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Anthropogenic emissions of sulfur dioxide (SO2) and nitrogen oxides(NOx) may affect concentration levels and composition of biogenicsecondary organic aerosols (BSOA) through photochemical reactions withbiogenic organic precursors to form organosulfates and nitrooxyorganosulfates. We investigated this influence in a field study from 19 Mayto 22 June, 2011 at two sampling sites in Denmark. Within the study, weidentified a substantial number of organic acids, organosulfates and nitrooxyorganosulfates in the ambient urban curbside and semi-rural background air. Ahigh degree of correlation in concentrations was found among a group ofspecific organic acids, organosulfates and nitrooxy organosulfates, which mayoriginate from various precursors, suggesting a common mechanism or factoraffecting their concentration levels at the sites. It was proposed that theformation of those species most likely occurred on a larger spatial scale,with the compounds being long-range transported to the sites on the days withthe highest concentrations. The origin of the long-range transported aerosolswas investigated using the Hybrid Single Particle Lagrangian IntegratedTrajectory (HYSPLIT) model in addition to modeled emissions of relatedprecursors, including isoprene and monoterpenes using the global Model ofEmissions of Gases and Aerosols from Nature (MEGAN) and SO2 emissionsusing the European Monitoring and Evaluation Program (EMEP) database. Thelocal impacts were also studied by examining the correlation between selectedspecies, which showed significantly enhanced concentrations at the urbancurbside site and the local concentrations of various gases, includingSO2, ozone (O3), NOx, aerosol acidity and othermeteorological conditions. This investigation showed that an inter-play ofthe local parameters such as the aerosol acidity, NOx, SO2,relative humidity (RH), temperature and global radiation seemed to affect theconcentration level of those species, suggesting the influence of aqueousaerosol chemistry. The local impacts, however, seemed minor compared to theregional impacts. The total concentrations of organosulfates and nitrooxyorganosulfates, on average, contributed to approximately 0.5–0.8% ofPM1 mass at the two sampling sites

atmospheric chemistry and physics

Understanding the anthropogenic influence on formation of biogenic secondary organic aerosols in Denmark via analysis of organosulfates and related oxidation products