Abstract. In the present-day atmosphere, sulfuric acid is the mostimportant vapour for aerosol particle formation and initial growth. However,the growth rates of nanoparticles (<10 nm) from sulfuric acidremain poorly measured. Therefore, the effect of stabilizing bases, thecontribution of ions and the impact of attractive forces on molecularcollisions are under debate. Here, we present precise growth ratemeasurements of uncharged sulfuric acid particles from 1.8 to 10 nm, performedunder atmospheric conditions in the CERN (EuropeanOrganization for Nuclear Research) CLOUD chamber. Our results showthat the evaporation of sulfuric acid particles above 2 nm is negligible,and growth proceeds kinetically even at low ammonia concentrations. Theexperimental growth rates exceed the hard-sphere kinetic limit for thecondensation of sulfuric acid. We demonstrate that this results fromvan der Waals forces between the vapour molecules and particles anddisentangle it from charge–dipole interactions. The magnitude of theenhancement depends on the assumed particle hydration and collisionkinetics but is increasingly important at smaller sizes, resulting in asteep rise in the observed growth rates with decreasing size. Including theexperimental results in a global model, we find that the enhanced growth rate ofsulfuric acid particles increases the predicted particle number concentrationsin the upper free troposphere by more than 50 %.
Role of iodine oxoacids in atmospheric aerosol nucleation
Iodic acid (HIO 3 ) is known to form aerosol particles in coastal marine regions, but predicted nucleation and growth rates are lacking. Using the CERN CLOUD (Cosmics Leaving Outdoor Droplets) chamber, we find that the nucleation rates of HIO 3 particles are rapid, even exceeding sulfuric acid–ammonia rates under similar conditions. We also find that ion-induced nucleation involves IO 3 − and the sequential addition of HIO 3 and that it proceeds at the kinetic limit below +10°C. In contrast, neutral nucleation involves the repeated sequential addition of iodous acid (HIO 2 ) followed by HIO 3 , showing that HIO 2 plays a key stabilizing role. Freshly formed particles are composed almost entirely of HIO 3 , which drives rapid particle growth at the kinetic limit. Our measurements indicate that iodine oxoacid particle formation can compete with sulfuric acid in pristine regions of the atmosphere.
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- 589 to 595
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- National Science Foundation
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