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A new model of secondary organic aerosol (SOA) formation is developed thatexplicitly takes into account multi-generational oxidation as well asfragmentation of gas-phase compounds, and assumes equilibrium gas-particlepartitioning. The model framework requires specification of a limited numberof tunable parameters to describe the kinetic evolution of SOA mass, theaverage oxygen-to-carbon atomic ratio and the mean particle volatility asoxidation proceeds. These parameters describe (1) the relationship betweenoxygen content and volatility, (2) the probability of fragmentation and (3)the amount of oxygen added per reaction. The time-evolution and absolutevalue of the simulated SOA mass depends sensitively on all tunableparameters. Of the tunable parameters, the mean O : C is most sensitive to theoxygen/volatility relationship, exhibiting only a weak dependence on theother relationships. The model mean particle O : C produced from a givencompound is primarily controlled by the number of carbon atoms comprisingthe SOA precursor, with some sensitivity to the specified oxygen/volatilityrelationship. The model is tested against laboratory measurements oftime-dependent SOA formation from the photooxidation of α-pinene and<i>n</i>-pentadecane and performs well (after tuning). The model can also accuratelysimulate the carbon-number dependence of aerosol yields previously observedfor oxidation of straight-chain alkanes. This model may provide ageneralized framework for the interpretation of laboratory SOA formationexperiments in which explicit consideration of multiple-generations ofproducts is required, which is true for all photo-oxidation experiments

Multi-generation gas-phase oxidation, equilibrium partitioning, and the formation and evolution of secondary organic aerosol