Aerosol size distribution modeling with the Community Multiscale Air Quality modeling system in the Pacific Northwest: 2. Parameterizations for ternary nucleation and nucleation mode processes

In order to test Community Multiscale Air Quality (CMAQ) model performance for ultrafine particle concentrations in the Pacific Northwest, CMAQ v4.4 was modified for ternary NH3-H2SO4-H2O nucleation and for atmospheric processing of ultrafine particles. Sulfuric acid from sulfur dioxide oxidation is iteratively partitioned into gaseous sulfuric acid, newly condensed aerosol sulfate, and aerosol sulfuric acid contained in new 1 nm particles. Freshly nucleated particles are either coagulated to larger particles or grown by sulfuric acid condensation to 10 nm at which point they are included in CMAQ's existing Aitken mode. Multiple nucleation parameterizations were implemented into CMAQ, and one other was investigated in a sensitivity analysis. For a case study in the Pacific Northwest where aerosol number concentration and size distributions were measured, standard binary nucleation in CMAQ produces nearly no particles for this case study. Ternary nucleation can produce millions of 1 nm particles per cm 3, but few of these particles survive coagulation loss and grow to 10 nm and into the Aitken mode. There are occasions when the additions to CMAQ increase the number of particles to within an order of magnitude of observations, but it is more common for number concentrations to remain underpredicted by, on average, one order of magnitude. Significant particle nucleation in CMAQ successfully produces a distinct Aitken and accumulation mode and an Aitken mode that is more prominent than the accumulation mode, although errors in the size distribution remain. A more recent ternary nucleation scheme including ammonium bisulfate clusters does not nucleate an appreciable number of particles.