Boundary layer versus free tropospheric submicron particle formation: A case study from NASA DC-8 observations in the Asian continental outflow during the KORUS-AQ campaign.

In this study, we contrasted major secondary inorganic species and processes responsible for submicron particle formation (SPF) events in the boundary layer (BL) and free troposphere (FT) over the Korean Peninsula during Korea-United States Air Quality (KORUS-AQ) campaign (May-June, 2016) using aircraft observations. The number concentration of ultrafine particles with diameters between 3 nm and 10 nm (N) during the entire KORUS-AQ period reached a peak (7,606 ± 12,003 cm ) at below 1 km altitude, implying that the particle formation around the Korean Peninsula primarily occurred in the daytime BL. During the BL SPF case (7 May, 2016), the SPF over Seoul metropolitan area was more attributable to oxidation of NO rather than SO-to-sulfate conversion. From the analysis of the relationship between nitrogen oxidation ratio (NOR) and temperature or relative humidity (RH), NOR showed a positive correlation only with temperature. This suggests that homogeneous gas-phase reactions of NO with OH or O contributed to nitrate formation. From the relationship between N (> 10,000 cm) and the NOR (or sulfur oxidation ratio) at Olympic Park in Seoul during the entire KORUS-AQ period, it was regarded that the relative importance of nitrogen oxidation was grown as the N increased. During the FT SPF case (31 May, 2016) over the yellow sea, the SO-to-sulfate conversion seemed to influence SPF highly. The sulfate/CO ratio had a positive correlation with both the temperature and RH, suggesting that aqueous-phase pathways as well as gas-phase reactions might be attributable to sulfate formation in the FT. In particular, FT SPF event on 31 May was possibly caused by the direct transport of SO precursors from the continent above the shallow marine boundary layer under favorable conditions for FT SPF events, such as decreased aerosol surface area and increased solar radiation.