Abstract
Classical theory of binary homogeneous nucleation is extended to the ternary system H2SO4‐NH3‐H2O. For NH3 mixing ratios exceeding about 1 ppt, the presence of NH3 enhances the binary H2SO4‐H2O nucleation rate by several orders of magnitude. The Gibbs free energies of formation of the critical H2SO4‐NH3‐H2O cluster, as calculated by two independent approaches, are in substantial agreement. The finding that the H2SO4‐NH3‐H2O ternary nucleation rate is independent of relative humidity over a large range of H2SO4 concentrations has wide atmospheric consequences. The limiting component for ternary H2SO4‐NH3‐H2O nucleation is, as in the binary H2SO4‐H2O case, H2SO4; however, the H2SO4 concentration needed to achieve significant nucleation rates is several orders of magnitude below that required in the binary case.
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