A sub-decadal trend in diacids in atmospheric aerosols in eastern Asia

Abstract

Change in secondary organic aerosols (SOAs) has been predicted to be highly uncertain in the future atmosphere in Asia. To better quantify the SOA change, we examine the sub-decadal (2001-2008) trend in major surrogate compounds (C-2-C-10 diacids) of SOA in atmospheric aerosols from Gosan site on Cheju Island, South Korea. The Gosan site is influenced by pollution outflows from eastern Asia. The molecular distributions of diacids were characterized by the predominance of oxalic (C-2) acid followed by malonic (C-3) and succinic (C-4) acids in each year. The seasonal variations in diacids in each year were characterized by the highest concentrations of saturated diacids in spring and unsaturated diacids in winter. The consistent molecular distributions and seasonal variations along with significantly similar air mass transport patterns are indicative of similar pollution sources for diacids in eastern Asia on a sub-decadal scale. However, the intensity of the pollution sources has increased as evidenced by the increases in major diacids at the rate of 3.9-47.4% per year, particularly in April. The temporal variations in atmospheric tracer compounds (carbon monoxide, levoglucosan, 2-methyltetrols, pinic acid, glyoxylic acid, glyoxal and methylglyoxal) suggest that the increases in diacids are due to enhanced precursor emissions associated with more anthropogenic than biogenic activities followed by the compounds' chemical processing in the atmosphere. The trends in diacids contrast with the reported decreases in sulfate, nitrate and ammonium in recent years in eastern Asia. This study demonstrates that recent pollution control strategies in eastern Asia were not able to decrease organic acidic species in the atmosphere. The increases in water-soluble organic acid fraction could modify the aerosol organic composition and its sensitivity to climate relevant physical properties.