Long-term measurement of sub-3nm particles and their precursor gases in the boreal forest

2020 
Abstract. The knowledge of the dynamics of sub-3nm particles in the atmosphere is crucial for our understanding of first steps of atmospheric new particle formation. Therefore, accurate and stable long-term measurements of the smallest atmospheric particles are needed. In this study, we analyzed over five years of particle concentrations in size classes 1.1–1.3 nm, 1.3–1.7 nm and 1.7–2.5 nm obtained with the Particle Size Magnifier (PSM) and three years of precursor vapor concentrations measured with the Chemical Ionization Atmospheric Pressure Interface Time-of-Flight mass spectrometer (CI-APi-ToF) at the SMEAR II station in Hyytiala, Finland. The results show that the 1.1–1.3 nm particle concentrations have a daytime maximum during all seasons, which is due to increased photochemical activity. There are significant seasonal differences in median concentrations of 1.3–1.7 nm and 1.7–2.5 nm particles, underlining the different frequency of new particle formation between seasons. In particular, concentrations of 1.3–1.7 nm and 1.7–2.5 nm particles are notably higher in spring than during other seasons. Aerosol precursor vapors have notable diurnal and seasonal differences as well. Sulfuric acid and highly oxygenated organic molecule (HOM) monomer concentrations have clear daytime maxima, while HOM dimers have their maxima during the night. HOM concentrations for both monomers and dimers are the highest during summer and the lowest during winter. Higher median concentrations during summer result from increased biogenic activity in the surrounding forest. Sulfuric acid concentrations are the highest during spring and summer, with autumn and winter concentrations being two to three times lower. A correlation analysis between the sub-3nm concentrations and aerosol precursor vapor concentrations indicates that HOMs, particularly their dimers, and sulfuric acid play a significant role in new particle formation in the boreal forest. Our analysis also suggests that there might be seasonal differences in new particle formation pathways that need to be investigated further.
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