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Kinetics of collision-sticking processes between vapor molecules andmolecular clusters of low volatile compounds facilitates the initial steps ofatmospheric clustering. Conventional theoretical models are quite inaccuratedue to the neglection of long-range interactions that essentially govern thekinetics of these microscopic phenomena. Here, we present a consistent andgeneric theoretical model for evaluating collision rates between molecules andmolecular clusters with intermolecular potentials properly incorporated. Themodel requires solely the elementary molecule-molecule potential as a-prioriinformation but predicts collision rates of molecular clusters at arbitrarysizes, with an accuracy comparable to all-atom molecular dynamics simulationswe performed for sulfuric acid-dimethylamine clusters, a typical example ofacid-base induced clustering. The carefully devised simulations validate thetheoretical model and elucidate the kinetics of the molecularcollision-sticking process. It is found that the vibrational coupling after thecollision between a sulfuric acid molecule and a sulfuric acid cluster can beoccasionally unsuccessful, i.e., no stable bond is formed after the collision.However, introducing dimethylamine molecules to the sulfuric acid cluster cannotably increase the probability of forming stable bonds and hence stableproduct clusters. The results offer fundamental insights into the initial stepsof molecular clustering and will facilitate the development of efficientkinetic approach-based nucleation models.

Collision-sticking kinetics of acid-base clusters and its influence on atmospheric new particle formation