Abstract. This paper describes the scientific and structural updates to the latest release of the Community Multiscale Air Quality (CMAQ) modeling system version 4.7 (v4.7) and points the reader to additional resources for further details. The model updates were evaluated relative to observations and results from previous model versions in a series of simulations conducted to incrementally assess the effect of each change. The focus of this paper is on five major scientific upgrades: (a) updates to the heterogeneous N 2 O 5 parameterization, (b) improvement in the treatment of secondary organic aerosol (SOA), (c) inclusion of dynamic mass transfer for coarse-mode aerosol, (d) revisions to the cloud model, and (e) new options for the calculation of photolysis rates. Incremental test simulations over the eastern United States during January and August 2006 are evaluated to assess the model response to each scientific improvement, providing explanations of differences in results between v4.7 and previously released CMAQ model versions. Particulate sulfate predictions are improved across all monitoring networks during both seasons due to cloud module updates. Numerous updates to the SOA module improve the simulation of seasonal variability and decrease the bias in organic carbon predictions at urban sites in the winter. Bias in the total mass of fine particulate matter (PM 2.5 ) is dominated by overpredictions of unspeciated PM 2.5 (PM other ) in the winter and by underpredictions of carbon in the summer. The CMAQv4.7 model results show slightly worse performance for ozone predictions.Correspondence to: K. M. Foley (foley.kristen@epa.gov) However, changes to the meteorological inputs are found to have a much greater impact on ozone predictions compared to changes to the CMAQ modules described here. Model updates had little effect on existing biases in wet deposition predictions.

The Community Multiscale Air Quality (CMAQ) model is a comprehensive multipollutant air quality modeling system developed and maintained by the US Environmental Protection Agency’s (EPA) Office of Research and Development (ORD). Recently, version 5.1 of the CMAQ model (v5.1) was released to the public, incorporating a large number of science updates and extended capabilities over the previous release version of the model (v5.0.2). These updates include the following: improvements in the meteorological calculations in both CMAQ and the Weather Research and Forecast (WRF) model used to provide meteorological fields to CMAQ, updates to the gas and aerosol chemistry, revisions to the calculations of clouds and photolysis, and improvements to the dry and wet deposition in the model. Sensitivity simulations isolating several of the major updates to the modeling system show that changes to the meteorological calculations result in enhanced afternoon and early evening mixing in the model, periods when the model historically underestimates mixing. This enhanced mixing results in higher ozone (O3) mixing ratios on average due to reduced NO titration, and lower fine particulate matter (PM2.5) concentrations due to greater dilution of primary pollutants (e.g., elemental and organic carbon). Updates to the clouds and photolysis calculations greatly improve consistency between the WRF and CMAQ models and result in generally higher O3 mixing ratios, primarily due to reduced cloudiness and attenuation of photolysis in the model. Updates to the aerosol chemistry result in higher secondary organic aerosol (SOA) concentrations in the summer, thereby reducing summertime PM2.5 bias (PM2.5 is typically underestimated by CMAQ in the summer), while updates to the gas chemistry result in slightly higher O3 and PM2.5 on average in January and July. Overall, the seasonal variation in simulated PM2.5 generally improves in CMAQv5.1 (when considering all model updates), as simulated PM2.5 concentrations decrease in the winter (when PM2.5 is generally overestimated by CMAQ) and increase in the summer (when PM2.5 is generally underestimated by CMAQ). Ozone mixing ratios are higher on average with v5.1 vs. v5.0.2, resulting in higher O3 mean bias, as O3 tends to be overestimated by CMAQ throughout most of the year (especially at locations where the observed O3 is low); however, O3 correlation is largely improved with v5.1. Sensitivity simulations for several hypothetical emission reduction scenarios show that v5.1 tends to be slightly more responsive to reductions in NOx (NO + NO2), VOC and SOx (SO2 + SO4) emissions than v5.0.2, representing an improvement as previous studies have shown CMAQ to underestimate the observed reduction in O3 due to large, widespread reductions in observed emissions.

Abstract.A parameterization was developed for the heterogeneous reaction probability (γ ) of N 2 O 5 as a function of temperature, relative humidity (RH), particle composition, and phase state, for use in advanced air quality models. The reaction probabilities on aqueous NH 4 HSO 4 , (NH 4 ) 2 SO 4 , and NH 4 NO 3 were modeled statistically using data and uncertainty values compiled from seven different laboratory studies. A separate regression model was fit to laboratory data for dry NH 4 HSO 4 and (NH 4 ) 2 SO 4 particles, yielding lower γ values than the corresponding aqueous parameterizations. The regression equations reproduced 80% of the laboratory data within a factor of two and 63% within a factor of 1.5. A fixed value was selected for γ on icecontaining particles based on a review of the literature. The combined parameterization was applied under atmospheric conditions representative of the eastern United States using 3-dimensional fields of temperature, RH, sulfate, nitrate, and ammonium. The resulting spatial distributions of γ were contrasted with three other parameterizations that have been applied in air quality models in the past and with atmospheric observational determinations of γ . Our equations lay the foundation for future research that will parameterize the suppression of γ when inorganic ammoniated particles are mixed or coated with organic material. Our analyses draw attention to a major uncertainty in the available laboratory data at high RH and highlight a critical need for future laboratory measurements of γ at low temperature and high RH to improve model simulations of N 2 O 5 hydrolysis during wintertime conditions.

Chemical processing of sea-salt particles in coastal environments significantly impacts concentrations of particle components and gas-phase species and has implications for human exposure to particulate matter and nitrogen deposition to sensitive ecosystems. Emission of sea-salt particles from the coastal surf zone is known to be elevated compared to that from the open ocean. Despite the importance of sea-salt emissions and chemical processing, the US EPA's Community Multiscale Air Quality (CMAQ) model has traditionally treated coarse sea-salt particles as chemically inert and has not accounted for enhanced surf-zone emissions. In this article, updates to CMAQ are described that enhance sea-salt emissions from the coastal surf zone and allow dynamic transfer of HNO₃, H₂SO₄, HCl, and NH₃ between coarse particles and the gas phase. Predictions of updated CMAQ models and the previous release version, CMAQv4.6, are evaluated using observations from three coastal sites during the Bay Regional Atmospheric Chemistry Experiment (BRACE) in Tampa, FL in May 2002. Model updates improve predictions of NO₃^&minus;, SO₄^2&minus;, NH₄⁺, Na⁺, and Cl^&minus; concentrations at these sites with only a 8% increase in run time. In particular, the chemically interactive coarse particle mode dramatically improves predictions of nitrate concentration and size distributions as well as the fraction of total nitrate in the particle phase. Also, the surf-zone emission parameterization improves predictions of total sodium and chloride concentration. Results of a separate study indicate that the model updates reduce the mean absolute error of nitrate predictions at coastal CASTNET and SEARCH sites in the eastern US. Although the new model features improve performance relative to CMAQv4.6, some persistent differences exist between observations and predictions. Modeled sodium concentration is biased low and causes under-prediction of coarse particle nitrate. Also, CMAQ over-predicts geometric mean diameter and standard deviation of particle modes at the BRACE sites. These over-predictions may cause too rapid particle dry deposition and partially explain the low bias in sodium predictions. Despite these shortcomings, the updates to CMAQ enable more realistic simulations of chemical processes in environments where marine air mixes with urban pollution. The model updates described in this article are included in the public release of CMAQv4.7 (<a href="http://www.cmaq-model.org" target="_blank">http://www.cmaq-model.org</a>)

Abstract. This paper examines the operational performance of the Community Multiscale Air Quality (CMAQ) model simulations for 2002-2006 using both 36-km and 12-km horizontal grid spacing, with a primary focus on the performance of the CMAQ model in predicting wet deposition of sulfate (SO = 4 ), ammonium (NH + 4 ) and nitrate (NO − 3 ). Performance of the wet deposition estimates from the model is determined by comparing CMAQ predicted concentrations to concentrations measured by the National Acid Deposition Program (NADP), specifically the National Trends Network (NTN). For SO = 4 wet deposition, the CMAQ model estimates were generally comparable between the 36-km and 12-km simulations for the eastern US, with the 12-km simulation giving slightly higher estimates of SO = 4 wet deposition than the 36-km simulation on average. The result is a slightly larger normalized mean bias (NMB) for the 12-km simulation; however both simulations had annual biases that were less than ±15 % for each of the five years. The model estimated SO = 4 wet deposition values improved when they were adjusted to account for biases in the model estimated precipitation. The CMAQ model underestimates NH wet deposition tend to be slightly lower for the 36-km simulation as compared to the 12-km simulation, particularly in the spring. The underestimation of NO − 3 wet deposition in the spring and summer is due in part to a lack of lightning generated NO emissions in the upper troposphere, which can be a large source of NO in the spring and summer when lightning activity is the high. CMAQ model simulations that include production of NO from lightning show a significant improvement in the NO − 3 wet deposition estimates in the eastern US in the summer. Overall, performance for the 36-km and 12-km CMAQ model simulations is similar for the eastern US, while for the western US the performance of the 36-km simulation is generally not as good as either eastern US simulation, which is not entire unexpected given the complex topography in the western US.