ALBERT

Description: Ten year simulations of North American current and future air-quality were carried out using a regional air-quality model driven by a regional climate model, in turn driven by a general circulation model. Three separate summer scenarios were performed: a scenario representing the years 1997 to 2006, and two SRES A2 climate scenarios for the years 2041 to 2050. The first future climate scenario makes use of 2002 anthropogenic precursor emissions, and the second applied emissions scaling factors derived from the IPCC Representative Concentration Pathway 6 (RCP 6) scenario to estimate emissions for 2050 from existing 2020 projections. Ten-year averages of ozone and PM2.5 at North American monitoring network stations were used to evaluate the model's current chemical climatology. The model was found to have a similar performance for ozone as when driven by an operational weather forecast model. The PM2.5 predictions had larger negative biases, likely resulting from the absence of rainwater evaporation, and from sub-regional negative biases in the surface temperature fields, in the version of the climate model used here. The differences between the two future climate simulations and the current climate simulation were used to predict the changes to air-quality that might be expected in a future warmer climate, if anthropogenic precursor emissions remain constant at their current levels, versus if the RCP 6 emissions controls were adopted. Metrics of concentration, human health, and ecosystem damage were compared for the simulations. The scenario with future climate and current anthropogenic emissions resulted in worse air-quality than for current conditions – that is, the effect of climate-change alone, all other factors being similar, would be a worsening of air-quality. These effects are spatially inhomogeneous, with the magnitude and sign of the changes varying with region. The scenario with future climate and RCP 6 emissions for 2050 resulted in an improved air-quality, with decreases in key pollutant concentrations, in acute human mortality associated with air-pollution, and in sulphur and ozone deposition to the ecosystem. The positive outcomes of the RCP 6 emissions reductions were found to be of greater magnitude than the negative outcomes of climate change alone. The RCP 6 scenario however resulted in an increase in the deposition of nitrogen, as a result of increased ammonia emissions expected in that scenario, compared to current ammonia emissions levels. The results of the study raise the possibility that simultaneous reductions of greenhouse gases and air pollution precursors may further reduce air pollution levels, with the added benefits of an immediate reduction in the impacts of air pollution on human and ecosystem health. Further scenarios to investigate this possibility are therefore recommended.

Description: Co-located measurements of fine particulate matter (PM2.5) organic carbon, elemental carbon, radiocarbon (14C), speciated volatile organic compounds (VOCs), and OH radical during the CalNex field campaign provide a unique opportunity to evaluate the Community Multiscale Air Quality (CMAQ) model's representation of organic species from VOCs to particles. Episode averaged daily 23 h average 14C analysis indicate PM2.5 carbon at Pasadena and Bakersfield during the CalNex field campaign was evenly split between contemporary and fossil origin. CMAQ predicts a higher contemporary carbon fraction than indicated by the 14C analysis at both locations. The model underestimates measured PM2.5 organic carbon at both sites with very little (7% in Pasadena) of the modeled mass represented by secondary production, which contrasts with the ambient based SOC/OC fraction of 63% at Pasadena. Measurements and predictions of gas-phase anthropogenic species, such as toluene and xylenes, are generally within a factor of 2, but the corresponding secondary organic carbon (SOC) tracer (2,3-dihydroxy-4-oxo-pentanioc acid) is systematically underpredicted by more than a factor of 2. Monoterpene VOCs and SOCs are underestimated at both sites. Isoprene is underestimated at Pasadena and over predicted at Bakersfield and isoprene SOC mass is underestimated at both sites. Systematic model underestimates in SOC mass coupled with reasonable skill (typically within a factor of 2) in predicting hydroxyl radical and VOC gas phase precursors suggests error(s) in the parameterization of semi-volatile gases to form SOC. Yield values (α) applied to semi-volatile partitioning species were increased by a factor of 4 in CMAQ for a sensitivity simulation, taking in account recent findings of underestimated yields in chamber experiments due to gas wall losses. This sensitivity resulted in improved model performance for PM2.5 organic carbon at both field study locations and at routine monitoring network sites in California. Modeled percent secondary contribution (22% at Pasadena) becomes closer to ambient based estimates but is still too primary compared with ambient estimates at the CalNex sites.

Description: Ten year simulations of North American current and future air-quality were carried out using a regional air-quality model driven by a regional climate model, in turn driven by a general circulation model. Three separate summer scenarios were performed: a scenario representing the years 1997 to 2006, and two SRES A2 climate scenarios for the years 2041 to 2050. The first future climate scenario makes use of 2002 anthropogenic precursor emissions, and the second applied emissions scaling factors derived from the IPCC Representative Concentration Pathway 6 (RCP 6) scenario to estimate emissions for 2050 from existing 2020 projections. Ten-year averages of ozone and PM2.5 at North American monitoring network stations were used to evaluate the model's current chemical climatology. The model was found to have a similar performance for ozone as when driven by an operational weather forecast model. The PM2.5 predictions had larger negative biases, likely resulting from the absence of rainwater evaporation, and from sub-regional negative biases in the surface temperature fields, in the version of the climate model used here. The differences between the two future climate simulations and the current climate simulation were used to predict the changes to air-quality that might be expected in a future warmer climate, if anthropogenic precursor emissions remain constant at their current levels, versus if the RCP 6 emissions controls were adopted. Metrics of concentration, human health, and ecosystem damage were compared for the simulations. The scenario with future climate and current anthropogenic emissions resulted in worse air-quality than for current conditions – that is, the effect of climate-change alone, all other factors being similar, would be a worsening of air-quality. These effects are spatially inhomogeneous, with the magnitude and sign of the changes varying with region. The scenario with future climate and RCP 6 emissions for 2050 resulted in an improved air-quality, with decreases in key pollutant concentrations, in acute human mortality associated with air-pollution, and in sulphur and ozone deposition to the ecosystem. The positive outcomes of the RCP 6 emissions reductions were found to be of greater magnitude than the negative outcomes of climate change alone. The RCP 6 scenario however resulted in an increase in the deposition of nitrogen, as a result of increased ammonia emissions expected in that scenario, compared to current ammonia emissions levels. The results of the study raise the possibility that simultaneous reductions of greenhouse gases and air pollution precursors may further reduce air pollution levels, with the added benefits of an immediate reduction in the impacts of air pollution on human and ecosystem health. Further scenarios to investigate this possibility are therefore recommended.

Description: 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−, SO42−, NH4+, Na+, and Cl− 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 (http://www.cmaq-model.org).

Description: This work evaluates particle size-composition distributions simulated by the Community Multiscale Air Quality (CMAQ) model using Micro-Orifice Uniform Deposit Impactor (MOUDI) measurements at 18 sites across North America. Size-resolved measurements of particulate SO42−, NO3−, NH4+, Na+, Cl−, Mg2+, Ca2+ and K+ are compared to CMAQ model output for discrete sampling periods between 2002 and 2005. The observation sites were predominantly in remote areas (e.g. National Parks) in the United States and Canada, and measurements were typically made for a period of roughly one month. For SO42− and NH4+, model performance was consistent across the US and Canadian sites, with the model slightly overestimating the peak particle diameter and underestimating the peak particle concentration compared to the observations. Na+ and Mg2+ size distributions were generally well represented at coastal sites, indicating reasonable simulation of emissions from sea spray. CMAQ is able to simulate the displacement of Cl− in aged sea spray aerosol, though the extent of Cl− depletion relative to Na+ is often underpredicted. The model performance for NO3− exhibited much more site-to-site variability than that of SO42− and NH4+, with the model ranging from an underestimation to overestimation of both the peak diameter and peak particle concentration across the sites. Computing PM2.5 from the modeled size distribution parameters rather than by summing the masses in the Aitken and accumulation modes resulted in differences in daily averages of up to 1 μg m−3 (10%), while the difference in seasonal and annual model performance compared to observations from the IMPROVE, CSN and AQS networks was very small. Two updates to the CMAQ aerosol model – changes to the assumed size and mode width of emitted particles and the implementation of gravitational settling – resulted in small improvements in modeled size distributions.

Description: Sea spray aerosols (SSA) impact the particle mass concentration and gas-particle partitioning in coastal environments, with implications for human and ecosystem health. Despite their importance, the emission magnitude of SSA remains highly uncertain with global estimates varying by nearly two orders of magnitude. In this study, the Community Multiscale Air Quality (CMAQ) model was updated to enhance fine mode SSA emissions, include sea surface temperature (SST) dependency, and reduce coastally-enhanced emissions. Predictions from the updated CMAQ model and those of the previous release version, CMAQv5.0.2, were evaluated using several regional and national observational datasets in the continental US. The updated emissions generally reduced model underestimates of sodium, chloride, and nitrate surface concentrations for an inland site of the Bay Regional Atmospheric Chemistry Experiment (BRACE) near Tampa, Florida. Including SST-dependency to the SSA emission parameterization led to increased sodium concentrations in the southeast US and decreased concentrations along parts of the Pacific coast and northeastern US. The influence of sodium on the gas-particle partitioning of nitrate resulted in higher nitrate particle concentrations in many coastal urban areas due to increased condensation of nitric acid in the updated simulations, potentially affecting the predicted nitrogen deposition in sensitive ecosystems. Application of the updated SSA emissions to the California Research at the Nexus of Air Quality and Climate Change (CalNex) study period resulted in modest improvement in the predicted surface concentration of sodium and nitrate at several central and southern California coastal sites. This SSA emission update enabled a more realistic simulation of the atmospheric chemistry in environments where marine air mixes with urban pollution.

Description: 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 N2O5 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 (PM2.5) is dominated by overpredictions of unspeciated PM2.5 (PMother) in the winter and by underpredictions of carbon in the summer. The CMAQ v4.7 model results show slightly worse performance for ozone predictions. 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.

Description: This work evaluates particle size–composition distributions simulated by the Community Multiscale Air Quality (CMAQ) model using micro-orifice uniform deposit impactor (MOUDI) measurements at 18 sites across North America. Size-resolved measurements of particulate SO42−, NO3−, NH4+, Na+, Cl−, Mg2+, Ca2+, and K+ are compared to CMAQ model output for discrete sampling periods between 2002 and 2005. The observation sites were predominantly in remote areas (e.g., National Parks) in the USA and Canada, and measurements were typically made for a period of roughly 1 month. For SO42− and NH4+, model performance was consistent across the USA and Canadian sites, with the model slightly overestimating the peak particle diameter and underestimating the peak particle concentration compared to the observations. Na+ and Mg2+ size distributions were generally well represented at coastal sites, indicating reasonable simulation of emissions from sea spray. CMAQ is able to simulate the displacement of Cl− in aged sea spray aerosol, though the extent of Cl− depletion relative to Na+ is often underpredicted. The model performance for NO3− exhibited much more site-to-site variability than that of SO42− and NH4+, with the model ranging from an underestimation to overestimation of both the peak diameter and peak particle concentration across the sites. Computing PM2.5 from the modeled size distribution parameters rather than by summing the masses in the Aitken and accumulation modes resulted in differences in daily averages of up to 1 μg m−3 (10 %), while the difference in seasonal and annual model performance compared to observations from the Interagency Monitoring of Protected Visual Environments (IMPROVE), Chemical Speciation Network (CSN), and Air Quality System (AQS) networks was very small. Two updates to the CMAQ aerosol model – changes to the assumed size and mode width of emitted particles and the implementation of gravitational settling – resulted in small improvements in modeled size distributions.

Description: 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−, SO42−, NH4+, Na+, and Cl− 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 (http://www.cmaq-model.org).

Description: Sea spray aerosols (SSAs) impact the particle mass concentration and gas-particle partitioning in coastal environments, with implications for human and ecosystem health. Model evaluations of SSA emissions have mainly focused on the global scale, but regional-scale evaluations are also important due to the localized impact of SSAs on atmospheric chemistry near the coast. In this study, SSA emissions in the Community Multiscale Air Quality (CMAQ) model were updated to enhance the fine-mode size distribution, include sea surface temperature (SST) dependency, and reduce surf-enhanced emissions. Predictions from the updated CMAQ model and those of the previous release version, CMAQv5.0.2, were evaluated using several coastal and national observational data sets in the continental US. The updated emissions generally reduced model underestimates of sodium, chloride, and nitrate surface concentrations for coastal sites in the Bay Regional Atmospheric Chemistry Experiment (BRACE) near Tampa, Florida. Including SST dependency to the SSA emission parameterization led to increased sodium concentrations in the southeastern US and decreased concentrations along parts of the Pacific coast and northeastern US. The influence of sodium on the gas-particle partitioning of nitrate resulted in higher nitrate particle concentrations in many coastal urban areas due to increased condensation of nitric acid in the updated simulations, potentially affecting the predicted nitrogen deposition in sensitive ecosystems. Application of the updated SSA emissions to the California Research at the Nexus of Air Quality and Climate Change (CalNex) study period resulted in a modest improvement in the predicted surface concentration of sodium and nitrate at several central and southern California coastal sites. This update of SSA emissions enabled a more realistic simulation of the atmospheric chemistry in coastal environments where marine air mixes with urban pollution.