Role of Dust and Iron Solubility in Sulfate Formation during the Long-Range Transport in East Asia Evidenced by 17O-Excess Signatures.

Numerical models have been developed to elucidate air pollution caused by sulfate aerosols (SO42-). However, typical models generally underestimate SO42-, and oxidation processes have not been validated. This study improves the modeling of SO42- formation processes using the mass-independent oxygen isotopic composition [17O-excess; Δ17O(SO42-)], which reflects pathways from sulfur dioxide (SO2) to SO42-, at the background site in Japan throughout 2015. The standard setting in the Community Multiscale Air Quality (CMAQ) model captured SO42- concentration, whereas Δ17O(SO42-) was underestimated, suggesting that oxidation processes were not correctly represented. The dust inline calculation improved Δ17O(SO42-) because dust-derived increases in cloud-water pH promoted acidity-driven SO42- production, but Δ17O(SO42-) was still overestimated during winter as a result. Increasing solubilities of the transition-metal ions, such as iron, which are a highly uncertain modeling parameter, decreased the overestimated Δ17O(SO42-) in winter. Thus, dust and high metal solubility are essential factors for SO42- formation in the region downstream of China. It was estimated that the remaining mismatch of Δ17O(SO42-) between the observation and model can be explained by the proposed SO42- formation mechanisms in Chinese pollution. These accurately modeled SO42- formation mechanisms validated by Δ17O(SO42-) will contribute to emission regulation strategies required for better air quality and precise climate change predictions over East Asia.

Improving Estimates of Sulfur, Nitrogen, and Ozone Total Deposition through Multi-Model and Measurement-Model Fusion Approaches.

Earth system and environmental impact studies need high quality and up-to-date estimates of atmospheric deposition. This study demonstrates the methodological benefits of multimodel ensemble and measurement-model fusion mapping approaches for atmospheric deposition focusing on 2010, a year for which several studies were conducted. Global model-only deposition assessment can be further improved by integrating new model-measurement techniques, including expanded capabilities of satellite observations of atmospheric composition. We identify research and implementation priorities for timely estimates of deposition globally as implemented by the World Meteorological Organization.

Impacts of COVID-19 lockdown, Spring Festival and meteorology on the NO2 variations in early 2020 over China based on in-situ observations, satellite retrievals and model simulations.

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.

Detectability of the potential climate change effect on transboundary air pollution pathways in the downwind area of China.

Long-term aerosol optical depth (AOD) datasets focused on the Pacific Ocean in the downwind area of China over a 19-year period from 2003 to 2021 were derived from satellite observations, reanalysis datasets, and numerical simulations. Considering the significant year-to-year changes in the amounts of aerosols transported from China to the Pacific Ocean during this period, we proposed a metric named RAOD. This is defined as the AOD over the ocean relative to that near the eastern coast of China within the same latitude band (25-30°N). RAOD was identified as a valuable metric for quantifying the long-term changes in transboundary air pollution pathways. Our analysis revealed a clear exponential decrease in RAOD values from China toward the Pacific Ocean; this was consistent with the prevailing meteorological conditions observed over the 19-year period. However, the possible long-term changes in RAOD due to climate change were found to be insignificant and were overshadowed by much larger year-to-year variations in the meteorological field. Additionally, significant seasonal variations in the absolute slope of the linear regression between RAOD and longitude were observed, and there correlated with wind patterns in the lower troposphere. Elevated slope values in the spring and winter suggested a west-to-east aerosol transport facilitated by strong winds, whereas the lower slope values in summer and autumn indicated a northward aerosol movement under weaker winds. In recent years, aerosols have become less likely to be transported far eastward from the coast of China. Based on these findings, to enhance the detectability of the climate change impacts on meteorological field affecting transboundary air pollution pathways, the RAOD metric derived using a continued long-term satellite observation of aerosols is proposed.

Severe level of photochemical oxidants (Ox) over the western coast of Japan during autumn after typhoon passing.

Photochemical oxidants (Ox; mainly O3) are a concern in East Asia. Because of the prevailing westerly wind in the midlatitudes, O3 concentration generally shows a high in spring over Kyushu Island, western Japan, and Ox warnings have been issued in spring. However, the record from 2000 to 2021 of Ox warning days in Kyushu Island contains one warning case in autumn 2020. Interestingly, a typhoon had passed the day before this Ox warning. To relate these events, a modelling simulation was conducted and it showed the transboundary O3 transport from the Asian continent to the western coast of Japan due to the strong wind field determined by the location of Typhoon Haishen (2020). The sensitivity simulations for changing Chinese anthropogenic sources suggested that both nitrogen oxides (NOx) and volatile organic compound (VOC) emission regulations in China could decrease high O3 over the downwind region of Japan. Furthermore, VOC emission regulation in China led to an overall O3 decrease in East Asia, whereas NOx emission regulation in China had complex effects of decreasing (increasing) O3 during the daytime (nighttime) over China. The association between air quality and meteorology related to typhoons should be considered along with global warming in the future.

Effectiveness of emission controls implemented since 2000 on ambient ozone concentrations in multiple timescales in Japan: An emission inventory development and simulation study.

It has been reported that ambient ozone concentrations in Japan have not been effectively suppressed by precursor emission controls. In this study, we developed an unprecedented long-term emission inventory of ozone precursors, including nitrogen oxide (NOX) and volatile organic compounds (VOCs), in Japan. The developed emission inventory, which explicitly represents changes in emissions caused by emission controls and variation in activities from 2000 to 2019, revealed that emission controls implemented for vehicles, large point sources, and fugitive VOC sources effectively reduced precursor emissions. The impact of emission changes on ozone concentrations at six different timescales was evaluated using air quality simulations. Three of them corresponded to annual mean values of daily ozone concentrations, and the others corresponded to annual high ozone concentrations. The simulations performed better at higher ozone concentrations. The simulation results suggested that emission controls have helped suppress annual high ozone concentrations, whereas the annual mean values of daily ozone concentrations may have increased in populated urban areas because reduced NOX emissions weakened the titration of ozone. Overall changes in the simulated ozone concentrations over different timescales were generally consistent with those in the observed ozone concentrations. These findings highlight the importance of evaluating the impact of emission controls on ozone concentrations over multiple timescales. The differences in the sensitivities of ozone concentrations to emission controls were clearly explained by the ozone sensitivity regimes implied by the ratios of formaldehyde to nitrogen dioxide. The outcomes of this study could assist countries beyond Japan in developing effective strategies to manage ozone pollution.

Source contributions of sulfate aerosol over East Asia estimated by CMAQ-DDM.

We applied the decoupled direct method (DDM), a sensitivity analysis technique for computing sensitivities accurately and efficiently, to determine the source-receptor relationships of anthropogenic SO(2) emissions to sulfate aerosol over East Asia. We assessed source contributions from East Asia being transported to Oki Island downwind from China and Korea during two air pollution episodes that occurred in July 2005. The contribution from China, particularly that from central eastern China (CEC), was found to dominate the sulfate aerosols. To study these contributions in more detail, CEC was divided into three regions, and the contributions from each region were examined. Source contributions exhibited both temporal and vertical variability, largely due to transport patterns imposed by the Asian summer monsoon. Our results are consistent with backward trajectory analyses. We found that anthropogenic SO(2) emissions from China produce significant quantities of summertime sulfate aerosols downwind of source areas. We used a parametric scaling method for estimating anthropogenic SO(2) emissions in China. Using column amounts of SO(2) derived from satellite data, and relationships between the column amounts of SO(2) and anthropogenic emissions, 2009 emissions were diagnosed. The results showed that 2009 emissions of SO(2) from China were equivalent to 2004 levels.

Returning long-range PM2.5 transport into the leeward of East Asia in 2021 after Chinese economic recovery from the COVID-19 pandemic.

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 into the leeward of 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 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 recovered to that before COVID-19.

Quantifying the wet deposition of reactive nitrogen over China: Synthesis of observations and models.

Accurate estimation on reaction nitrogen (Nr) deposition is highly demanded for assessing the impacts on the environment and human beings. This study investigated the wet deposition of inorganic nitrogen (IN) in mainland China by measurements from over 500 sites from five observational networks/databases and ensemble results of eleven chemical transport models (CTMs). Each data source has its focus and limitations and together formed a comprehensive view over China. But the inconsistency among different sources may hinder the appropriate usage of data. Model evaluation results demonstrated the models' deficiency in simulating the wet NO3- deposition over Southeast China (40 % underestimation) and showed an overall underestimation of wet NH4+ deposition over the hotspot regions (5-60 % underestimation). A synthesis of this study and twelve reference studies was conducted to quantify the national amount of wet IN deposition. The estimations by CTMs ranged 2.4-3.9 Tg(N) yr-1 for wet NOy deposition and 4-6.7 Tg(N) yr-1 for wet NHx deposition, after adjusting the results with 10-19 % underestimations in wet NOy deposition and 1-40 % underestimations in wet NHx deposition. The estimations by ground observations ranged 7.1-9 Tg(N) yr-1 for wet NOy deposition and 8-13.1 Tg(N) yr-1 for wet NHx deposition, which were 20-275 % higher than the estimation by CTMs, but the results were strongly influenced by the abundances and representative of measurements. Studies using statistical techniques to interpolate site observations predicted 3-5.5 Tg(N) yr-1 for wet NOy deposition and 3.9-7.2 Tg(N) yr-1 for wet NHx deposition. This approach benefited from high accuracy and good robustness of the statistical models, but the uncertainty in the interpolation methods could be a potential drawback.

How have Divergent Global Emission Trends Influenced Long-range Transported Ozone to North America?

Several locations across the United States in non-compliance with the national standard for ground-level ozone (O3) are thought to have sizeable influences from distant extra-regional emission sources or natural stratospheric O3, which complicates design of local emission control measures. To quantify the amount of long-range transported O3 (LRT O3), its origin, and change over time, we conduct and analyze detailed sensitivity calculations characterizing the response of O3 to emissions from different source regions across the Northern Hemisphere in conjunction with multi-decadal simulations of tropospheric O3 distributions and changes. Model calculations show that the amount of O3 at any location attributable to sources outside North America varies both spatially and seasonally. On a seasonal-mean basis, during 1990-2010, LRT O3 attributable to international sources steadily increased by 0.06-0.2 ppb yr-1 at locations across the United States and arose from superposition of unequal and contrasting trends in individual source-region contributions, which help inform attribution of the trend evident in O3 measurements. Contributions of emissions from Europe steadily declined through 2010, while those from Asian emissions increased and remained dominant. Steadily rising NOx emissions from international shipping resulted in increasing contributions to LRT O3, comparable to those from Asian emissions in recent years. Central American emissions contribute a significant fraction of LRT O3 in southwestern United States. In addition to the LRT O3 attributable to emissions outside of North America, background O3 across the continental United States is comprised of a sizeable and spatially variable fraction that is of stratospheric origin (29-78%).

Incorporation of volcanic SO2 emissions in the Hemispheric CMAQ (H-CMAQ) version 5.2 modeling system and assessing their impacts on sulfate aerosol over the Northern Hemisphere.

The state-of-the-science Community Multiscale Air Quality (CMAQ) Modeling System has recently been extended for hemispheric-scale modeling applications (referred to as H-CMAQ). In this study, satellite-constrained estimation of the degassing SO2 emissions from 50 volcanoes over the Northern Hemisphere is incorporated into H-CMAQ, and their impact on tropospheric sulfate aerosol ( SO 4 2 - ) levels is assessed for 2010. The volcanic degassing improves predictions of observations from the Acid Deposition Monitoring Network in East Asia (EANET), the United States Clean Air Status and Trends Network (CASTNET), and the United States Integrated Monitoring of Protected Visual Environments (IMPROVE). Over Asia, the increased SO 4 2 - concentrations were seen to correspond to the locations of volcanoes, especially over Japan and Indonesia. Over the USA, the largest impacts that occurred over the central Pacific were caused by including the Hawaiian Kilauea volcano, while the impacts on the continental USA were limited to the western portion during summertime. The emissions of the Soufrière Hills volcano located on the island of Montserrat in the Caribbean Sea affected the southeastern USA during the winter season. The analysis at specific sites in Hawaii and Florida also confirmed improvements in regional performance for modeled SO 4 2 - by including volcanoes SO2 emissions. At the edge of the western USA, monthly averaged SO 4 2 - enhancements greater than 0.1µgm-3 were noted within the boundary layer (defined as surface to 750hPa) during June- September. Investigating the change on SO 4 2 - concentration throughout the free troposphere revealed that although the considered volcanic SO2 emissions occurred at or below the middle of free troposphere (500hPa), compared to the simulation without the volcanic source, SO 4 2 - enhancements of more than 10% were detected up to the top of the free troposphere (250hPa). Our model simulations and comparisons with measurements across the Northern Hemisphere indicate that the degassing volcanic SO2 emissions are an important source and should be considered in air quality model simulations assessing background SO 4 2 - levels and their source attribution.

Trends of sulfur and nitrogen deposition from 2003 to 2017 in Japanese remote areas.

Emissions of sulfur (S) and nitrogen (N) compounds in East Asia has drastically changed over the last two decades. To assess the influence of the drastic changes in air pollution on ecosystems in Japan, we investigated the trends of S and N deposition during 2003-2017 at remote sites of Acid Deposition Monitoring Network in East Asia (EANET). We measured wet deposition and inferentially estimated dry deposition of S and N using monitoring data from 2003 to 2017 at eight sites. We estimated dry deposition using the inferential method with an updated parameterization for gaseous surface resistance. The linear regression method and nonparametric Mann-Kendall test was used to analyze the temporal trends based on the monthly data sets. High S and N deposition amounts over 10 kg ha-1 year-1 were frequently found at most sites. There were significant increase trends in N deposition to S deposition (N/S) ratio at all sites throughout the 15-year period. Some trends were significantly found when the 15-year period was divided into three: 2003-2007, 2008-2012, and 2013-2017. S deposition had significantly decreased over a wide area in Japan, especially at Sado-seki, Happo, Oki, Hedo, and Ogasawara, in 2013-2017. Significant decreases in oxidized N deposition at Sado-seki and Oki were also found in 2013-2017. Because of almost flat N deposition mainly contributed by reduced N deposition, the N/S ratio clearly increased. These trends were associated with the recent reductions in SO2 and NOx emissions in China. The NOx emission reduction of China has not caught up with that of SO2, and NH3 emissions have not been reduced. This caused the significant increases in the N/S ratio not only in 2013-2017 but also in 2003-2017.

Nitrogen burden from atmospheric deposition in East Asian oceans in 2010 based on high-resolution regional numerical modeling.

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.

Disentangling the contribution of the transboundary out-flow from the Asian continent to Tokyo, Japan.

We assessed the contribution of transboundary air pollutants (TAPs) transported from China to Tokyo using the Pb(0.5

Modeling stratospheric intrusion and trans-Pacific transport on tropospheric ozone using hemispheric CMAQ during April 2010 - Part 1: Model evaluation and air mass characterization for stratosphere-troposphere transport.

Stratospheric intrusion and trans-Pacific transport have been recognized as a potential source of tropospheric ozone over the US. The state-of-the-science Community Multiscale Air Quality (CMAQ) modeling system has recently been extended for hemispheric-scale modeling applications (referred to as H-CMAQ). In this study, H-CMAQ is applied to study the stratospheric intrusion and trans-Pacific transport during April 2010. The results will be presented in two companion papers. In this Part 1 paper, model evaluation for tropospheric ozone (O3) is presented. Observations at the surface, by ozonesondes and airplane, and by satellite across the Northern Hemisphere are used to evaluate the model performance for O3. H-CMAQ is able to capture surface and boundary layer (defined as surface to 750hPa) O3 with a normalized mean bias (NMB) of -10%; however, a systematic underestimation with an NMB up to -30% is found in the free troposphere (defined as 750-250hPa). In addition, a new air mass characterization method is developed to distinguish influences of stratosphere-troposphere transport (STT) from the effects of photochemistry on O3 levels. This method is developed based on the ratio of O3 and an inert tracer indicating stratospheric O3 to examine the importance of photochemistry, and sequential intrusion from upper layer. During April 2010, on a monthly average basis, the relationship between surface O3 mixing ratios and estimated stratospheric air masses in the troposphere show a slight negative slope, indicating that high surface O3 values are primarily affected by other factors (i.e., emissions), whereas this relationship shows a slight positive slope at elevated sites, indicating that STT has a possible impact at elevated sites. STT shows large day-to-day variations, and STT impacts can either originate from the same air mass over the entire US with an eastward movement found during early April, or stem from different air masses at different locations indicated during late April. Based on this newly established air mass characterization technique, this study can contribute to understanding the role of STT and also the implied importance of emissions leading to high surface O3. Further research focused on emissions is discussed in a subsequent paper (Part 2).

Modeling stratospheric intrusion and trans-Pacific transport on tropospheric ozone using hemispheric CMAQ during April 2010 - Part 2: Examination of emission impacts based on the higher-order decoupled direct method.

The state-of-the-science Community Multiscale Air Quality (CMAQ) modeling system, which has recently been extended for hemispheric-scale modeling applications (referred to as H-CMAQ), is applied to study the trans-Pacific transport, a phenomenon recognized as a potential source of air pollution in the US, during April 2010. The results of this analysis are presented in two parts. In the previous paper (Part 1), model evaluation for tropospheric ozone (O3) was presented and an air mass characterization method was developed. Results from applying this newly established method pointed to the importance of emissions as the factor to enhance the surface O3 mixing ratio over the US. In this subsequent paper (Part 2), emission impacts are examined based on mathematically rigorous sensitivity analysis using the higher-order decoupled direct method (HDDM) implemented in H-CMAQ. The HDDM sensitivity coefficients indicate the presence of a NO x -sensitive regime during April 2010 over most of the Northern Hemisphere. By defining emission source regions over the US and east Asia, impacts from these emission sources are examined. At the surface, during April 2010, the emission impacts of the US and east Asia are comparable over the western US with a magnitude of about 3ppbv impacts on monthly mean O3 all-hour basis, whereas the impact of domestic emissions dominates over the eastern US with a magnitude of about 10ppbv impacts on monthly mean O3. The positive correlation (r = 0.63) between surface O3 mixing ratios and domestic emission impacts is confirmed. In contrast, the relationship between surface O3 mixing ratios and emission impacts from east Asia exhibits a flat slope when considering the entire US. However, this relationship has strong regional differences between the western and eastern US; the western region exhibits a positive correlation (r = 0.36-0.38), whereas the latter exhibits a flat slope (r <0.1). Based on the comprehensive evaluation of H-CMAQ, we extend the sensitivity analysis for O3 aloft. The results reveal the significant impacts of emissions from east Asia on the free troposphere (defined as 750 to 250hPa) over the US (impacts of more than 5ppbv) and the dominance of stratospheric air mass on upper model layer (defined as 250 to 50hPa) over the US (impacts greater than 10ppbv). Finally, we estimate changes of trans-Pacific transport by taking into account recent emission trends from 2010 to 2015 assuming the same meteorological condition. The analysis suggests that the impact of recent emission changes on changes in the contribution of trans-Pacific transport to US O3 levels was insignificant at the surface level and was small (less than 1ppbv) over the free troposphere.

Paradigm shift in aerosol chemical composition over regions downwind of China.

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.

Chinese province-scale source apportionments for sulfate aerosol in 2005 evaluated by the tagged tracer method.

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 (SO42-), has a large-scale impact due to long range transport. In this study we evaluate the source-receptor relationships of SO42- over East Asia for 2005, when anthropogenic sulfur dioxide (SO2) emissions from China peaked. SO2 emissions from China have been declining since 2005-2006, so the possible maximum impact of Chinese contributions of SO42- 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 SO42- 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 SO2 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 SO2 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.

Long-term inverse modeling of Chinese CO emission from satellite observations.

Carbon monoxide (CO) emissions in China in 2005-2010 were estimated by inversion, using the Green's function method from vertical CO profiles derived from MOPITT Version 5 satellite data and a tagged CO simulation, and validated with independent in situ observations from the World Data Centre for Greenhouse Gases. Modeling with a posteriori emission successfully reproduced CO outflow from the continent to the East China Sea, Sea of Japan, and Japanese islands during winter and spring, and compensated for underestimates in central and eastern China in summer. A posteriori emissions showed large seasonal variations in which December and March emissions were on average 23% larger than August emissions, consistent with other studies. Estimated Chinese CO emissions were 184.4, 173.1, 184.6, 158.4, 157.4, and 157.3 Tg/year for 2005-2010, respectively. The decrease after 2007 is partly attributed to Chinese socioeconomic conditions and improved combustion efficiency.