Aerosol formation during PARFORCE: Ternary nucleation of H2SO4, NH3, and H2O

Abstract

A new version of a ternary nucleation (sulphuric acid‐ammonia‐water) model based on classical nucleation theory, but with an improved ability to predict nucleation rates over a larger temperature range (258–303 K) compared with previous work, is presented. The modeled nucleation rates are given as a function of temperature and ambient acid and ammonia concentrations. For the first time the predicted ternary nucleation rates are compared to the observed particle production rates using measured ambient sulphuric acid and ammonia concentrations as input data. The ambient gas concentrations were measured simultaneously to aerosol formation rates during the 1999 New Particle Formation and Fate in the Coastal Environment (PARFORCE) coastal field campaign at Mace Head. According to the results, daytime ambient acid and ammonia concentrations were significantly higher than required by model calculations to induce the formation of new particles by homogeneous ternary nucleation. However, binary nucleation of sulphuric acid‐water molecules is not able to predict new particle formation since the binary nucleation rate is far too small. We conclude that all particle formation events observed at coastal sites can be initiated by ternary nucleation of sulphuric acid, ammonia, and water vapor. However, related studies illustrate that ambient sulphuric acid concentrations are, nevertheless, insufficient to explain observed rapid growth of particles from 1 to 3 nm sizes which can be detected by current instrumentation.