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In this study, we developed a data assimilation (DA) system for chemical transport model (CTM) simulations using an ensemble Kalman filter (EnKF) technique. This DA technique is easy to implement in an existing system without seriously modifying the original CTM and can provide flow-dependent corrections based on error covariance by short-term ensemble propagations. First, the PM2.5 observations at ground stations were assimilated in this DA system every 6 h over South Korea for the period of the KORUS–AQ campaign from 1 May to 12 June 2016. The DA performances with the EnKF were then compared to a control run (CTR) without DA and a run with three-dimensional variational (3D-Var) DA. Consistent improvements owing to the initial conditions (ICs) assimilated with the EnKF were found in the DA experiments at a 6 h interval compared to the CTR run and to the run with 3D-Var. In addition, we attempted to assimilate the ground observations from China to examine the impacts of improved boundary conditions (BCs) on the PM2.5 predictability over South Korea. The contributions of the ICs and BCs to improvements in the PM2.5 predictability were also quantified. For example, the relative reductions in terms of the normalized mean bias (NMB) were found to be approximately 27.2 % for the 6 h reanalysis run. A series of 24 h PM2.5 predictions were additionally conducted each day at 00:00 UTC with the optimized ICs. The relative reduction of the NMB was 17.3 % for the 24 h prediction run when the updated ICs were applied at 00:00 UTC. This means that after the application of the updated BCs, an additional 9.0 % reduction in the NMB was achieved for 24 h PM2.5 predictions in South Korea.

Changes in the aerosol composition of sulfate (SO42−) and nitrate (NO3−) from 2012 to 2019 have been captured as a paradigm shift in the region downwind of China. Specifically, SO42− dramatically decreased and NO3− dramatically increased over downwind locations such as western Japan due to the faster reduction of SO2 emissions than NOx emissions and the almost constant trend of NH3 emissions from China. Emissions from China sharply decreased during COVID-19 lockdowns in February–March 2020, after which China’s economic situation seemed to recover going into 2021. Given this substantial change in Chinese emissions, it is necessary to clarify the impact of long-range PM2.5 transport over East Asia. In this study, ground-based aerosol compositions observed at three sites in western Japan were analysed. The concentrations of PM2.5, SO42− and NO3− decreased in 2020 (during COVID-19) compared with 2018–2019 (before COVID-19). In 2021 (after COVID-19), PM2.5 and NO3− increased and SO42− was unchanged. This suggests the returning impact of long-range PM2.5 transport in 2021. From numerical simulations, the status of Chinese emissions during COVID-19 did not explain this returning impact in 2021. This study shows that the status of Chinese emissions in 2021 was close to that before COVID-19.

In this study, we developed a data assimilation (DA) system for chemical transport model (CTM) simulations using an ensemble Kalman filter (EnKF) technique. This DA technique is easy to implement to an existing system without seriously modifying the original CTM, and can provide flow-dependent corrections based on error covariance by short-term ensemble propagations. First, the PM2.5 observations at ground stations were assimilated in this DA system every 6 hours over South Korea for the period of the KORUS–AQ campaign, from 1 May to 12 June, 2016. The DA performances with the EnKF were then compared to a control run (CTR) without DA, as well as a run with three-dimensional variational (3DVAR) DA. Consistent improvements due to the ICs assimilated with the EnKF were found in the DA experiments with 6 h interval, compared to the CTR run, and to the run with 3DVAR. In addition, we attempted to assimilate the ground observations from China to examine the impacts of improved boundary concentrations (BCs) on the PM2.5 predictability over South Korea. The contributions of the ICs and BCs to improvements in the PM2.5 predictability were also quantified. For example, the relative reductions in terms of the normalized mean bias (NMB) were found to be about 27.2 % for the 6 h reanalysis run. A series of 24 hour PM2.5 predictions were additionally conducted each day at 00 UTC with the optimized initial concentrations (ICs). The relative reduction of the NMB was 17.3 % for the 24 h prediction run, when the updated ICs were applied at 00 UTC. This means that after the application of the updated BCs, an additional 9.0 % reduction in the NMB was achieved for 24 h PM2.5 predictions in South Korea.

The black carbon (BC) and carbon monoxide (CO) emission ratios were estimated and compiled from long-term, harmonized observations of the ΔBC∕ΔCO ratios under conditions unaffected by wet deposition at four sites in East Asia, including two sites in South Korea (Baengnyeong and Gosan) and two sites in Japan (Noto and Fukuoka). Extended spatio-temporal coverage enabled estimation of the full seasonality and elucidation of the emission ratio in North Korea for the first time. The estimated ratios were used to validate the Regional Emission inventory in ASia (REAS) version 2.1 based on six study domains (“East China”, “North China”, “Northeast China”, South Korea, North Korea, and Japan). We found that the ΔBC∕ΔCO ratios from four sites converged into a narrow range (6.2–7.9 ng m−3 ppb−1), suggesting consistency in the results from independent observations and similarity in source profiles over the regions. The BC∕CO ratios from the REAS emission inventory (7.7 ng m−3 ppb−1 for East China – 23.2 ng m−3 ppb−1 for South Korea) were overestimated by factors of 1.1 for East China to 3.0 for South Korea, whereas the ratio for North Korea (3.7 ng m−3 ppb−1 from REAS) was underestimated by a factor of 2.0, most likely due to inaccurate emissions from the road transportation sector. Seasonal variation in the BC∕CO ratio from REAS was found to be the highest in winter (China and North Korea) or summer (South Korea and Japan), whereas the measured ΔBC∕ΔCO ratio was the highest in spring in all source regions, indicating the need for further characterization of the seasonality when creating a bottom-up emission inventory. At levels of administrative districts, overestimation in Seoul, the southwestern regions of South Korea, and Northeast China was noticeable, and underestimation was mainly observed in the western regions in North Korea, including Pyongyang. These diagnoses are useful for identifying regions where revisions in the inventory are necessary, providing guidance for the refinement of BC and CO emission rate estimates over East Asia.

The Taklimakan Desert is known to be one of the world’s major sources of aeolian dust particles. Continuous images with 10-min temporal and 2-km spatial resolutions from a new-generation geostationary meteorological satellite captured the lifecycle (generation, evolution and outflow) of a previously unrecognized type of Taklimakan dust storm. The dust storm showed an anti-clockwise spiral structure and a clear core and behaved like a “dust vortex”. From image analysis, the horizontal scale and temporal lifetime of the dust vortex were estimated to be 600 km and 36 hours, respectively. We found that a strong pressure trough (cut-off low), along with a cold air mass located on the northwestern side of the Taklimakan Desert and the high mountains surrounding the Taklimakan Desert, played important roles in the formation and evolution of the dust vortex.

East Asian oceans are possibly affected by a high nitrogen (N) burden because of the intense anthropogenic emissions in this region. Based on high-resolution regional chemical transport modeling with horizontal grid scales of 36 and 12 km, we investigated the N burden into East Asian oceans via atmospheric deposition in 2010. We found a high N burden of 2–9 kg N ha-1 yr-1 over the Yellow Sea, East China Sea (ECS), and Sea of Japan. Emissions over East Asia were dominated by ammonia (NH3) over land and nitrogen oxides (NOx) over oceans, and N deposition was dominated by reduced N over most land and open ocean, whereas it was dominated by oxidized N over marginal seas and desert areas. The verified numerical modeling identified that the following processes were quantitatively important over East Asian oceans: the dry deposition of nitric acid (HNO3), NH3, and coarse-mode (aerodynamic diameter greater than 2.5 μm) NO3-, and wet deposition of fine-mode (aerodynamic diameter less than 2.5 μm) NO3- and NH4+. The relative importance of the dry deposition of coarse-mode NO3- was higher over open ocean. The estimated N deposition to the whole ECS was 390 Gg N yr-1; this is comparable to the discharge from the Yangtze River to the ECS, indicating the significant contribution of atmospheric deposition. Based on the high-resolution modeling over the ECS, a tendency of high deposition in the western ECS and low deposition in the eastern ECS was found, and a variety of deposition processes were estimated. The dry deposition of coarse-mode NO3- and wet deposition of fine-mode NH4+ were the main factors, and the wet deposition of fine-mode NO3- over the northeastern ECS and wet deposition of coarse-mode NO3- over the southeastern ECS were also found to be significant processes determining N deposition over the ECS.

There has been little study on the effect of Asian dust exposure on respiratory symptoms among children who are vulnerable to environmental factors. In this panel study, we investigated the effect of Asian dust on respiratory symptoms among children with and without asthma, and their sensitivity. Children attending two elementary schools (137 total), and 23 children with asthma from cooperating medical institutions in Fukuoka prefecture were recruited. Subjects measured peak expiratory flow rate (PEF), and recorded asthma-like symptoms, cough, nasal symptoms and use of medication in a diary from April 1, 2013 to June 30, 2013. To assess exposure to Asian dust, we used Light Detection and Ranging (LIDAR) data. For the analysis of the association between Asian dust and respiratory symptoms, the case-crossover design and generalized estimating equation (GEE) models were used. Taking individual sensitivity to respiratory aggravation into consideration, the subjects were classified into three groups: children without asthma, children with asthma who do not use long-term preventive medication (CA) and children with asthma who use long-term preventive medication (CA-LTM). For CA, Asian dust exposure was significantly associated with asthma-like symptoms, with a hazard ratio of 5.17 (95%CI: 1.02=26.12) at Lag0, and the change in %maxPEF, -1.65% (95%CI:-2.82, -0.48) at Lag0. For children without asthma, a statistically significant association was found between Asian dust exposure and the change in %maxPEF, -0.56% (95%CI: -1.31, -0.08) at Lag1. However, no adverse effects were observed in CA-LTM. Temperature had significant effects on %maxPEF for three groups. Asian dust, photochemical oxidant and pollen caused simultaneously additive adverse effects on nasal symptoms for children without asthma. This study suggests the possibility that long-term preventive medication to manage asthma may suppress aggravation of respiratory symptoms due to Asian dust and may be an effective prevention.

The effect of the nonsphericity of mineral dust aerosols on its deposition and transport was investigated based on model simulation for a typical dust event over northern China from April 6 to 12, 2018. The settling velocity related to morphological change in dust size was considered in Nested Air Quality Prediction Modeling System (NAQPMS) to simulate the dust spatial distribution. Comparison of these results with observations showed that the model reproduced the temporal variability in the mass concentration of particles along the dust plume pathway. The most frequently reported aspect ratio (λ) was 1.7 ± 0.2 for Asian dust aerosols. Changing the nonsphericity of the particle from typical prolate ellipsoids (λ = 1.7) to spherical ellipsoids (λ = 1) caused an ~3% decrease in the surface dust concentration on average. For particles with diameters5 μm, nonsphericity caused a change in the surface dust concentration up to 10%, especially at the periphery of the dust source region. The overall effects on the fine dust (2.5 μm) were not significant. A sensitivity study using a more extreme nonspherical shape (λ = 2) showed that the differences in PM

Acidifying species in precipitation can have severe impacts on ecosystems. The chemical composition of precipitation is directly related to the amount of precipitation; accordingly, it is difficult to identify long-term variation in chemical concentrations. The ratio of the nitrate (NO3−) to non-sea-salt sulfate (nss-SO42−) concentration in precipitation on an equivalent basis (hereinafter, Ratio) is a useful index to investigate the relative contributions of these acidifying species. To identify the long-term record of acidifying species in precipitation over East Asia, the region with the highest emissions worldwide, we compiled ground-based observations of the chemical composition of precipitation over China, Korea, and Japan from 2001 to 2015 based on the Acid Deposition Monitoring Network in East Asia (EANET). The spatial coverage was limited, but additional monitoring data for Japan, southern China, and northern China around Beijing were utilized. The period of analysis was divided into three phases: Phase I (2001–2005), Phase II (2006–2010), and Phase III (2011–2015). The behaviors of NO3− and nss-SO42− concentrations and hence the Ratio in precipitation were related to these precursors. The anthropogenic NOx and SO2 emissions and the NOx ∕ SO2 emission ratio were analyzed. Further, satellite observations of the NO2 and SO2 column density to capture the variation in emissions were applied. We found that the long-term trend in the NO3− concentration in precipitation was not related to the variation in NOx emission and the NO2 column. In comparison, the nss-SO42− concentration in precipitation over China, Korea, and Japan was partially connected to the changes in SO2 emissions from China, but the trends were not significant. The long-term trends of Ratio over China, Korea, and Japan were nearly flat during Phase I, increased significantly during Phase II, and were essentially flat again during Phase III. This variation in Ratio in East Asia clearly corresponded to the NOx ∕ SO2 emission ratio and the NO2 ∕ SO2 column ratio in China. The initial flat trend during Phase I was due to increases in both NOx and SO2 emissions in China, the significantly increasing trend during Phase II was triggered by the increase in NOx emissions and decrease in SO2 emissions in China, and the return to a flat trend during Phase III was caused by declines in both NOx and SO2 emissions in China. These results suggest that emissions in China had a significant impact not only on China but also on downwind precipitation chemistry during the 15-year period of 2001–2015. In terms of wet deposition, the NO3− wet deposition over China, Korea, and Japan did not change dramatically, but the nss-SO42− wet deposition declined over China, Korea, and Japan from Phase II to III. These declines were caused by a strong decrease in the nss-SO42− concentration in precipitation accompanied by a reduction in SO2 emission from China, which counteracted the increase in precipitation. These findings indicated that the acidity of precipitation shifted from sulfur to nitrogen.

The emission characteristics of refractory black carbon (rBC) from biomass burning are essential information for numerical simulations of regional pollution and climate effects. We conducted combustion experiments in the laboratory to investigate the emission ratio and mixing state of rBC from the burning of wheat straw and rapeseed plants, which are the main crops cultivated in the Yangtze River Delta region of China. A single particle soot photometer (SP2) was used to measure rBC-containing particles at high temporal resolution and with high accuracy. The combustion state of each burning case was indicated by the modified combustion efficiency (MCE), which is calculated using the integrated enhancement of carbon dioxide and carbon monoxide concentrations relative to their background values. The mass size distribution of the rBC particles showed a lognormal shape with a mode mass equivalent diameter (MED) of 189 nm (ranging from 152 to 215 nm), assuming an rBC density of 1.8 g cm−3. rBC particles less than 80 nm in size (the lower detection limit of the SP2) accounted for ∼ 5 % of the total rBC mass, on average. The emission ratios, which are expressed as ΔrBC ∕ ΔCO (Δ indicates the difference between the observed and background values), displayed a significant positive correlation with the MCE values and varied between 1.8 and 34 ng m−3 ppbv−1. Multi-peak fitting analysis of the delay time (Δt, or the time of occurrence of the scattering peak minus that of the incandescence peak) distribution showed that rBC-containing particles with rBC MED = 200 ± 10 nm displayed two peaks at Δt = 1.7 µs and Δt = 3.2 µs, which could be attributed to the contributions from both flaming and smoldering combustion in each burning case. Both the Δt values and the shell / core ratios of the rBC-containing particles clearly increased as the MCE decreased from 0.98 (smoldering-dominant combustion) to 0.86 (flaming-dominant combustion), implying the great importance of the rapid condensation of semi-volatile organics. This laboratory study found that the mixing state of rBC particles from biomass burning strongly depends on its combustion processes, and overall MCE should be taken carefully into consideration while the climate effect of rBC particles from open biomass burning is simulated.

The impact of heterogeneous reactions on the chemical components and mixing state of dust particles are investigated by observations and an air quality model over northern China between March 27, 2015 and April 2, 2015. Synergetic observations were conducted using a polarization optical particle counter (POPC), a depolarized two-wavelength Lidar and filter samples in Beijing. During this period, dust plume passed through Beijing on March 28, and flew back on March 29 because of synoptic weather changes. Mineral dust mixed with anthropogenic pollutants was simulated using the Nested Air Quality Prediction Modeling System (NAQPMS) to examine the role of heterogeneous processes on the dust. A comparison of observations shows that the NAQPMS successfully reproduces the time series of the vertical profile, particulate matter concentration, and chemical components of fine mode (diameter ≤ 2.5 μm) and coarse mode (2.5 μm

High PM2. 5 concentrations of around 100 µg m−3 were observed twice during an intensive observation campaign in January 2015 at Fukuoka (33.52° N, 130.47° E) in western Japan. These events were analyzed comprehensively with a regional chemical transport model and synergetic ground-based observations with state-of-the-art measurement systems, which can capture the behavior of secondary inorganic aerosols (SO42−, NO3−, and NH4+). The first episode of high PM2. 5 concentration was dominated by NO3− (type N) and the second episode by SO42− (type S). The concentration of NH4+ (the counterion for SO42− and NO3−) was high for both types. A sensitivity simulation in the chemical transport model showed that the dominant contribution was from transboundary air pollution for both types. To investigate the differences between these types further, the chemical transport model results were examined, and a backward trajectory analysis was used to provide additional information. During both types of episodes, high concentrations of NO3− were found above China, and an air mass that originated from northeast China reached Fukuoka. The travel time from the coastline of China to Fukuoka differed between types: it was 18 h for type N and 24 h for type S. The conversion ratio of SO2 to SO42− (Fs) was less than 0.1 for type N, but reached 0.3 for type S as the air mass approached Fukuoka. The higher Fs for type S was related to the higher relative humidity and the concentration of HO2, which produces H2O2, the most effective oxidant for the aqueous-phase production of SO42−. Analyzing the gas ratio as an indicator of the sensitivity of NO3− to changes in SO42− and NH4+ showed that the air mass over China was NH3-rich for type N, but almost NH3-neutral for type S. Thus, although the high concentration of NO3− above China gradually decreased during transport from China to Fukuoka, higher NO3− concentrations were maintained during transport owing to the lower SO42− for type N. In contrast, for type S, the production of SO42− led to the decomposition of NH4NO3, and more SO42− was transported. Notably, the type N transport pattern was limited to western Japan, especially the island of Kyushu. Transboundary air pollution dominated by SO42− (type S) has been recognized as a major pattern of pollution over East Asia. However, our study confirms the importance of transboundary air pollution dominated by NO3−, which will help refine our understanding of transboundary heavy PM2. 5 pollution in winter over East Asia.

Mixing state of aerosols and optical properties including lidar ratio, particle depolarization ratio, and Angstrom exponent were investigated at Fukuoka in western Japan using a multi-wavelength Mie–Raman lidar (MMRL), various aerosol mass-concentration measurements, and a polarization optical particle counter during Winter–Spring 2015. Aerosol extinction coefficient, backscatter coefficient, and depolarization at 355 and 532 nm and attenuated backscatter coefficient at 1064 nm are obtained from the MMRL measurements. Ten aerosol episodes were classified into three categories (air pollution, mineral dust, and marine aerosol) based on aerosol mass-concentration measurements in the fine-mode (particle diameter Dp

A rapid decrease in PM2.5 concentrations in China has been observed in response to the enactment of strong emission control policies. From 2012 to 2017, total emissions of SO2 and NOx from China decreased by approximately 63% and 24%, respectively. Simultaneously, decreases in the PM2.5 concentration in Japan have been observed since 2014, and the proportion of stations that satisfy the PM2.5 environmental standard (daily, 35 µg/m3; annual average, 15 µg/m3) increased from 37.8% in fiscal year (FY) 2014 (April 2014 to March 2015) to 89.9% in FY 2017. However, the quantitative relationship between the PM2.5 improvement in China and the PM2.5 concentration in downwind regions is not well understood. Here, we (1) quantitatively evaluate the impacts of Chinese environmental improvements on downwind areas using source/receptor analysis with a chemical transport model, and (2) show that these rapid emissions reductions improved PM2.5 concentrations both in China and its downwind regions, but the difference between SO2 and NOx reduction rates led to greater production of nitrates (e.g., NH4NO3) due to a chemical imbalance in the ammonia–nitric acid–sulfuric acid–water system. Observations from a clean remote island in western Japan and numerical modeling confirmed this paradigm shift.

The BC/CO emission ratios were estimated and compiled from long-term, harmonized observations of the ΔBC/ΔCO ratios under conditions unaffected by wet deposition at four sites in East Asia, including two sites in Korea (Baengnyeong and Gosan) and two sites in Japan (Noto and Fukuoka). Extended spatio-temporal coverage enabled estimation of full seasonality and elucidation of the emission ratio in North Korea, for the first time. The estimated ratios were used to validate the Regional Emission inventory in Asia (REAS) version 2.1 based on six study domains (East China, North China, Northeast China, South Korea, North Korea, and Japan). We found that the ΔBC/ΔCO ratios from four sites converged into a narrow range (6.2–7.9 ng m−3 ppb−1), suggesting consistency in the results from independent observations and similarity in source profiles over the regions. The BC/CO ratios from the REAS emission inventory (7.7 ng m−3 ppb−1 for East China – 23.2 ng m−3 ppb−1 for South Korea) were overestimated by factors of 1.1 for East China to 3.0 for South Korea, whereas the ratio for North Korea (3.7 ng m−3 ppb−1 from REAS) was underestimated by a factor of 2.0, most likely due to inaccurate emissions from the road transportation sector. Seasonal variation in the BC/CO ratio from REAS was found to be the highest in winter (China and North Korea) or summer (South Korea and Japan), whereas the measured ΔBC/ΔCO ratio was highest in spring in all source regions, indicating the need for further characterization of seasonality when creating a bottom-up emission inventory. At levels of administrative districts, overestimation in Seoul, the southwest regions of South Korea, and Northeast China was noticeable, and underestimation was mainly observed in the western regions in North Korea, including Pyongyang. These diagnoses are useful for identifying the regions where revisions in the inventory are necessary, providing guidance for refinement of BC and CO emission rate estimates over East Asia.

Atmospheric aerosols over polar regions have attracted considerable attention for their pivotal effects on climate change. In this study, temporospatial variations in single-particle-based depolarization ratios (δ

Long-term synergetic fine and coarse mode aerosol observations were analyzed at 1-h intervals at Fukuoka, Japan, from January to June 2015. The GEOS-Chem chemical transport model, including dust and sea-salt acid uptake processes, was used for detailed analysis of observation data. Several Asian dust events and long-range anthropogenic aerosol transport events were observed during our analysis period, and the numerical model generally explained the observed time variation for both fine and coarse mode aerosols. We found that (i) the majority of fine mode NO3– can be considered as long-range transport (LRT) outside of Japan during the cold season, and (ii) the peak timing of fine mode NO3– coincided with that of SO4–, indicating that both aerosols are controlled by LRT. Also, an observed mass concentration ratio of NO3–/SO42– > 0.9 occurred during the cold season, indicating the importance of NO3– as a major contributor to the PM2.5 mass fraction. Finally, we clearly showed that large-scale dust-nitrate outflow from China to Fukuoka was confirmed in all cases of dust events, indicating that the anthropogenic NOx is converted to dust-nitrate and transported to Japan with dust. These results demonstrate the importance of anthropogenic NO3– LRT during the cold season and dust-nitrate LRT for all dust events (even in June).

Two regional chemical transport models were applied to simulate high concentrations of particulate matters (PM) observed in East Asia in January 2015; the first model is the Nested Air Quality Prediction Modeling System (NAQPMS) and the second is the Community Multi-scale Air Quality Model (CMAQ). The variation of PM2.5 in both models showed well agreement with measurements over both eastern China and western Japan. Based on the model results and the aerosol compositions observed in Fukuoka in western Japan, three types of PM long-range transport (LRT) were identified: N-, S-, and D-type. The N episode showed higher fine-mode nitrate (fNO3–) concentrations than fine-mode sulfate (fSO42–), indicating the importance of NO3– LRT. The S episode showed the highest fSO42– concentrations (28.9 µg m–3), which were 3.4-fold higher than fNO3–, due to high relative humidity. During the D episode, dust stagnated in Fukuoka for three days, due to the influence of low- and high-pressure systems; thus, dust LRT is also important in winter besides spring. Both models reasonable explained variations in aerosol components during both N and S episodes; however, both underestimated fSO42– especially during D episode, suggesting that they may miss certain emissions or chemical mechanisms. High coarse-mode NO3– (cNO3–) concentrations (maximum: 6.3 µg m–3), and high cNO3–/fNO3– ratios (maximum: 1.2) were observed during D episode. NAQPMS successfully captured this cNO3– peak after including heterogeneous reactions on dust. Our results emphasize the importance of such heterogeneous processes for understanding the LRT of dust and anthropogenic pollutants over East Asia.

Appropriate policies to improve air quality by reducing anthropogenic emissions are urgently needed. This is typified by the particulate matter (PM) problem and it is well known that one type of PM, sulfate aerosol (SO 4 2− ), has a large-scale impact due to long range transport. In this study we evaluate the source–receptor relationships of SO 4 2− over East Asia for 2005, when anthropogenic sulfur dioxide (SO 2 ) emissions from China peaked. SO 2 emissions from China have been declining since 2005–2006, so the possible maximum impact of Chinese contributions of SO 4 2− is evaluated. This kind of information provides a foundation for policy making and the estimation of control effects. The tagged tracer method was applied to estimate the source apportionment of SO 4 2− for 31 Chinese province-scale regions. In addition, overall one-year source apportionments were evaluated to clarify the seasonal dependency. Model performance was confirmed by comparing with ground-based observations over mainland China, Taiwan, Korea, and Japan, and the model results fully satisfied the performance goal for PM. We found the following results. Shandong and Hebei provinces, which were the largest and second largest SO 2 sources in China, had the greatest impact over the whole of East Asia with apportionments of around 10–30% locally and around 5–15% in downwind receptor regions during the year. Despite large SO 2 emissions, the impact of south China (e.g., Guizhou, Guangdong, and Sichuan provinces) was limited to local impact. These results suggest that the reduction policy in south China contributes to improving the local air quality, whereas policies in north and central China are beneficial for both the whole of China and downwind regions. Over Taiwan, Korea, and Japan, the impact of China was dominant; however, local contributions were important during summer.

Ground-based observation of the polarization properties of aerosol particles using a polarization optical particle counter (POPC) was made from 27 October 2013, to 31 December 2015, at a suburban site in the Kyushu area of Japan. We found that the depolarization ratio (DR, the fraction of s-polarized signal in the total backward light scattering signal) of aerosol particles showed prominent seasonal variability, with peaks in spring (0.21–0.23) and winter (0.19–0.23), and a minimum value (0.09–0.14) in summer. The aerosol compositions in both fine mode (aerodynamic diameter of particle, Dp Dp Dp > 1 µm) particles. Occurrence of substandard air quality days in Kyushu was closely related with mixed type (coexistence of anthropogenic pollutants and dust particles in the atmosphere), especially in winter and spring, indicating that dust events in the Asian continent played a key role in the cross-boundary transport of continental pollution. Backward trajectory analysis demonstrated that air masses originating from the western Pacific contained large amounts of spherical particles due to the influence of sea salt, especially in summer; however, for air masses from the Asian continent, the dependence of number fraction of spherical particles on air relative humidity was insignificant, indicating the predominance of less-hygroscopic substances (e.g., mineral dust), although the mass concentrations of anthropogenic pollutants were elevated.

The atmospheric input of anthropogenic total reactive oxygenated nitrogen (NOy) to ocean regions in East Asia during 2002–2004 was revisited with an updated regional chemical transport model and the latest emissions inventory. The updated model treats both fine- and coarse-mode nitrate (NO3−). Coarse-mode NO3− is produced by the reaction of nitric acid (HNO3) and sea salt particles. The modeling system reproduced the atmospheric concentration and wet deposition amount of NO3− quantitatively compared with observations. The fraction of coarse-mode NO3− was also well captured. NOy deposition amounts over marginal seas and open oceans were 733 and 730 Gg N/yr, which are increases of 1.6- and 2.2-fold, respectively, by including coarse-mode NO3−. Anthropogenic NOx emissions from China were 5377 Gg N/yr, and 3060 Gg N/yr was exported from China; therefore, the NOy deposition amount over ocean regions in East Asia (1463 Gg N/yr) corresponded to almost half (48%) of the export amounts.

The lockdown measures due to COVID-19 affected the industry, transportation and other human activities within China in early 2020, and subsequently the emissions of air pollutants. The decrease of atmospheric NO2 due to the COVID-19 lockdown and other factors were quantitively analyzed based on the surface concentrations by in-situ observations, the tropospheric vertical column densities (VCDs) by different satellite retrievals including OMI and TROPOMI, and the model simulations by GEOS-Chem. The results indicated that due to the COVID-19 lockdown, the surface NO2 concentrations decreased by 42% ± 8% and 26% ± 9% over China in February and March 2020, respectively. The tropospheric NO2 VCDs based on both OMI and high quality (quality assurance value (QA) ≥ 0.75) TROPOMI showed similar results as the surface NO2 concentrations. The daily variations of atmospheric NO2 during the first quarter (Q1) of 2020 were not only affected by the COVID-19 lockdown, but also by the Spring Festival (SF) holiday (January 24–30, 2020) as well as the meteorology changes due to seasonal transition. The SF holiday effect resulted in a NO2 reduction from 8 days before SF to 21 days after it (i.e. January 17 - February 15), with a maximum of 37%. From the 6 days after SF (January 31) to the end of March, the COVID-19 lockdown played an important role in the NO2 reduction, with a maximum of 51%. The meteorology changes due to seasonal transition resulted in a nearly linear decreasing trend of 25% and 40% reduction over the 90 days for the NO2 concentrations and VCDs, respectively. Comparisons between different datasets indicated that medium quality (QA ≥ 0.5) TROPOMI retrievals might suffer large biases in some periods, and thus attention must be paid when they are used for analyses, data assimilations and emission inversions., Graphical abstract Image 1, Highlights • NO2 in China decreased by 42% and 26% in February and March 2020 due to COVID-19. • The NO2 VCDs by satellites were consistent with the surface NO2 concentrations. • Spring Festival holiday led to a NO2 decrease in 30 days with a maximum of 37%. • COVID-19 led to a NO2 decrease from 6 days after SF with a maximum of 51%. • NO2 concentrations and VCDs decreased by 25% and 40% in 90 days due to meteorology.

Depolarization ratio (δ) of backscattered light from aerosol particle is an applicable parameter for real-time distinguishing spherical and non-spherical particles, which has been widely adopted by ground-based Lidar observation and satellite remote sensing. From November 2016 to February of 2017, it consecutively suffered from numbers of severe air pollution at Beijing with daily averaged mass concentration of PM2.5 (aerodynamic diameter less than 2.5 μm) larger than 150 μg/m3. We preformed concurrent measurements of water-soluble chemical species and depolarization properties of aerosol particles on the basis of a continuous dichotomous Aerosol Chemical Speciation Analyzer (ACSA-14) and a bench-top optical particle counter with a polarization detection module (POPC). We found that δ value of ambient particles generally decrease as mass concentration of PM2.5 increased at unfavorable meteorological condition. Ratio of mass concentration of nitrate (NO3−) to that of sulfate (SO42−) in PM2.5 was 1.5 ± 0.6, indicating of great importance of NOx in the formation of heavy pollution. Mass concentration of NO3− in PM2.5 (fNO3) was generally an order of magnitude higher than that in coarse mode (cNO3) with a mean fNO3 / cNO3 ratio of 14 ± 10. Relatively high allocation (fNO3/cNO3 = 5) of NO3− in coarse mode could be partially attributed to hygroscopic growth/coagulation of nitrate-rich fine mode particles under higher relative humidity condition. As a result, δ values of particles with Dp = 2 μm (δDp = 2) and 5 μm (δDp = 5) decreased evidently as the mass fraction of water-soluble species (NO3− and SO42−) increase in both PM2.5 and PM2.5–10, respectively. In particular, due to synergistic effect of RH, δDp = 5 value could decrease by 50 % as mass fraction of NO3− in PM2.5–10 increased from 8 % to 23 %. It suggested that alteration of non-sphericity of mineral dust particles was evident owing to coating with pollutants and heterogeneous reactions on the surface of the particle during heavy pollution period. This study brings the attention to great variability of morphological changes of aerosol particles along the transport, which have great complex effects in evaluating their climate and health effect.

East Asia is suffering from a severe air pollution problem due to intensive emissions of anthropogenic pollutants and mineral dust aerosols. During transport, both Asian dust and pollutants undergo complex mixing processes, which result in great impacts on regional air quality, human health and climate. To characterize these mixing processes, we conducted long-term observations using an optical particle counter equipped with a polarization detection module (POPC) in the megacity of Beijing. Mass concentrations of PM 2.5 (aerodynamic diameters of less than 2.5 μm) and PM 10 derived from POPC compared well with ground-based measurements. Based on size-resolved polarization measurements, anthropogenic pollutants, mineral dust and mixed-type mineral dust (dust particle with pollutant coatings) were well distinguished. We found that the depolarization ratio (DR, termed as the ratio of the intensity of the s-polarized signal to the intensity of the backward scattering signal [s/(s + p)]) for aerosol particles with optical diameters of 2.0 μm has a pronounced seasonal variation trend, with a winter–spring high and a summer low pattern. Aerosols that originated from Mongolia and western China normally demonstrate non-spherical shapes, with a DR centred on 0.3, whereas the value for fine-mode particles was usually less than 0.1 due to the predominance of secondary water-soluble matter. In Beijing, the morphology of mineral dust changed obviously, particularly in humid conditions. Higher relative humidity accelerated the liquid phase reaction and promoted water absorption due to the coating of hygroscopic soluble compounds on the dust surface. This study also found that 48 % of substandard air quality days featured high coarse-mode particles in the winter–spring time, which implies the great influence of heterogeneous processes on the surface of mineral dust on smog formation.

Changes in anthropogenic emissions in East Asia will cause substantial variations in the precipitation chemistry. In particular, the effects of changes in China, where NOx emissions have been rising continuously and SO2 emissions peaked in 2005–2006, are important. The absolute chemical concentration in precipitation is inherently linked to the amount of precipitation; therefore, in this work we used the ratio of nitrate (NO3−) to non-seasalt sulfate nss-SO42- concentration in precipitation on an equivalent basis (hereinafter, Ratio). Here, we extend the method in our previous study (Itahashi et al., 2014a) to Korea and China. We analyzed the long-term behavior of Ratio in precipitation during 2000–2011 and investigated the factors responsible for variations of Ratio in precipitation by using a model simulation with sensitivity analysis for emission changes in China. Ratio over Japan, Korea, and China decreased slightly or remained constant during 2000–2005 (first 6 years of 2000–2011) and subsequently increased during 2006–2011 (last 6 years of 2000–2011). Linear regression analysis of the observations showed significant increases in Ratio during 2006–2011: +3.4 ± 1.0%/year, +13.2 ± 4.1%/year, and +9.8 ± 2.5%/year for Japan, Korea, and China, respectively (each p

Open biomass burning (OBB) emits significant amounts of non-methane hydrocarbons (NMHCs), and the mixing of OBB with urban plumes could exacerbate regional ozone (O3) pollution. In the present study, an observational field campaign was performed in a rural area at the northern edge of the Yangtze River Delta region (YRDR) from 15 May to 24 June 2010, during intensive open burning of wheat residues. The net photochemical production rate of oxidant (Ox = O3 + NO2) at the site was evaluated based on a box model (Regional Atmospheric Chemical Mechanism, Version 2) constrained by real-time ambient measurements (e.g., O3, volatile organic compounds (VOCs), NOx (NO2 + NO), J values). Our results showed that both in situ photochemistry and direct transport from urban areas in the YRDR were responsible for the high Ox concentration at the site. During an OBB-impact case, net photochemical production of Ox in the daytime was pronounced, with a 6 h averaged Ox production rate of 13 ± 4 ppbv h−1 (maximum value of 21 ppbv h−1 at 12:00 CST). Photochemical Oxproduction changed from VOC-limited in the morning to NOx-limited in the afternoon due to the rapid photochemical consumption of NOx during the day. A combined analysis with positive matrix factorization demonstrated that O3 pollution in the rural area of the YRDR was largely affected by urban emission, and OBB-related emissions also contributed to in situ photochemical production, particularly in the afternoon. Our study suggested that a joint effort in reducing both NMHCs (e.g., aromatics) and NOx emissions in the urban area, as well as local OBB activities, may be effective in eliminating high-O3 pollution risk in the rural areas of the YRDR.

We observed a long-lasting dust event from 25 May to 2 June 2014, using a polarization optical particle counter (POPC). The transport of dust plumes over East Asia was verified on the basis of observations of Moderate Resolution Imaging Spectroradiometer, a lidar network, and surface synoptic observation stations. Mixing of dust and anthropogenic pollutants was investigated according to the variation in the depolarization ratio as a function of particle size. The nonsphericity of dust particles varied due to the impact of anthropogenic pollutants on their pathway. In the coarse mode, dust particles always had a clear nonspherical configuration, although large amounts of nitrate were also present. Supermicron particles are occasionally present in a spherical configuration, possibly due to the complex mixing of natural dust and anthropogenic particles. Statistically, ~64% of the total nitrate mass was deemed to be transported from outside of Japan due to a trapping effect in the dust plume.

The behavior of tropospheric NO2 vertical column density (VCD) over continental Southeast Asia (Cambodia, Laos, Myanmar, Thailand, and Vietnam) was systematically analyzed using observations from the SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY) and a regional chemical transport model (CTM) during 2003–2008. NO2 VCD over continental Southeast Asia showed a distinctive large peak from winter (December) to early spring (April). The regional CTM was configured with anthropogenic emissions taken from the Regional Emission inventory in Asia (REAS) version 2.1 and biomass burning emissions taken from the Global Fire Emissions Database (GFED) version 3.1. Overall, the model could reproduce the NO2 VCD observed by space-borne sensors. A mismatch between satellite observations and the regional CTM was found only in January over Cambodia. A likely reason for this mismatch was diurnal variation in biomass burning emissions. During the analysis period, the largest biomass burning event was reported from December 2003 to April 2004, and a sensitivity analysis was conducted by omitting the biomass burning emissions in the CTM. It was found that the seasonal variations of NO2 VCD, with the peak during winter to early spring, were caused by biomass burning emissions in all countries in continental Southeast Asia. The contribution of biomass burning emissions to NO2 VCD over continental Southeast Asia was an average of 28% during this period and a maximum of 58% in March 2004.

Emission source contributions of tropospheric ozone (O3) were comprehensively investigated by using the higher-order decoupled direct method (HDDM) for sensitivity analysis and the ozone source apportionment technology (OSAT) for mass balance analysis in the comprehensive air-quality model with extensions (CAMx). The response of O3 to emissions reductions at various levels in mainland China, Korea, and Japan were estimated and compared with results calculated by the brute force method (BFM) where one model parameter is varied at a time. Emissions were assessed at three receptor sites in Japan that experienced severe pollution events in May 2009. For emissions from China, HDDM assessed O3 response with a bias of only up to 3 ppbv (a relative error of 4.5%) even for a 50% reduction but failed to assess a more extreme reduction. OSAT was reasonably accurate at 100% reduction, with a −4 ppbv (−7%) bias, but was less accurate at moderate ranges of reduction (∼50–70%). For emissions from Korea and Japan, HDDM captured the nonlinear response at all receptor sites and at all reduction levels to within 1% in all but one case; however, the bias of OSAT increased with the increasing reduction of emissions. One possible reason for this is that OSAT does not account for NO titration. To address this, a term for potential ozone (PO; O3 and NO2 together) was introduced. Using of PO instead of O3 improved the performance of OSAT, especially for emissions reductions from Korea and Japan. The proposed approach with PO refined the OSAT results and did not degrade HDDM performance.

Acidifying species in precipitation can cause severe impacts on ecosystem. The chemical concentration of precipitation is directly related to the precipitation amount, so it is partly difficult to identify the long-term variation from precipitation concentration. The ratio of nitrate (NO3−) to non-seasalt sulfate (nss-SO42−) concentration in precipitation on an equivalent basis (hereinafter, Ratio) will be a useful index. To identify the long-term record of acidifying species in precipitation over East Asia, where is the highest emission region in the world, we have compiled the ground-based observations of the chemical concentration of precipitation over China, Korea, and Japan from 2001 to 2015 based on the Acid Deposition Monitoring Network in East Asia (EANET). The period was partly limited but other monitoring data in Japan, southern China, and northern China around Beijing were additionally utilized. The analyzed period was categorized into three phases: Phase I (2001–2005), Phase II (2006–2010), and Phase III (2011–2015). The behavior of NO3− and nss-SO42− concentration, and hence Ratio in precipitation will be related to these precursors. The anthropogenic NOx and SO2 emission amount, and NOx/SO2 emission ratio are analyzed. Further, satellite observations of NO2 and SO2 column density to capture the variation in emission was applied. We found that the long-term trend of NO3− concentration in precipitation was not related to the variation in NOx emission and the NO2 column. In comparison, the nss-SO42− concentration in precipitation over China, Korea, and Japan was partly connected to the changes in SO2 emission from China, but the trends were not significant. The long-term trend of Ratio over China, Korea, and Japan were nearly flat during Phase I, increasing significantly during Phase II, and almost flat again during Phase III. These variations of Ratio in East Asia clearly corresponded to the NOx/SO2 emission ratio and the NO2/SO2 column ratio in China. The first flat trend during Phase I was due to both increases in NOx and SO2 emissions in China, the significant increasing trend during Phase II was triggered by the increase in NOx emission and decrease in SO2 emission in China, and the returned flat trend during Phase III was caused by both declines in NOx and SO2 emissions in China. This suggests that China’s emission has a significant impact not only on China but also on downwind precipitation chemistry during the analyzed 15–year period of 2001–2015. In terms of wet depositions, the NO3− wet deposition amount over China, Korea, and Japan has not changed dramatically, but the nss-SO42− wet deposition amount declined over China, Korea, and Japan from Phase II to III. These declines were caused by a strong decrease in nss-SO42− concentration in precipitation accompanied by a reduction in SO2 emission from China, which counteracted an increase in precipitation amount. It was indicated the decision on the acidity of precipitation would be shift from sulfur to nitrogen.