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To better understand the distributions and sources of low-molecular-weight (LMW) monocarboxylic acids (monoacids) in the forest atmosphere, we conducted simultaneous collection of gaseous and particulate samples at a deciduous broadleaf forest site in northern Japan. LMW normal (C1–C10), branched (iC4–iC6), hydroxyl (glycolic and lactic) and aromatic (benzoic) monoacids were detected in the gas and particle phases. The dominant LMW monoacids in gas phase were formic (mean: 953 ng m−3) and acetic (528 ng m−3) acids followed by propionic (37 ng m−3) or isopentanoic (42 ng m−3) acid. In the particle phase, isopentanoic (159 ng m−3) was dominant, followed by acetic (104 ng m−3) and formic (71 ng m−3) or lactic (65 ng m−3) acids. Concentrations of LMW monoacids did not show correlations with anthropogenic tracers such as nss-SO42- and NO3-, indicating that anthropogenic contribution is not important. Concentrations of C1–C6 monoacids in the gas phase showed positive correlations (r2=0.21–0.91) with isobutyric acid (iC4), which may be produced by microbial activity in soil. The forest soil may be a source of gaseous C1–C6 monoacids in the forest atmosphere. Acetic acid in the particle phase positively correlated with nonanoic acid (C9) (r2=0.63), suggesting that formation of acetic and nonanoic acids is associated with the oxidation of biogenic unsaturated fatty acids in the aerosol phase, in addition to photochemical oxidation of biogenic volatile organic compounds. The particle-phase fractions (Fp) of formic and acetic acids showed negative correlation with ambient temperature (C1: r2=0.49, C2: r2=0.60) but showed positive correlation with relative humidity (C1: r2=0.30, C2: r2=0.55) in daytime, suggesting that these meteorological parameters are important for the gas and particle portioning of monoacids in the forest atmosphere.

The present study reports on carbonaceous, water-soluble species and trace metals in PM10 aerosols collected at Bharati station during the austral summer (December 17, 2016 to February 2, 2017) over East Antarctica. Organic matter was the predominant among all measured species followed by nss-Ca2+ and nss-SO42-. Two distinct air masses that arrive from high-altitude-troposphere (HTAs) and low-altitude-troposphere (LTAs) regions which clearly showed significant differences in concentrations of measured chemical and metal species as inferred from the air mass backward trajectory analysis and mixed layer height variations. Based on significant positive correlations among chemical species, aerosol liquid water content (ALWC), and PM10 mass, we confirmed that the aqueous-phase formation of secondary aerosols followed by atmospheric processing are possible sources in HTAs while primary emissions associated with soil/dust from ice-free regions and in-situ emissions are major sources in LTAs. This result further supported by significant (p < 0.05) higher concentrations of specific trace metals (for example, Fe, Ti, and Pb) in LTAs. Moreover, higher cation-to-anion (Σ+/Σ−) ratios suggesting the alkaline nature of aerosols at Bharati. The present study demonstrates that ice-free regions over East Antarctica may act as major sources of particulate matter, thus significant implications toward climate change over the global environment.

To better understand the impact of East Asian pollutants on the molecular composition of marine organic aerosols, we conducted long-term (2001–2013) observations of water-soluble dicarboxylic acids and related compounds in total suspended particulate samples collected at Chichijima Island in the western North Pacific (WNP). Seasonal variations of all the diacids and related compounds showed maxima in winter and spring and minima in summer, except for azelaic acid (C9), which maximized in summer to autumn. The overall annual concentrations of the total diacids, ω-oxoacids and α-dicarbonyls showed an increase during 2001–2013. We found a significant (p 0.05) acids, and methylglyoxal (MeGly). In contrast, phthalic acid (p < 0.05) and glyoxal (Gly) showed a decrease in their trends. We also found a significant decrease in the trend of the Gly/MeGly mass ratios. These results demonstrate that the enhanced concentrations of diacids over the WNP are majorly attributed to the aqueous-phase photooxidation of biogenic volatile organic compounds from East Asia followed by long-range atmospheric transport. Further, positive matrix factorization analysis showed a biogenic photochemical contribution (42%) was the dominant source of oxalic acid in the WNP.