Abstract. To investigate the seasonal changes in biogenic water-soluble organic carbon (WSOC) aerosols in a boreal forest, aerosol samples were collected continuously in the canopy of a deciduous forest in northern Japan during 2009–2010. Stable carbon isotopic composition of WSOC (δ13CWSOC) in total suspended particulate matter (TSP) exhibited a distinct seasonal cycle, with lower values from June through September (−25.5±0.5 ‰). This cycle follows the net CO2 exchange between the forest ecosystem and the atmosphere, indicating that δ13CWSOC likely reflects the biological activity at the forest site. WSOC concentrations showed the highest values in early summer and autumn. Positive matrix factorization (PMF) analysis indicated that the factor in which biogenic secondary organic aerosols (BSOAs) dominated accounted for ~40 % of the highest concentrations of WSOC, where BSOAs mostly consisted of α-/β-pinene SOA. In addition, primary biological aerosol particles (PBAPs) made similar contributions (~57 %) to the WSOC near the forest floor in early summer. This finding indicates that the production of both primary and secondary WSOC aerosols is important during the growing season in a deciduous forest. The methanesulfonic acid (MSA) maximum was also found in early summer and had a distinct vertical gradient with larger concentrations near the forest floor. Together with the similar vertical gradients found for WSOC and δ13CWSOC as well as the α-/β-pinene SOA tracers, our results indicate that the forest floor, including ground vegetation and soil, acts as a significant source of WSOC in TSP within a forest canopy at the study site.

[1] Semicontinuous measurements of submicrometer water-soluble organic aerosols and particle size distributions were conducted at a deciduous forest site in northern Japan in August 2010. Increases in particle number concentration were frequently observed in daytime, accompanied by an increase in the concentrations of water-soluble organic carbon (WSOC). We found that daily averaged WSOC concentrations positively correlated with gross primary production of CO 2 by the forest ecosystem (r 2 = 0.63) and ambient temperature during daytime. These relations suggest that the formation of WSOC is closely linked to photosynthetic activity by the forest ecosystem, which depends on both temperature and solar radiation. Off-line chemical analysis of samples of particles with aerodynamic diameter smaller than 1 mm collected during a 2 day event of elevated WSOC levels suggests that photochemical aging of both a-and b-pinene and isoprene oxidation products contributes to the particle growth and the WSOC mass. Organic tracers of primary biological aerosol particles (PBAPs) showed distinct diurnal variations with a maximum around noontime, also indicating that higher temperature and light intensity induce emissions of PBAPs. However, their contribution to the submicrometer WSOC mass was likely insignificant. During the day, the concentrations of 3-methyl-1,2,3-butanetricarboxylic acid (3-MBTCA) showed a strong dependence on temperature, and the ratios of WSOC to particle volume concentration increased with an increase in the concentration ratios of 3-MBTCA to pinonic acid (PA). This result supports a previous proposal that the 3-MBTCA/PA ratios in submicrometer particles can be a useful tracer for chemical aging of biogenic secondary organic aerosol from forest vegetation.Citation: Miyazaki, Y., J. Jung, P. Fu, Y. Mizoguchi, K. Yamanoi, and K. Kawamura (2012), Evidence of formation of submicrometer water-soluble organic aerosols at a deciduous forest site in northern Japan in summer,

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