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BSTRACT Primary (i.e. sugars and sugar-alcohols) and secondary (i.e. carboxylic acids) water-soluble organic compounds (WSOCs) in size-segregated aerosols from the urban and mountain atmosphere of China and from the marine atmosphere in the outflow region of East Asia were characterized on a molecular level. Levoglucosan is the most abundant compound among the quantified WSOCs in the urban and mountain atmosphere, whose concentration at the urban site was 1-2 orders of magnitude higher than that at the mountain and marine sites. In contrast, malic, succinic and phthalic acids were dominant among the measured WSOCs at the marine site. In the urban air, sugars except levoglucosan gave a bimodal size distribution with a large peak in fine range (<2.1 μm) and a small peak in coarse range (≥2.1 μm) during winter, being opposite to those in spring. In contrast, these WSOCs at the mountain and marine sites dominated in the coarse range but diminished and even disappeared in the fine range. Geometric mean diameters (GMDs) of the measured WSOCs in the fine mode at the urban site were larger in winter than in spring. Levoglucosan and carboxylic acids except for azelaic and benzoic acids showed a larger GMD in the coarse mode at the marine site probably due to an increased hygroscopic growth. [ABSTRACT FROM AUTHOR]