and the ability of the particle to act as a cloud condensation nuclei (CCN). Recent field studies have shown that carbonate minerals are preferentially associated with nitrates whereas aluminum silicates (i.e., clay minerals) are preferentially associated with sulfates. To better understand how this association can impact the climate effects of mineral dust particles, we have measured the CCN activity of a number of pure and internal mixtures of aerosols relevant to these recent field studies. The CCN activity of CaCO ₃ -Ca(NO ₃ ) ₂ aerosol, simulating the activity of mineral dust aerosol that has been partially processed by nitrogen oxides in the atmosphere, is significantly enhanced relative to CaCO₃ aerosol of the same diameter. Similar results are obtained for a clay mineral, kaolinite, internally mixed with (NH ₄ ) ₂ SO ₄ . For example, at 0.3% supersaturation, a 200 nm particle containing a soluble nitrate or sulfate component is 2 to 4 times more active than an unreacted particle. The results presented here show that when determining the contribution of mineral dust aerosol to the overall impact of the aerosol indirect effect on radiative forcing, changes in chemical composition due to atmospheric processing cannot be ignored.

Acknowledgments

This material is based upon work supported by the National Science Foundation under Grant Nos. CHE0503854 and ATM0613124. Any opinions, findings, and conclusions or recommendations expressed in this material are those of the authors and do not necessarily reflect the views of the National Science Foundation. The authors would like to thank Jean Ross of the Central Microscopy Research Facility for her assistance in obtaining TEM images. VHG would like to thank Professor Kim Prather and Ryan Sullivan for helpful discussions.

Notes

^a Lognormal distribution: y = Aexp [].

^a Reported error based on the calculated sigmoidal fit of the data shown in Figure 5.

^b S_c is outside the range of the CCN counter.