Korea-United States Air Quality Study Research Articles

Ozone, nitrogen dioxide, and PM2.5 estimation from observation-model machine learning fusion over S. Korea: Influence of observation density, chemical transport model resolution, and geostationary remotely sensed AOD

High-resolution multi-component estimates of ground-level air pollutants are necessary for assessing their impacts to human health, agriculture, and ecosystems. We demonstrate a high-resolution fusion and downscaling approach over South Korea for May 2016 and May 2021. Daily 1 km fine particulate matter (PM2.5), ozone (O3), and nitrogen dioxide (NO2) concentrations are calculated at ground level using a random forest machine learning (ML) algorithm, with predictors including reanalysis meteorology, satellite aerosol optical depth (AOD), and gridded surface fields from chemical transport models (CTM). The ML model is tested for May 2016, coinciding with the Korea-United States Air Quality Study (KORUS-AQ) intensive field campaign, and for May 2021, to allow incorporation of observations from the Geostationary Environment Monitoring Spectrometer (GEMS). In the tests for May 2016, the correlation coefficients (R) and root mean squared errors (RMSE) relative to withheld observations of daily-averaged pollutants in 10-fold cross-validation are promising: 0.93 (5.5 μg/m3), 0.90 (5.5 ppbv), and 0.95 (4.7 ppbv) for PM2.5, O3, and NO2, respectively. Relative performance is assessed for alternate choices of predictors: (a) 80-km global reanalysis Copernicus Atmosphere Monitoring Service (CAMS) vs. 4-km regional Weather Research and Forecasting model coupled with Chemistry (WRF-Chem); (b) AOD polar-orbiting Moderate Resolution Image Spectroradiometer (MODIS) Multi-Angle Implementation of Atmospheric Correction (MAIAC) vs. geostationary GEMS; and (c) variations in surface observation density. This study is among the very first to incorporate both CTM and GEMS AOD for building surface high resolution multiple air pollution predictions over South Korea.

Adjusting elemental carbon emissions in Northeast Asia using observed surface concentrations of downwind area and simulated contributions

In this study, we developed a practical approach to augment elemental carbon (EC) emissions to improve the reproducibility of the most recent air quality with photochemical grid modeling in support of source-receptor relationship analysis. We demonstrated the usefulness of this approach with a series of simulations for EC concentrations over Northeast Asia during the 2016 Korea-United States Air Quality study. Considering the difficulty of acquiring EC observational data in foreign countries, our approach takes two steps: (1) augmenting upwind EC emissions based on simulated upwind contributions and observational data at a downwind EC monitor considered as the most representative monitor for upwind influences and (2) adjusting downwind EC emissions based on simulated downwind contributions, including the effects of updated upwind emissions from the first step and observational data at the downwind EC monitors. The emission adjustment approach resulted in EC emissions 2.5 times higher than the original emissions in the modeling domain. The EC concentration in the downwind area was observed to be 1.0 μg m−3 during the study period, while the simulated EC concentration was 0.5 μg m−3 before the emission adjustment. After the adjustment, the normalized mean error of the daily mean EC concentration decreased from 48 % to 22 % at ground monitor locations. We found that the EC simulation results were improved at high altitudes, and the contribution of the upwind areas was greater than that of the downwind areas for EC concentrations downwind with or without emission adjustment. This implies that collaborating with upwind regions is essential to alleviate high EC concentrations in downwind areas. The developed emission adjustment approach can be used for any upwind or downwind area when transboundary air pollution mitigation is needed because it provides better reproducibility of the most recent air quality through modeling with improved emission data.

Nocturnal Boundary Layer Height Uncertainty in Particulate Matter Simulations during the KORUS-AQ Campaign

Vertical mixing in the planetary boundary layer (PBL) is an important factor in the prediction of particulate matter (PM) concentrations; however, PBL height (PBLH) in the stable atmosphere remains poorly understood. In particular, the assessment of uncertainties related to nocturnal PBLH (nPBLH) is challenging due to the absence of stable atmosphere observations. In this study, we explored nPBLH–PM2.5 interactions by comparing model results and observations during the Korea–United States Air Quality Study (KORUS-AQ) campaign (1–31 May 2016). Remote sensing measurements (e.g., aerosol and wind Doppler lidar) and on-line WRF-Chem modeling results were used by applying three different PBL parameterizations: Yonsei University (YSU), Mellor–Yamada–Janjic (MYJ), and Asymmetrical Convective Model v2 (ACM2). Our results indicated that the uncertainties of PBLH–PM interactions were not large in daytime, whereas the uncertainties of nPBLH–PM2.5 interactions were significant. All WRF-Chem experiments showed a clear tendency to underestimate nighttime nPBLH by a factor of ~3 compared with observations, and shallow nPBLH clearly led to extremely high PM2.5 peaks during the night. These uncertainties associated with nPBLH and nPBLH–PM2.5 simulations suggest that PM2.5 peaks predicted from nighttime or next-morning nPBLH simulations should be interpreted with caution. Additionally, we discuss uncertainties among PBL parameterization schemes in relation to PM2.5 simulations.

Aerosol Layer Height Retrieval Over Ocean From the Advanced Himawari Imager Using Spectral Reflectance Sensitivity

Aerosol layer height (ALH) has been retrieved using multi-angle observations or the O2–O2 and O2–A/B absorption bands. This study attempted to retrieve ALH using the Advanced Himawari Imager (AHI), a single passive imager onboard Himawari-8 and -9. ALH retrieval using geostationary Earth orbit (GEO) satellites is advantageous for monitoring diurnal changes in ALH and understanding long-range transport. Before retrieving the ALH, the aerosol optical properties (AOPs) are retrieved using the green-near infrared (NIR) band, which is relatively insensitive to aerosol height. The retrieved AOPs are used as input to the radiative transfer calculation to compute the top-of-atmosphere (TOA) reflectance of a highly sensitive band (the blue band in this study). Then, the ALH is retrieved using the observed and calculated TOA reflectances. Since the retrieval accuracy of the aerosol optical depth (AOD) is better over the ocean, the retrieval was performed only over the ocean during the Korea–United States Air Quality Study (KORUS-AQ) campaign period. The retrieved ALH was validated using the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) and high-spectral-resolution Lidar (HSRL).

Impacts of uncertainties in emissions on aerosol data assimilation and short-term PM2.5 predictions over Northeast Asia

To improve PM2.5 predictions in Northeast Asia, we estimated a new background error covariance matrix (BEC) for aerosol data assimilation using surface PM2.5 observations. In contrast to the conventional method of BEC estimation that uses perturbations in meteorological data, this method additionally considered the perturbations using two different emission inventories. By taking the emission uncertainty into account, we found that the standard deviations in the BEC were significantly increased. The standard deviations became around three times larger than those in the conventional method at the surface. The impacts of the new BEC were then tested for the prediction of surface PM2.5 over Northeast Asia using the Community Multiscale Air Quality (CMAQ) model initialized by three-dimensional variational method (3D-VAR). The surface PM2.5 data measured at 154 sites in South Korea and 1535 sites in China were assimilated every 6 h during the campaign period of the Korea-United States Air Quality Study (KORUS-AQ) (1 May–14 June 2016). The data assimilation with the new BEC showed better agreement with the surface PM2.5 observations than with the BEC from the conventional method. Our method was also more consistent with the observations in 24-h PM2.5 predictions than the conventional method (specifically, with a ∼44% reduction of negative biases). We concluded that increased standard deviations, together with updated horizontal and vertical length scales in the new BEC, improved the data assimilation and short-term predictions of the surface PM2.5. This paper also suggests several research efforts to further improve the BEC for better short-term PM2.5 predictions in Northeast Asia.

Contributions to OH reactivity from unexplored volatile organic compounds measured by PTR-ToF-MS – a case study in a suburban forest of the Seoul metropolitan area during the Korea–United States Air Quality Study (KORUS-AQ) 2016

Abstract. We report OH reactivity observations by a chemical ionization mass spectrometer–comparative reactivity method (CIMS-CRM) instrument in a suburban forest of the Seoul metropolitan area (SMA) during the Korea–United States Air Quality Study (KORUS-AQ 2016) from mid-May to mid-June of 2016. A comprehensive observational suite was deployed to quantify reactive trace gases inside of the forest canopy including a high-resolution proton transfer reaction time-of-flight mass spectrometer (PTR-ToF-MS). An average OH reactivity of 30.7±5.1 s−1 was observed, while the OH reactivity calculated from CO, NO+NO2 (NOx), ozone (O3), sulfur dioxide (SO2), and 14 volatile organic compounds (VOCs) was 11.8±1.0 s−1. An analysis of 346 peaks from the PTR-ToF-MS accounted for an additional 6.0±2.2 s−1 of the total measured OH reactivity, leaving 42.0 % missing OH reactivity. A series of analyses indicate that the missing OH reactivity most likely comes from VOC oxidation products of both biogenic and anthropogenic origin.

Airborne formaldehyde and volatile organic compound measurements over the Daesan petrochemical complex on Korea’s northwest coast during the Korea-United States Air Quality study

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.

Validation of XCO<sub>2</sub> and XCH<sub>4</sub> retrieved from a portable Fourier transform spectrometer with those from in situ profiles from aircraft-borne instruments

Abstract. Column-averaged dry-air mole fractions of carbon dioxide (XCO2) and methane (XCH4) measured by a solar viewing portable Fourier transform spectrometer (FTS, EM27/SUN) have been characterized and validated by comparison using in situ profile measurements made during the transfer flights of two aircraft campaigns: Korea-United States Air Quality Study (KORUS-AQ) and Effect of Megacities on the Transport and Transformation of Pollutants at Regional and Global Scales (EMeRGe). The aircraft flew over two Total Carbon Column Observing Network (TCCON) sites: Rikubetsu, Japan (43.46∘ N, 143.77∘ E), for the KORUS-AQ campaign and Burgos, Philippines (18.53∘ N, 120.65∘ E), for the EMeRGe campaign. The EM27/SUN was deployed at the corresponding TCCON sites during the overflights. The mole fraction profiles obtained by the aircraft over Rikubetsu differed between the ascending and the descending flights above approximately 8 km for both CO2 and CH4. Because the spatial pattern of tropopause heights based on potential vorticity values from the ERA5 reanalysis shows that the tropopause height over the Rikubetsu site was consistent with the descending profile, we used only the descending profile to compare with the EM27/SUN data. Both the XCO2 and XCH4 derived from the descending profiles over Burgos were lower than those from the ascending profiles. Output from the Weather Research and Forecasting Model indicates that higher CO2 for the ascending profile originated in central Luzon, an industrialized and densely populated region about 400 km south of the Burgos TCCON site. Air masses observed with the EM27/SUN overlap better with those from the descending aircraft profiles than those from the ascending aircraft profiles with respect to their properties such as origin and atmospheric residence times. Consequently, the descending aircraft profiles were used for the comparison with the EM27/SUN data. The EM27/SUN XCO2 and XCH4 data were derived by using the GGG2014 software without applying air-mass-independent correction factors (AICFs). The comparison of the EM27/SUN observations with the aircraft data revealed that, on average, the EM27/SUN XCO2 data were biased low by 1.22 % and the EM27/SUN XCH4 data were biased low by 1.71 %. The resulting AICFs of 0.9878 for XCO2 and 0.9829 for XCH4 were obtained for the EM27/SUN. Applying AICFs being utilized for the TCCON data (0.9898 for XCO2 and 0.9765 for XCH4) to the EM27/SUN data induces an underestimate for XCO2 and an overestimate for XCH4.

Semi-continuous Measurements of Water-soluble Organic Carbon and Ionic Composition of PM2.5 in Baengnyeong Island during the 2016 KORUS-AQ (Korea-United States Air Quality Study)

This study characterized the water-soluble organic carbon (WSOC) and ionic components of PM2.5 (particles less than 2.5 µm in diameter) from April to June 2016, at Baengnyeong Island The study utilized a particle-into-liquid sampler (PILS) coupled with a total organic carbon (TOC) analyzer and ion chromatography (PILS-TOC-IC). The PM2.5 mean concentration in this study was 23.8±16.7 µg m−3, and the mean of WSOC concentration was 1.6±1.5 µg m−3. Ionic compounds increased by 3.8% in the period in which the air quality standard of PM2.5 (35 µg m−3) was exceeded because the concentration of ionic components increased due to generation by chemical reactions and emissions from a primary source in a nearby urban area. The wind direction and speed were mostly in the northwest and southwest directions and the higher concentration of PM2.5 was also shown in the same directions. In comparison with the previous study, the WSOC/OC ratio was 0.5±0.3 in Baengnyeong Island, which was higher than that at roadside and urban sites and lower than at the background site (Sweden, Aspvreten). It was considered that insoluble OC constituted a major proportion of primary OC that was emitted in urban areas, and the higher WSOC/OC ratios of rural and background sites were affected by inflow. The ratio of nitrate and sulfate in Baengnyeong Island was lower than urban areas in China in other studies, because of emitted aerosols from coal combustion or vehicle emission. The results indicate that Baengnyeong Island was affected by formation of secondary aerosols by chemical reactions and inflow from China as well as domestic emissions. The slope of H+Aersol/SO42− in Baengnyeong Island was 0.079, which was a result of neutralized particle acidity in ambient air. The molar ratio of nitrate and ammonium with sulfate in Baengnyeong Island showed ammoniumrich conditions because ammonium nitrate was increased to homogeneous reaction of ammonia and nitric acid in the gas-phase.

Analysis of the factors influencing PM2.5 concentration

미세먼지 문제는 삶의 질을 떨어뜨리는 대표적인 환경문제로, 최근 미세먼지 및 초미세먼지농도가 높아짐에 따라 개인 건강의 문제 뿐 만 아니라 국가 경제에도 영향을 미치고 있는 것으로 나타나고 있다. 2016년에 수행된 한미대기질합동연구에 따르면 미세먼지 오염은 국내 배출원이 지배적 기여를 하며, 해외로부터의 영향은 작은 것으로 알려졌다. 이 뿐만 아니라, 기상상태 가운데서는 풍속이 미세먼지 오염에 영향을 준다는 연구결과 역시 알려졌다. 본 논문에서는 배출원을 제외하면 미세먼지농도에 가장 큰 영향을 주는 것으로 알려진 풍향 및 풍속 등의 기상상태가 초미세먼지 농도에 어떠한 영향을 주는지를 파악하기 위해 일반화가법모형을 이용하였다. 분석결과 풍속 뿐 만 아니라, 풍향 역시 초미세먼지 농도에 영향을 주는 것으로 나타났으며, 봄, 여름 및 가을에는 남서풍 및 서풍의 영향을 주로 받으며, 겨울에는 남동풍에서 서풍에 이르는 광범위한 범위에서 초미세먼지 농도에 영향을 주는 것으로 나타났다. 초미세먼지 농도를 낮추기 위한 다양한 국가정책이 시행되고 있는 가운데, 초미세먼지 농도에 영향을 주는 요인에 대한 면밀한 파악이 필요하며, 본 논문의 분석결과가 이에 기여할 수 있을 것으로 기대된다.The fine dust problem is getting serious that deteriorates the quality of life. Recently, the concentration of PM10 and PM2.5 has increased, and it has been known that it affects not only the public health but also the national economy. KORUS-AQ(Korea-United States Air Quality Study) conducted in 2016 reported that the contribution of domestic emission sources for the fine fust pollution dominate other sources from abroad. In addition, research has also been reported that the primary reason for the concentration of fine dust is wind speed in weather conditions. In this paper, the generalized additive model was applied to investigate how the weather conditions such as wind direction and wind speed affect the PM2.5 concentration without consideration of the emission sources. The result of analysis showed that not only wind speed, but also wind direction influenced the concentration of PM2.5, mainly affected by southwest and west wind in spring, summer and fall, and a wide range from southeast to west wind in winter. To reduce the concentration of the fine dust, the factors affecting the concentration of the fine dust should be identified clearly, and the analysis results of this paper can be contributable.

Assessment of NO2 observations during DISCOVER-AQ and KORUS-AQ field campaigns.

NASA’s Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ, conducted in 2011–2014) campaign in the United States and the joint NASA and National Institute of Environmental Research (NIER) Korea–United States Air Quality Study (KORUS-AQ, conducted in 2016) in South Korea were two field study programs that provided comprehensive, integrated datasets of airborne and surface observations of atmospheric constituents, including nitrogen dioxide (NO2), with the goal of improving the interpretation of spaceborne remote sensing data. Various types of NO2 measurements were made, including in situ concentrations and column amounts of NO2 using ground- and aircraft-based instruments, while NO2 column amounts were being derived from the Ozone Monitoring Instrument (OMI) on the Aura satellite. This study takes advantage of these unique datasets by first evaluating in situ data taken from two different instruments on the same aircraft platform, comparing coincidently sampled profile-integrated columns from aircraft spirals with remotely sensed column observations from ground-based Pandora spectrometers, intercomparing column observations from the ground (Pandora), aircraft (in situ vertical spirals), and space (OMI), and evaluating NO2 simulations from coarse Global Modeling Initiative (GMI) and high-resolution regional models. We then use these data to interpret observed discrepancies due to differences in sampling and deficiencies in the data reduction process. Finally, we assess satellite retrieval sensitivity to observed and modeled a priori NO2 profiles. Contemporaneous measurements from two aircraft instruments that likely sample similar air masses generally agree very well but are also found to differ in integrated columns by up to 31.9 %. These show even larger differences with Pandora, reaching up to 53.9 %, potentially due to a combination of strong gradients in NO2 fields that could be missed by aircraft spirals and errors in the Pandora retrievals. OMI NO2 values are about a factor of 2 lower in these highly polluted environments due in part to inaccurate retrieval assumptions (e.g., a priori profiles) but mostly to OMI’s large footprint (> 312 km2).

Development of Korean Air Quality Prediction System version 1 (KAQPS v1) with focuses on practical issues

Abstract. For the purpose of providing reliable and robust air quality predictions, an 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 Multiscale 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 (SO42-), nitrate (NO3-), ammonium (NH4+), 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 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 (index of agreement IOA =0.60; mean bias 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 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 peroxyacetyl nitrates – 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 (MLHs) 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 3D variational (3DVAR) method and ensemble Kalman filter (EnK) are being tested and will be introduced to the Korean air quality prediction system (KAQPS).

Observation-based modeling of ozone chemistry in the Seoul metropolitan area during the Korea-United States Air Quality Study (KORUS-AQ)

The Seoul Metropolitan Area (SMA) has a population of 24 million and frequently experiences unhealthy levels of ozone (O3). In this work, measurements taken during the Korea-United States Air Quality Study (KORUS-AQ, 2016) are used to explore regional gradients in O3 and its chemical precursors, and an observationally-constrained 0-D photochemical box model is used to quantify key aspects of O3 production including its sensitivity to precursor gases. Box model performance was evaluated by comparing modeled concentrations of select secondary species to airborne measurements. These comparisons indicate that the steady state assumption used in 0-D box models cannot describe select intermediate species, highlighting the importance of having a broad suite of trace gases as model constraints. When fully constrained, aggregated statistics of modeled O3 production rates agreed with observed changes in O3, indicating that the box model was able to represent the majority of O3 chemistry. Comparison of airborne observations between urban Seoul and a downwind receptor site reveal a positive gradient in O3 coinciding with a negative gradient in NOx, no gradient in CH2O, and a slight positive gradient in modeled rates of O3 production. Together, these observations indicate a radical-limited (VOC-limited) O3 production environment in the SMA. Zero-out simulations identified C7+ aromatics as the dominant VOC contributors to O3 production, with isoprene and anthropogenic alkenes making smaller but appreciable contributions. Simulations of model sensitivity to decreases in NOx produced results that were not spatially uniform, with large increases in O3 production predicted for urban Seoul and decreases in O3 production predicted for far-outlying areas. The policy implications of this work are clear: Effective O3 mitigation strategies in the SMA must focus on reducing local emissions of C7+ aromatics, while reductions in NOx emissions may increase O3 in some areas but generally decrease the regional extent of O3 exposure.

Characterization, sources and reactivity of volatile organic compounds (VOCs) in Seoul and surrounding regions during KORUS-AQ

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.

Integration of airborne and ground observations of nitryl chloride in the Seoul metropolitan area and the implications on regional oxidation capacity during KORUS-AQ 2016

Abstract. Nitryl chloride (ClNO2) is a radical reservoir species that releases chlorine radicals upon photolysis. An integrated analysis of the impact of ClNO2 on regional photochemistry in the Seoul metropolitan area (SMA) during the Korea–United States Air Quality Study (KORUS-AQ) 2016 field campaign is presented. Comprehensive multiplatform observations were conducted aboard the NASA DC-8 and at two ground sites (Olympic Park, OP; Taehwa Research Forest, TRF), representing an urbanized area and a forested suburban region, respectively. Positive correlations between daytime Cl2 and ClNO2 were observed at both sites, the slope of which was dependent on O3 levels. The possible mechanisms are explored through box model simulations constrained with observations. The overall diurnal variations in ClNO2 at both sites appeared similar but the nighttime variations were systematically different. For about half of the observation days at the OP site the level of ClNO2 increased at sunset but rapidly decreased at around midnight. On the other hand, high levels were observed throughout the night at the TRF site. Significant levels of ClNO2 were observed at both sites for 4–5 h after sunrise. Airborne observations, box model calculations, and back-trajectory analysis consistently show that these high levels of ClNO2 in the morning are likely from vertical or horizontal transport of air masses from the west. Box model results show that chlorine-radical-initiated chemistry can impact the regional photochemistry by elevating net chemical production rates of ozone by ∼25 % in the morning.

Validation, comparison, and integration of GOCI, AHI, MODIS, MISR, and VIIRS aerosol optical depth over East Asia during the 2016 KORUS-AQ campaign

Abstract. Recently launched multichannel geostationary Earth orbit (GEO) satellite sensors, such as the Geostationary Ocean Color Imager (GOCI) and the Advanced Himawari Imager (AHI), provide aerosol products over East Asia with high accuracy, which enables the monitoring of rapid diurnal variations and the transboundary transport of aerosols. Most aerosol studies to date have used low Earth orbit (LEO) satellite sensors, such as the Moderate Resolution Imaging Spectroradiometer (MODIS) and the Multi-angle Imaging Spectroradiometer (MISR), with a maximum of one or two overpass daylight times per day from midlatitudes to low latitudes. Thus, the demand for new GEO observations with high temporal resolution and improved accuracy has been significant. In this study the latest versions of aerosol optical depth (AOD) products from three LEO sensors – MODIS (Dark Target, Deep Blue, and MAIAC), MISR, and the Visible/Infrared Imager Radiometer Suite (VIIRS), along with two GEO sensors (GOCI and AHI), are validated, compared, and integrated for a period during the Korea–United States Air Quality Study (KORUS-AQ) field campaign from 1 May to 12 June 2016 over East Asia. The AOD products analyzed here generally have high accuracy with high R (0.84–0.93) and low RMSE (0.12–0.17), but their error characteristics differ according to the use of several different surface-reflectance estimation methods. High-accuracy near-real-time GOCI and AHI measurements facilitate the detection of rapid AOD changes, such as smoke aerosol transport from Russia to Japan on 18–21 May 2016, heavy pollution transport from China to the Korean Peninsula on 25 May 2016, and local emission transport from the Seoul Metropolitan Area to the Yellow Sea in South Korea on 5 June 2016. These high-temporal-resolution GEO measurements result in more representative daily AOD values and make a greater contribution to a combined daily AOD product assembled by median value selection with a 0.5∘×0.5∘ grid resolution. The combined AOD is spatially continuous and has a greater number of pixels with high accuracy (fraction within expected error range of 0.61) than individual products. This study characterizes aerosol measurements from LEO and GEO satellites currently in operation over East Asia, and the results presented here can be used to evaluate satellite measurement bias and air quality models.

Radiance-based retrieval bias mitigation for the MOPITT instrument: the version 8 product

Abstract. The MOPITT (Measurements of Pollution in the Troposphere) satellite instrument has been making nearly continuous observations of atmospheric carbon monoxide (CO) since 2000. Satellite observations of CO are routinely used to analyze emissions from fossil fuels and biomass burning, as well as the atmospheric transport of those emissions. Recent enhancements to the MOPITT retrieval algorithm have resulted in the release of the version 8 (V8) product. V8 products benefit from updated spectroscopic data for water vapor and nitrogen used to develop the operational radiative transfer model and exploit a new method for minimizing retrieval biases through parameterized radiance bias correction. In situ datasets used for algorithm development and validation include the NOAA (National Oceanic and Atmospheric Administration) and HIPPO (HIAPER Pole-to-Pole Observations) datasets used for earlier MOPITT validation work in addition to measurements from the ACRIDICON-CHUVA (Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems – Cloud processes of the main precipitation systems in Brazil: A contribution to cloud resolving modeling and to the GPM (Global Precipitation Measurement)), KORUS-AQ (The Korea-United States Air Quality Study), and ATom (The Atmospheric Tomography Mission) programs. Validation results illustrate clear improvements with respect to long-term bias drift and geographically variable retrieval bias. For example, whereas bias drift for the V7 thermal-infrared (TIR)-only product exceeded 0.5 % yr−1 for levels in the upper troposphere (e.g., at 300 hPa), bias drift for the V8 TIR-only product is found to be less than 0.1 % yr−1 at all levels. Also, whereas upper-tropospheric (300 hPa) retrieval bias in the V7 TIR-only product exceeded 10 % in the tropics, corresponding V8 biases are less than 5 % (in terms of absolute value) at all latitudes and do not exhibit a clear latitudinal dependence.

The first evaluation of formaldehyde column observations by improved Pandora spectrometers during the KORUS-AQ field study.

The Korea-United States Air Quality Study (KORUS-AQ) conducted during May-June 2016 offered the first opportunity to evaluate direct-sun observations of formaldehyde (HCHO) total column densities with improved Pandora spectrometer instruments. The measurements highlighted in this work were conducted both in the Seoul megacity area at the Olympic Park site (37.5232° N, 27.1260° E; 26 ma.s.l.) and at a nearby rural site downwind of the city at the Mount Taehwa research forest site (37.3123° N, 127.3106° E; 160ma.s.l.). Evaluation of these measurements was made possible by concurrent ground-based in situ observations of HCHO at both sites as well as overflight by the NASA DC-8 research aircraft. The flights provided in situ measurements of HCHO to characterize its vertical distribution in the lower troposphere (0-5km). Diurnal variation in HCHO total column densities followed the same pattern at both sites, with the minimum daily values typically observed between 6:00 and 7:00 local time, gradually increasing to a maximum between 13:00 and 17:00 before decreasing into the evening. Pandora vertical column densities were compared with those derived from the DC-8 HCHO in situ measured profiles augmented with in situ surface concentrations below the lowest altitude of the DC-8 in proximity to the ground sites. A comparison between 49 column densities measured by Pandora vs. aircraft-integrated in situ data showed that Pandora values were larger by 16% with a constant offset of 0.22DU (Dobson units; R 2 = 0.68). Pandora HCHO columns were also compared with columns calculated from the surface in situ measurements over Olympic Park by assuming a well-mixed lower atmosphere up to a ceilometer-measured mixed-layer height (MLH) and various assumptions about the small residual HCHO amounts in the free troposphere up to the tropopause. The best comparison (slope = 1.03±0.03; intercept = 0.29±0.02DU; and R 2 = 0.78±0.02) was achieved assuming equal mixing within ceilometer-measured MLH combined with an exponential profile shape. These results suggest that diurnal changes in HCHO surface concentrations can be reasonably estimated from the Pandora total column and information on the mixed-layer height. More work is needed to understand the bias in the intercept and the slope relative to columns derived from the in situ aircraft and surface measurements.

Impact of urban aerosol properties on cloud condensation nuclei (CCN) activity during the KORUS-AQ field campaign

Ground measurements of physical, chemical and hygroscopic properties of aerosols were made at the Olympic Park, Seoul, as part of the KORea-United States Air Quality study (KORUS-AQ) campaign in May–June 2016. The average number concentrations of aerosols larger than 10 nm in diameter and cloud condensation nuclei (CCN) at 0.6% supersaturation (S) were 10800 cm−3 and 3400 cm−3, respectively. The average geometric mean diameter (Dg) was 44 nm, and size-resolved aerosol hygroscopicity (κ) from HTDMA ranged from 0.11 to 0.24 for particle diameters in the range of 30–150 nm. Aerosols were classified into three types based on mixing state and hygroscopic growth factor (GF): Type 1 (externally mixed aerosol), Type 2 (Internally mixed and growth aerosol) and Type 3 (internally mixed and non-growth aerosol). These three aerosol types showed distinct diurnal patterns. The difference in physical and chemical properties of aerosols for different air mass sources crucially impacted aerosol hygroscopicity. Using the external mixture assumption with measured hygroscopicity data improved the results of CCN prediction compared to those from the simple internal mixture assumption because externally mixed aerosols comprised a significant portion of aerosols in this urban area. Moreover, the simple assumption of aerosol size distribution with a fixed chemical composition sufficiently explained more than 50 percent of the variation of CCN number concentrations, although the information of chemical composition was still meaningful. Overall, the measured data showed consistency with Megacity Air Pollution Studies (MAPS-Seoul) campaign held during May–June 2015, implying that these results may represent urban aerosols in spring/summer in the Korean Peninsula.