Development and application of the model of aerosol dynamics, reaction, ionization, and dissolution (MADRID)

[1] A new aerosol model, the Model of Aerosol Dynamics, Reaction, Ionization, and Dissolution ( MADRID) has been developed to simulate atmospheric particulate matter (PM). MADRID and the Carnegie-Mellon University (CMU) bulk aqueous-phase chemistry have been incorporated into the three-dimensional Models-3/Community Multiscale Air Quality model (CMAQ). The resulting model, CMAQ-MADRID, is applied to simulate the August 1987 episode in the Los Angeles basin. Model performance for ozone and PM is consistent with current performance standards. However, organic aerosol was underpredicted at most sites owing to underestimation of primary organic PM emissions and secondary organic aerosol (SOA) formation. Nitrate concentrations were also sometimes underpredicted, mainly owing to overpredictions in vertical mixing, underpredictions in relative humidity, and uncertainties in the emissions of primary pollutants. Including heterogeneous reactions changed hourly O-3 by up to 17% and 24-hour average PM2.5, sulfate(2.5), and nitrate(2.5) concentrations by up to 3, 7, and 19%, respectively. A SOA module with a mechanistic representation provides results that are more consistent with observations than that with an empirical representation. The moving-center scheme for particle growth predicts more accurate size distributions than a typical semi-Lagrangian scheme, which causes an upstream numerical diffusion. A hybrid approach that simulates dynamic mass transfer for coarse PM but assumes equilibrium for fine PM can predict a realistic particle size distribution under most conditions, and the same applies under conditions with insignificant concentrations of reactive coarse particles to a bulk equilibrium approach that allocates transferred mass to different size sections based on condensational growth law. In contrast, a simple bulk equilibrium approach that allocates transferred mass based on a given distribution tends to cause a downstream numerical diffusion in the predicted particle size distribution.