Ozone sensitivity to high energy demand day electricity and onroad emissions during LISTOS.

Using a high-resolution, 1.33 km by 1.33 km coupled Weather Research and Forecasting-Community Multi-scale Air Quality Model (WRF-CMAQ), we quantify the impact of emissions of nitrogen oxides (NOx) from high energy demand day (HEDD) electricity generating units (EGU) and onroad vehicles on ambient ozone air quality in the Long Island Sound Tropospheric Ozone Study (LISTOS) region covering New York City (NYC); Long Island, NY; coastal Connecticut; and neighboring areas. We test sensitivity scenarios to quantify HEDD EGU NOx contributions to ozone: (1) zero out HEDD EGU emissions, (2) dispatch HEDD EGUs starting with the lowest NOx emitting units first, (3) reduce onroad emissions by 90%, (4) combine zero out HEDD EGU emissions and reducing onroad emissions by 90%, and (5) dispatch HEDD EGUs starting with the lowest emitting units coupled with a reduction in onroad emissions by 90%. Results determine that HEDD EGUs lead to highly localized impacts on ambient concentrations of ozone while onroad emission reductions lead to large-scale regional concentration impacts. Further, reducing onroad emissions by 90% leads to spatially smaller VOC-limited regions and spatially larger transitional and NOX-limited regions around NYC. Despite the limited scale at which the EGU emission reductions occur, modifying HEDD EGU NOX emissions still provides substantial benefits in reducing ozone concentrations in the region, particularly at elevated ozone concentrations above 70 ppb.Implications: High-resolution coupled meteorology-chemistry modeling was used to quantify the impacts of high energy demand day (HEDD) electricity generating units (EGUs) and onroad transportation emissions changes on ozone air quality in the LISTOS region. Despite being highly localized and variable, HEDD EGUs NOX emissions sensitivity tests led to quantifiable changes in ozone. Further, reducing onroad emissions by 90% produced large decreases in ozone concentrations and led to a more NOX-sensitive ozone photochemical regime. With a transition to greater NOX-sensitivity, urban NOX-titration weakens and ozone is more likely to decline with the removal of additional NOX from sources like HEDD EGUs.

An Analysis of CMAQ Gas Phase Dry Deposition over North America Through Grid-Scale and Land-Use Specific Diagnostics in the Context of AQMEII4.

The fourth phase of the Air Quality Model Evaluation International Initiative (AQMEII4) is conducting a diagnostic intercomparison and evaluation of deposition simulated by regional-scale air quality models over North America and Europe. In this study, we analyze annual AQMEII4 simulations performed with the Community Multiscale Air Quality Model (CMAQ) version 5.3.1 over North America. These simulations were configured with both the M3Dry and Surface Tiled Aerosol and Gas Exchange (STAGE) dry deposition schemes available in CMAQ. A comparison of observed and modeled concentrations and wet deposition fluxes shows that the AQMEII4 CMAQ simulations perform similarly to other contemporary regional-scale modeling studies. During summer, M3Dry has higher ozone (O3) deposition velocities (Vd) and lower mixing ratios than STAGE for much of the eastern U.S. while the reverse is the case over eastern Canada and along the West Coast. In contrast, during winter STAGE has higher O3 Vd and lower mixing ratios than M3Dry over most of the southern half of the modeling domain while the reverse is the case for much of the northern U.S. and southern Canada. Analysis of the diagnostic variables defined for the AQMEII4 project, i.e. grid-scale and land-use (LU) specific effective conductances and deposition fluxes for the major dry deposition pathways, reveals generally higher summertime stomatal and wintertime cuticular grid-scale effective conductances for M3Dry and generally higher soil grid-scale effective conductances (for both vegetated and bare soil) for STAGE in both summer and winter. On a domain-wide basis, the stomatal grid-scale effective conductances account for about half of the total O3 Vd during daytime hours in summer for both schemes. Employing LU-specific diagnostics, results show that daytime Vd varies by a factor of 2 between LU categories. Furthermore, M3Dry vs. STAGE differences are most pronounced for the stomatal and vegetated soil pathway for the forest LU categories, with M3Dry estimating larger effective conductances for the stomatal pathway and STAGE estimating larger effective conductances for the vegetated soil pathway for these LU categories. Annual domain total O3 deposition fluxes differ only slightly between M3Dry (74.4 Tg/year) and STAGE (76.2 Tg/yr), but pathway-specific fluxes to individual LU types can vary more substantially on both annual and seasonal scales which would affect estimates of O3 damages to sensitive vegetation. A comparison of two simulations differing only in their LU classification scheme shows that the differences in LU cause seasonal mean O3 mixing ratio differences on the order of 1 ppb across large portions of the domain, with the differences generally largest during summer and in areas characterized by the largest differences in the fractional coverages of the forest, planted/cultivated, and grassland LU categories. These differences are generally smaller than the M3Dry vs. STAGE differences outside the summer season but have a similar magnitude during summer. Results indicate that the deposition impacts of LU differences are caused both by differences in the fractional coverages and spatial distributions of different LU categories as well as the characterization of these categories through variables like surface roughness and vegetation fraction in look-up tables used in the land-surface model and deposition schemes. Overall, the analyses and results presented in this study illustrate how the diagnostic grid-scale and LU-specific dry deposition variables adopted for AQMEII4 can provide insights into similarities and differences between the CMAQ M3Dry and STAGE dry deposition schemes that affect simulated pollutant budgets and ecosystem impacts from atmospheric pollution.

A single-point modeling approach for the intercomparison and evaluation of ozone dry deposition across chemical transport models (Activity 2 of AQMEII4).

A primary sink of air pollutants and their precursors is dry deposition. Dry deposition estimates differ across chemical transport models, yet an understanding of the model spread is incomplete. Here, we introduce Activity 2 of the Air Quality Model Evaluation International Initiative Phase 4 (AQMEII4). We examine 18 dry deposition schemes from regional and global chemical transport models as well as standalone models used for impact assessments or process understanding. We configure the schemes as single-point models at eight Northern Hemisphere locations with observed ozone fluxes. Single-point models are driven by a common set of site-specific meteorological and environmental conditions. Five of eight sites have at least 3 years and up to 12 years of ozone fluxes. The interquartile range across models in multiyear mean ozone deposition velocities ranges from a factor of 1.2 to 1.9 annually across sites and tends to be highest during winter compared with summer. No model is within 50 % of observed multiyear averages across all sites and seasons, but some models perform well for some sites and seasons. For the first time, we demonstrate how contributions from depositional pathways vary across models. Models can disagree with respect to relative contributions from the pathways, even when they predict similar deposition velocities, or agree with respect to the relative contributions but predict different deposition velocities. Both stomatal and nonstomatal uptake contribute to the large model spread across sites. Our findings are the beginning of results from AQMEII4 Activity 2, which brings scientists who model air quality and dry deposition together with scientists who measure ozone fluxes to evaluate and improve dry deposition schemes in the chemical transport models used for research, planning, and regulatory purposes.

Sensitivity of northeastern US surface ozone predictions to the representation of atmospheric chemistry in the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMMv1.0).

Chemical mechanisms describe how emissions of gases and particles evolve in the atmosphere and are used within chemical transport models to evaluate past, current, and future air quality. Thus, a chemical mechanism must provide robust and accurate predictions of air pollutants if it is to be considered for use by regulatory bodies. In this work, we provide an initial evaluation of the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMMv1.0) by assessing CRACMMv1.0 predictions of surface ozone (O3) across the northeastern US during the summer of 2018 within the Community Multiscale Air Quality (CMAQ) modeling system. CRACMMv1.0 O3 predictions of hourly and maximum daily 8 h average (MDA8) ozone were lower than those estimated by the Regional Atmospheric Chemistry Mechanism with aerosol module 6 (RACM2_ae6), which better matched surface network observations in the northeastern US (RACM2_ae6 mean bias of +4.2 ppb for all hours and +4.3 ppb for MDA8; CRACMMv1.0 mean bias of +2.1 ppb for all hours and +2.7 ppb for MDA8). Box model calculations combined with results from CMAQ emission reduction simulations indicated a high sensitivity of O3 to compounds with biogenic sources. In addition, these calculations indicated the differences between CRACMMv1.0 and RACM2_ae6 O3 predictions were largely explained by updates to the inorganic rate constants (reflecting the latest assessment values) and by updates to the representation of monoterpene chemistry. Updates to other reactive organic carbon systems between RACM2_ae6 and CRACMMv1.0 also affected ozone predictions and their sensitivity to emissions. Specifically, CRACMMv1.0 benzene, toluene, and xylene chemistry led to efficient NO x cycling such that CRACMMv1.0 predicted controlling aromatics reduces ozone without rural O3 disbenefits. In contrast, semivolatile and intermediate-volatility alkanes introduced in CRACMMv1.0 acted to suppress O3 formation across the regional background through the sequestration of nitrogen oxides (NO x ) in organic nitrates. Overall, these analyses showed that the CRACMMv1.0 mechanism within the CMAQ model was able to reasonably simulate ozone concentrations in the northeastern US during the summer of 2018 with similar magnitude and diurnal variation as the current operational Carbon Bond (CB6r3_ae7) mechanism and good model performance compared to recent modeling studies in the literature.

The pathway of impacts of aerosol direct effects on secondary inorganic aerosol formation.

Airborne aerosols reduce surface solar radiation through light scattering and absorption (aerosol direct effects, ADEs), influence regional meteorology, and further affect atmospheric chemical reactions and aerosol concentrations. The inhibition of turbulence and the strengthened atmospheric stability induced by ADEs increases surface primary aerosol concentration, but the pathway of ADE impacts on secondary aerosol is still unclear. In this study, the online coupled meteorological and chemistry model (WRF-CMAQ; Weather Research and Forecasting-Community Multiscale Air Quality) with integrated process analysis was applied to explore how ADEs affect secondary aerosol formation through changes in atmospheric dynamics and photolysis processes. The meteorological condition and air quality in the Jing-Jin-Ji area (denoted JJJ, including Beijing, Tianjin, and Hebei Province in China) in January and July 2013 were simulated to represent winter and summer conditions, respectively. Our results show that ADEs through the photolysis pathway inhibit sulfate formation during winter in the JJJ region and promote sulfate formation in July. The differences are attributed to the alteration of effective actinic flux affected by single-scattering albedo (SSA). ADEs through the dynamics pathway act as an equally or even more important route compared with the photolysis pathway in affecting secondary aerosol concentration in both summer and winter. ADEs through dynamics traps formed sulfate within the planetary boundary layer (PBL) which increases sulfate concentration in winter. Meanwhile, the impact of ADEs through dynamics is mainly reflected in the increase of gaseous-precursor concentrations within the PBL which enhances secondary aerosol formation in summer. For nitrate, reduced upward transport of precursors restrains the formation at high altitude and eventually lowers the nitrate concentration within the PBL in winter, while such weakened vertical transport of precursors increases nitrate concentration within the PBL in summer, since nitrate is mainly formed near the surface ground.

Performance Evaluation of the Meteorology and Air Quality Conditions From Multiscale WRF-CMAQ Simulations for the Long Island Sound Tropospheric Ozone Study (LISTOS).

The Long Island Sound (LIS) Tropospheric Ozone Study was a multi-agency collaborative field campaign conducted during the summer of 2018 to improve the understanding of ozone chemistry and transport from New York City to areas downstream, especially the LIS and adjacent Connecticut coastline. Measurements made during this campaign were leveraged to test and evaluate the coupled WRF-CMAQ model at 12 km, 4 and 1.33 km horizontal grid spacing. Special attention was placed on the model's representation of sea breeze circulations, low level jets, and boundary layer evolution. The evaluation suggests using higher resolutions resulted in improved surface meteorology statistics throughout the whole summer, with temperature biases seeing the biggest statistical improvements when using 1.33-km grid spacing, going from -0.12 to 0.08 K. Additionally, 4-km grid spacing provided the biggest advantage when simulating ozone over the region of interest, with biases being reduced from 2.40 to 0.57 to 0.37 ppbV with increased resolution. Case studies of two high ozone concentration events (July 10 and August 6) revealed that sound breezes and low-level jets had a critical role in transporting pollutant-rich, shallow marine air masses from the LIS inland over the Connecticut coast. Modifications were made to the representation of sea surface temperatures, which subsequently improved the simulation of surface ozone predictions.

Technical note: AQMEII4 Activity 1: evaluation of wet and dry deposition schemes as an integral part of regional-scale air quality models.

We present in this technical note the research protocol for phase 4 of the Air Quality Model Evaluation International Initiative (AQMEII4). This research initiative is divided into two activities, collectively having three goals: (i) to define the current state of the science with respect to representations of wet and especially dry deposition in regional models, (ii) to quantify the extent to which different dry deposition parameterizations influence retrospective air pollutant concentration and flux predictions, and (iii) to identify, through the use of a common set of detailed diagnostics, sensitivity simulations, model evaluation, and reduction of input uncertainty, the specific causes for the current range of these predictions. Activity 1 is dedicated to the diagnostic evaluation of wet and dry deposition processes in regional air quality models (described in this paper), and Activity 2 to the evaluation of dry deposition point models against ozone flux measurements at multiple towers with multiyear observations (to be described in future submissions as part of the special issue on AQMEII4). The scope of this paper is to present the scientific protocols for Activity 1, as well as to summarize the technical information associated with the different dry deposition approaches used by the participating research groups of AQMEII4. In addition to describing all common aspects and data used for this multi-model evaluation activity, most importantly, we present the strategy devised to allow a common process-level comparison of dry deposition obtained from models using sometimes very different dry deposition schemes. The strategy is based on adding detailed diagnostics to the algorithms used in the dry deposition modules of existing regional air quality models, in particular archiving diagnostics specific to land use-land cover (LULC) and creating standardized LULC categories to facilitate cross-comparison of LULC-specific dry deposition parameters and processes, as well as archiving effective conductance and effective flux as means for comparing the relative influence of different pathways towards the net or total dry deposition. This new approach, along with an analysis of precipitation and wet deposition fields, will provide an unprecedented process-oriented comparison of deposition in regional air quality models. Examples of how specific dry deposition schemes used in participating models have been reduced to the common set of comparable diagnostics defined for AQMEII4 are also presented.

The Community Multiscale Air Quality (CMAQ) model versions 5.3 and 5.3.1: system updates and evaluation.

The Community Multiscale Air Quality (CMAQ) model version 5.3 (CMAQ53), released to the public in August 2019 and followed by version 5.3.1 (CMAQ531) in December 2019, contains numerous science updates, enhanced functionality, and improved computation efficiency relative to the previous version of the model, 5.2.1 (CMAQ521). Major science advances in the new model include a new aerosol module (AERO7) with significant updates to secondary organic aerosol (SOA) chemistry, updated chlorine chemistry, updated detailed bromine and iodine chemistry, updated simple halogen chemistry, the addition of dimethyl sulfide (DMS) chemistry in the CB6r3 chemical mechanism, updated M3Dry bidirectional deposition model, and the new Surface Tiled Aerosol and Gaseous Exchange (STAGE) bidirectional deposition model. In addition, support for the Weather Research and Forecasting (WRF) model's hybrid vertical coordinate (HVC) was added to CMAQ53 and the Meteorology-Chemistry Interface Processor (MCIP) version 5.0 (MCIP50). Enhanced functionality in CMAQ53 includes the new Detailed Emissions Scaling, Isolation and Diagnostic (DESID) system for scaling incoming emissions to CMAQ and reading multiple gridded input emission files. Evaluation of CMAQ531 was performed by comparing monthly and seasonal mean daily 8 h average (MDA8) O3 and daily PM2.5 values from several CMAQ531 simulations to a similarly configured CMAQ521 simulation encompassing 2016. For MDA8 O3, CMAQ531 has higher O3 in the winter versus CMAQ521, due primarily to reduced dry deposition to snow, which strongly reduces wintertime O3 bias (2-4 ppbv monthly average). MDA8 O3 is lower with CMAQ531 throughout the rest of the year, particularly in spring, due in part to reduced O3 from the lateral boundary conditions (BCs), which generally increases MDA8 O3 bias in spring and fall ( 0.5 µg m-3). For daily 24 h average PM2.5, CMAQ531 has lower concentrations on average in spring and fall, higher concentrations in summer, and similar concentrations in winter to CMAQ521, which slightly increases bias in spring and fall and reduces bias in summer. Comparisons were also performed to isolate updates to several specific aspects of the modeling system, namely the lateral BCs, meteorology model version, and the deposition model used. Transitioning from a hemispheric CMAQ (HCMAQ) version 5.2.1 simulation to a HCMAQ version 5.3 simulation to provide lateral BCs contributes to higher O3 mixing ratios in the regional CMAQ simulation in higher latitudes during winter (due to the decreased O3 dry deposition to snow in CMAQ53) and lower O3 mixing ratios in middle and lower latitudes year-round (due to reduced O3 over the ocean with CMAQ53). Transitioning from WRF version 3.8 to WRF version 4.1.1 with the HVC resulted in consistently higher (1.0-1.5 ppbv) MDA8 O3 mixing ratios and higher PM2.5 concentrations (0.1-0.25 µg m-3) throughout the year. Finally, comparisons of the M3Dry and STAGE deposition models showed that MDA8 O3 is generally higher with M3Dry outside of summer, while PM2.5 is consistently higher with STAGE due to differences in the assumptions of particle deposition velocities to non-vegetated surfaces and land use with short vegetation (e.g., grasslands) between the two models. For ambient NH3, STAGE has slightly higher concentrations and smaller bias in the winter, spring, and fall, while M3Dry has higher concentrations and smaller bias but larger error and lower correlation in the summer.

Establishing the Suitability of the Model for Prediction Across Scales for Global Retrospective Air Quality Modeling.

The U.S. EPA is leveraging recent advances in meteorological modeling to construct an air quality modeling system to allow consistency from global to local scales. The Model for Prediction Across Scales-Atmosphere (MPAS-A or MPAS) has been developed by the National Center for Atmospheric Research (NCAR) as a global complement to the Weather Research and Forecasting model (WRF). Patterned after a regional coupled system with WRF, the Community Multiscale Air Quality (CMAQ) modeling system has been coupled within MPAS to explore global-to-local chemical transport modeling. Several options were implemented into MPAS for retrospective applications. Nudging-based data assimilation was added to support continuous simulations of past weather to minimize error growth that exists with a weather forecast configuration. The Pleim-Xiu land-surface model, the Asymmetric Convective Model 2 boundary layer scheme, and the Pleim surface layer scheme were added as the preferred options for retrospective air quality applications with WRF. Annual simulations were conducted using this EPA-enhanced MPAS configuration on two different mesh structures and compared against WRF. MPAS generally compares well with WRF over the conterminous United States. Errors in MPAS surface meteorology are comparable to WRF throughout the year. Precipitation statistics indicate MPAS performs slightly better than WRF. Solar radiation in MPAS is higher than WRF and measurements, suggesting fewer clouds in MPAS than WRF. Upper-air meteorology is well-simulated by MPAS, but errors are slightly higher than WRF. These comparisons lend confidence to use MPAS for retrospective air quality modeling and suggest ways it can be further improved in the future.

A comparative study of two-way and offline coupled WRF v3.4 and CMAQ v5.0.2 over the contiguous US: performance evaluation and impacts of chemistry-meteorology feedbacks on air quality.

The two-way coupled Weather Research and Forecasting and Community Multiscale Air Quality (WRF-CMAQ) model has been developed to more realistically represent the atmosphere by accounting for complex chemistry-meteorology feedbacks. In this study, we present a comparative analysis of two-way (with consideration of both aerosol direct and indirect effects) and offline coupled WRF v3.4 and CMAQ v5.0.2 over the contiguous US. Long-term (5 years from 2008 to 2012) simulations using WRF-CMAQ with both offline and two-way coupling modes are carried out with anthropogenic emissions based on multiple years of the U.S. National Emission Inventory and chemical initial and boundary conditions derived from an advanced Earth system model (i.e., a modified version of the Community Earth System Model/Community Atmospheric Model). The comprehensive model evaluations show that both two-way WRF-CMAQ and WRF-only simulations perform well for major meteorological variables such as temperature at 2 m, relative humidity at 2 m, wind speed at 10 m, precipitation (except for against the National Climatic Data Center data), and shortwave and longwave radiation. Both two-way and offline CMAQ also show good performance for ozone (O3) and fine particulate matter (PM2.5). Due to the consideration of aerosol direct and indirect effects, two-way WRF-CMAQ shows improved performance over offline coupled WRF and CMAQ in terms of spatiotemporal distributions and statistics, especially for radiation, cloud forcing, O3, sulfate, nitrate, ammonium, elemental carbon, tropospheric O3 residual, and column nitrogen dioxide (NO2). For example, the mean biases have been reduced by more than 10 W m-2 for shortwave radiation and cloud radiative forcing and by more than 2 ppb for max 8 h O3. However, relatively large biases still exist for cloud predictions, some PM2.5 species, and PM10 that warrant follow-up studies to better understand those issues. The impacts of chemistry-meteorological feedbacks are found to play important roles in affecting regional air quality in the US by reducing domain-average concentrations of carbon monoxide (CO), O3, nitrogen oxide (NO x ), volatile organic compounds (VOCs), and PM2.5 by 3.1% (up to 27.8%), 4.2% (up to 16.2%), 6.6% (up to 50.9%), 5.8% (up to 46.6%), and 8.6% (up to 49.1%), respectively, mainly due to reduced radiation, temperature, and wind speed. The overall performance of the two-way coupled WRF-CMAQ model achieved in this work is generally good or satisfactory and the improved performance for two-way coupled WRF-CMAQ should be considered along with other factors in developing future model applications to inform policy making.

New Bidirectional Ammonia Flux Model in an Air Quality Model Coupled With an Agricultural Model.

Ammonia surface flux is bidirectional; that is, net flux can be either upward or downward. In fertilized agricultural croplands and grasslands there is usually more emission than deposition especially in midday during warmer seasons. In North America, most of the ammonia emissions are from agriculture with a significant fraction of that coming from fertilizer. A new bidirectional ammonia flux modeling system has been developed in the Community Multiscale Air Quality (CMAQ) model, which has close linkages with the Environmental Policy Integrated Climate (EPIC) agricultural ecosystem model. Daily inputs from EPIC are used to calculate soil ammonia concentrations that are combined with air concentrations in CMAQ to calculate bidirectional surface flux. The model is evaluated against surface measurements of NH3 concentrations, NH4 + and SO4 2- aerosol concentrations, NH4 + wet deposition measurements, and satellite retrievals of NH3 concentrations. The evaluation shows significant improvement over the base model without bidirectional ammonia flux. Comparisons to monthly average satellite retrievals show similar spatial distribution with the highest ammonia concentrations in the Central Valley of California (CA), the Snake River valley in Idaho, and the western High Plains. In most areas the model underestimates, but in the Central Valley of CA, it generally overestimates ammonia concentration. Case study analyses indicate that modeled high fluxes of ammonia in CA are often caused by anomalous high soil ammonia loading from EPIC for particular crop types. While further improvements to parameterizations in EPIC and CMAQ are recommended, this system is a significant advance over previous ammonia bidirectional surface flux models.

Long-term trends in the ambient PM2.5- and O3-related mortality burdens in the United States under emission reductions from 1990 to 2010.

Concentrations of both fine particulate matter (PM2.5) and ozone (O3) in the United States (US) have decreased significantly since 1990, mainly because of air quality regulations. Exposure to these air pollutants is associated with premature death. Here we quantify the annual mortality burdens from PM2.5 and O3 in the US from 1990 to 2010, estimate trends and inter-annual variability, and evaluate the contributions to those trends from changes in pollutant concentrations, population, and baseline mortality rates. We use a fine-resolution (36 km) self-consistent 21-year simulation of air pollutant concentrations in the US from 1990 to 2010, a health impact function, and annual county-level population and baseline mortality rate estimates. From 1990 to 2010, the modeled population-weighted annual PM2.5 decreased by 39 %, and summertime (April to September) 1 h average daily maximum O3 decreased by 9 % from 1990 to 2010. The PM2.5-related mortality burden from ischemic heart disease, chronic obstructive pulmonary disease, lung cancer, and stroke steadily decreased by 54% from 123 700 deaths year-1 (95% confidence interval, 70 800-178 100) in 1990 to 58 600 deaths year-1 (24 900-98 500) in 2010. The PM2.5-related mortality burden would have decreased by only 24% from 1990 to 2010 if the PM2.5 concentrations had stayed at the 1990 level, due to decreases in baseline mortality rates for major diseases affected by PM2.5. The mortality burden associated with O3 from chronic respiratory disease increased by 13% from 10 900 deaths year-1 (3700-17 500) in 1990 to 12 300 deaths year-1 (4100-19 800) in 2010, mainly caused by increases in the baseline mortality rates and population, despite decreases in O3 concentration. The O3-related mortality burden would have increased by 55% from 1990 to 2010 if the O3 concentrations had stayed at the 1990 level. The detrended annual O3 mortality burden has larger inter-annual variability (coefficient of variation of 12%) than the PM2.5-related burden (4%), mainly from the inter-annual variation of O3 concentration. We conclude that air quality improvements have significantly decreased the mortality burden, avoiding roughly 35 800 (38%) PM2.5-related deaths and 4600 (27%) O3-related deaths in 2010, compared to the case if air quality had stayed at 1990 levels (at 2010 baseline mortality rates and population).

Historical Trends in PM2.5-Related Premature Mortality during 1990-2010 across the Northern Hemisphere.

BACKGROUND: Air quality across the northern hemisphere over the past two decades has witnessed dramatic changes, with continuous improvement in developed countries in North America and Europe, but a contrasting sharp deterioration in developing regions of Asia. OBJECTIVE: This study investigates the historical trend in the long-term exposure to PM2.5 and PM2.5-related premature mortality (PM2.5-mortality) and its response to changes in emission that occurred during 1990-2010 across the northern hemisphere. Implications for future trends in human exposure to air pollution in both developed and developing regions of the world are discussed. METHODS: We employed the integrated exposure-response model developed by Health Effects Institute to estimate the PM2.5-mortality. The 1990-2010 annual average PM2.5 concentrations were obtained from the simulations using the WRF-CMAQ model. Emission mitigation efficiencies of sulfur dioxide (SO2), nitrogen oxides (NOx), ammonia (NH3), and primary PM are estimated from the PM2.5-mortality responses to the emission variations. RESULTS: Estimated PM2.5-mortalities in East Asia and South Asia increased by 21% and 85% respectively, from 866,000 and 578,000 in 1990, to 1,048,000 and 1,068,000 in 2010. PM2.5-mortalities in developed regions (i.e., Europe and high-income North America) decreased substantially by 67% and 58% respectively. CONCLUSIONS: Over the past two decades, correlations between population and PM2.5 have become weaker in Europe and North America due to air pollution controls but stronger in East Asia due to deteriorating air quality. Mitigation of primary PM appears to be the most efficient way for increasing health benefits (i.e., providing the largest mortality reduction per unit emissions). However, reductions in emissions of NH3 are needed to maximize the effectiveness of NOx emission controls. Citation: Wang J, Xing J, Mathur R, Pleim JE, Wang S, Hogrefe C, Gan CM, Wong DC, Hao J. 2017. Historical trends in PM2.5-related premature mortality during 1990-2010 across the northern hemisphere. Environ Health Perspect 125:400-408; http://dx.doi.org/10.1289/EHP298.

Improving the simulation of convective dust storms in regional-to-global models.

Convective dust storms have significant impacts on atmospheric conditions and air quality and are a major source of dust uplift in summertime. However, regional-to-global models generally do not accurately simulate these storms, a limitation that can be attributed to (1) using a single mean value for wind speed per grid box, i.e., not accounting for subgrid wind variability and (2) using convective parametrizations that poorly simulate cold pool outflows. This study aims to improve the simulation of convective dust storms by tackling these two issues. Specifically, we incorporate a probability distribution function for surface wind in each grid box to account for subgrid wind variability due to dry and moist convection. Furthermore, we use lightning assimilation to increase the accuracy of the convective parameterization and simulated cold pool outflows. This updated model framework is used to simulate a massive convective dust storm that hit Phoenix, AZ, on 6 July 2011. The results show that lightning assimilation provides a more realistic simulation of precipitation features, including timing and location, and the resulting cold pool outflows that generated the dust storm. When those results are combined with a dust model that accounts for subgrid wind variability, the prediction of dust uplift and concentrations are considerably improved compared to the default model results. This modeling framework could potentially improve the simulation of convective dust storms in global models, regional climate simulations, and retrospective air quality studies.

A Photosynthesis-based Two-leaf Canopy Stomatal Conductance Model for Meteorology and Air Quality Modeling with WRF/CMAQ PX LSM.

A coupled photosynthesis-stomatal conductance model with single layer sunlit and shaded leaf canopy scaling is developed for the Pleim-Xiu land surface model (LSM) option in the meteorology and air quality modeling system - WRF/CMAQ (Weather Research and Forecast model and Community Multiscale Air Quality model). The photosynthesis-based model for the PX LSM (PX PSN) is implemented and evaluated in a diagnostic box model that has evapotranspiration and ozone deposition components taken directly from WRF/CMAQ. We evaluate PX PSN for latent heat (LH) estimation at four FLUXNET sites with different vegetation types and landscape characteristics and at one FLUXNET site with ozone flux measurements against the simple Jarvis approach used in the current PX LSM. Overall, the PX PSN simulates LH as well as the PX Jarvis approach. The PX PSN, however, shows distinct advantages over the PX Jarvis approach on grassland that likely results from its treatment of C3 and C4 plants for CO2 assimilation estimation. Simulations using Moderate Resolution Imaging Spectroradiometer (MODIS) LAI rather than LAI observations assess how the model would perform with the grid averaged data available in the Eulerian grid model (WRF/CMAQ). While MODIS LAI generally follows the seasonality of the observed LAI, it cannot capture the extreme highs and lows of the site measurements. MODIS LAI estimates degrade model performance at all sites but one site having old and tall trees. Ozone deposition velocity and ozone flux along with LH are simulated especially well by PX PSN as compared to significant PX Jarvis overestimation.

Extending the Community Multiscale Air Quality (CMAQ) Modeling System to Hemispheric Scales: Overview of Process Considerations and Initial Applications.

The Community Multiscale Air Quality (CMAQ) modeling system is extended to simulate ozone, particulate matter, and related precursor distributions throughout the Northern Hemisphere. Modelled processes were examined and enhanced to suitably represent the extended space and time scales for such applications. Hemispheric scale simulations with CMAQ and the Weather Research and Forecasting (WRF) model are performed for multiple years. Model capabilities for a range of applications including episodic long-range pollutant transport, long-term trends in air pollution across the Northern Hemisphere, and air pollution-climate interactions are evaluated through detailed comparison with available surface, aloft, and remotely sensed observations. The expansion of CMAQ to simulate the hemispheric scales provides a framework to examine interactions between atmospheric processes occurring at various spatial and temporal scales with physical, chemical, and dynamical consistency.

Impacts of aerosol direct effects on tropospheric ozone through changes in atmospheric dynamics and photolysis rates.

Aerosol direct effects (ADEs), i.e., scattering and absorption of incoming solar radiation, reduce radiation reaching the ground and the resultant photolysis attenuation can decrease ozone (O3) formation in polluted areas. One the other hand, evidence also suggests that ADE-associated cooling suppresses atmospheric ventilation, thereby enhancing surface-level O3. Assessment of ADE impacts is thus important for understanding emission reduction strategies that seek co-benefits associated with reductions in both particuate matter and O3 levels. This study quantifies the impacts of ADEs on tropospheric ozone by using a two-way online coupled meteorology and atmospheric chemistry model, WRF- CMAQ, using a process analysis methodology. Two mani-festations of ADE impacts on O3 including changes in atmospheric dynamics (ᐃDynamics) and changes in photolysis rates (∆Photolysis) were assessed separately through multiple scenario simulations for January and July of 2013 over China. Results suggest that ADEs reduced surface daily maxima 1 h O3 (DM1O3) in China by up to 39µgm-3 through the combination of ∆Dynamics and ∆Photolysis in January but enhanced surface DM1O3 by up to 4µgm-3 in July. Increased O3 in July is largely attributed to ∆Dynamics, which causes a weaker O3 sink of dry deposition and a stronger O3 source of photochemistry due to the stabilization of the at-mosphere. Meanwhile, surface OH is also enhanced at noon in July, though its daytime average values are reduced in January. An increased OH chain length and a shift towards more volatile organic compound (VOC)-limited conditions are found due to ADEs in both January and July. This study suggests that reducing ADEs may have the potential risk of increasing O3 in winter, but it will benefit the reduction in maxima O3 in summer.