Seasonality of speciated aerosol transport over the Great Lakes region

[1] The Community Multiscale Air Quality model (CMAQ) is used to simulate aerosol mass and composition in the Great Lakes region of North America in an annual study for 2002. Model predictions are evaluated against daily and weekly average speciated fine particle (PM2.5) and bulk (PM2.5 and PM10) mass concentration measurements taken throughout the region by the Interagency Monitoring of Protected Visual Environments (IMPROVE), Speciation Trends Network (STN), and Clean Air Status and Trends Network (CASTNet) monitoring networks, and number concentration is evaluated using hourly observations at a rural site. Through detailed evaluation of model-measurement agreement over urban and remote areas, major features of aerosol seasonality are examined. Whereas nitrate (winter maximum) and sulfate (summer maximum) seasonal patterns are driven by climatic influence on aerosol thermodynamics, seasonality of ammonium and organic mass (OM) is driven by emissions. Production of anthropogenic secondary organic aerosol (SOA) and summertime ozone formation both reach regional maxima over the southern Great Lakes, where they are also most strongly temporally correlated. Although primary OM is more prevalent, insufficient SOA formation leads to summertime OM underprediction of more than 50%. By comparing temporal patterns in aerosol species between model and observations, we find that elemental carbon, OM, and PM2.5 are overly correlated in CMAQ, suggesting that the model misses chemical, transport, or emissions processes differentiating these constituents. In contrast, sulfate and PM2.5 are not sufficiently correlated in CMAQ, although CMAQ simulates sulfate with a high level of skill. Performance relative to ad hoc regional modeling goals and previous studies is average to excellent for most species throughout the year, and seasonal patterns are captured.