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Secondary organic aerosol (SOA) formation in the atmosphere is currently often modeled using a multiple lumped "two-product" (N&middot;2p) approach. The N&middot;2p approach neglects: 1) variation of activity coefficient (ζi) values and mean molecular weight MW in the particulate matter (PM) phase; 2) water uptake into the PM; and 3) the possibility of phase separation in the PM. This study considers these effects by adopting an (N&middot;2p)ζpMW,ζ approach (θ is a phase index). Specific chemical structures are assigned to 25 lumped SOA compounds and to 15 representative primary organic aerosol (POA) compounds to allow calculation of ζi and MW values. The SOA structure assignments are based on chamber-derived 2p gas/particle partition coefficient values coupled with known effects of structure on vapor pressure pL,io (atm). To facilitate adoption of the (N&middot;2p)ζpMW,θ approach in large-scale models, this study also develops CP-Wilson.1 (Chang-Pankow-Wilson.1), a group-contribution ζi-prediction method that is more computationally economical than the UNIFAC model of Fredenslund et al. (1975). Group parameter values required by CP-Wilson.1 are obtained by fitting ζi values to predictions from UNIFAC. The (N&middot;2p)ζpMW,θ approach is applied (using CP-Wilson.1) to several real α-pinene/O3 chamber cases for high reacted hydrocarbon levels (ΔHC≈400 to 1000 μg m−3) when relative humidity (RH) &asymp;50%. Good agreement between the chamber and predicted results is obtained using both the (N&middot;2p)ζpMW,θ and N&middot;2p approaches, indicating relatively small water effects under these conditions. However, for a hypothetical α-pinene/O3 case at &Delta;HC=30 μg m−3 and RH=50%, the (N&middot;2p)ζpMW,θ approach predicts that water uptake will lead to an organic PM level that is more double that predicted by the N&middot;2p approach. Adoption of the (N&middot;2p)ζpMW,θ approach using reasonable lumped structures for SOA and POA compounds is recommended for ambient PM modeling

atmospheric chemistry and physics

Organic particulate matter formation at varying relative humidity using surrogate secondary and primary organic compounds with activity corrections in the condensed phase obtained using a method based on the Wilson equation