UC Irvine

Atmospheric aerosols represent one of the greatest uncertainties in predicting the Earth’s future climate. Secondary organic aerosols (SOA) are particularly complicated because they are highly susceptible to change upon exposure to different conditions, such as varying temperatures and relative humidities (RHs), sunlight, and different atmospheric pollutants. The goal of this work was to increase our understanding of the contribution of SOA to the Earth’s radiation budget by exploring how different environmental conditions can affect aerosol properties and processes.

The first project investigated the effect of viscosity on photochemical kinetics of probe molecules embedded in laboratory-generated SOA. Temperature and RH of the system were varied independently to adjust the viscosity of the SOA and the samples were irradiated. At lower temperatures and humidities both systems exhibited lower photoreaction rates, suggesting that increased viscosity hinders the motion of the molecules in the SOA slowing down their photochemical reactions. This means that molecules trapped inside SOA in cold, dry parts of the atmosphere will photodegrade slower than in warm and humid areas.

The next stage of this work was to study the effect of RH on the mass loading and composition of SOA formed from toluene photooxidation. When the RH was increased from 0% to 75%, the yield of toluene SOA made under low NOx conditions decreased by an order of magnitude. High resolution mass spectrometry revealed a significant reduction in the fraction of oligomers present in the SOA made under humid conditions compared to dry conditions. These results suggest that water vapor suppresses oligomer formation in low NOx toluene SOA, reducing aerosol yield. This means that concentrations of toluene SOA in the atmosphere will be dependent on the RH and NOx concentrations.

The last stage of this work investigated the interaction between SOA and ammonia. SOA made from toluene, n-hexadecane, or limonene in a chamber was exposed to gaseous ammonia while the mass loading and composition was monitored. These experiments indicated that ammonia could be taken up into SOA, leaving less ammonia in the atmosphere to neutralize atmospheric acids. This leads to a reduction of inorganic aerosols in the atmosphere.