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. New particle formation (NPF) is known to be an important sourceof atmospheric particles that impacts air quality, hydrological cycle, andclimate. Although laboratory measurements indicate that ammonia enhances NPF,the physicochemical processes underlying the observed effect of ammonia onNPF are yet to be understood. Here we present a comprehensivekinetically based H2 SO4 – H2O – NH3 ternary ion-mediated nucleation (TIMN) model that is based on thethermodynamic data derived from both quantum-chemical calculations andlaboratory measurements. NH3 was found to reduce nucleationbarriers for neutral, positively charged, and negatively charged clustersdifferently, due to large differences in the binding strength of NH3 , H2O , and H2 SO4 to small clusters ofdifferent charging states. The model reveals the general favor of nucleationof negative ions, followed by nucleation on positive ions and neutralnucleation, for which higher NH3 concentrations are needed, inexcellent agreement with Cosmics Leaving OUtdoor Droplets (CLOUD)measurements. The TIMN model explicitly resolves dependences of nucleationrates on all the key controlling parameters and captures the absolutevalues of nucleation rates as well as the dependence of TIMN rates onconcentrations of NH3 and H2 SO4 , ionizationrates, temperature, and relative humidity observed in the well-controlledCLOUD measurements well. The kinetic model offers physicochemical insights intothe ternary nucleation process and provides a physics-based approach tocalculate TIMN rates under a wide range of atmospheric conditions.

atmospheric chemistry and physics

H&amp;lt;sub&amp;gt;2&amp;lt;/sub&amp;gt;SO&amp;lt;sub&amp;gt;4&amp;lt;/sub&amp;gt;–H&amp;lt;sub&amp;gt;2&amp;lt;/sub&amp;gt;O–NH&amp;lt;sub&amp;gt;3&amp;lt;/sub&amp;gt; ternary ion-mediated nucleation (TIMN): kinetic-based model and comparison with CLOUD measurements