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The absence of up-to-date emissions has been a major impediment to accurately simulating aspects of atmospheric chemistry and to precisely quantifying the impact of changes in emissions on air pollution. Hence, a nonlinear joint analytical inversion (Gauss–Newton method) of both volatile organic compounds (VOCs) and nitrogen oxide ( NOx ) emissions is made by exploiting the Smithsonian Astrophysical Observatory (SAO) Ozone Mapping and Profiler Suite Nadir Mapper (OMPS-NM) formaldehyde (HCHO) and the National Aeronautics and Space Administration (NASA) Ozone Monitoring Instrument (OMI) tropospheric nitrogen dioxide ( NO2 ) columns during the Korea–United States Air Quality (KORUS-AQ) campaign over East Asia in May–June 2016. Effects of the chemical feedback of NOx and VOCs on both NO2 and HCHO are implicitly included by iteratively optimizing the inversion. Emission uncertainties are greatly narrowed (averaging kernels > 0.8 , which is the mathematical presentation of the partition of information gained from the satellite observations with respect to the prior knowledge) over medium- to high-emitting areas such as cities and dense vegetation. The prior amount of total NOx emissions is mainly dictated by values reported in the MIX-Asia 2010 inventory. After the inversion we conclude that there is a decline in emissions (before, after, change) for China ( 87.94±44.09 Gg d −1 , 68.00±15.94 Gg d −1 , −23 %), North China Plain (NCP) ( 27.96±13.49 Gg d −1 , 19.05±2.50 Gg d −1 , −32 %), Pearl River Delta (PRD) ( 4.23±1.78 Gg d −1 , 2.70±0.32 Gg d −1 , −36 %), Yangtze River Delta (YRD) ( 9.84±4.68 Gg d −1 , 5.77±0.51 Gg d −1 , −41 %), Taiwan ( 1.26±0.57 Gg d −1 , 0.97±0.33 Gg d −1 , −23 %), and Malaysia ( 2.89±2.77 Gg d −1 , 2.25±1.34 Gg d −1 , −22 %), all of which have effectively implemented various stringent regulations. In contrast, South Korea ( 2.71±1.34 Gg d −1 , 2.95±0.58 Gg d −1 , + 9 %) and Japan ( 3.53±1.71 Gg d −1 , 3.96±1.04 Gg d −1 , +12 %) are experiencing an increase in NOx emissions, potentially due to an increased number of diesel vehicles and new thermal power plants. We revisit the well-documented positive bias (by a factor of 2 to 3) of MEGAN v2.1 (Model of Emissions of Gases and Aerosols from Nature) in terms of biogenic VOC emissions in the tropics. The inversion, however, suggests a larger growth of VOCs (mainly anthropogenic) over NCP (25 %) than previously reported (6 %) relative to 2010. The spatial variation in both the magnitude and sign of NOx and VOC emissions results in nonlinear responses of ozone production and loss. Due to a simultaneous decrease and increase in NOx∕VOC over NCP and YRD, we observe a ∼53 % reduction in the ratio of the chemical loss of NOx ( LNOx ) to the chemical loss of ROx ( RO2+HO2 ) over the surface transitioning toward NOx -sensitive regimes, which in turn reduces and increases the afternoon chemical loss and production of ozone through NO2+OH ( −0.42 ppbv h −1 ) ∕HO2 (and RO2 ) +NO ( +0.31 ppbv h −1 ). Conversely, a combined decrease in NOx and VOC emissions in Taiwan, Malaysia, and southern China suppresses the formation of ozone. Simulations using the updated emissions indicate increases in maximum daily 8 h average (MDA8) surface ozone over China (0.62 ppbv), NCP (4.56 ppbv), and YRD (5.25 ppbv), suggesting that emission control strategies on VOCs should be prioritized to curb ozone production rates in these regions. Taiwan, Malaysia, and PRD stand out as regions undergoing lower MDA8 ozone levels resulting from the NOx reductions occurring predominantly in NOx -sensitive regimes.

Atmospheric ammonia is a significant pollutant throughout the year, necessitating standardized measurement and identification of emission factors. We performed a quantized evaluation of ammonia concentrations at various locations in and around Seoul, South Korea. The established testing methods of the Radiello Passive Sampler were used for ammonia sampling, and the method was validated using annular denuder sampling. Urban and suburban areas were studied to gain a deeper understanding of the factors responsible for ammonia pollution. This study aimed to establish the fluctuations in concentration over one year, by analyzing the seasonal and regional variation in ammonia concentration. Livestock and agricultural areas recorded the highest concentration of ammonia among all sites, with the highest concentration recorded in autumn. However, at most of the other studied sites, the highest and lowest ammonia concentrations were recorded during summer and winter, respectively. This study attempted to establish a correlation between ammonia concentration and temperature, as well as ammonia concentration and altitude.

Geostationary satellite sensors over East Asia (GOCI and AHI) are now providing continuous mapping of aerosol optical depth (AOD) at 550 nm to improve monitoring of fine particulate matter (PM2.5) air quality. Here we evaluate our understanding of the physical relationships between AOD and PM2.5 over East Asia by using the GEOS-Chem atmospheric chemistry model to simulate observations from multiple sources: 1) the joint NASA-NIER Korea – United States Air Quality aircraft campaign over South Korea (KORUS-AQ; May–June 2016); 2) AODs from the AERONET ground-based network; 3) AOD from a new GOCI/AHI fused product; and 4) surface PM2.5 networks in South Korea and China. The KORUS-AQ data show that 550 nm AOD is mainly contributed by sulfate-nitrate-ammonium (SNA) and organic aerosols in the planetary boundary layer (PBL), despite large dust concentrations in the free troposphere, reflecting the optically effective size and the high hygroscopicity of the PBL aerosols. Although GEOS-Chem is successful in reproducing the KORUS-AQ vertical profiles of aerosol mass, its ability to link AOD to PM2.5 is limited by under-accounting of coarse PM and by a large overestimate of nighttime PM2.5 nitrate. A broader analysis of the GOCI/AHI AOD data over East Asia in different seasons shows agreement with AERONET AODs and a spatial distribution consistent with surface PM2.5 network data. The AOD observations over North China show a summer maximum and winter minimum, opposite in phase to surface PM2.5. This is due to low PBL depths compounded by high residential coal emissions in winter, and high relative humidity (RH) in summer. Seasonality of AOD and PM2.5 over South Korea is much weaker, reflecting weaker variation of PBL depth and lack of residential coal emissions. Physical interpretation of the satellite AOD data in terms of surface PM2.5 is sensitive to accurate information on aerosol size distributions, PBL depths, RH, the role of coarse particles, and diurnal variation of PM2.5.

High concentrations of PM2.5 have become a serious environmental issue in South Korea, which ranked 1st or 2nd among OECD countries in terms of population exposure to PM2.5. Quantitative understanding of PM2.5 source attribution is thus crucial for developing efficient air quality mitigation strategies. Here we use a suite of extensive observations of PM2.5 and its precursors concentrations during the international KORea-US cooperative Air Quality field study in Korea (KORUS-AQ) in May–June 2016 to investigate source contributions to PM2.5 in South Korea under various meteorological conditions. For the quantitative analysis, we updated a 3-D chemical transport model, GEOS-Chem, and its adjoint with the latest regional emission inventory and other recent findings. The updated model is evaluated by comparing against observed daily PM2.5 and its component concentrations from six ground sites (Bangnyung, Bulkwang, Olympic park, Gwangju, Ulsan, and Jeju). Overall, simulated concentrations of daily PM2.5 and its components are in a good agreement with observations over the peninsula. We conduct an adjoint sensitivity analysis for simulated surface level PM2.5 concentrations at five ground sites (except for Bangnyung because of its small population) under four different meteorological conditions: dynamic weather, stagnant, extreme pollution, and blocking periods. Source contributions by regions vary greatly depending on synoptic meteorological conditions. Chinese contribution accounts for almost 68% of PM2.5 in surface air in South Korea during the extreme pollution period of the campaign, whereas an enhanced contribution from domestic sources (57%) occurs for the blocking period. Results from our sensitivity analysis suggest that the reduction of domestic anthropogenic NH3 emissions could be most effective in reducing population exposure to PM2.5 in South Korea (effectiveness = 14%) followed by anthropogenic SO2 emissions from Shandong region (effectiveness = 11%), domestic anthropogenic NOx emissions (effectiveness = 10%), anthropogenic NH3 emissions from Shandong region (effectiveness = 8%), anthropogenic NOx emissions from Shandong region (effectiveness = 7%), domestic anthropogenic OC emissions (effectiveness = 7%), and domestic anthropogenic BC emissions (effectiveness = 5%).

The Korea-United States Air Quality (KORUS-AQ) field study was conducted during May–June 2016 to understand the factors controlling air quality in South Korea. Extensive aircraft and ground network observations from the campaign offer an opportunity to address issues in current air quality models and reduce model-observation disagreements. This study examines these issues using model evaluation against the KORUS-AQ observations and intercomparisons between models. Six regional and two global chemistry transport models using identical anthropogenic emissions participated in the model intercomparison study and were used to conduct air quality simulations focusing on ozone (O3), aerosols, and their precursors for the campaign. Using the KORUSv5 emissions inventory, which has been updated from KORUSv1, the models successfully reproduced observed nitrogen oxides (NOx) and volatile organic compounds mixing ratios in surface air, especially in the Seoul Metropolitan Area, but showed systematic low biases for carbon monoxide (CO), implying possible missing CO sources in the inventory in East Asia. Although the DC-8 aircraft-observed O3 precursor mixing ratios were well captured by the models, simulated O3 levels were lower than the observations in the free troposphere in part due to too low stratospheric O3 influxes, especially in regional models. During the campaign, the synoptic meteorology played an important role in determining the observed variability of PM2.5 (PM diameter ≤ 2.5 μm) concentrations in South Korea. The models successfully simulated the observed PM2.5 variability with significant inorganic sulfate-nitrate-ammonium aerosols contribution, but failed to reproduce that of organic aerosols, causing a large inter-model variability. From the model evaluation, we find that an ensemble of model results, incorporating individual models with differing strengths and weaknesses, performs better than most individual models at representing observed atmospheric compositions for the campaign. Ongoing model development and evaluation, in close collaboration with emissions inventory development, are needed to improve air quality forecasting.

Nonmethane volatile organic compounds (NMVOCs) result in ozone and aerosol production that adversely affects the environment and human health. For modeling purposes, anthropogenic NMVOC emissions have been typically compiled using the “bottom-up” approach. To minimize uncertainties of the bottom-up emission inventory, “top-down” NMVOC emissions can be estimated using formaldehyde (HCHO) observations. In this study, HCHO vertical column densities (VCDs) obtained from the Geostationary Trace gas and Aerosol Sensor Optimization spectrometer during the Korea–United States Air Quality campaign were used to constrain anthropogenic volatile organic compound (AVOC) emissions in South Korea. Estimated top-down AVOC emissions differed from those of the up-to-date bottom-up inventory over major anthropogenic source regions by factors of 1.0 ± 0.4 to 6.9 ± 3.9. Our evaluation using a 3D chemical transport model indicates that simulated HCHO mixing ratios using the top-down estimates were in better agreement with observations onboard the DC-8 aircraft during the campaign relative to those with the bottom-up emission, showing a decrease in model bias from –25% to –13%. The top-down analysis used in this study, however, has some limitations related to the use of HCHO yields, background HCHO columns, and AVOC speciation in the bottom-up inventory, resulting in uncertainties in the AVOC emission estimates. Our attempt to constrain diurnal variations of the AVOC emissions using the aircraft HCHO VCDs was compromised by infrequent aircraft observations over the same source regions. These limitations can be overcome with geostationary satellite observations by providing hourly HCHO VCDs.

We present trace gas vertical profiles observed by instruments on the NASA DC-8 and at a ground site during the Korea-US air quality study (KORUS) field campaign in May to June 2016. We focus on the region near the Seoul metropolitan area and its surroundings where both anthropogenic and natural emission sources play an important role in local photochemistry. Integrating ground and airborne observations is the major research goal of many atmospheric chemistry field campaigns. Although airborne platforms typically aim to sample from near surface to the free troposphere, it is difficult to fly very close to the surface especially in environments with complex terrain or a populated area. A detailed analysis integrating ground and airborne observations associated with specific concentration footprints indicates that reactive trace gases are quickly oxidized below an altitude of 700 m. The total OH reactivity profile has a rapid decay in the lower part of troposphere from surface to the lowest altitude (700 m) sampled by the NASA DC-8. The decay rate is close to that of very reactive biogenic volatile organic compounds such as monoterpenes. Therefore, we argue that photochemical processes in the bottom of the boundary layer, below the typical altitude of aircraft sampling, should be thoroughly investigated to properly assess ozone and secondary aerosol formation.

Biogenic volatile organic compound (BVOCs) emissions are the largest VOC emission source globally, and are precursors to ozone and secondary organic aerosols, both of which are strong, short-lived climate pollutants. BVOC emissions are usually estimated using the Model of Emissions of Gases and Aerosols from Nature (MEGAN), which requires Plant Functional Types (PFTs) and Leaf Area Indexes (LAIs) as inputs. Herein, the effects of refined input data on regional BVOC emission estimates are analyzed. For LAIs, lower resolution MODerate-resolution Imaging Spectroradiometer (MODIS), and higher spatio-temporal resolution Spatial and Temporal Adaptive Reflectance Fusion Model (STARFM) LAI were generated. For PFTs, local land cover maps were developed, in addition to MODIS PFT. In South Korea, annual emissions of isoprene and monoterpenes in 2015 were estimated as 384 and 160 Gg/year, respectively, using STARFM LAI and Local PFT (Case 4). For North Korea, 340 Gg/year isoprene and 72 Gg/year monoterpenes emissions were estimated using STARFM LAI and MODIS PFT. These estimates were 14&ndash, 110% higher than when using MODIS LAI and MODIS PFT (Case 1). Inter-comparison with satellite-based inverse isoprene emission estimates from GlobEmission shows 32% (North Korea) to 34% (South Korea) overestimation in bottom-up data. Our new vegetation inputs improve MEGAN performance and resulting BVOC emission estimations. Performance of Weather Research and Forecasting (WRF) meteorological modeling requires improvement, especially for solar radiation, to avoid overestimation of isoprene emissions.

For the purpose of improving PM prediction skills in East Asia, we estimated a new background error covariance matrix (BEC) for aerosol data assimilation using surface PM2.5 observations that accounts for the uncertainties in anthropogenic emissions. In contrast to the conventional method to estimate the BEC that uses perturbations in meteorological data, this method additionally considered the perturbations using two different emission inventories. The impacts of the new BEC were then tested for the prediction of surface PM2.5 over East Asia using Community Multi-scale Air Quality (CMAQ) initialized by three-dimensional variational method (3D-VAR). The surface PM2.5 data measured at 154 sites in South Korea and 1,535 sites in China were assimilated every six hours during the Korea-United States Air Quality Study (KORUS-AQ) campaign period (1 May–14 June 2016). Data assimilation with our new BEC showed better agreement with the surface PM2.5 observations than that with the conventional method. Our method also showed closer agreement with the observations in 24-hour PM2.5 predictions with ~ 44 % fewer negative biases than the conventional method. We conclude that increased standard deviations, together with horizontal and vertical length scales in the new BEC, tend to improve the data assimilation and short-term predictions for the surface PM2.5. This paper also suggests further research efforts devoted to estimating the BEC to improve PM2.5 predictions.

The absence of up-to-date emissions has been a major impediment to accurately simulate aspects of atmospheric chemistry, and to precisely quantify the impact of changes of emissions on air pollution. Hence, a non-linear joint analytical inversion (Gauss–Newton method) of both volatile organic compounds (VOC) and nitrogen oxides (NOx) emissions is made by exploiting the Smithsonian Astrophysical Observatory (SAO) Ozone Mapping and Profile Suite Nadir Mapper (OMPS-NM) formaldehyde (HCHO) and the National Aeronautics and Space Administration (NASA) Ozone Monitoring Instrument (OMI) tropospheric nitrogen dioxide (NO2) retrievals during the Korea-United States Air Quality (KORUS-AQ) campaign over East Asia in May–June 2016. Effects of the chemical feedback of NOx and VOCs on both NO2 and HCHO are implicitly included through iteratively optimizing the inversion. Emissions estimates are greatly improved (averaging kernels > 0.8) over medium- to high-emitting areas such as cities and dense vegetation. The amount of total NOx emissions is mainly dictated by values reported in the MIX-Asia 2010 inventory. After the inversion we conclude a decline in the emissions (before, after, change) for China (87.94 ± 44.09 Gg/day, 68.00 ± 15.94 Gg/day, −23 %), North China Plain (NCP) (27.96 ± 13.49 Gg/day, 19.05 ± 2.50 Gg/day, −32 %), Pearl River Delta (PRD) (4.23 ± 1.78 Gg/day, 2.70 ± 0.32 Gg/day, −36 %), Yangtze River Delta (YRD) (9.84 ± 4.68 Gg/day, 5.77 ± 0.51 Gg/day, −41 %), Taiwan (1.26 ± 0.57 Gg/day, 0.97 ± 0.33 Gg/day, −23 %), and Malaysia (2.89 ± 2.77 Gg/day, 2.25 ± 1.34 Gg/day, −22 %), all of which have effectively implemented various stringent regulations. In contrast, South Korea (2.71 ± 1.34 Gg/day, 2.95 ± 0.58 Gg/day, +9 %) and Japan (3.53 ± 1.71 Gg/day, 3.96 ± 1.04 Gg/day, +12 %) experience an increase in NOx emissions potentially due to risen number of diesel vehicles and new thermal power plants. We revisit the well-documented positive bias of the model in terms of biogenic VOC emissions in the tropics. The inversion, however, suggests a larger growth of VOC (mainly anthropogenic) over NCP (25 %) than previously reported (6 %) relative to 2010. The spatial variation in both magnitude and sign of NOx and VOC emissions results in non-linear responses of ozone production/loss. Due to simultaneous decrease/increase of NOx/VOC over NCP and YRD, we observe an ~ 53 % reduction in the ratio of the chemical loss of NOx (LNOx) to the chemical loss of ROx (RO2 + HO2) transitioning toward NOx-sensitive regimes, which in turn, reduces/increases the afternoon chemical loss/production of ozone through NO2 + OH (−0.42 ppbv hr−1)/HO2 (and RO2) + NO (+0.31 ppbv hr−1). Conversely, a combined decrease in NOx and VOC emissions in Taiwan, Malaysia, and the southern China suppresses the formation of ozone. Ultimately, model simulations indicate enhancements of maximum daily 8-hour average (MDA8) surface ozone over China (0.62 ppbv), NCP (4.56 ppbv), and YRD (5.25 ppbv) due to the non-linear ozone chemistry, suggesting that emissions standards should be extended to regulate VOCs to be able to curb ozone production rates. Taiwan, Malaysia, and PRD stand out as the regions undergoing lower MDA8 ozone levels resulting from the NOx reductions occurring predominantly in NOx-sensitive regimes.

We examine O3 production and its sensitivity to precursor gases and boundary layer mixing in Korea by using a 3-D global chemistry transport model and extensive observations during the KORea-US cooperative Air Quality field study in Korea, which occurred in May–June 2016. During the campaign, observed aromatic species onboard the NASA DC-8 aircraft, especially toluene, showed high mixing ratios of up to 10 ppbv, emphasizing the importance of aromatic chemistry in O3 production. To examine the role of VOCs and NOx in O3 chemistry, we first implement a detailed aromatic chemistry scheme in the model, which reduces the normalized mean bias of simulated O3 mixing ratios from –26% to –13%. Aromatic chemistry also increases the average net O3 production in Korea by 37%. Corrections of daytime PBL heights, which are overestimated in the model compared to lidar observations, increase the net O3 production rate by ~10%. In addition, increasing NOx emissions by 50% in the model shows best performance in reproducing O3 production characteristics, which implies that NOx emissions are underestimated in the current emissions inventory. Sensitivity tests show that a 30% decrease in anthropogenic NOx emissions in Korea increases the O3 production efficiency throughout the country, making rural regions ~2 times more efficient in producing O3 per NOx consumed. Simulated O3 levels overall decrease in the peninsula except for urban and other industrial areas, with the largest increase (~6 ppbv) in the Seoul Metropolitan Area (SMA). However, with simultaneous reductions in both NOx and VOCs emissions by 30%, O3 decreases in most of the country, including the SMA. This implies the importance of concurrent emission reductions for both NOx and VOCs in order to effectively reduce O3 levels in Korea.

Accurate and consistent monitoring of anthropogenic combustion is imperative because of its significant health and environmental impacts, especially at city-to-regional scale. Here, we assess the performance of the Copernicus Atmosphere Monitoring Service (CAMS) global prediction system using measurements from aircraft, ground sites, and ships during the Korea-United States Air Quality (KORUS-AQ) field study in May to June 2016. Our evaluation focuses on CAMS CO and CO2 analyses as well as two higher-resolution forecasts (16 and 9 km horizontal resolution) to assess their capability in predicting combustion signatures over east Asia. Our results show a slight overestimation of CAMS CO2 with a mean bias against airborne CO2 measurements of 2.2, 0.7, and 0.3 ppmv for 16 and 9 km CO2 forecasts, and analyses, respectively. The positive CO2 mean bias in the 16 km forecast appears to be consistent across the vertical profile of the measurements. In contrast, we find a moderate underestimation of CAMS CO with an overall bias against airborne CO measurements of − 19.2 (16 km), − 16.7 (9 km), and − 20.7 ppbv (analysis). This negative CO mean bias is mostly seen below 750 hPa for all three forecast/analysis configurations. Despite these biases, CAMS shows a remarkable agreement with observed enhancement ratios of CO with CO2 over the Seoul metropolitan area and over the West (Yellow) Sea, where east Asian outflows were sampled during the study period. More efficient combustion is observed over Seoul ( d CO / d CO 2 = 9 ppbv ppmv −1 ) compared to the West Sea ( d CO / d CO 2 = 28 ppbv ppmv −1 ). This “combustion signature contrast” is consistent with previous studies in these two regions. CAMS captured this difference in enhancement ratios (Seoul: 8–12 ppbv ppmv −1 , the West Sea: ∼30 ppbv ppmv −1 ) regardless of forecast/analysis configurations. The correlation of CAMS CO bias with CO2 bias is relatively high over these two regions (Seoul: 0.64–0.90, the West Sea: ∼0.80 ) suggesting that the contrast captured by CAMS may be dominated by anthropogenic emission ratios used in CAMS. However, CAMS shows poorer performance in terms of capturing local-to-urban CO and CO2 variability. Along with measurements at ground sites over the Korean Peninsula, CAMS produces too high CO and CO2 concentrations at the surface with steeper vertical gradients ( ∼0.4 ppmv hPa −1 for CO2 and 3.5 ppbv hPa −1 for CO) in the morning samples than observed ( ∼0.25 ppmv hPa −1 for CO2 and 1.7 ppbv hPa −1 for CO), suggesting weaker boundary layer mixing in the model. Lastly, we find that the combination of CO analyses (i.e., improved initial condition) and use of finer resolution (9 km vs. 16 km) generally produces better forecasts.

We report the results of year-long PM2.5 (particulate matter less than 2.5 µm in diameter) simulations over Northeast Asia for the base year of 2013 under the framework of the Long-range Transboundary Air Pollutants in Northeast Asia (LTP) project. LTP is a tripartite project launched by China, Japan, and Korea for cooperative monitoring and modeling of the long-range transport (LRT) of air pollutants. In the modeling aspect in the LTP project, each country’s modeling group employs its own original air quality model and options. The three regional air quality models employed by the modeling groups are WRF-CAMx, NHM-RAQM2, and WRF-CMAQ. PM2.5 concentrations were simulated in remote exit-and-entrance areas associated with the LRT process over China, Japan, and Korea. The results showed apparent bias that remains unexplored due to a series of uncertainties from emission estimates and inherent model limitations. The simulated PM10 levels at seven remote exit-and-entrance sites were underestimated with the normalized mean bias of 0.4 ± 0.2. Among the four chemical components of PM2.5 (SO42−, NO3−, organic carbon (OC), and elemental carbon (EC)), the largest inter-model variability was in OC, with the second largest discrepancy in NO3−. Our simulation results also indicated that under considerable SO42− levels, favorable environments for ammonium nitrate formation were found in exit-and-entrance areas between China and Korea, and gas-aerosol partitioning for semi-volatile species of ammonium nitrate could be fully achieved prior to arrival at the entrance areas. Other chemical characteristics, including NO3−/SO42− and OC/EC ratios, are discussed to diagnose the LRT characteristics of PM2.5 in exit-and-entrance areas associated with transboundary transport over China, Japan, and Korea.

Enforcement of an air quality standard for PM2.5 in the Seoul metropolitan area (SMA) was enacted in 2015. From May to June of 2016, an international airborne and surface measurement campaign took place to investigate air pollution mechanisms in the SMA. The total and speciated PM2.5 concentrations since 2008 have been measured at an intensive monitoring site for the SMA operated by the National Institute of Environmental Research (NIER). To gain insight on the trends and sources of PM2.5 in the SMA in May, we analyze PM2.5 concentrations from 2009 to 2013 using the measurements and simulations from a 3-dimensional global chemical transport model, GEOS-Chem and its adjoint. The model is updated here with the latest regional emission inventory and diurnally varying NH3 emissions. Monthly average PM2.5 concentration measured by β-ray attenuation ranges from 28 (2010) to 45 (2013) μg/m3, decreased from 2009 to 2010, and then continuously increased until 2013. The model shows good agreement with the measurements for the daily average PM2.5 concentrations (R ≥ 0.5), and reproduces 10 out of 17 measured episodes exceeding the daily air quality standard (50 μg/m3). Using the GEOS-Chem adjoint model, we find that anthropogenic emissions from the Shandong region have the largest modeled influence on PM2.5 in Seoul in May. Average contributions to the high PM2.5 episodes simulated by the model are 39% from the Shandong region, 16% from the Shanghai region, 14% from the Beijing region, and 15% from South Korea. Anthropogenic SO2 emissions from South Korea are negligible with 90% of the total contribution originating from China. Findings from this study may guide interpretation of observations obtained in the KORUS-AQ measurement campaign.

The MIX inventory is developed for the years 2008 and 2010 to support the Model Inter-Comparison Study for Asia (MICS-Asia) and the Task Force on Hemispheric Transport of Air Pollution (TF HTAP) by a mosaic of up-to-date regional emission inventories. Emissions are estimated for all major anthropogenic sources in 29 countries and regions in Asia. We conducted detailed comparisons of different regional emission inventories and incorporated the best available ones for each region into the mosaic inventory at a uniform spatial and temporal resolution. Emissions are aggregated to five anthropogenic sectors: power, industry, residential, transportation, and agriculture. We estimate the total Asian emissions of 10 species in 2010 as follows: 51.3 Tg SO2, 52.1 Tg NOx, 336.6 Tg CO, 67.0 Tg NMVOC (non-methane volatile organic compounds), 28.8 Tg NH3, 31.7 Tg PM10, 22.7 Tg PM2.5, 3.5 Tg BC, 8.3 Tg OC, and 17.3 Pg CO2. Emissions from China and India dominate the emissions of Asia for most of the species. We also estimated Asian emissions in 2006 using the same methodology of MIX. The relative change rates of Asian emissions for the period of 2006–2010 are estimated as follows: −8.1 % for SO2, +19.2 % for NOx, +3.9 % for CO, +15.5 % for NMVOC, +1.7 % for NH3, −3.4 % for PM10, −1.6 % for PM2.5, +5.5 % for BC, +1.8 % for OC, and +19.9 % for CO2. Model-ready speciated NMVOC emissions for SAPRC-99 and CB05 mechanisms were developed following a profile-assignment approach. Monthly gridded emissions at a spatial resolution of 0.25° × 0.25° are developed and can be accessed from http://www.meicmodel.org/dataset-mix.

This study examines the effects of different foreign anthropogenic emissions inventories on predicted ozone concentrations in the Seoul Metropolitan Area (SMA), South Korea, and estimates changes in ozone due to emissions reductions. We ran the Community Multi-Scale Air Quality (CMAQ) model using the High-Order Decoupled Direct Method with three inventories of foreign anthropogenic emissions: (1) the Intercontinental Chemical Transport Experiment, Phase B (INTEX-B) 2006; (2) the Comprehensive Regional Emissions inventory for Atmospheric Transport Experiment (CREATE) 2010; and (3) the Model Inter-Comparison Study (MICS)-Asia 2010. All three inventories have different spatial distributions of emissions, yielding different modeled ozone concentrations. However, the ozone concentrations modeled for the SMA differ less than those modeled for large, foreign cities in the modeling domain. The simulations using INTEX-B 2006 and CREATE 2010 suggested greater reduction in ozone with NOx control than with VOCs control. All simulations show that (1) simultaneous reduction in NOx and VOCs leads to less ozone reduction than the sum of ozone reductions for individual NOx and VOCs controls and (2) ozone reductions are stronger for high ozone days than for low ozone days. Comparing the modeled reductions in the relative sense yields smaller differences between high and low ozone days than comparing the modeled reductions in the absolute sense. With a 20% reduction in only NOx emissions, the differences in MDA1O3 among the three inventories were between 0.3 and 0.7 ppb. Because air-quality planning often leads to defined tonnage reductions, we examined the model’s response to such a defined emissions reduction. Using the NOx reduction in China estimated by Zhao et al. (2013), we estimated that the differences in MDA1O3 among the three inventories were between 1.50 and 1.78 ppb. Based on these results, we recommend using different foreign anthropogenic emissions inventories to test future scenarios for air-quality control

Spatial and temporal variations of mercury, including dry and wet deposition fluxes, were assessed over Northeast Asia, targeting the Yellow Sea, using meteorology and chemistry models. Four modeling periods, each representative of one of the four seasons, were selected. Modeling results captured general patterns and behaviors, and fell within similar ranges with respect to observations. However, temporal variations of mercury were not closely matched, possibly owing to the effects of localized emissions. Modeling results indicated that dry deposition is correlated with wind speed, while wet deposition is correlated with precipitation amount. Overall, the wet deposition flux of 66 ng/m2-day was about twice as large as the dry deposition flux of 32 ng/m2-day, when averaged over the four modeling periods. Dry deposition occurred predominantly in the form of reactive gaseous mercury (RGM). In contrast, RGM accounted for only about two-thirds of wet deposition, while particulate mercury accounted for the remainder.

We have developed the Integrated Climate and Air Quality Modeling System (ICAMS) through the one-way nesting of global–regional models to examine the changes in the surface ozone concentrations over East Asia under future climate scenarios. Model simulations have been conducted for the present period of 1996–2005 to evaluate the performance of ICAMS. The simulated surface ozone concentrations reproduced the observed monthly mean concentrations at sites in East Asia with high R2 values (0.4–0.9), indicating a successful simulation to capture both spatial and temporal variability. We then performed several model simulations with the six IPCC SRES scenarios (A2, A1B, A1FI, A1T, B1, and B2) for the next three periods, 2016–2025 (the 2020s), 2046–2055 (the 2050s), and 2091–2100 (the 2090s). The model results show that the projected changes of the annual daily mean maximum eight-hour (DM8H) surface ozone concentrations in summertime for East Asia are in the range of 2–8 ppb, −3 to 8 ppb, and −7 to 9 ppb for the 2020s, the 2050s, and the 2090s, respectively, and are primarily determined based on the emission changes of NOx and NMVOC. The maximum increases in the annual DM8H surface ozone and high-ozone events occur in the 2020s for all scenarios except for A2, implying that the air quality over East Asia is likely to get worse in the near future period (the 2020s) than in the far future periods (the 2050s and the 2090s). The changes in the future environment based on IPCC SRES scenarios would also influence the change in the occurrences of high-concentrations events more greatly than that of the annual DM8H surface ozone concentrations. Sensitivity simulations show that the emissions increase is the key factor in determining future regional surface ozone concentrations in the case of a developing country, China, whereas a developed country, Japan would be influenced more greatly by effects of the regional climate change than the increase in emissions.

We investigate ozone air quality changes in 2050 caused by global changes in climate and anthropogenic emissions of ozone precursors by using a global chemical transport model driven by meteorological fields from a general circulation model. We use projected emissions based on the Representative Concentration Pathway (RCP) scenarios and conduct model simulations to quantify the effects of climate and emission changes on future air quality, focusing on ozone in surface air. Our model results show that annual mean concentrations of surface ozone will be lower in 2050 relative to 2000 by −3.3, −3.7, and −4.2 ppbv under RCP6.0, RCP4.5, and RCP2.6, respectively. In contrast, the RCP8.5 projection results in a slight increase of 2.1 ppbv caused by a methane increase. The ozone reductions are driven primarily by decreases in NOx emission, which dominate the climate penalty on ozone driven by temperature increases. We also estimate the effect of 21st century climate change on ozone air quality, assuming no changes in anthropogenic emissions of ozone precursors in the future. We further use a statistical method to analyze the results in order to quantify the effect of each meteorological variable change on ozone concentration in summer. Temperature increase is found to result in ozone increases of up to 2.2 ppbv over land. Ozone over the oceans, however, is largely reduced with specific humidity increase, particularly in the Northern Hemisphere, where the ozone concentration decreases by 0.8 ppbv. We find that future increases in natural NOx emissions from lightning and soil make an important contribution to the formation of nitric acid and might seriously offset future decreases in nitrogen deposition caused by anthropogenic NOx emission reduction.

We use a 3-D regional atmospheric chemistry transport model (WRF-Chem) to examine ozone dry deposition in East Asia, which is an important but uncertain research area because of insufficient observation and numerical studies focusing on East Asia. Here we compare two widely used dry deposition parameterization schemes, the Wesely and M3DRY schemes, which are used in the WRF-Chem and Community Multiscale Air Quality (CMAQ) models, respectively. Simulated ozone dry deposition velocities with the two schemes under identical meteorological conditions show considerable differences (a factor of 2) owing to surface resistance parameterization discrepancies. Resulting ozone concentrations differ by up to 10 ppbv for a monthly mean in May when the peak ozone typically occurs in East Asia. An evaluation of the simulated dry deposition velocities shows that the Wesely scheme calculates values with more pronounced diurnal variation than the M3DRY and results in a good agreement with the observations. However, we find significant changes in simulated ozone concentrations using the Wesely scheme but with different surface type data sets, indicating the high sensitivity of ozone deposition calculations to the input data. The need is high for observations to constrain the dry deposition parameterization and its input data to improve the use of air quality models for East Asia.

Plant functional type (PFT) distributions affect the results of biogenic emission modeling as well as O3 and particulate matter (PM) simulations using chemistry-transport models (CTMs). This paper analyzes the variations of both surface biogenic volatile organic compound (BVOC) emissions and O3 concentrations due to changes in the PFT distributions in the Seoul Metropolitan Areas, Korea. The Fifth-Generation NCAR/Pennsylvania State Meso-scale Model (MM5)/the Model of Emissions of Gases and Aerosols from Nature (MEGAN)/the Sparse Matrix Operator Kernel Emissions (SMOKE)/the Community Multiscale Air Quality (CMAQ) model simulations were implemented over the Seoul Metropolitan Areas in Korea to predict surface O3 concentrations for the period of 1 May to 31 June 2008. Starting from a performance check of CTM predictions, we consecutively assessed the effects of PFT area deviations on the MEGAN BVOC and CTM O3 predictions, and we further considered the basis of geospatial and statistical analyses. The three PFT data sets considered were (1) the Korean PFT, developed with Korea-specific vegetation database; (2) the CDP PFT, adopted from the community data portal (CDP) of US National Center for Atmospheric Research in the United States (NCAR); (3) MODIS PFT, reclassified from the NASA Terra and Aqua combined land cover products. Although the CMAQ performance check reveals that all of the three different PFT data sets are applicable choices for regulatory modeling practice, noticeable primary data (i.e., PFT and Leaf Area Index (LAI)) was observed to be missing in many geographic locations. Based on the assessed effect of such missing data on CMAQ O3 predictions, we found that this missing data can cause spatially increased bias in CMAQ O3. Thus, it must be resolved in the near future to obtain more accurate biogenic emission and chemistry transport modeling results. Comparisons of MEGAN biogenic emission results with the three different PFT data showed that broadleaf trees (BTs) are the most significant contributor, followed by needleleaf trees (NTs), shrub (SB), and herbaceous plants (HBs) to the total BVOCs. In addition, isoprene from BTs and terpene from NTs were recognized as significant primary and secondary BVOC species in terms of BVOC emissions distributions and O3-forming potentials in the study domain. A geographically weighted regression analysis with locally compensated ridge (LCR-GWR) with the different PFT data (δO3 vs. δPFTs) suggests that addition of BT, SB, and NT areas can contribute to O3 increase, whereas addition of an HB area contributes to O3 decrease in the domain. Assessment results of the simulated spatial and temporal changes of O3 distributions with the different PFT scenarios reveal that hourly and local impacts from the different PFT distributions on occasional inter-deviations of O3 are quite noticeable, reaching up to 13 ppb. The simulated maximum 1 h O3 inter-deviations between different PFT scenarios have an asymmetric diurnal distribution pattern (low in the early morning, rising during the day, peaking at 05:00 p.m., and decreasing during the night) in the study domain. Exponentially diverging hourly BVOC emissions and O3 concentrations with increasing ambient temperature suggest that the use of different PFT distribution data requires much caution when modeling (or forecasting) O3 air quality in complicated urban atmospheric conditions in terms of whether uncertainties in O3 prediction results are expected to be mild or severe.

Significant differences were found between two particulate sulfate size-distributions measured using a MOUDI impactor at Gosan, Jeju Island, Korea, and simulated via the Lagrangian photochemical model under a condition of aerosol internal mixing between mineral dust and urban pollution particles. It was suspected that these differences might have resulted from: (1) the assumption of aerosol internal mixing and (2) the uses of identical reaction probabilities (γ) of the gaseous sulfate precursors (SO2 and H2SO4) onto both urban pollution particles and mineral dust in the Lagrangian photochemical model simulations. In this study; therefore, some cases of aerosol external mixing between urban-derived pollution aerosols and mineral dust were investigated, with different magnitudes of γ for the gas-phase sulfate precursors onto the two different condensing media. The model simulations under the external mixing condition, with different magnitudes of the reaction probabilities (γi,urban and γi,dust) onto urban pollution particles and mineral dust, successfully reproduced the size-dependent particulate sulfate formation measured at the Gosan station. Further attempts were made to approximate the magnitudes of γSO2,urban and γH2SO4,dust under external mixing state conditions with the fixed γSO2,dust and γH2SO2,urban values of 10−4 and 1.0. The best-estimates of γSO2,urban and γH2SO4,dust found in this study were in the orders of 10−4–10−5 and 10−2–10−3, respectively.

We examine the effects of below-cloud scavenging on regional aerosol simulations over East Asia using wet deposition fluxes observed at Acid Deposition Monitoring Network in East Asia (EANET) sites and the Community Multiscale Air Quality (CMAQ) model together with a new below-cloud-scavenging scheme. Typical air quality models, including CMAQ, assume below-cloud scavenging as a simple first-order process with a constant or simple form depending on rain intensity. The scheme used here accounts for the collection efficiency, terminal velocity of raindrops, raindrop-size distributions, and particle-size distributions, which are important factors affecting below-cloud scavenging. We conduct model simulations for spring 2001, including baseline and sensitivity simulations. Our analysis mainly focuses on May 2001 to rule out the effect of dust aerosols. Simulated wet deposition fluxes of SO42−, NO3−, and NH4+ by the new scheme are increased by 103, 16, and 108%, respectively, relative to the baseline simulation and show better agreement with observations. The effect of below-cloud scavenging on coarse particles is even greater, producing wet deposition fluxes two orders of magnitude higher than the baseline. The resulting changes in the model indicate the considerable impacts of below-cloud scavenging on regional aerosol simulations over East Asia, where both anthropogenic emissions and natural sources of aerosols are present throughout the year. An accurate wet scavenging simulation is critical to simulate the atmospheric burden and wet deposition fluxes of both fine-mode and coarse-mode aerosols over East Asia.

South Korea has recently achieved developed country status with the second largest megacity in the world, the Seoul Metropolitan Area (SMA). This study provides insights into future changes in air quality for rapidly emerging megacities in the East Asian region. We present total OH reactivity observations in the SMA conducted at an urban Seoul site (May–June, 2015) and a suburban forest site (Sep, 2015). The total OH reactivity in an urban site during the daytime was observed at similar levels (∼15 s−1) to those previously reported from other East Asian megacity studies. Trace gas observations indicate that OH reactivity is largely accounted for by NOX (∼50%) followed by volatile organic compounds (VOCs) (∼35%). Isoprene accounts for a substantial fraction of OH reactivity among the comprehensive VOC observational dataset (25–47%). In general, observed total OH reactivity can be accounted for by the observed trace gas dataset. However, observed total OH reactivity in the suburban forest area cannot be largely accounted for (∼70%) by the trace gas measurements. The importance of biogenic VOC (BVOCs) emissions and oxidations used to evaluate the impacts of East Asian megacity outflows for the regional air quality and climate contexts are highlighted in this study.

We examine the meteorological responses due to the probable eruption of Mt. Baekdu using an off-line Climate-Chemistry model that is composed of the National Center for Atmospheric Research (NCAR) Climate Atmosphere Model version 3 (CAM3) and a global chemistry transport model (GEOS-Chem). Using the aerosol dataset from the GEOS-Chem driven by GEOS-5 meteorology, experiment and control simulations of the climate model are performed and their meteorological differences between the two simulations are analyzed. The magnitudes of volcanic eruption and column injection height were presumably set to 1/200 of the Mt. Pinatubo eruption and 9 km, respectively. Significant temperature drop in the lower troposphere (850 hPa), which is mainly due to a direct effect of prescribed volcanic aerosols from Mt. Baekdu, has been simulated up to about −4 K. The upper atmosphere (150 hPa) right above the volcano, however, shows significant warming due to the absorption of the infrared radiation by volcanic aerosols. As a result of the volcanic eruption in the climate model, wave-like patterns are shown in both the geopotential height and horizontal wind. The changes in the lower atmospheric temperature are well associated with the modification of the atmospheric circulation through the hydrostatic balance. In spite of limitations in our current simulations due to several underlying assumptions, our results could give a clue to understanding the meteorological impacts from Mt. Baekdu eruptions that are currently attracting considerable public attention.

We examine the impacts of aerosols on regional meteorology due to intense Siberian forest fires occurred in May 2003 using both reanalysis data and global model simulations. Our analysis of the NCEP-DOE reanalysis data shows 99% statistical significant changes in meteorological variables over East Asia in May 2003 relative to the 30 years climatology. In particular a significant surface cooling was observed up to −3.5 K over Siberia and extended to the North Pacific region with the surface pressure increases up to 5.6 hPa. Whereas, smoke aerosols affected the large-scale circulations and resulted in the increases in rainfall rates of 2.9 mm day −1 averaged over the NW Pacific (10–35°N, 130–170°E). We use the climate model simulations with and without biomass burning emissions over Siberia to examine the effects of smoke aerosols on the regional meteorology. The simulated results show consistent changes in meteorological variables including surface temperature, surface pressure and precipitation rates with the observations over East Asia and the NW Pacific, which support that the observed changes are likely due to smoke aerosols from the Siberian forest fires. The implication is that smoke aerosols from the forest fires should be properly considered to correctly simulate both regional climate and synoptic scale weather patterns.

We estimated the source contributions to carbonaceous aerosol concentration in Korea on the basis of Intercontinental Chemical Transport Experiment Phase B (INTEX-B) anthropogenic emissions and satellite-derived biomass burning emissions by using a nested version of GEOS-Chem with a spatial resolution of 0.5 � � 0.667 � for the period March 2006eFebruary 2007. First, we evaluated the model by comparing the simulated and observed aerosol concentrations at East Asia Network (EANET) sites and at a site in Korea. The results indicate that the model reproduces the variability and magnitudes of the observed SO4 2� ,N O 3 � , and NH 4 þ concentrations in Korea and those of the observed PM 10 concentrations in East Asia. However, the organic carbon (OC) and black carbon (BC) aerosol concentrations estimated by the model are lower than those observed in Korea by a factor of 2, especially in winter. This underestimation is likely due to extremely low domestic anthropogenic emissions and lack in seasonal variation. Source adjustments using a simple fitting and the Emission Database for Global Atmospheric Research (EDGAR) monthly allocation factors for seasonal variation yield significantly improved model results (R 2

Elevated levels of formaldehyde (HCHO) along the ship corridors have been observed by satellite sensors, such as ESA/ERS-2 GOME (Global Ozone Monitoring Experiment), and were also simulated by global 3-D chemistry-transport models. In this study, three likely sources of the elevated HCHO levels in the ship plumes as well as their contributions to the elevated HCHO levels (budget) were investigated using a newly-developed ship-plume photochemical/dynamic model: (1) primary HCHO emission from ships; (2) secondary HCHO production via the atmospheric oxidation of non-methane volatile organic compounds (NMVOCs) emitted from ships; and (3) atmospheric oxidation of CH4 within the ship plumes. For this ship-plume modelling study, the ITCT 2K2 (Intercontinental Transport and Chemical Transformation 2002) ship-plume experiment, which was carried out about 100 km off the coast of California on 8 May 2002 (11:00 local standard time), was chosen as a base study case because it is the best defined in terms of (1) meteorological data, (2) in-plume chemical composition, and (3) background chemical composition. From multiple ship-plume model simulations for the ITCT 2K2 ship-plume experiment case, CH4 oxidation by elevated levels of in-plume OH radicals was found to be the main factor responsible for the elevated levels of HCHO in the ITCT 2K2 ship-plume. More than ~88% of the HCHO for the ITCT 2K2 ship-plume is produced by this atmospheric chemical process, except in the areas close to the ship stacks where the main source of the elevated HCHO levels would be primary HCHO from the ships (due to the deactivation of CH4 oxidation from the depletion of in-plume OH radicals). Because of active CH4 oxidation by OH radicals, the instantaneous chemical lifetime of CH4 (τCH4) decreased to ~0.45 yr inside the ship plume, which is in contrast to τCH4 of ~1.1 yr in the background (up to ~41% decrease) for the ITCT 2K2 ship-plume case. A variety of likely ship-plume situations at three different latitudinal locations within the global ship corridors was also studied to determine the enhancements in the HCHO levels in the marine boundary layer (MBL) influenced by ship emissions. It was found that the ship-plume HCHO levels could be 19.9–424.9 pptv higher than the background HCHO levels depending on the latitudinal locations of the ship plumes (i.e., intensity of solar radiation and temperature), MBL stability and NOx emission rates. On the other hand, NMVOC emissions from ships were not found to be a primary source of photochemical HCHO production inside ship plumes due to their rapid and individual dilution. However, the diluted NMVOCs would contribute to the HCHO productions in the background air.

Household fuel use in developing countries, particularly as biomass and coal, is a major source of carbonaceous aerosols and other air pollutants affecting health and climate. Using state-of-the-art emission inventories, a global three-dimensional photochemical tracer/transport model of the troposphere, and a global radiative transfer model based on methods presented in the latest IPCC Assessment Report (2007-AR4), we estimate the radiative forcing (RF) attributable to household fuel combustion in Asia in terms of current global annual-mean RF and future global integrated RF for a one-year pulse of emissions (2000) over two time horizons (100 and 20 years). Despite the significant emissions of black carbon (BC) aerosols, these estimates indicate that shorter-lived (non-Kyoto) air pollutants from household fuel use in the region overall seem to exert a small net negative RF because of the strong influence of reflective aerosols. There are, however, major uncertainties in emission estimates for solid fuel burning, and about the sustainability of household fuel wood harvesting in Asia (the carbon neutrality of harvesting). In addition, there is still substantial uncertainty associated with the BC radiative forcing. As a result we find that the sign of the RF from household biomass burning in the region cannot be established. While recognizing the value of integrating climate change and air pollution policies, we are concerned that for a ‘Kyoto style’ post-Kyoto treaty (with global cap-and-trade and the Global Warming Potential as the metric) expanding the basket of components with a selection of short-lived species without also including the wider range of co-emitted species may lead to unintended consequences for global-scale climate. Additional measurement, modelling, and policy research is urgently needed to reduce the uncertainties so that the net impact on climate of emissions and mitigation measures in this sector can be accurately assessed.

In this study, background concentration sites of Deokjeok and Gosan, which were deemed suitable for monitoring the impact of long-range transported air pollutants, were selected. An investigation of the source types of pollutants, their locations, and relative quantitative contributions to the particulate concentrations at both sites using appropriate methodologies to make initial estimations was conducted. Episodic measurements of PM2.5, PM10, and size distribution, along with its ion and carbon components were performed from 2005 to 2007, and a comprehensive analysis of the results was conducted utilizing back trajectory analysis. As for frequency of wind direction, it was quite apparent that the two sites are heavily influenced by air masses originating from the eastern and northern regions of China. For PM2.5 and PM10, the mass concentrations from north and east China were higher than other cases, originating from the ocean. In the northerly-wind case, meteorological properties for Deokjeok and Gosan and the influence of carbon emissions from northwest Korea resulted in a changing of air mass properties during transport. As was the case with mass concentration, the highest contribution for ionic and carbon components of PM2.5 and PM10 for both sites appeared for the westerly wind case. A specially high relative contribution, greater than 1.4 times, was apparent in the secondary aerosol case because of a large influence of long-range transported pollutants from east China. Carbon components exhibited different behaviors for the northerly and westerly wind cases compared with secondary aerosol. The major reason for this discrepancy appears to be the carbon emissions from northwest Korea.

An assessment of how future climate change will impact regional air quality requires projecting emissions many decades into the future in a consistent manner. An approach that integrates the impact of both the current regulations and the longer-term national and global trends is developed to construct an emissions inventory (EI) for North America for the mid-century in support of a regional modeling study of ozone and particulate matter (PM) less than or equal to 2.5 microm (PM2.5). Because the time horizon of such a distant projection is beyond that of EIs used in typical modeling studies, it is necessary to identify a practical approach that allows the emission projections to account for emission controls and climatic and energy-use changes. However, a technical challenge arises because this requires integration of various different types of information with which emissions from human activities are associated. Often, emission information in global models has less detail and uses coarser spatiotemporal resolution. The method developed here is based on data availability, spatiotemporal coverage and resolution, and future-scenario consistency (i.e., Intergovernmental Panel on Climate Change Special Report on Emissions Scenarios [IPCC SRES] A1B), and consists of two major steps: (1) near-future EI projection (to the year 2020), and (2) longer-term EI projection (to mid-century). The first step is based closely on the U.S. Environmental Protection Agency Clean Air Interstate Rule EI, the Environment Canada EI, as well estimates of Mexico's EI; whereas the second step follows approaches proposed by the EI from the Integrated Model to Assess the Global Environment (IMAGE), developed by Netherlands's National Institute for Public Health and the Environment (RIVM). For the United States, the year-2050 emissions for nitrogen oxides (NOx), sulfur dioxide (SO2), PM2.5, anthropogenic volatile organic compounds (VOCs), and ammonia are projected to change by -55, -55, -30, -40, and +20%, respectively, compared with 2001. NOx and SO2 emission changes are very similar in total amount but different in sectoral contribution. The projected emission trends for Canada and Mexico differ considerably. After taking into account the modeled climate changes, biogenic VOC emission increases from three countries overwhelm the decreases in anthropogenic VOC emissions, leading to a net small increase (approximately 2%) in overall VOC emissions.

Potential impacts of global climate and emissions changes on regional air quality over southern (western and eastern) Canada and northern Mexico are examined by comparing future summers' (i.e., 2049–2051) average regional O3 and PM2.5 concentrations with historic concentrations (i.e., 2000–2002 summers). Air quality modeling was conducted using CMAQ and meteorology downscaled from the GISS-GCM using MM5. Emissions for North America are found using US EPA, Mexican and Canadian inventories and projected emissions following CAIR and IPCC A1B emissions scenario. Higher temperatures for all sub-regions and regional changes in mixing height, insolation and precipitation are forecast in the 2049-2051 period. Future emissions are calculated to be lower over both Canadian sub-regions, but higher over northern Mexico. Global climate change, alone, is predicted to affect PM2.5 concentrations more than O3 for the projections used in this study: average daily maximum eight (8) hour O3 (M8hO3) concentrations are estimated to be slightly different in all examined sub-regions while average PM2.5 concentrations are estimated to be higher over both Canadian sub-regions (8% over western and 3% over eastern) but 11% lower over northern Mexico. More days are forecast where M8hO3 concentrations are over 75 ppb in all examined sub-regions but the number of days where PM2.5 concentration will be over 15 μg/m3 is projected higher only over western Canada. Climate change combined with the projected emissions lead to greater change in pollutant concentrations: average M8hO3 concentrations are simulated to be 6% lower over western Canada and 8% lower over eastern Canada while average PM2.5 concentrations are simulated to be 5% lower over western Canada and 11% lower over eastern Canada. Although future emissions over northern Mexico are projected higher, pollutant concentrations are simulated to be lower due to US emissions reductions. Global climate change combined with the projected emissions will decrease average M8hO3 4% and PM2.5 17% over northern Mexico. Significant reductions in the number of days where M8hO3 concentrations are over 75 ppb and PM2.5 concentration over 15 μg/m3 are also projected with a significant reduction in peak values.

An inverse modeling method using the four-dimensional variational data assimilation approach is developed to provide a top-down estimate of mercury emission inventory in China. The mercury observations on board the C130 aircraft during the Asian Pacific Regional Aerosol Characterization Experiment (ACE-Asia) campaign in April 2001 are assimilated into a regional chemical transport model, STEM. Using a 340 Mg of elemental mercury emitted in 1999, the assimilation results in an increase in Hg 0 emissions for China to 1140 Mg in 2001. This is an upper limit amount of the elemental mercury required in China. The average emission-scaling factor is ∼3.4 in China. The spatial changes in the mercury emissions after the assimilation are also evaluated. The largest changes are estimated on the China north-east coastal areas and the areas of north-center China. The influences of the observation and inventory uncertainties and the initial and boundary conditions on the emission estimates are discussed. Increasing the boundary conditions of Hg from 1.2 to 1.5 ng m −3 , results in a top-down estimate of Hg 0 emissions for China of 718 Mg, and leads the average scaling factor from 3.4 to 2.1.

In this study, the accuracy of NH3 emissions in East Asia is evaluated by a comparison of measured and predicted NH4NO3 concentrations. For the prediction of particulate NH4NO3 concentrations, this study uses the USEPA Models-3/Community Multi-scale Air Quality (Models-3/CMAQ) model. The measurement data are collected from 4 ground-based stations (Beijing, Shanghai, Qingdao, and Kangwha) and ACE-ASIA C130 Flights #6, #7, and #10. The four ground-based stations and air flight tracks are located in and around the Yellow Sea in East Asia. According to the results, the predicted fine-mode NH4+concentrations are 1.2–3.8 times overestimated compared to those measured on the mass basis, and fine-mode NO3− concentrations are 1.9–7.6 times overestimated on the mass basis. It is also revealed in this study that aberrantly high predicted fine-mode NO3− concentrations in East Asia can be attributed to the overestimated NH3 emissions. The predicted gas-phase NH3 concentrations and estimated NH3 emissions are likely to be 1.2–3.8 times overestimated in East Asia on the mass basis. Therefore, it is recommended that approximately 20–75% reduced NH3 emission fields should be used in future modeling studies for East Asia.

Long-range transport of pollutants influenced by anthropogenic and natural emission sources in East Asia is investigated by using backward trajectory analysis along the NASA TRACE-P flight tracks and a numerical simulation with the three-dimensional chemical transport model (STEM-2k1). Observation-based regional distributions of trace gases are reconstructed using the observations obtained by measurements on board the DC-8 and P3-B aircrafts. Systematic features of the spatial distribution for each species are identified. It is found that the observed concentrations of CO and some NMHCs, and the ratios between these species, are highly associated with the source distribution features and their regional characteristics. Reconstructed fields of the observed and modeled ethane/CO and ethane/propane are found to reproduce well the estimated emission ratios in East Asia. We also investigated the time rate of change of the concentration of species and their ratio along the trajectory. From this analysis the propane/ethane and propane/acetylene ratios are shown to preserve their emission ratios during regional transport. However systematic differences in the propane vs. acetylene/CO relationships are found between the model and observation values. This analysis suggests that further efforts are needed to improve the estimates of biomass burning emissions in SE Asia. The results presented in this paper also suggest ways to further extend the capabilities to derive observation-based inventories.

The relationship between SO 2 emissions and the effective particle radius of low-level water clouds ( r e ) over China was investigated to determine anthropogenic effects on clouds. Sulfur dioxide emission values were obtained from a statistical inventory, and r e origins were retrieved by satellite remote sensing on a 0.5° grid. Comparisons between annual mean SO 2 emissions and r e showed generally decreasing r e values, explained by the Twomey effect. The existence of the Twomey effect is supported by comparisons with simulated aerosol optical depths. Results further suggest that clouds over land show sensitivity to the Twomey effect as well as clouds over the ocean.

Emissions in East Asia for 1993 by administrative units and source types are estimated to support regional emission assessments and transport modeling studies. Total emission of SOx, NOx, soil NOx, N2O, and NH3 are 24 150, 12 610, 1963, 908, and 8263 kton yr-1, respectively.China's emission contribution is the highest for every species.The area sources are the most significant source type for SOx and NOx, but the fraction due to mobile source is highest for NOx. Major LPSs are located from the middle to the east part of China, south and middle-west part of South Korea, and the east part of Japan. The area sources of SOx show a pattern similar to population density, whereas NH3 shows a strong landuse dependency. Detail emissions analysis reveals higher SOx emission `cores' within each province. The estimated emissions are used to estimate sulfur deposition in the regions. The seasonal average sulfur distribution amounts are estimated from the ATMOS2 chemical transport model. The results showed anti-correlation with temperature for sulfur (SO2 + SO4-2) concentrations and a positive correlation with rainfall for deposition.

An intercomparison study involving eight long-range transport models for sulfur deposition in East Asia has been initiated. The participating models included Eulerian and Lagrangian frameworks, with a wide variety of vertical resolutions and numerical approaches. Results from this study, in which models used common data sets for emissions, meteorology, and dry, wet and chemical conversion rates, are reported and discussed. Model results for sulfur dioxide and sulfate concentrations, wet deposition amounts, for the period January and May 1993, are compared with observed quantities at 18 surface sites in East Asia. At many sites the ensemble of models is found to have high skill in predicting observed quantities. At other sites all models show poor predictive capabilities. Source–receptor relationships estimated by the models are also compared. The models show a high degree of consistency in identifying the main source–receptor relationships, as well as in the relative contributions of wet/dry pathways for removal. But at some locations estimated deposition amounts can vary by a factor or 5. The influence of model structure and parameters on model performance is discussed. The main factors determining the deposition fields are the emissions and underlying meteorological fields. Model structure in terms of vertical resolution is found to be more important than the parameterizations used for chemical conversion and removal, as these processes are highly coupled and often work in compensating directions.

Uncertainties in calculated impacts of climate forecasts on future regional air quality are investigated using downscaled MM5 meteorological fields from the NASA GISS and MIT IGSM global models and the CMAQ model in 2050 in the continental US. Differences between three future scenarios: high-extreme, low-extreme and base case, are used for quantifying effects of climate uncertainty on regional air quality. GISS, with the IPCC A1B scenario, is used for the base case simulations. IGSM results, in the form of probabilistic distributions, are used to perturb the base case climate to provide the high- and low-extreme scenarios. Impacts of the extreme climate scenarios on concentrations of summertime fourth-highest daily maximum 8-h average ozone are predicted to be up to 10 ppbV (about one-seventh of the current US ozone standard of 75 ppbV) in urban areas of the Northeast, Midwest and Texas due to impacts of meteorological changes, especially temperature and humidity, on the photochemistry of tropospheric ozone formation and increases in biogenic VOC emissions, though the differences in average peak ozone concentrations are about 1–2 ppbV on a regional basis. Differences between the extreme and base scenarios in annualized PM2.5 levels are very location dependent and predicted to range between −1.0 and +1.5 μg m−3. Future annualized PM2.5 is less sensitive to the extreme climate scenarios than summertime peak ozone since precipitation scavenging is only slightly affected by the extreme climate scenarios examined. Relative abundances of biogenic VOC and anthropogenic NOx lead to the areas that are most responsive to climate change. Overall, planned controls for decreasing regional ozone and PM2.5 levels will continue to be effective in the future under the extreme climate scenarios. However, the impact of climate uncertainties may be substantial in some urban areas and should be included in assessing future regional air quality and emission control requirements., United States. Environmental Protection Agency (Science To Achieve Results (STAR) grant No. RD83096001), United States. Environmental Protection Agency (Science To Achieve Results (STAR) grant No. RD82897602), United States. Environmental Protection Agency (Science To Achieve Results (STAR) grant No. RD83107601), East Tennessee State University

Responses of ozone and PM2.5 to emission changes are coupled because of interactions between their precursors. Here we show the interdependencies of ozone and PM2.5 responses to emission changes in 2001 and 2050, with the future case accounting for both currently planned emission controls and climate change. Current responses of ozone and PM2.5 to emissions are quantified and linked on a daily basis for five cities in the continental United States: Atlanta, Chicago, Houston, Los Angeles, and NewYork. Reductions in anthropogenic NO(x) emissions decrease 24-h average PM2.5 levels but may either increase or decrease daily maximum 8-h average ozone levels. Regional ozone maxima for all the cities are more sensitive to NO(x) reductions than at the city center, particularly in New York and Chicago. Planned controls of anthropogenic NO(x) emissions lead to more positive responses to NO(x) reductions in the future. Sensitivities of ozone and PM2.5 to anthropogenic VOC emissions are predicted to decrease between 2001 and 2050. Ammonium nitrate formation is predicted to be less ammonia-sensitive in 2050 than 2001 while the opposite is true for ammonium sulfate. Sensitivity of PM2.5 to SO2 and NO(x) emissions changes little between 2001 and 2050. Both ammonium sulfate and ammonium nitrate are predicted to decrease in sensitivity to SO2 and NO(x) emissions between 2001 and 2050. The complexities, linkages, and daily changes in the pollutant responses to emission changes suggest that strategies developed to meet specific air quality standards should consider other air quality impacts as well.

[1] Potential impacts of global climate change and emissions on the total nitrogen and sulfur deposition over the US are investigated. Three future years' annual average deposition rates (i.e., 2049–2051) are compared with historic ones (i.e., 2000–2002) accounting for existing US and individual State's emission regulations and strategies. Impacts of global climate change alone on regional nitrogen and sulfur deposition are small compared to impacts from emission control-related reductions for the projections used in this study. The combined effect of climate change and emission reductions is a decrease in the annual average nitrogen and sulfur deposition over the US. Reduced nitrogen species dominate oxidized nitrogen deposition in the future. Spatial distribution plots for both components show lower deposition rates in the future mainly in the middle and eastern States where reductions in NOx and SO2 emissions are more pronounced.

Simulated future summers (i.e., 2049-2051) and annual (i.e., 2050) average regional O 3 and PM2.5 concentrations over North America are compared with historic (i.e., 2000-2002 summers and all of 2001) levels to investigate the potential impacts of global climate change on regional air quality. Meteorological inputs to the CMAQ chemical transport model are developed by downscaling the GISS Global Climate Model simulations using an MM5-based regional climate model. Future-year emissions for North America are developed by growing the US EPA CAIR inventory, Mexican and Canadian emissions and by using the IMAGE model with the IPCC A1B emissions scenario that is also used in projecting future climate. Reductions of more than 50% in NOX and SO2 emissions are forecast. The impacts of global climate change alone on regional air quality are small compared to impacts from emission control-related reductions in the US and Canada. The combined effect of climate change and emission reductions lead to a 20% decrease (regionally varying from -11% to -28% regionally) in the mean summer maximum daily 8-hr ozone levels (M8hO3) over the US, -8% over Canada and -10% over Northern Mexico. The mean annual PM2.5 concentrations are estimated to be 23% lower (varies from -9% tomore » -32%) over the US, -7% and -15% over Western and Eastern Canada, respectively and -25% over Northern Mexico. Major reductions are expected in sulfate, nitrate and ammonium fractions of annually-averaged PM2.5 for all sub-regions. The limited reduction in organic carbon over the US and Northern Mexico and the higher concentrations over Canada suggests that organic carbon will be the dominant component of PM2.5 mass over most of the continent in the future. Regionally, the Eastern US benefits more than the rest of the regions from reductions in both M8hO3 and PM2.5, due to both spatial variations in the meteorological and emissions changes. Reduction in the higher M8hO3 concentrations is also estimated for all sub-regions and less days with M8hO3 above the air quality standards in urban sites with Atlanta in the Southeast benefiting most.« less

[1] The regional radiative impact of biomass-burning aerosols in Asia is estimated using the new and detailed emission data during the experimental period of Transport and Chemical Evolution over the Pacific (TRACE-P) in March 2001. Integration of the USA National Oceanic and Atmospheric Administration (NOAA) Hybrid Single-Particle Lagrangian Integrated Transport model (HYSPLIT) and a solar radiative transfer model (CLIRAD-SW) allow us to simulate the spatial and temporal distributions of black carbon (BC) and organic carbon (OC) aerosols from biomass burning in the South Asian region. It also allows us to estimate further their aerosol optical properties and radiative forcing. We find that an anticyclone over Bay of Bengal dominates the transport of pollutants of the South Asian region. The monthly mean surface concentration of OC and BC is 1.1 μg m−3 in this region. Western Myanmar has the maximum value, with the concentration reaching 12.5 μg m−3. The monthly mean clear-sky direct shortwave radiative forcing ranges from −1.9 to 0.4 W m−2 at the top of the atmosphere and from −0.5 to −12.0 W m−2 at surface, resulting in an increase of the atmospheric heating rate from 0.01 to 0.3°C day−1. Owing to the spatial distributions of the aerosol optical depth ratio (OC/BC) and the surface albedo, there is a strong gradient of heating rate near the source regions, which may modify local circulations.

[1] Mercury tracer model simulations are performed to support the analysis of the total gas phase mercury (TGM) observations on 15 flights of the NSF/NCAR C-130 aircraft during the Asian Pacific Regional Aerosol Characterization Experiment (ACE-Asia) campaign conducted during April 2001. Ninety-seven percent of the observed mercury concentrations are greater than 1.2 ng/m3. The mean value of the observations is 1.9 ng/m3. No simple relationships between Hg-CO and Hg-total sulfur are found; however, strong correlations are observed in individual flight segments. Backward trajectory analysis is used to help characterize regional of Hg/CO ratios, and these are compared with emission-based ratios from the various sectors. Model predictions using new Hg emission estimates are presented and compared to the observations. Under the condition of a mercury background level of 1.2 ng/m3 the tracer model underestimates the observations when the flights were over the Yellow Sea but is consistent with the observations when the flights were over the Japan Sea. Further analysis suggests that Hg emissions are underestimated in north central China and the eastern coastal areas of China. Model sensitivity studies indicate that the emissions of China may be underestimated by 80–200%.

International audience; One of the main uncertainties in the estimation of the climatic impact of aerosols is linked to our knowledge of gas and aerosol emissions. This is particularly crucial over Asia, where a strong regional fingerprint is observed, with different emission types, depending on the various vegetation and climate conditions (biomass burning emissions) and on the very fast changes of the population and industrialization (biofuel and fossil fuel emissions). The main contribution of this work is to derive a biomass burning inventory of 1° × 1° over Asia (the Asian biomass burning inventory (ABBI)) for gases and particles for the Aerosol Characterization Experiment-Asia (ACE-Asia) and Transport and Chemical Evolution Over the Pacific (TRACE-P) campaign period (March to May 2001) in 2001. In this paper we apply new estimates of burnt biomass area to estimate emissions. The method is based on burnt areas (GBA2000 project; Tansey et al. (2002) and Grégoire et al. (2003)) obtained from 1 km resolution SPOT-VEGETATION satellite data. Regional-scale maps of burnt areas are produced, and then spatial and temporal emission distribution are obtained from biomass density and emission factors. Strength and weaknesses associated with the use of satellite products are discussed, including the problem of subpixel classification and the lack of validation data for the accuracy assessment of the products for the studied area. Estimated emissions are compared with ACE-Asia and TRACE-P Modeling and Emission Support System (ACESS) climatological estimates. In addition, interannual variability is estimated by preparing inventories for the years 2000 and 2001

[1] Measurements from the Transport and Chemical Evolution over the Pacific (TRACE-P) and Asian Pacific Regional Aerosol Characterization Experiment (ACE-Asia) field experiments obtained during the period of March–April 2001 are used to evaluate the impact of megacity emissions on regional air quality in east Asia. A classification method built upon back trajectory analysis and sensitivity runs using the Sulfur Transport and Emissions Model 2001 (STEM-2K1) regional chemical transport model are used to identify the aircraft observations that were influenced by megacity emissions. More than 30% of measurement points are classified as urban points, with a significant number of plumes found to have originated from Shanghai, Qingdao, Beijing, Taiyuan, Tianjin and Guiyang, Seoul, and Pusan. These data are then analyzed, and chemical characteristics of these megacities are compared. Emission estimates for the megacities are also presented and discussed in the context of expected similarities and differences in the chemical signals in the ambient air impacted by these cities. Comparisons of the observation-based ratios with emission-based estimates are presented and provide a means to test for the consistency of the emission estimates. The observation-based ratios are shown to be generally consistent with the emissions ratios. The megacity emissions are used in the STEM-2K1 model to study the effects of these emissions on criteria and photochemical species in the region. Over large portions of the Japan Sea, Yellow Sea, western Pacific Ocean, and the Bay of Bengal, megacity emissions contribute in excess of 10% of the near-surface ambient levels of O3, CO, SO2, H2SO4, HCHO, and NOz. The megacity emissions are also used to study ozone levels in Asia under a scenario where all cities evolve their emissions in a manner such that they end up with the same VOC/NOx emission ratio as that for Tokyo. Monthly mean ozone levels are found to increase by at least 5%.

[1] We evaluate the TRACE-P emission inventories for gaseous and particulate pollutants from East Asia using chemical measurements made at a rural site in China during the China-MAP Field Intensive in conjunction with a coupled regional climate/chemical transport modeling system. Time-dependent, three-dimensional fields for trace gas and particulate matter concentrations over East Asia are simulated by an updated version of the Regional Acid Deposition Model (RADM) driven by the TRACE-P emission inventories along with meteorology fields calculated by the NCAR Regional Climate Model (RegCM) for the month of November 1999. Model-calculated SO2 is in good agreement with measurements, while CO and particulate carbon (PC) are significantly smaller, and particulate sulfate (SO4� ) is somewhat smaller. Our calculations suggest that increases in the TRACE-P emission inventory of CO by � 50% and PC by 60–90% would bring the model-calculated CO, PC, and particulate sulfate concentration into agreement with the China-MAP observations. If these increases were spread uniformly throughout China and the year, it would require that there be additional emissions in China of CO and PC of 60 Tg yr � 1 and 2.5–4 Tg yr � 1 , respectively. Further analysis of high resolution gas species measurements suggests that the missing CO emissions are likely to be associated with SO2 emissions from coal burning. This in turn suggests that coal-burning facilities in China are operating at significantly lower efficiencies than currently assumed. INDEX TERMS: 0322 Atmospheric Composition and Structure: Constituent sources and sinks; 0345 Atmospheric Composition and Structure: Pollution—urban and regional (0305); 0365 Atmospheric Composition and Structure: Troposphere—composition and chemistry; 0368 Atmospheric Composition and Structure: Troposphere—constituent transport and chemistry; KEYWORDS: anthropogenic emissions, East Asia, regional modeling

Although continental-scale plumes of Asian dust and pollution reduce the amount of solar radiation reaching the earth's surface and perturb the chemistry of the atmosphere, our ability to quantify these effects has been limited by a lack of critical observations, particularly of layers above the surface. Comprehensive surface, airborne, shipboard, and satellite measurements of Asian aerosol chemical composition, size, optical properties, and radiative impacts were performed during the Asian Pacific Regional Aerosol Characterization Experiment (ACE-Asia) study. Measurements within a massive Chinese dust storm at numerous widely spaced sampling locations revealed the highly complex structure of the atmosphere, in which layers of dust, urban pollution, and biomass-burning smoke may be transported long distances as distinct entities or mixed together. The data allow a first-time assessment of the regional climatic and atmospheric chemical effects of a continental-scale mixture of dust and pollution. Our results show that radiative flux reductions during such episodes are sufficient to cause regional climate change.

In this paper, aerosol composition and size distributions in east Asia are simulated using a comprehensive chemical transport model. Three-dimensional aerosol simulations for the TRACE-P and ACE-Asia periods are performed and used to help interpret actual observations. The regional chemical transport model, STEM-2K3, which includes the on-line gas-aerosol thermodynamic module SCAPE II, and explicitly considers chemical aging of dust, is used in the analysis. The model is found to represent many of the important observed features. The Asian outflow during March and April of 2001 is heavily polluted with high aerosol loadings. Under conditions of low dust loading, SO_2 condensation and gas phase ammonia distribution determine the nitrate size and gas-aerosol distributions along air mass trajectories, a situation that is analyzed in detail for two TRACE-P flights. Dust is predicted to alter the partitioning of the semivolatile components between the gas and aerosol phases as well as the size distributions of the secondary aerosol constituents. Calcium in the dust affects the gas-aerosol equilibrium by shifting the equilibrium balance to an anion-limited status, which benefits the uptake of sulfate and nitrate, but reduces the amount of aerosol ammonium. Surface reactions on dust provide an additional mechanism to produce aerosol nitrate and sulfate. The size distribution of dust is shown to be a critical factor in determining the size distribution of secondary aerosols. As much of the dust mass is found in the supermicron mode (70–90%), appreciable amounts of sulfate and nitrate are found in the supermicron particles. For sulfate the observations and the analysis indicate that 10–30% of sulfate is in the supermicron fraction during dust events; in the case of nitrate, more than 80% is found in the supermicron fraction.