Aerosol samples were collected in the urban atmosphere of Beijing, China, by deploying a tethered balloon. Coarse particles (d > 1 ¿m) were individually analyzed using electron microscopes, to investigate the extent of dust modification by acidic gases in the atmosphere. Based on the elemental composition, irregularly shaped mineral dust was separated into carbonate and silicate groups. Both sulfate and nitrate were found to accumulate on carbonate more readily than silicate particles. Interestingly, spherical particles resembling Ca-carbonate in composition were spotted frequently in the samples. These Ca-rich spherical particles were more abundant under humid conditions, suggesting that they are deliquesced carbonate particles that formed in the atmosphere following the uptake of acidic gases. Sulfate and nitrate were more frequently detected in the Ca-rich spherical particles than in carbonate in the original solid form, indicating that the gas uptake efficiency of carbonate is further enhanced after the phase transition.