A ternary nucleation model for the H2SO4-NH3-H20 system is presented in an effort to examine the effect of NH 3 on heteromolecular homogeneous nucleation in the marine boundary layer (MBL). The results from this nucleation model suggest that ammonia could, in fact, enhance the nucleation rate over that of the binary system, H2SO4-H20. The magnitude of this enhancement is introduced as an enhancement ratio, which, in principle, is applicable to any binary nucleation rate for H2SO4-H20. Also presented are preliminary results from a simple aerosol model using this enhancement ratio. These results suggest that under conditions typical of the marine environment it may be possible to produce enough particles to balance the various particle sinks characteristic of the MBL.
Introduction
It has long been maintained that in situ homogeneousnucleation is an important source of particles in the atmosphere [cf. Kiang et al., 1975]. In describing the aerosol population of the marine boundary layer (MBL), such nucleation has often been parameterized in terms of a binary nucleation process involving H2SO 4 and H20 [Lin et al., 1992; Hegg et al., 1992; Raes and Van Dingenen, 1991]. However, nucleation rates calculated utilizing binary nucleation theory for average MBL conditions have yielded negligible particle production. While atypical conditions have yielded quite significant nucleation, it has been both spatially and temporally variable. It is by no means clear that this production, when averaged over the MBL, is sufficient to offset the various particle sinks. Certainly, such episodic, intense nucleation has been rarely observed. Furthermore, an issue has arisen in that it is similarly unclear that the newly created particles, given the calculated nucleation rates, have a sufficiently long lifetime to grow to such a size that they can become cloud condensation nuclei (CCN). Indeed, a number of recent studies have dealt with possible ways of reconciling calculated nucleation rates with the CCN budget [Lin et al., 1992; Hegg, 1990; Raes and Van Dingenen, 1992; Hoppel et al., 1990]. Considering the possible linkage of the CCN number population to global climate [Charlson et al., 1987], the issue of the proper nucleation theory to use in modeling the MBL aerosol may be of considerable importance.One process which could possibly reconcile particle nucleation rates, growth rates, and particle lifetimes and possibly eliminate the need for intense, episodic nucleation is that of ternary as opposed to binary nucleation. For example, several studies have been conducted in recent years to predict the nucleation rates in the ternary system, H20-H2SO4-methane sulfonic acid [e.g., Kreidenweis and Seinfeld, 1988; Van Dingenen and Raes, 1993]. However, while these assessments have suggested an impact of the third component (i.e., methane sulfonic acid (MSA)) on particle growth, no significant impact on the nucleation rate has been established. Another atmospheric gas with great potential for impact on nucleation rates, especially for the H2...