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This paper describes and evaluates a new framework for modeling kineticgas-particle partitioning of secondary organic aerosol (SOA) that takes intoaccount diffusion and chemical reaction within the particle phase. Theframework uses a combination of  (a) an analytical quasi-steady-statetreatment for the diffusion–reaction process within the particle phase forfast-reacting organic solutes, and (b) a two-film theory approach for slow-and nonreacting solutes. The framework is amenable for use in regional andglobal atmospheric models, although it currently awaits specification of thevarious gas- and particle-phase chemistries and the related physicochemicalproperties that are important for SOA formation. Here, the new framework isimplemented in the computationally efficient Model for Simulating AerosolInteractions and Chemistry (MOSAIC) to investigate the competitive growthdynamics of the Aitken and accumulation mode particles. Results show thatthe timescale of SOA partitioning and the associated size distributiondynamics depend on the complex interplay between organic solute volatility,particle-phase bulk diffusivity, and particle-phase reactivity (asexemplified by a pseudo-first-order reaction rate constant), each of whichcan vary over several orders of magnitude. In general, the timescale of SOApartitioning increases with increase in volatility and decrease in bulkdiffusivity and rate constant. At the same time, the shape of the aerosolsize distribution displays appreciable narrowing with decrease in volatilityand bulk diffusivity and increase in rate constant. A proper representationof these physicochemical processes and parameters is needed in the nextgeneration models to reliably predict not only the total SOA mass, but alsoits composition- and number-diameter distributions, all of which togetherdetermine the overall optical and cloud-nucleating properties

atmospheric chemistry and physics

Modeling kinetic partitioning of secondary organic aerosol and size distribution dynamics: representing effects of volatility, phase state, and particle-phase reaction