Abstract
ABSTRACT The effects of two gas-phase chemical kinetic mechanisms, Regional Atmospheric Chemistry Mechanism version 2 (RACM2) and Carbon-Bond 05 (CB05), and two secondary organic aerosol (SOA) modules, the Secondary Organic Aerosoi Model (SORGAM) and AER/EPRI/Caltech model (AEC), on fine (aerodynamic diameter ≤2.5 μm) particulate matter (PM2.5) formation is studied. The major sources of uncertainty in the chemistry of SOA formation are investigated. The use of all major SOA precursors and the treatment of SOA oligomerization are found to be the most important factors for SOA formation, leading to 66% and 60% more SOA, respectively. The explicit representation of high-NOx and low-NOx gas-phase chemical regimes is also important with increases in SOA of 30–120% depending on the approach used to implement the distinct SOA yields within the gas-phase chemical kinetic mechanism; further work is needed to develop gas-phase mechanisms that are fully compatible with SOA formation algorithms. The treatment of isoprene SOA as hydrophobic or hydrophilic leads to a significant difference, with more SOA being formed in the latter case. The activity coefficients may also be a major source of uncertainty, as they may differ significantly between atmospheric particles, which contain a myriad of SOA, primary organic aerosol (POA), and inorganic aerosol species, and particles formed in a smog chamber from a single precursor under dry conditions. Significant interactions exist between the uncertainties of the gas-phase chemistry and those of the SOA module. IMPLICATIONS The current state of the science is more advanced for the gas-phase chemistry of ozone formation than for the chemistry and gas/particle partitioning of particulate matter (PM) formation. As a result, there are larger uncertainties associated with aerosol modules than with gas-phase chemical kinetic mechanisms. Nevertheless, the uncertainties associated with those modules are not additive in an air quality model and there are close interactions between the gas-phase chemical mechanism and the secondary aerosol formation. In particular, the effect of the NOx regime on SOA formation should be explicitly treated in air quality models.
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