Atmospheric aerosol particulate matter was directly collected in the free troposphere over the Japan Sea coast between 1992 and 1993 using an aircraft-borne nine-stage cascade impactor (particle size range: 0.1-8 mu m). The water-soluble components in the aerosol particulate matter were analyzed by ion chromatography. Particulate sulfate and ammonium were detected in most of the samples and their size distributions showed noticeable peaks below the 1 mu m particle size range. Water-soluble calcium (Ca(2+)) was detected in half of the samples; the size distribution showed that the maximum particle size was larger than 1 mu m. Highly concentrated Ca(2+) in larger particles was possibly due to transport of Kosa aerosols from the Asian continent in the free troposphere. The concentration of fine particulate sulfate and ammonium tended to increase whenever Ca(2+) was detected, which suggests possible mixing of Kosa aerosols and non-Kosa aerosols during long-range transport of air masses containing Kosa particles. (C) 1999 Elsevier Science Ltd. All rights reserved.