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For the first time, mobile campaign and building monitoring experiments were conducted in downtown Seoul, Korea during the 2018/2019 winter period to assess the possibility of the co-benefit of CO2 emission reduction and air quality improvement. Given that CO2 and air pollutants in cities both originate from fossil fuel combustion, monitoring urban CO2 concentrations using a mobile vehicle and from the top of tall buildings can be a potentially effective approach for diagnosing the air quality. The local enhancement values (△species) related to urban emission sources were estimated by eliminating baseline concentrations. The results obtained showed high correlation coefficients between △CO2 and △air pollutants (i.e., 0.753, 0.505, and 0.525 for △CO, △NOX, and △NO2), confirming the applicability of CO2 as an indicator of air pollutant sources in downtown Seoul. The evaluation of the air quality in the study area using air pollutant ratios, including the ratios of CO and NOX/NO2, relative to CO2 showed that the ratios of △CO, △NOX, and △NO2 relative to △CO2 were 5.76, 1.89, and 0.21 ppb ppm−1. The estimated △NO2/△NOX ratio (11%) and a comparison of the △NOX/△CO2 ratios obtained with those reported for other cities in different countries suggested the possibility of a relationship between the current air quality in downtown Seoul and the use of diesel vehicles. Results suggest that the development of municipal policies aimed at mitigating climate change should consider the co-benefit of air quality improvement so as to ensure the effective reduction of CO2 and air pollutant emissions.

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.

With the increasing importance of monitoring and verifying urban CO2 concentrations to mitigate carbon emissions from cities, a high-resolution ground networks of low-cost CO2 sensors are emerging that have a price advantage over existing high-cost sensors. This study develops a low-cost CO2 instrument called the Seoul National University CO2 Measurement (SNUCO2M) to monitor and analyze intra-city CO2 concentrations over Seoul, Korea. The first step of establishing this low-cost CO2 sensor network involved installing the SNUCO2M at the Yongsan Building (YSB; 113 m MASL) and Namsan Seoul Tower-High (NSTH; 385 m MASL) on October 18, 2018 and July 8, 2019, respectively. For comparison with the SNUCO2M, we utilized CO2 concentrations measured by the Picarro instrument (high-cost CO2 sensor) at Gwanak Mountain (GWA) background measurement site and the lower part of the NST (NSTL). The initial CO2 measurements from the SNUCO2M, show that 1) the SNUCO2M has a 0.71% maximum error range and is sufficient to measure urban atmospheric CO2 concentrations; and 2) the SNUCO2M captures 26.92 and 20.30 ppm of Seoul’s summer and winter time CO2 enhancement compared to the GWA background site. Our results suggest that the low-cost sensors such as SNUCO2M successfully detect urban CO2 characteristics over the megacity and has great potential to replace high-cost sensors with cost and management limitations.

The Geostationary Environment Monitoring Spectrometer (GEMS) is scheduled for launch in February 2020 to monitor air quality (AQ) at an unprecedented spatial and temporal resolution from a geostationary Earth orbit (GEO) for the first time. With the development of UV–visible spectrometers at sub-nm spectral resolution and sophisticated retrieval algorithms, estimates of the column amounts of atmospheric pollutants (O3, NO2, SO2, HCHO, CHOCHO, and aerosols) can be obtained. To date, all the UV–visible satellite missions monitoring air quality have been in low Earth orbit (LEO), allowing one to two observations per day. With UV–visible instruments on GEO platforms, the diurnal variations of these pollutants can now be determined. Details of the GEMS mission are presented, including instrumentation, scientific algorithms, predicted performance, and applications for air quality forecasts through data assimilation. GEMS will be on board the Geostationary Korea Multi-Purpose Satellite 2 (GEO-KOMPSAT-2) satellite series, which also hosts the Advanced Meteorological Imager (AMI) and Geostationary Ocean Color Imager 2 (GOCI-2). These three instruments will provide synergistic science products to better understand air quality, meteorology, the long-range transport of air pollutants, emission source distributions, and chemical processes. Faster sampling rates at higher spatial resolution will increase the probability of finding cloud-free pixels, leading to more observations of aerosols and trace gases than is possible from LEO. GEMS will be joined by NASA’s Tropospheric Emissions: Monitoring of Pollution (TEMPO) and ESA’s Sentinel-4 to form a GEO AQ satellite constellation in early 2020s, coordinated by the Committee on Earth Observation Satellites (CEOS).

The air quality in Republic of Korea, especially in cities such as Seoul, has been a serious public health concern over the years. The key pollutant in the atmosphere leading to poor air quality in Korea is fine particulate matter (PM2.5). Here, we use a 3-D global chemistry model (GEOS-Chem) to conduct source attribution to PM2.5 in Korea from international and domestic emissions. The modeling was done for 2015 and 2016 to account for different meteorological conditions. We ran the GEOS-Chem model for both years, conducted model evaluation using ground and aloft observations, and then conducted sensitivity simulations without domestic anthropogenic emissions and Chinese anthropogenic emissions, respectively. Results show that the Chinese influence on PM2.5 in Korea varies from month to month with the highest contribution during spring when observed concentrations are also the highest. Chinese contributions to PM2.5 concentrations in South Korea reach a maximum of up to ~60% in January and February and gradually decrease until August when they reach a minimum at about 20%. On an annual basis, our analysis estimated that in 2016, Chinese anthropogenic emissions contributed 45% to PM2.5 in South Korea. The 2016 contribution from China was generally 3–5% lower than in 2015 because of emissions reductions in China. Compared to the Chinese contribution, the rest of the world contributions (which also include contributions from natural emissions worldwide) were minor except for summer in the South Sea.

The emission of pollution from Chinese point sources, and its migration to Korea, downwind of China, is an important issue in terms of Korean air quality management. Therefore, this study intended to improve the Asian Emission Inventory, NIER/KU-CREATE, by improving information about the point source emissions, their location, and discharge conditions, in China. By using the Global dataset, we can establish point source location information for Coal Power Plants and Non-Coal Power Plants in the Chinese power sector, and calculate and allocate emissions in the inventory. In addition, the emission inventory of NH3, as a by-product of NOx abatement processing, was regarded as being insufficiently characterized in the previous emission inventory, and has been re-estimated. As a result, 3798 LPSs in China were identified, and NH3 emissions from those power plants have increased significantly. In addition, the vertical distribution of emissions through the allocation stack height parameters showed atmospheric injection heights of between 250 m and 1000 m. Using this information, HY-SPLIT trajectory modeling found that during periods of active westerly from China to Korea, emissions from the higher injection height were more prone to move towards Korea, than those from the lower height.

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%).

In this work, we investigate the NOx emissions inventory in Seoul, South Korea, using a regional ozone monitoring instrument (OMI) NO2 product derived from the standard NASA product. We first develop a regional OMI NO2 product by recalculating the air mass factors using a high-resolution (4 km × 4 km) WRF-Chem model simulation, which better captures the NO2 profile shapes in urban regions. We then apply a model-derived spatial averaging kernel to further downscale the retrieval and account for the subpixel variability. These two modifications yield OMI NO2 values in the regional product that are 1.37 times larger in the Seoul metropolitan region and >2 times larger near substantial point sources. These two modifications also yield an OMI NO2 product that is in better agreement with the Pandora NO2 spectrometer measurements acquired during the South Korea–United States Air Quality (KORUS-AQ) field campaign. NOx emissions are then derived for the Seoul metropolitan area during the KORUS-AQ field campaign using a top-down approach with the standard and regional NASA OMI NO2 products. We first apply the top-down approach to a model simulation to ensure that the method is appropriate: the WRF-Chem simulation utilizing the bottom-up emissions inventory yields a NOx emissions rate of 227±94 kt yr −1 , while the bottom-up inventory itself within a 40 km radius of Seoul yields a NOx emissions rate of 198 kt yr −1 . Using the top-down approach on the regional OMI NO2 product, we derive the NOx emissions rate from Seoul to be 484±201 kt yr −1 , and a 353±146 kt yr −1 NOx emissions rate using the standard NASA OMI NO2 product. This suggests an underestimate of 53 % and 36 % in the bottom-up inventory using the regional and standard NASA OMI NO2 products respectively. To supplement this finding, we compare the NO2 and NOy simulated by WRF-Chem to observations of the same quantity acquired by aircraft and find a model underestimate. When NOx emissions in the WRF-Chem model are increased by a factor of 2.13 in the Seoul metropolitan area, there is better agreement with KORUS-AQ aircraft observations and the recalculated OMI NO2 tropospheric columns. Finally, we show that by using a WRF-Chem simulation with an updated emissions inventory to recalculate the air mass factor (AMF), there are small differences ( ∼8 %) in OMI NO2 compared to using the original WRF-Chem simulation to derive the AMF. This suggests that changes in model resolution have a larger effect on the AMF calculation than modifications to the South Korean emissions inventory. Although the current work is focused on South Korea using OMI, the methodology developed in this work can be applied to other world regions using TROPOMI and future satellite datasets (e.g., GEMS and TEMPO) to produce high-quality region-specific top-down NOx emissions estimates.

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.

The Korea–United States Air Quality (KORUS-AQ) field study was conducted during May–June 2016. The effort was jointly sponsored by the National Institute of Environmental Research of South Korea and the National Aeronautics and Space Administration of the United States. KORUS-AQ offered an unprecedented, multi-perspective view of air quality conditions in South Korea by employing observations from three aircraft, an extensive ground-based network, and three ships along with an array of air quality forecast models. Information gathered during the study is contributing to an improved understanding of the factors controlling air quality in South Korea. The study also provided a valuable test bed for future air quality–observing strategies involving geostationary satellite instruments being launched by both countries to examine air quality throughout the day over Asia and North America. This article presents details on the KORUS-AQ observational assets, study execution, data products, and air quality conditions observed during the study. High-level findings from companion papers in this special issue are also summarized and discussed in relation to the factors controlling fine particle and ozone pollution, current emissions and source apportionment, and expectations for the role of satellite observations in the future. Resulting policy recommendations and advice regarding plans going forward are summarized. These results provide an important update to early feedback previously provided in a Rapid Science Synthesis Report produced for South Korean policy makers in 2017 and form the basis for the Final Science Synthesis Report delivered in 2020.

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.

The U.S. National Aeronautics and Space Administration in partnership with Korea’s National Institute of Environmental Research embarked on the Korea-United States Air Quality (KORUS-AQ) study to address air quality issues over the Korean peninsula. Underestimation of volatile organic compound (VOC) emissions from various large facilities on South Korea’s northwest coast may contribute to this problem, and this study focuses on quantifying top-down emissions of formaldehyde (CH2O) and VOCs from the largest of these facilities, the Daesan petrochemical complex, and comparisons with the latest emission inventories. To accomplish this and additional goals discussed herein, this study employed a number of measurements acquired during KORUS-AQ onboard the NASA DC-8 aircraft during three Daesan overflights on June 2, 3, and 5, 2016, in conjunction with a mass balance approach. The measurements included fast airborne measurements of CH2O and ethane from an infrared spectrometer, additional fast measurements from other instruments, and a suite of 33 VOC measurements acquired by the whole air sampler. The mass balance approach resulted in consistent top-down yearly Daesan VOC emission flux estimates, which averaged (61 ± 14) × 103 MT/year for the 33 VOC compounds, a factor of 2.9 ± 0.6 (±1.0) higher than the bottom-up inventory value. The top-down Daesan emission estimate for CH2O and its four primary precursors averaged a factor of 4.3 ± 1.5 (± 1.9) times higher than the bottom-up inventory value. The uncertainty values in parentheses reflect upper limits for total uncertainty estimates. The resulting averaged top-down Daesan emission estimate for sulfur dioxide (SO2) yielded a ratio of 0.81–1.0 times the bottom-up SO2 inventory, and this provides an important cross-check on the accuracy of our mass balance analysis.

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.

With global anthropogenic black carbon (BC) emissions increasing, automobiles are significantly contributing as the major source of emissions. However, the appropriate regulations of BC emissions from vehicles are not in place. This study examined BC emissions following fuel types (gasoline, liquefied petroleum gas (LPG), and diesel) and engine combustion (gasoline direct injection (GDI) and multi-port injection (MPI) for gasoline vehicles) with emission regulations. To this end, chassis dynamometer and aethalometer (AE33) were used. Driving modes created by the National Institute of Environmental Research (NIER) and emission certification modes (CVS-75 and NEDC) for vehicles in Korea were used to determine BC emissions for various vehicle speeds. In addition, the contributions of biomass and coal combustion to the data of AE33 were analyzed to determine the possibility of tracking the BC sources. MPI, LPG, and EURO 6 with diesel particulate filter (DPF) vehicles emitted the lowest BC emissions in NIER modes. Among gasoline vehicles, MPI vehicles showed the lower BC content in PM emissions. Also, older vehicles in MPI vehicles emitted the high PM and BC emissions. The BC emissions of EURO 3 vehicles without DPF were the highest as the results of previous studies, and it was found that as emissions regulations were tightened, the level of BC results of diesel vehicles became similar with MPI vehicles. The average absorption &Aring, ngstr&ouml, m exponent (AAE) from difference emissions sources were biomass combustion (oak wood) &gt, coal combustion (the power plant stack) &gt, automobile emissions (gasoline, LPG, diesel).

Substantial mitigation of air pollutants emissions has been performed since 2013 around Beijing, and changes in the atmospheric characteristics have been expected over the downstream area of Beijing. In this study, both WRF-Chem simulation and on-site measurements were utilized for the Baengnyeong (island) supersite, one of the representative regional background sites located in the Yellow Sea, the entrance area of the long-range transport process in Korea. The changes in the chemical compositions of inorganic aerosols were examined for spring-time during the Chinese emission mitigation period from 2014 to 2016. The measured ratio of ionic species to PM2.5 at the Baengnyeong supersite showed changes in aerosol inorganic chemical compositions from sulfate in 2014 to nitrate in 2015–2016. The modeling results also showed that nitrate was low in 2014 and significantly increased in 2015 and 2016, and the acidic aerosol condition had also changed toward a more neutralized status in both the simulation and the observations. The WRF-Chem modeling study further indicated that the sulfur was not neutralized in 2014. However, in 2015 and 2016, SO2 was more sufficiently neutralized as sulfur emissions were substantially reduced in China, while at the same time nitrate had begun to increase in such a ‘SO2–poor’ condition in Beijing area in China, and thus approaching more enhanced neutralization over the Yellow Sea area. The causes of the higher nitrate based on the modeled characteristics of the ammonia-sulfate-nitrate aerosol formation in response to the SO2 emissions reduction in China are also discussed in this paper.

The Korea-United States Air Quality Study (KORUS-AQ) took place in spring 2016 to better understand air pollution in Korea. In support of KORUS-AQ, 2554 whole air samples (WAS) were collected aboard the NASA DC-8 research aircraft and analyzed for 82 C1–C10 volatile organic compounds (VOCs) using multi-column gas chromatography. Together with fast-response measurements from other groups, the air samples were used to characterize the VOC composition in Seoul and surrounding regions, determine which VOCs are major ozone precursors in Seoul, and identify the sources of these reactive VOCs. (1) The WAS VOCs showed distinct signatures depending on their source origins. Air collected over Seoul had abundant ethane, propane, toluene and n-butane while plumes from the Daesan petrochemical complex were rich in ethene, C2–C6 alkanes and benzene. Carbonyl sulfide (COS), CFC-113, CFC-114, carbon tetrachloride (CCl4) and 1,2-dichloroethane were good tracers of air originating from China. CFC-11 was also elevated in air from China but was surprisingly more elevated in air over Seoul. (2) Methanol, isoprene, toluene, xylenes and ethene were strong individual contributors to OH reactivity in Seoul. However methanol contributed less to ozone formation based on photochemical box modeling, which better accounts for radical chemistry. (3) Positive Matrix Factorization (PMF) and other techniques indicated a mix of VOC source influences in Seoul, including solvents, traffic, biogenic, and long-range transport. The solvent and traffic sources were roughly equal using PMF, and the solvents source was stronger in the KORUS-AQ emission inventory. Based on PMF, ethene and propene were primarily associated with traffic, and toluene, ethylbenzene and xylenes with solvents, especially non-paint solvents for toluene and paint solvents for ethylbenzene and xylenes. This suggests that VOC control strategies in Seoul could continue to target vehicle exhaust and paint solvents, with additional regulations to limit the VOC content in a variety of non-paint solvents.

Global coupled chemistry-climate models underestimate carbon monoxide (CO) in the Northern Hemisphere, exhibiting a pervasive, negative bias against measurements peaking in late winter and early spring. While this bias has been commonly attributed to underestimation of direct anthropogenic and biomass burning emissions, chemical production and loss via OH reaction from emissions of anthropogenic and biogenic VOCs play an important role. Here we investigate the reasons for this underestimation using aircraft measurements taken in May and June 2016 from the Korea United States Air Quality (KORUS‐AQ) experiment in South Korea and the Air chemistry Research In Asia (ARIAs) in the North China Plain (NCP). For reference, multispectral CO retrievals (V8J) from the Measurements of Pollution in the Troposphere (MOPITT) are jointly assimilated with meteorological observations using an Ensemble Adjustment Kalman Filter (EAKF) within the global Community Atmosphere Model with Chemistry (CAM-chem) and the Data Assimilation Research Testbed (DART). With regard to KORUS-AQ data, CO is underestimated by 42 % in the Control-Run and by 12 % with the MOPITT assimilation run. The inversion suggests an underestimation of anthropogenic CO sources in many regions, by up to 80 % for Northern China, with large increments over the Liaoning province and the North China Plains (NCP). Yet, an often-overlooked aspect of these inversions is that correcting the underestimation in anthropogenic CO emissions also improves the comparison with observational O3 datasets, and observationally constrained box model simulations of OH and HO2. Running a CAM-chem simulation with the updated emissions of anthropogenic CO reduces the bias by 29 % for CO, 18 % for ozone, 11 % for HO2 and 27 % for OH. Longer lived anthropogenic VOCs whose model errors are correlated with CO are also improved while short-lived VOCs, including formaldehyde, are difficult to constrain solely by assimilating satellite retrievals of CO. During an anticyclonic episode, better simulation of O3, with an average underestimation of 5.5 ppbv and a reduction in the bias of surface formaldehyde and oxygenated VOCs can be achieved by separately increasing by a factor of two the modeled biogenic emissions for the plant functional types found in Korea. Results also suggest that controlling VOC and CO emissions, in addition to wide spread NOx controls, can improve pollution ozone over East Asia.; Global coupled chemistry-climate models underestimate carbon monoxide (CO) in the Northern Hemisphere, exhibiting a pervasive, negative bias against measurements peaking in late winter and early spring. While this bias has been commonly attributed to underestimation of direct anthropogenic and biomass burning emissions, chemical production and loss via OH reaction from emissions of anthropogenic and biogenic VOCs play an important role. Here we investigate the 40 reasons for this underestimation using aircraft measurements taken in May and June 2016 from the Korea United States Air Quality (KORUS-AQ) experiment in South Korea and the Air chemistry Research In Asia (ARIAs) in the North China Plain (NCP). For reference, multispectral CO retrievals (V8J) from the Measurements of Pollution in the Troposphere (MOPITT) are jointly assimilated with meteorological observations using an Ensemble Adjustment Kalman Filter 45 (EAKF) within the global Community Atmosphere Model with Chemistry (CAM-chem) and the Data Assimilation Research Testbed (DART). With regard to KORUS-AQ data, CO is underestimated by 42 % in the Control-Run and by 12 % with the MOPITT assimilation run. The 2 inversion suggests an underestimation of anthropogenic CO sources in many regions, by up to 80 % for Northern China, with large increments over the Liaoning province and the North China 50 Plains (NCP). Yet, an often-overlooked aspect of these inversions is that correcting the underestimation in anthropogenic CO emissions also improves the comparison with observational O 3 datasets, and observationally constrained box model simulations of OH and HO 2. Running a CAM-chem simulation with the updated emissions of anthropogenic CO reduces the bias by 29 % for CO, 18 % for ozone, 11 % for HO 2 and 27 % for OH. Longer lived anthropogenic VOCs whose 55 model errors are correlated with CO are also improved while short-lived VOCs, including formaldehyde, are difficult to constrain solely by assimilating satellite retrievals of CO. During an anticyclonic episode, better simulation of O 3 , with an average underestimation of 5.5 ppbv and a reduction in the bias of surface formaldehyde and oxygenated VOCs can be achieved by separately increasing by a factor of two the modeled biogenic emissions for the plant functional types found 60 in Korea. Results also suggest that controlling VOC and CO emissions, in addition to wide spread NOx controls, can improve pollution ozone over East Asia.

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.

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.

Understanding how ozone (O3) and fine particulate matter (PM) formation respond to the precursor concentrations in the presence of biogenic emissions (BEs) and thereby changes in health effects can be a key step to design effective air quality management plans. This is particularly true in the Seoul Metropolitan Area (SMA), where future significant controls of anthropogenic sources of O3 and PM2.5 precursors are expected. In this paper, we investigate the effects of BEs on O3 and fine PM (PM2.5) concentrations during a strong photochemical air pollution season in the SMA in Korea. O3 and PM2.5 levels are modeled with and without BEs in June 2008. Further, we perform the health impact assessments (HIA) of O3 and PM2.5 concentration changes due to BEs to seek useful implications for air quality management by utilizing the adjusted exposure concentration fields for O3 and PM2.5 with an observation fusing (OBF) method. With BEs, daily maximum 8-h average O3 (maximum 8-h O3) and secondary organic aerosol (SOA) concentrations in the SMA increase by 17 and 474%, respectively. These increments are associated with significant consumption of photochemical oxidants (Ox), such as a ~ 60% reduction in OH∙ radicals. The reduction in Ox, conversely, lowers the production of secondary inorganic aerosols (SIOAs) by 2.7%. Adjusted O3 and PM2.5 exposure metrics and the subsequent HIA reveal that large mean increments of O3, about 8.43 ppb, due to BEs are responsible for approximately 62 all-cause premature mortalities in the SMA in June. However, mean increment of PM2.5 due to BEs is approximately 0.3 μg m−3 and results in negligible impacts on the all-cause mortality. Significant correlations of O3 and mortality rates (MR) with the VOC/NOx ratios across the SMA suggest that controlling volatile organic compounds (VOCs) from anthropogenic sources can be a priority to reduce O3 levels and population health risks in the SMA. Specifically, linear relationships of log [O3] and log [MR] to log [VOC/NOx] ensure that a 10% decrease in the VOC/NOx ratios through the VOC abatements would lead to a 1.5% decrease in the O3 levels and a 4.3% decrease in the MR on average across the SMA.

Fast economic growth and urbanization of China have been causing air pollution not only over its domestic but transboundary atmosphere. Recent high fine particle pollution episodes in China made the government move toward more stringent air pollution control policies - which are mostly fuel switching and emissions control. In this research, we tried to understand characteristics of Chinese emissions and their change by analyzing its emissions inventory by year, sector, and region. From the inter-comparison of existing bottom-up emission inventories, we found relatively good agreements (

The characteristics of primary gas/aerosol and secondary aerosol emissions were identified for small passenger vehicles using typical fuel types in South Korea (gasoline, liquefied petroleum gas (LPG), and diesel). The generation of secondary organic aerosol (SOA) was explored using the potential aerosol mass (PAM) oxidation flow reactor. The primary emissions did not vary significantly between fuel types, combustion technologies, or aftertreatment systems, while the amount of NH3 was higher in gasoline and LPG vehicle emissions than that in diesel vehicle emissions. The SOA emission factor was 11.7–66 mg kg-fuel−1 for gasoline vehicles, 2.4–50 mg kg-fuel−1 for non-diesel particulate filter (non-DPF) diesel vehicles (EURO 2–3), 0.4–40 mg kg-fuel−1 for DPF diesel vehicles (EURO 4–6), and 3–11 mg kg-fuel−1 for LPG vehicles (lowest). The carbonaceous aerosols (equivalent black carbon (eBC) + primary organic aerosol + SOA) of diesel vehicles in EURO 4–6 were reduced by up to 95% compared to those in EURO 2–3. The expected SOA yield increased through the hot-condition combustion section of a vehicle, over the SOA range of 0.2–155 μg m−3. These results provide the necessary data to analyze all types of SOA generated by the gas-phase oxidation in vehicle emissions in metropolitan areas.

Climate change is an important issue, with many researches examining not only future climatic conditions, but also the interaction of climate and air quality. In this study, a new version of the emissions processing software tool - Python-based PRocessing Operator for Climate and Emission Scenarios (PROCES) - was developed to support climate and atmospheric chemistry modeling studies. PROCES was designed to cover global and regional scale modeling domains, which correspond to GEOS-Chem and CMAQ/CAMx models, respectively. This tool comprises of one main system and two units of external software. One of the external software units for this processing system was developed using the GIS commercial program, which was used to create spatial allocation profiles as an auxiliary database. The SMOKE-Asia emissions modeling system was linked to the main system as an external software, to create model-ready emissions for regional scale air quality modeling. The main system was coded in Python version 2.7, which includes several functions allowing general emissions processing steps, such as emissions interpolation, spatial allocation and chemical speciation, to create model-ready emissions and auxiliary inputs of SMOKE-Asia, as well as user-friendly functions related to emissions analysis, such as verification and visualization. Due to its flexible software architecture, PROCES can be applied to any pre-gridded emission data, as well as regional inventories. The application results of our new tool for global and regional (East Asia) scale modeling domain under RCP scenario for the years 1995-2006, 2015-2025, and 2040-2055 was quantitatively in good agreement with the reference data of RCPs.

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.

Recent regulatory policies in East Asia reduce ozone precursors, but these changes are spatially and temporally nonuniform. This study investigates variations in the long-term trends of tropospheric NO2, HCHO, and HCHO/NO2 ratios to diagnose ozone sensitivity to changes in NOx and volatile organic compound using the Ozone Monitoring Instrument (OMI). Using an adaptive-degree polynomial filter, we identify extremums of time series of NO2 to determine when and how NO2 change. Due to the regulations in China, trends which were predominantly upward turned downward. The years undergoing these changes primarily happened in 2011 and 2012. OMI column densities, however, suggest that NOx sources in South Korea, the Pearl River Delta (PRD), Taiwan, and Japan have not consistently decreased. Specifically, as Chinese exports of NO2 started subsiding, increasing trends in NO2 columns over several Korean cities, including Seoul, become evident. To quantify the changes in NOx emissions from summertime 2010 to 2014, we conduct a 3D-Var inverse modeling using a regional model with MIX-Asia inventory and estimate NOx emissions (in 2010 and 2014) for the PRD (1.6 and 1.5 Gg/d), the Yangtze River Delta (3.9 and 3.0 Gg/d), north China (15.6 and 14.3 Gg/d), South Korea (1.6 and 1.5 Gg/d), and Japan (2.7 and 2.6 Gg/d). OMI HCHO shows upward trends in East Asia resulting from anthropogenic effects; however, the magnitudes are negative in the PRD, Japan, North Korea, and Taiwan. OMI HCHO/NO2 ratios reveal that while South Korea, Japan, and the south of China have undergone toward more NOx-sensitive regime, areas around the Bohai Sea have become more NOx saturated.

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

For the purpose of providing reliable and robust air quality predictions, an operational air quality prediction system was developed for the main air quality criteria species in South Korea (PM10, PM2.5, CO, O3, and SO2). The main caveat of the system is to prepare the initial conditions (ICs) of the Community Multi-scale Air Quality (CMAQ) model simulations using observations from the Geostationary Ocean Color Imager (GOCI) and ground-based monitoring networks in northeast Asia. The performance of the air quality prediction system was evaluated during the Korea-United States Air Quality Study (KORUS-AQ) campaign period (1 May–12 June 2016). Data assimilation (DA) of optimal interpolation (OI) with Kalman filter was used in this study. One major advantage of the system is that it can predict not only particulate matter (PM) concentrations but also PM chemical composition including five main constituents: sulfate, nitrate, ammonium, organic aerosols (OAs), and elemental carbon (EC). In addition, it is also capable of predicting the concentrations of gaseous pollutants (CO, O3 and SO2). In this sense, this new operational air quality prediction system is comprehensive. The results with the ICs (DA RUN) were compared with those of the CMAQ simulations without ICs (BASE RUN). For almost all of the species, the application of ICs led to improved performance in terms of correlation, errors, and biases over the entire campaign period. The DA RUN agreed reasonably well with the observations for PM10 (IOA = 0.60; MB = −13.54) and PM2.5 (IOA = 0.71; MB = −2.43) as compared to the BASE RUN for PM10 (IOA = 0.51; MB = −27.18) and PM2.5 (IOA = 0.67; MB = −9.9). A significant improvement was also found with the DA RUN in terms of bias. For example, for CO, the MB of −0.27 (BASE RUN) was greatly enhanced to −0.036 (DA RUN). In the cases of O3 and SO2, the DA RUN also showed better performance than the BASE RUN. Further, several more practical issues frequently encountered in the operational air quality prediction system were also discussed. In order to attain more accurate ozone predictions, the DA of NO2 mixing ratios should be implemented with careful consideration of the measurement artifacts (i.e., inclusion of alkyl nitrates, HNO3, and PANs in the ground-observed NO2 mixing ratios). It was also discussed that, in order to ensure accurate nocturnal predictions of the concentrations of the ambient species, accurate predictions of the mixing layer heights (MLH) should be achieved from the meteorological modeling. Several advantages of the current air quality prediction system, such as its non-static free parameter scheme, dust episode prediction, and possible multiple implementations of DA prior to actual predictions, were also discussed. These configurations are all possible because the current DA system is not computationally expensive. In the ongoing and future works, more advanced DA techniques such as the three-dimensional variational (3DVAR) method and ensemble Kalman filter (EnK) are being tested and will be introduced to the Korean operational air quality forecasting system.

Author(s): Tang, Wenfu; Emmons, Louisa K; Jr, Arellano Avelino F; Gaubert, Benjamin; Knote, Christoph; Tilmes, Simone; Buchholz, Rebecca R; Pfister, Gabriele G; Diskin, Glenn S; Blake, Donald R; Blake, Nicola J; Meinardi, Simone; DiGangi, Joshua P; Choi, Yonghoon; Woo, Jung-Hun; He, Cenlin; Schroeder, Jason R; Suh, Inseon; Lee, Hyo-Jung; Jo, Hyun-Young; Kanaya, Yugo; Jung, Jinsang; Lee, Youngjae; Kim, Danbi

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.

A bottom-up emissions inventory is one of the most important data sets needed to understand air quality (AQ) and climate change (CC). Several emission inventories have been developed for Asia, including Transport and Chemical Evolution over the Pacific (TRACE-P), Regional Emission Inventory in Asia (REAS), and Inter-Continental Chemical Transport Experiment (INTEX) and, while these have been used successfully for many international studies, they have limitations including restricted amounts of information on pollutant types and low levels of transparency with respect to the polluting sectors or fuel types involved. To address these shortcomings, we developed: 1) a base-year, bottom-up anthropogenic emissions inventory for Asia, using the most current parameters and international frameworks (i.e., the Greenhouse gas—Air pollution INteractions and Synergies (GAINS) model); and 2) a base-year, natural emissions inventory for biogenic and biomass burning. For 1), we focused mainly on China, South Korea, and Japan; however, we also covered emission inventories for other regions in Asia using data covering recent energy/industry statistics, emission factors, and control technology penetration. The emissions inventory (Comprehensive Regional Emissions inventory for Atmospheric Transport Experiment (CREATE)) covers 54 fuel classes, 201 subsectors, and 13 pollutants, namely SO2, NOx, CO, non-methane volatile organic compounds (NMVOC), NH3, OC, BC, PM10, PM2.5, CO2, CH4, N2O, and Hg. For the base-year natural emissions inventory, the Model of Emissions of Gases and Aerosols from Nature (MEGAN) and BlueSky-Asia frameworks were used to estimate biogenic and biomass burning emissions, respectively. Since the CREATE emission inventory was designed/developed using international climate change/air quality (CC/AQ) assessment frameworks, such as GAINS, and has been fully connected with the most comprehensive emissions modeling systems—such as the US Environmental Protection Agency (EPA) Chemical Manufacturing Area Source (CMAS) system—it can be used to support various climate and AQ integrated modeling studies, both now and in the future.

Anthropogenic emissions in East Asia have changed dramatically in recent years. To measure these changing emissions in support of air-quality modeling, we developed a top-down emission update system using surface observations and a geographical information system spatial-allocation technique. We deploy a data-processing system to construct adjustment factors to prefecture-level SO2 emissions by comparing surface and modeled observations. A case study is conducted over East Asia for 2016 in which we update Chinese SO2 emissions using measurements from around 1500 surface monitoring sites. Model simulations using updated SO2 emissions are improved relative to the existing simulation system (e.g., R = 0.23 to R = 0.8), suggesting that the newly designed system provides an efficient, practical forecast solution. Finally, estimated SO2 emissions are compared with existing emission inventories, agreeing well with recent reports of reduced SO2 emissions from Chinese anthropogenic sources.

To improve short-term particulate matter (PM) forecasts in South Korea, the initial distribution of PM composition, particularly over the upwind regions, is primarily important. To prepare the initial PM composition, the aerosol optical depth (AOD) data retrieved from a geostationary equatorial orbit (GEO) satellite sensor, GOCI (Geostationary Ocean Color Imager) which covers a part of Northeast Asia (113–146° E; 25–47° N), were used. Although GOCI can provide a higher number of AOD data in a semicontinuous manner than low Earth orbit (LEO) satellite sensors, it still has a serious limitation in that the AOD data are not available at cloud pixels and over high-reflectance areas, such as desert and snow-covered regions. To overcome this limitation, a spatiotemporal-kriging (STK) method was used to better prepare the initial AOD distributions that were converted into the PM composition over Northeast Asia. One of the largest advantages in using the STK method in this study is that more observed AOD data can be used to prepare the best initial AOD fields compared with other methods that use single frame of observation data around the time of initialization. It is demonstrated in this study that the short-term PM forecast system developed with the application of the STK method can greatly improve PM10 predictions in the Seoul metropolitan area (SMA) when evaluated with ground-based observations. For example, errors and biases of PM10 predictions decreased by ∼ 60 and ∼ 70 %, respectively, during the first 6 h of short-term PM forecasting, compared with those without the initial PM composition. In addition, the influences of several factors on the performances of the short-term PM forecast were explored in this study. The influences of the choices of the control variables on the PM chemical composition were also investigated with the composition data measured via PILS-IC (particle-into-liquid sampler coupled with ion chromatography) and low air-volume sample instruments at a site near Seoul. To improve the overall performances of the short-term PM forecast system, several future research directions were also discussed and suggested.

Landsat optical images have enough spatial and spectral resolution to analyze vegetation growth characteristics. But, the clouds and water vapor degrade the image quality quite often, which limits the availability of usable images for the time series vegetation vitality measurement. To overcome this shortcoming, simulated images are used as an alternative. In this study, weighted average method, spatial and temporal adaptive reflectance fusion model (STARFM) method, and multilinear regression analysis method have been tested to produce simulated Landsat normalized difference vegetation index (NDVI) images of the Korean Peninsula. The test results showed that the weighted average method produced the images most similar to the actual images, provided that the images were available within 1 month before and after the target date. The STARFM method gives good results when the input image date is close to the target date. Careful regional and seasonal consideration is required in selecting input images. During summer season, due to clouds, it is very difficult to get the images close enough to the target date. Multilinear regression analysis gives meaningful results even when the input image date is not so close to the target date. Average R 2 values for weighted average method, STARFM, and multilinear regression analysis were 0.741, 0.70, and 0.61, respectively.

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.

Many studies have found that larger parks might be needed to counteract the Urban Heat Island effects typical in densely populated Asian megacities. However, it is not easy to establish large parks to serve as urban cool islands in Asian megacities, where little space exists for large urban neighborhood parks. Officials in these cities would rather use small areas by replacing heat-absorbing artificial land cover with natural cover. The main objective of this study was to understand the cooling effect of changes in land cover on surface and air temperatures in urban micro-scale environments for supporting sustainable green-space planning and policy in densely built-up areas. This was achieved using measurements at different heights (ground surface, 0.1 m, and 1.5 m) for five land cover types (LCTs) and modeling with the micro-scale climate model ENVI-met. At all vertical measuring points, the average temperature over the entire measurement period had the same hot-to-cold order: asphalt > soil > grass > water > forest. However, the value dramatically decreased as the measuring points became higher. The intensity of hot and cool spots showed the highest value at surface by 18.2 degrees C, and declined with the height, showing 4.1 degrees C at 0.1 m and 3.1 degrees C at 1.5 m. The modeling results indicated that the well-known diurnal variation in surface insolation also occurred in our small domain, among the various LCTs. Based on these findings, providing small-scale green infrastructure in densely built-up areas could be an effective way to improve urban micro-scale thermal conditions.

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

Measurements of gaseous SO2, NH3, and O3 using IVL passive sampler technology were obtained during a pilot measurement program initiated as a key component of the newly established WMO/GAW Urban Research Meteorology and Environment (GURME) project. Monthly measurements were obtained at 50 stations in Asia, Africa, South America, and Europe. The median SO2 concentrations vary from a high of 13 ppb at Linan, China, to