A. M. K. Hansen

Volatility of Organic Aerosol: Evaporation of Ammonium Sulfate/Succinic Acid Aqueous Solution Droplets

Condensation and evaporation modify the properties and effects of atmospheric aerosol particles. We studied the evaporation of aqueous succinic acid and succinic acid/ammonium sulfate droplets to obtain insights on the effect of ammonium sulfate on the gas/particle partitioning of atmospheric organic acids. Droplet evaporation in a laminar flow tube was measured in a Tandem Differential Mobility Analyzer setup. A wide range of droplet compositions was investigated, and for some of the experiments the composition was tracked using an Aerosol Mass Spectrometer. The measured evaporation was compared to model predictions where the ammonium sulfate was assumed not to directly affect succinic acid evaporation. The model captured the evaporation rates for droplets with large organic content but overestimated the droplet size change when the molar concentration of succinic acid was similar to or lower than that of ammonium sulfate, suggesting that ammonium sulfate enhances the partitioning of dicarboxylic acids to aqueous particles more than currently expected from simple mixture thermodynamics. If extrapolated to the real atmosphere, these results imply enhanced partitioning of secondary organic compounds to particulate phase in environments dominated by inorganic aerosol.

Characterization of humic-like substances in Arctic aerosols

Humic-like substances (HULIS) are a complex group of relatively high molecular weight organic compounds which contribute considerably to the mass of organic carbon (OC) and influence the light-absorbing properties of aerosols. In this work, HULIS were investigated for the first time in the high-Arctic atmosphere, focusing on the chemical characterization and mass contribution of HULIS to the total suspended particle (TSP) mass using weekly aerosol samples collected at Station Nord, northeast Greenland every fourth week during 2010. Average HULIS-C concentration was 11 ng C m−3 during the darker months (November–April) and 4 ng C m−3 during the other months (May–October) with an annual mass concentration of 0.02 ± 0.01 µg m−3. HULIS-C contributed to 3–16% of water-soluble organic carbon (WSOC), whereas HULIS accounted for 0.7–4.1% of TSP mass, with TSP typically below 1.0 µg m−3. Concentrations of OC, WSOC, HULIS, selected HULIS functional groups (carboxylic acids, aromatic carboxylic acids, and organosulfates) and levoglucosan overlapped with the typical Arctic haze pattern with elevated concentrations during winter to early spring. The aromatic carboxylic acid portion accounted for a larger share of total carboxylic acid of HULIS during the darker months (7%) compared to the brighter months (3%). The more abundant aromatic carboxylic acid functional groups and the moderate correlation between HULIS and levoglucosan concentrations during the darker months both indicate that biomass burning aerosols and thereby emissions of aromatic compounds could contribute to HULIS in the Arctic, especially during late winter. During the brighter months, relatively higher average molecular weight of HULIS was observed.

Effect of Organic Coatings, Humidity and Aerosol Acidity on Multiphase Chemistry of Isoprene Epoxydiols.

Multiphase chemistry of isomeric isoprene epoxydiols (IEPOX) has been shown to be the dominant source of isoprene-derived secondary organic aerosol (SOA). Recent studies have reported particles composed of ammonium bisulfate (ABS) mixed with model organics exhibit slower rates of IEPOX uptake. In the present study, we investigate the effect of atmospherically relevant organic coatings of α-pinene (AP) SOA on the reactive uptake of trans-β-IEPOX onto ABS particles under different conditions and coating thicknesses. Single particle mass spectrometry was used to characterize in real-time particle size, shape, density, and quantitative composition before and after reaction with IEPOX. We find that IEPOX uptake by pure sulfate particles is a volume-controlled process, which results in particles with uniform concentration of IEPOX-derived SOA across a wide range of sizes. Aerosol acidity was shown to enhance IEPOX-derived SOA formation, consistent with recent studies. The presence of water has a weaker impact on IEPOX-derived SOA yield, but significantly enhanced formation of 2-methyltetrols, consistent with offline filter analysis. In contrast, IEPOX uptake by ABS particles coated with AP-derived SOA is lower compared to that of pure ABS particles, strongly dependent on particle composition, and therefore on particle size.