Year-round observations of water-soluble ionic species and trace metals in Sapporo aerosols: implication for significant contributions from terrestrial biological sources in Northeast Asia

Abstract. High aerosol loadings are prevalent in the atmosphere of East Asia, where the aerosols impact the Earth's climate system and human health; however, their sources and seasonal variations are not clearly understood. To better understand the sources of water-soluble ionic species and trace metals in Northeast Asia, we studied atmospheric aerosol samples collected in Sapporo, northern Japan for one-year period. SO₄²⁻ (average 3.47 ± 1.03 μg m⁻³) was found as the most abundant ionic species, which accounted for on average 43 ± 15% of the measured total ionic mass followed by Cl⁻ (13 ± 12%) ≈ NO₃⁻ ≈ Na⁺ > NH₄⁺ > Ca²⁺ > Mg²⁺ > K⁺ > MSA⁻. Among the metals determined, Ca was found as the most abundant (45 ± 5.2%) followed by Fe (27 ± 4.5%), Al (21± 3.1%), Zn (3.2 ± 1.7), Ti, Mn, Ni, Pb, Cu, V, As, Cr and Cd. Based on factor analysis, linear relations of selected species with biomarkers, and backward air mass trajectories, we found that long-range atmospheric transport of soil dust (∼ 33%) from arid regions of Mongolia and/or Northeast China is a major source for Sapporo aerosols as well as terrestrial biogenic emissions (≥ 24%) including microbial activities and biomass burning mostly from distant source region(s) (e.g. Siberia). We also found that the contributions of soil dust to the aerosols maximized in early spring whereas those of vegetational emissions maximized in spring/summer. Contributions of microbial activities to aerosols peaked in autumn whereas forest fires/biomass burning peaked in autumn/winter. On the contrary, fossil fuel combustion/industrial activities and oceanic emissions to Sapporo aerosols are suggested to be rather minor. This study also suggests that fungal spores contribute to some trace metals (i.e. Ni, Cu, As) while pollen contributes to Zn in aerosols.