Source apportionment and impact of long-range transport on carbonaceous aerosol particles in central Germany during HCCT-2010

The identification of different sources of the carbonaceous aerosol (organics and black carbon) was investigated at a mountain forest site located in central Germany from September to October 2010 to characterize incoming air masses during the Hill Cap Cloud Thuringia 2010 (HCCT-2010) experiment. The near-PM1 chemical composition, as measured by a high-resolution time-offlight aerosol mass spectrometer (HR-ToF-AMS), was dominated by organic aerosol (OA; 41 %) followed by sulfate (19 %) and nitrate (18 %). Source apportionment of the OA fraction was performed using the multilinear engine (ME-2) approach, resulting in the identification of the following five factors: hydrocarbon-like OA (HOA; 3% of OA mass), biomass burning OA (BBOA; 13 %), semi-volatilelike OA (SV-OOA; 19 %), and two oxygenated OA (OOA) factors. The more oxidized OOA (MO-OOA, 28 %) was interpreted as being influenced by aged, polluted continental air masses, whereas the less oxidized OOA (LO-OOA, 37 %) was found to be more linked to aged biogenic sources. Equivalent black carbon (eBC), measured by a multi-angle absorption photometer (MAAP) represented 10% of the total particulate matter (PM). The eBC was clearly associated with HOA, BBOA, and MO-OOA factors (all together R-2=0 :83). Therefore, eBC's contribution to each factor was achieved using a multi-linear regression model. More than half of the eBC (52 %) was associated with long-range transport (i.e., MO-OOA), whereas liquid fuel eBC (35 %) and biomass burning eBC (13 %) were associated with local emissions, leading to a complete apportionment of the carbonaceous aerosol. The separation between local and transported eBC was well supported by the mass size distribution of elemental carbon (EC) from Berner impactor samples. Air masses with the strongest marine influence, based on back trajectory analysis, corresponded with a low particle mass concentration (6.4-7.5 mu gm(-3)/ and organic fraction (approximate to 30 %). However, they also had the largest contribution of primary OA (HOA approximate to 4% and BBOA 15 %-20 %), which was associated with local emissions. Continental air masses had the highest mass concentration (11.4-12.6 mu gm(-3)), and a larger fraction of oxygenated OA (approximate to 45 %) indicated highly processed OA. The present results emphasize the key role played by long-range transport processes not only in the OA fraction but also in the eBC mass concentration and the importance of improving our knowledge on the identification of eBC sources.

Automated summary

The study investigated the sources of carbonaceous aerosols at a mountain forest site in central Germany, identifying organic aerosols as the dominant component, influenced by biomass burning and oxidation processes. Black carbon was associated with both local emissions and long-range transport, with highly oxidized OA linked to continental pollution and less oxidized OA associated with aged biogenic sources.