Received for review June 14, 2004

Revised manuscript received August 30, 2004

Accepted September 21, 2004

Abstract:

The trends in secondary organic aerosol at a remote location are studied using atmospheric fine particulate matter samples collected at Seney National Wildlife Refuge (NWR) in northern Michigan. Detailed analysis of particle-phase organic compounds revealed very low concentra tions of primary anthropogenic emissions and relatively high levels of organic di-, tri-, and tetracarboxylic acids thought to be indicators of secondary organic aerosols. Seasonal changes in these organic compounds were tracked by analyzing composites of monthly average samples. The concentration of aromatic and aliphatic dicarboxylic acids peak in July and taper off in the fall, which coincides with fine particle organic carbon concentration. In contrast, a chemical mass balance model used to quantify primary sources of particulate matter shows higher contributions from primary emissions in the winter. Complementing the monthly average concentrations, event-based composites of high volume samples were used to track the different species of secondary organic aerosol at the Seney NWR location. The distribution of aliphatic diacids and the aromatic di- and triacids varied with different atmospheric conditions, which suggests different precursor gases for these secondary organic aerosol components. The aliphatic diacid concentrations track with ambient concentrations of particle-phase pinonic acid. In addition, back-trajectories for the eight event-based composites are compared to the organic acid distributions and are linked to the distribution of organic acids present in the composites.

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