Organic aerosol spatial/temporal patterns: Perspectives of measurements and model

Ambient measurements from SEARCH and model results from CMAQ-MADRID are analyzed side by side for the southeastern United States to understand the strengths and weaknesses of an air quality model in reproducing key spatial and temporal patterns related to organic aerosol (OA), with inferences regarding secondary organic aerosol (SOA). The model predicts a larger difference in OA concentrations between an urban (JST) and a rural site (YRK) than indicated by measurements. Modeled OA concentrations at JST and YRK are more strongly correlated than measurements. On average, models may understate urban OA emissions, while overstating urban SOA production; measurements indicate that SOA production takes place on the regional scale. Modeled diurnal fluctuations for OA are stronger than measured, due partially to overestimations of the temperature dependence parameters (Delta H-vap) for SOA in the model. Urban-rural differences in the composition of SOA, inferred from the variations of estimated Delta H-vap, are not properly captured by the model, which does not represent multiple generations of SOA or varied reaction pathways as a function of chemical regimes. Model results are hampered by day-of-the-week and diurnal allocation issues related to EC and OA emissions. Top quintile (20%) afternoon OA concentrations are observed in both warm and cold seasons at the urban site. The frequency of high OA in the cold season is overstated in the model. The model predicts the warm vs cold season frequency of elevated OA episodes better at YRK than at JST, suggesting that regional emissions, chemistry, and transport are better simulated than urban processes.