Two extreme types of mixing of dust with urban aerosols observed in Kosa particles: 'After' mixing and 'on-the-way' mixing

Besides well-known episodic Kosa during spring, high concentrations of Ca²⁺ in aerosols were observed early in summer as well as in the semi-continuous data of the aerosols at the summit of Mt. Fuji. We further analysed the data to study the chemical characteristics of the high calcium event during early summer. The back trajectory analyses of the event indicated that Ca was transported from arid and semi-arid regions (e.g. the Taklamakan desert) through the westerly-dominated troposphere higher than the height of the summit of Fuji. The amount of SO₄^2- was always equivalent to that of NH₄⁺ unlike the case of the normal Kosa period where SO₄^2- is in excess with respect to NH₄⁺. This shows the 'after' mixing of unreacted CaCO₃ of Kosa origin with (NH₄)₂SO₄, which was only realized by the downward injection of Kosa particles from higher altitudes to the air masses of different origin. In the case of normal Kosa, the air bearing Kosa particles passed through the polluted area to absorb unneutralized acids ('on-the-way' mixing), whereas in the case of the Kosa-like phenomena in summer, the acids from the polluted area have been neutralized by NH₄⁺ and become inactive before mixing with CaCO₃ ("after" mixing). We have simplified the chemistry of aerosols using their three major components, Ca²⁺, SO₄^2- and NH₄⁺, and introduced a new triangle diagram with the three assumed end-members of CaCO₃, CaSO₄ and (NH₄)₂SO₄ to quantify the contribution of the 'after' mixing to the aerosols (AMI; 'after' mixing index). Based on the back trajectories of some high AMI cases, CaCO₃ in Kosa particles was transported through the middle troposphere (5000-7000 m) and descended to meet another air mass where SO₄^2- had been already neutralized by NH₃.