Abstract

Abstract. Ambient aerosol samples (TSP, n = 50) were collected for 12 months at subtropical Okinawa Island, Japan, an outflow region of Asian dusts in the western North Pacific and analysed for organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC), water-soluble total nitrogen (WSTN), water-soluble organic nitrogen (WSON) and major ions to better understand the formation and transformation of East Asian aerosols during long-range atmospheric transport. Concentration ranges of these components are; OC: 0.76–7.1 μg m−3 (av. 1.7 ± 1.0 μg m−3), EC: 0.07–0.96 μg m−3 (0.28 ± 0.19 μg m−3), WSOC: 0.27–1.9 μg m−3 (0.73 ± 0.38 μg m−3), WSTN: 0.77 to 3.0 μg m−3 (0.58 ± 0.46 μg m−3) and WSON: 0.0–2.2 μg m−3 (0.12 ± 0.23 μg m−3). Higher OC concentrations were obtained in active biota seasons; spring (av. 2.4 μg m−3) and summer (1.8 μg m−3). EC and WSOC concentrations maximized in spring (av. 0.41 μg m−3 and 0.95 μg m−3, respectively) followed by winter (0. 70 and 0.90 μg m−3) whereas they became lowest in summer (0.19 and 0.52 μg m−3). In contrast, WSTN concentrations were highest in winter (0.86 μg m−3) and lowest in summer (0.37 μg m−3) and autumn (0.34 μg m−3). Concentrations of WSON are higher in early summer (av. 0.26 μg m−3) due to the emission from marine biota. The high ratios of OC / EC (av. 7.6) and WSOC / OC (44%) suggest a secondary formation of organic aerosols. Strong correlation between OC and MSA- (0.81) in spring suggests that springtime aerosols are influenced by additional marine and terrestrial biogenic sources. The positive correlation of Ca2+ and TSP in spring (r = = 0.81) demonstrates a significant contribution of Asian dust whereas high abundances of NO3- and nss-SO42- in winter suggest an important contribution from anthropogenic sources including biomass burning, vehicular emission and coal combustion. NH4-N/WSTN ratios peaked in winter (0.56), indicating a significant contribution of biomass burning to WSTN in cold season. In contrast, higher NO3-N/WSTN ratio in spring than winter suggests that the atmospheric transport of vehicular emissions maximizes in spring. Correlation analyses of major ions suggest that NH4+ and Ca2+ play major role in the neutralization of acidic aerosols forming NH4HSO4, (NH4)2SO4 and CaSO4.

Highlights

  • Aerosols affect the Earth’s radiative forcing directly by scattering and absorbing light and indirectly by acting as cloud condensation nuclei (Buseck and Posfai, 1999)

  • We found a strong correlation (r = 0.87) between organic carbon (OC) and biomass burning tracer in autumn, indicating a significant influence of biomass burning on organic aerosols

  • We found a positive correlation between NO−3 and biomass burning tracer (r = 0.65) in winter, suggesting that NO−3 is associated with biomass burning

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Summary

Introduction

Aerosols affect the Earth’s radiative forcing directly by scattering and absorbing light and indirectly by acting as cloud condensation nuclei (Buseck and Posfai, 1999). Organic aerosols that contain water-soluble species play an important role in climate forcing (Novakov and Penner, 1993) and cloud condensation nuclei (CCN) activity (Saxena et al, 1995). Cape Hedo is located on the northern edge of Okinawa and has been used as a supersite of Atmospheric Brown Clouds (ABC) project to study the atmospheric transport of Chinese aerosols and their chemical transformation in East Asia (Takami et al, 2007). We report one-year observations of OC, EC, WSOC, WSTN and major ions in ambient atmospheric aerosols collected at Cape Hedo, Okinawa. No studies were conducted for a long-term measurement of OC, EC, WSOC, WSTN, WSON and major ions in atmospheric aerosols from Cape Hedo, Okinawa Island

Sampling site and aerosol collection
Chemical analysis
Estimate of organic matter and secondary organic carbon
Estimate of sea salt and non-sea salt component
Estimate of chlorine loss
Backward air mass trajectory analysis
Aerosols mass loading
Seasonal variations of carbonaceous and nitrogenous components
Seasonal variations of inorganic species
Ion balance and correlations among major ions
Sea salt and non-sea salt ions
Neutralization factor and ionic composition
Summary and conclusions
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