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Urban aerosol measurements are necessary to establish associations between air pollution and human health outcomes and to evaluate the efficacy of air quality legislation and emissions standards. The measurement of urban aerosol particle size distributions (PSDs) is of particular importance as they enable characterization of size-dependent processes that govern a particle's transport, transformation, and fate in the urban atmosphere. PSDs also improve our ability to link air pollution to health effects through evaluation of particle deposition in the respiratory system and inhalation toxicity. To inform future measurements of urban aerosol observations, this paper reviews and critically analyzes the current state of knowledge on urban aerosol PSD measurements by synthesizing 737 PSD observations made between 1998 to 2017 in 114 cities in 43 countries around the globe. Significant variations in the shape and magnitude of urban aerosol number and mass PSDs were identified among different geographical regions. In general, number PSDs in Europe (EU) and North America, Australia, and New Zealand (NAAN) are dominated by nucleation- and Aitken-mode particles. PSDs in Central, South, and Southeast Asia (CSSA) and East Asia (EA) are shifted to larger sizes, with a meaningful contribution from the accumulation mode. Urban mass PSDs are typically bimodal, presenting a dominant mode in the accumulation mode and a secondary mode in the coarse mode. Most PSD observations published in the literature are short-term, with only 14 % providing data for longer than 6 months. There is a paucity of PSDs measured in Africa (AF), CSSA, Latin America (LA), and West Asia (WA), demonstrating the need for long-term aerosol measurements across wide size ranges in many cities around the globe. Geographical variations in urban aerosol effective densities were also reviewed. Size-resolved urban aerosol effective density functions from 3 to 10 000 nm were established for different geographical regions and intra-city sampling locations in order to accurately translate number PSDs to mass PSDs, with significant variations observed between near-road and urban background sites. The results of this study demonstrate that global initiatives are urgently needed to develop infrastructure for routine and long-term monitoring of urban aerosol PSDs spanning the nucleation to coarse mode. Doing so will advance our understanding of spatiotemporal trends in urban PSDs throughout the world and provide a foundation to more reliably elucidate the impact of urban aerosols on atmospheric processes, human health, and climate. [ABSTRACT FROM AUTHOR]

The concentration of carbonaceous aerosols, black carbon (BC) and organic aerosol (OA), in the atmosphere is related to co-emitted or co-produced trace gases. In this study, we investigate the most relevant proportional relationships between both BC and OA with the following trace gases: carbon monoxide (CO), formaldehyde (HCHO), nitrogen dioxide (NO2), ozone (O3), and sulfur dioxide (SO2). One motivation for selecting these trace gases is that they can be observed using remote sensing measurements from satellite instrumentation, and could therefore be used to predict spatial changes in the amounts of BC and OA. Airborne measurements are optimal for the analysis of both the composition of aerosols and trace gases in different environments ranging from unpolluted oceanic air masses to those in heavily polluted city plumes. The two aircraft campaigns of the EMeRGe (Effect of Megacities on the Transport and Transformation of Pollutants on the Regional to Global Scales) project have created a unique database, with flight plans dedicated to studying city plumes in two regions, Europe (2017) and East Asia (2018), along with identical instrumental payload. Using linear regression analysis, three relevant relationships between carbonaceous aerosol and trace gases are identified: - The BC/OA ratio observed in the Asian campaign is three times higher (≈ 0.3) than in the European campaign (≈ 0.1), whereas the Pearson correlation coefficient (R) between BC and OA is much higher in Europe (R ≈ 0.8) than in Asia (R ≈ 0.6). - The CO/BC ratio is also observed higher in the Asian campaign (≈ 240) than in the European campaign (≈ 170), whereas the R-value between CO and BC is similar for both campaigns (R ≈ 0.7). - The HCHO/OA ratio is similar in both campaigns (≈0.32), but the observed R-values between HCHO and OA is higher in Europe than in the Asia (R ≈ 0.7 compared to ≈ 0.3). By focusing on heavily polluted air masses sampled downwind in the city plumes, the ratios between the observed carbonaceous aerosols and the five trace gases change, and the R-values increase with O3 for both BC and OA (R ≈ 0.5). To assess the performance of atmospheric models with respect to the most relevant observed relationships, an air quality model ensemble is used to represent the current state of atmospheric modeling, consisting of two global and two regional simulations. The evaluation shows that these proportional relationships are not satisfactorily reproduced by the model ensemble. The relationships between BC and OA or between CO and BC are modeled with stronger correlations than the observed ones, and their higher ratios observed in Asia compared to Europe are not reproduced. Furthermore, the modeled HCHO/OA ratio is underestimated in the Asian campaign and overestimated in the European campaign. This analysis of the proportional relationships between carbonaceous aerosols and trace gases implies that the observed relationships can be used to constrain models and improve anthropogenic emission inventories. In addition, it implies that information about the lower tropospheric concentration of carbonaceous aerosols can potentially be inferred from satellite retrievals of trace gases, particularly in the plumes from megacities. [ABSTRACT FROM AUTHOR]

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

In this study, the WRF-Chem v4.4 model was utilized to evaluate the sensitivity of O 3 simulations with three bottom-up emission inventories (EDGAR-HTAP v2 and v3 and KORUS v5) using surface and aircraft data in East Asia during the Korea-United States Air Quality (KORUS-AQ) campaign period in 2016. All emission inventories were found to reproduce the diurnal variations of O 3 and its main precursor NO 2 as compared to the surface monitor data. However, the spatial distributions of the daily maximum 8 h average (MDA8) O 3 in the model do not completely align with the observations. The model MDA8 O 3 had a negative (positive) bias north (south) of 30° N over China. All simulations underestimated the observed CO by 50 %–60 % over China and South Korea. In the Seoul Metropolitan Area (SMA), EDGAR-HTAP v2 and v3 and KORUS v5 simulated the vertical shapes and diurnal patterns of O 3 and other precursors effectively, but the model underestimated the observed O 3 , CO, and HCHO concentrations. Notably, the model aromatic volatile organic compounds (VOCs) were significantly underestimated with the three bottom-up emission inventories, although the KORUS v5 shows improvements. The model isoprene estimations had a positive bias relative to the observations, suggesting that the Model of Emissions of Gases and Aerosols from Nature (MEGAN) version 2.04 overestimated isoprene emissions. Additional model simulations were conducted by doubling CO and VOC emissions over China and South Korea to investigate the causes of the model O 3 biases and the effects of the long-range transport on the O 3 over South Korea. The doubled CO and VOC emission simulations improved the model O 3 simulations for the local-emission-dominant case but led to the model O 3 overestimations for the transport-dominant case, which emphasizes the need for accurate representations of the local VOC emissions over South Korea. [ABSTRACT FROM AUTHOR]

Air quality network data in China and South Korea show very high year-round mass concentrations of coarse particulate matter (PM), as inferred by the difference between PM 10 and PM 2.5. Coarse PM concentrations in 2015 averaged 52 µ g m -3 in the North China Plain (NCP) and 23 µ g m -3 in the Seoul Metropolitan Area (SMA), contributing nearly half of PM 10. Strong daily correlations between coarse PM and carbon monoxide imply a dominant source from anthropogenic fugitive dust. Coarse PM concentrations in the NCP and the SMA decreased by 21 % from 2015 to 2019 and further dropped abruptly in 2020 due to COVID-19 reductions in construction and vehicle traffic. Anthropogenic coarse PM is generally not included in air quality models but scavenges nitric acid to suppress the formation of fine particulate nitrate, a major contributor to PM 2.5 pollution. GEOS-Chem model simulation of surface and aircraft observations from the Korea–United States Air Quality (KORUS-AQ) campaign over the SMA in May–June 2016 shows that consideration of anthropogenic coarse PM largely resolves the previous model overestimate of fine particulate nitrate. The effect is smaller in the NCP which has a larger excess of ammonia. Model sensitivity simulations for 2015–2019 show that decreasing anthropogenic coarse PM directly increases PM 2.5 nitrate in summer, offsetting 80 % the effect of nitrogen oxide and ammonia emission controls, while in winter the presence of coarse PM increases the sensitivity of PM 2.5 nitrate to ammonia and sulfur dioxide emissions. Decreasing coarse PM helps to explain the lack of decrease in wintertime PM 2.5 nitrate observed in the NCP and the SMA over the 2015–2021 period despite decreases in nitrogen oxide and ammonia emissions. Continuing decrease of fugitive dust pollution means that more stringent nitrogen oxide and ammonia emission controls will be required to successfully decrease PM 2.5 nitrate. [ABSTRACT FROM AUTHOR]

Nitrogen oxides (NO x≡ NO + NO 2) are of central importance for air quality, climate forcing, and nitrogen deposition to ecosystems. The Geostationary Environment Monitoring Spectrometer (GEMS) is now providing hourly NO 2 satellite observations over East Asia, offering the first direct measurements of NO 2 diurnal variation from space to guide understanding of NO x emissions and chemistry. The NO 2 retrieval requires independent vertical profile information from a chemical transport model (CTM) to compute the air mass factor (AMF) that relates the NO 2 column measured along the line of sight to the NO 2 vertical column. Here, we use aircraft observations from the Korea-United States Air Quality (KORUS-AQ) campaign over the Seoul metropolitan area (SMA) and around the Korean Peninsula in May–June 2016 to better understand the factors controlling the NO 2 vertical profile, its diurnal variation, the implications for the AMFs, and the ability of the GEOS-Chem CTM to compute the NO 2 vertical profiles used for AMFs. Proper representation of oxidant chemistry is critical for the CTM simulation of NO 2 vertical profiles and is achieved in GEOS-Chem through new model developments, including aerosol nitrate photolysis, reduced uptake of hydroperoxy (HO 2) radicals by aerosols, and accounting for atmospheric oxidation of volatile chemical products (VCPs). We find that the tropospheric NO 2 columns measured from space in the SMA are mainly contributed by the planetary boundary layer (PBL) below 2 km altitude, reflecting the highly polluted conditions. Repeated measurements of NO 2 vertical profiles over the SMA at different times of day show that diurnal change in mixing depth affecting the NO 2 vertical profile induces a diurnal variation in AMFs of comparable magnitude to the diurnal variation in the NO 2 column. GEOS-Chem captures this diurnal variation in AMFs and more generally the variability in the AMFs for the KORUS-AQ NO 2 vertical profiles (2.7 % mean bias, 7.6 % precision), with some outliers in the morning due to errors in the timing of mixed-layer growth. [ABSTRACT FROM AUTHOR]

Using European Centre for Medium-Range Weather Forecasts fifth-generation (ERA5) and second Modern-Era Retrospective analysis for Research and Applications (MERRA-2) reanalysis and surface meteorological observation data, this study explores the possible impact of sudden stratospheric warming (SSW) events on air quality in the Beijing–Tianjin–Hebei (BTH) region. Major SSW events are divided into polar vortex displacement SSW and polar vortex split SSW. As the duration of split SSW events is longer and the stratospheric signal pulses propagate further downward than displacement SSWs, subseasonal variability of the atmospheric particulates in the BTH is larger during split SSWs. The air particulate concentration is light before the SSW onset due to the enhanced perturbation in the troposphere associated with strengthened planetary waves. The air particulate concentration around the SSW onset dates begins to rise due to weakening of the tropospheric disturbance as the enhanced planetary waves enter the stratosphere. In the decaying period of the SSW, the air particulate concentration decreases as the stratospheric negative northern annular mode (NAM) signal propagates downward. Specifically, in the pre-SSW period of displacement (split) SSW events, a wavenumber-1-like (wavenumber-2-like) anomaly pattern is strengthened. The East Asian winter monsoon intensifies as the East Asian trough is deepened, especially before the split SSW event onset, leading to a cleaning period. Around the SSW onset period as the tropospheric perturbation diminishes and the East Asian winter monsoon weakens, a surge of air particulate concentration is observed. After the SSW onset, due to the downward propagation of the stratospheric negative NAM signal, cold anomalies form in northeastern East Asia, especially for split SSWs, corresponding to a cleaning period in the BHT region. The local meteorological conditions during the SSWs are also discussed. [ABSTRACT FROM AUTHOR]

High levels of fine particulate matter (PM2.5) pollution in East Asia often exceed local air quality standards. Observations from the Korea–United States Air Quality (KORUS-AQ) field campaign in May and June 2016 showed that development of extreme pollution (haze) occurred through a combination of long-range transport and favorable meteorological conditions that enhanced local production of PM2.5. Atmospheric models often have difficulty simulating PM2.5 chemical composition during haze, which is of concern for the development of successful control measures. We use observations from KORUS-AQ to examine the ability of the GEOS-Chem chemical transport model to simulate PM2.5 composition throughout the campaign and identify the mechanisms driving the pollution event. At the surface, the model underestimates sulfate by - 64 % but overestimates nitrate by + 36 %. The largest underestimate in sulfate occurs during the pollution event, for which models typically struggle to generate elevated sulfate concentrations due to missing heterogeneous chemistry in aerosol liquid water in the polluted boundary layer. Hourly surface observations show that the model nitrate bias is driven by an overestimation of the nighttime peak. In the model, nitrate formation is limited by the supply of nitric acid, which is biased by + 100 % against aircraft observations. We hypothesize that this is due to a large missing sink, which we implement here as a factor of 5 increase in dry deposition. We show that the resulting increased deposition velocity is consistent with observations of total nitrate as a function of photochemical age. The model does not account for factors such as the urban heat island effect or the heterogeneity of the built-up urban landscape, resulting in insufficient model turbulence and surface area over the study area that likely results in insufficient dry deposition. Other species such as NH3 could be similarly affected but were not measured during the campaign. Nighttime production of nitrate is driven by NO2 hydrolysis in the model, while observations show that unexpectedly elevated nighttime ozone (not present in the model) should result in N2O5 hydrolysis as the primary pathway. The model is unable to represent nighttime ozone due to an overly rapid collapse of the afternoon mixed layer and excessive titration by NO. We attribute this to missing nighttime heating driving deeper nocturnal mixing that would be expected to occur in a city like Seoul. This urban heating is not considered in air quality models run at large enough scales to treat both local chemistry and long-range transport. Key model failures in simulating nitrate, mainly overestimated daytime nitric acid, incorrect representation of nighttime chemistry, and an overly shallow and insufficiently turbulent nighttime mixed layer, exacerbate the model's inability to simulate the buildup of PM2.5 during haze pollution. To address the underestimate in sulfate most evident during the haze event, heterogeneous aerosol uptake of SO2 is added to the model, which previously only considered aqueous production of sulfate from SO2 in cloud water. Implementing a simple parameterization of this chemistry improves the model abundance of sulfate but degrades the SO2 simulation, implying that emissions are underestimated. We find that improving model simulations of sulfate has direct relevance to determining local vs. transboundary contributions to PM2.5. During the haze pollution event, the inclusion of heterogeneous aerosol uptake of SO2 decreases the fraction of PM2.5 attributable to long-range transport from 66 % to 54 %. Locally produced sulfate increased from 1 % to 25 % of locally produced PM2.5 , implying that local emissions controls could have a larger effect than previously thought. However, this additional uptake of SO2 is coupled to the model nitrate prediction, which affects the aerosol liquid water abundance and chemistry driving sulfate–nitrate–ammonium partitioning. An additional simulation of the haze pollution with heterogeneous uptake of SO2 to aerosol and simple improvements to the model nitrate simulation results in 30 % less sulfate due to 40 % less nitrate and aerosol water, and this results in an underestimate of sulfate during the haze event. Future studies need to better consider the impact of model physical processes such as dry deposition and nighttime boundary layer mixing on the simulation of nitrate and the effect of improved nitrate simulations on the overall simulation of secondary inorganic aerosol (sulfate + nitrate + ammonium) in East Asia. Foreign emissions are rapidly changing, increasing the need to understand the impact of local emissions on PM2.5 in South Korea to ensure continued air quality improvements. [ABSTRACT FROM AUTHOR]

Air quality simulations in which the global chemical transport model CHASER and the regional chemical transport model WRF/chem are coupled have been developed to consider the dynamic transport of chemical species across the boundaries of the domain of the regional chemical transport model. The simulation captures the overall seasonal variations of surface ozone, but overestimates its concentration over Japanese populated areas by approximately 20 ppb from summer to early winter. It is deduced that ozone formation around Northeast China and Japan in summer is overestimated in the simulation. On the other hand, the simulation well reproduces the interannual variability and the long-term trend of observed surface ozone over Japan. Sensitivity experiments have been performed to investigate the influence of the variation in inflow to East Asia on the interannual variability and the long-term trend of surface ozone over Japan during 1996-2005. The inflow defined in this paper includes the recirculation of species with sources within the East Asian region as well as the transport of species with sources out of the East Asian region. Results of sensitivity experiments suggest that inflow to East Asia accounts for approximately 30% of the increasing trend of surface ozone, whereas it has much less influence on the interannual variability of observed surface ozone compared to meteorological processes within East Asia. [ABSTRACT FROM AUTHOR]

We present the WRF-GC model v2.0, an online two-way coupling of the Weather Research and Forecasting (WRF) meteorological model (v3.9.1.1) and the GEOS-Chem model (v12.7.2). WRF-GC v2.0 is built on the modular framework of WRF-GC v1.0 and further includes aerosol–radiation interaction (ARI) and aerosol–cloud interaction (ACI) based on bulk aerosol mass and composition, as well as the capability to nest multiple domains for high-resolution simulations. WRF-GC v2.0 is the first implementation of the GEOS-Chem model in an open-source dynamic model with chemical feedbacks to meteorology. In WRF-GC, meteorological and chemical calculations are performed on the exact same 3-D grid system; grid-scale advection of meteorological variables and chemical species uses the same transport scheme and time steps to ensure mass conservation. Prescribed size distributions are applied to the aerosol types simulated by GEOS-Chem to diagnose aerosol optical properties and activated cloud droplet numbers; the results are passed to the WRF model for radiative and cloud microphysics calculations. WRF-GC is computationally efficient and scalable to massively parallel architectures. We use WRF-GC v2.0 to conduct sensitivity simulations with different combinations of ARI and ACI over China during January 2015 and July 2016. Our sensitivity simulations show that including ARI and ACI improves the model's performance in simulating regional meteorology and air quality. WRF-GC generally reproduces the magnitudes and spatial variability of observed aerosol and cloud properties and surface meteorological variables over East Asia during January 2015 and July 2016, although WRF-GC consistently shows a low bias against observed aerosol optical depths over China. WRF-GC simulations including both ARI and ACI reproduce the observed surface concentrations of PM 2.5 in January 2015 (normalized mean bias of - 9.3 %, spatial correlation r of 0.77) and afternoon ozone in July 2016 (normalized mean bias of 25.6 %, spatial correlation r of 0.56) over eastern China. WRF-GC v2.0 is open source and freely available from http://wrf.geos-chem.org (last access: 20 June 2021). [ABSTRACT FROM AUTHOR]

This study compares the performance of 12 regional chemical transport models (CTMs) from the third phase of the Model Inter-Comparison Study for Asia (MICS-Asia III) on simulating the particulate matter (PM) over East Asia (EA) in 2010. The participating models include the Weather Research and Forecasting model coupled with Community Multiscale Air Quality (WRF-CMAQ; v4.7.1 and v5.0.2), the Regional Atmospheric Modeling System coupled with CMAQ (RAMS-CMAQ; v4.7.1 and v5.0.2), the Weather Research and Forecasting model coupled with chemistry (WRF-Chem; v3.6.1 and v3.7.1), Goddard Earth Observing System coupled with chemistry (GEOS-Chem), a non-hydrostatic model coupled with chemistry (NHM-Chem), the Nested Air Quality Prediction Modeling System (NAQPMS) and the NASA-Unified WRF (NU-WRF). This study investigates three model processes as the possible reasons for different model performances on PM. (1) Models perform very differently in the gas–particle conversion of sulfur (S) and oxidized nitrogen (N). The model differences in sulfur oxidation ratio (50 %) are of the same magnitude as that in SO42- concentrations. The gas–particle conversion is one of the main reasons for different model performances on fine mode PM. (2) Models without dust emission modules can perform well on PM 10 at non-dust-affected sites but largely underestimate (up to 50 %) the PM 10 concentrations at dust sites. The implementation of dust emission modules in the models has largely improved the model accuracies at dust sites (reduce model bias to -20 %). However, both the magnitude and distribution of dust pollution are not fully captured. (3) The amounts of modeled depositions vary among models by 75 %, 39 %, 21 % and 38 % for S wet, S dry, N wet and N dry depositions, respectively. Large inter-model differences are found in the washout ratios of wet deposition (at most 170 % in India) and dry deposition velocities (generally 0.3–2 cm s -1 differences over inland regions). [ABSTRACT FROM AUTHOR]

Horizontal grid resolution has a profound effect on model performances on meteorology and air quality simulations. In contribution to MICS-Asia Phase III, one of whose goals was to identify and reduce model uncertainty in air quality prediction, this study examined the impact of grid resolution on meteorology and air quality simulation over East Asia, focusing on the North China Plain (NCP) region. The NASA Unified Weather Research and Forecasting (NU-WRF) model has been applied with the horizontal resolutions at 45, 15, and 5 km. The results revealed that, in comparison with ground observations, no single resolution can yield the best model performance for all variables across all stations. From a regional average perspective (i.e., across all monitoring sites), air temperature modeling was not sensitive to the grid resolution but wind and precipitation simulation showed the opposite. NU-WRF with the 5 km grid simulated the wind speed best, while the 45 km grid yielded the most realistic precipitation as compared to the site observations. For air quality simulations, finer resolution generally led to better comparisons with observations for O3 , CO, NOx , and PM 2.5. However, the improvement of model performance on air quality was not linear with the resolution increase. The accuracy of modeled surface O3 of the 15 km grid was greatly improved over the one from the 45 km grid. A further increase in grid resolution to 5 km, however, showed diminished impact on model performance improvement on O3 prediction. In addition, a 5 km resolution grid showed large advantage in better capturing the frequency of high-pollution occurrences. This was important for the assessment of noncompliance with ambient air quality standards, which was key to air quality planning and management. Balancing the modeling accuracy and resource limitation, a 15 km grid resolution was suggested for future MICS-Asia air quality modeling activity if the research region remained unchanged. This investigation also found a large overestimate of ground-level O3 and an underestimate of surface NOx and CO, likely due to missing emissions of NOx and CO. [ABSTRACT FROM AUTHOR]

Anthropogenic emissions of short-lived climate forcers (SLCFs) affect both air quality and climate. How much regional temperatures are affected by ambitious SLCF emission mitigation policies is, however, still uncertain. We investigate the potential temperature implications of stringent air quality policies by applying matrices of regional temperature responses to new pathways for future anthropogenic emissions of aerosols, methane (CH4), and other short-lived gases. These measures have only a minor impact on CO2 emissions. Two main options are explored, one with climate optimal reductions (i.e., constructed to yield a maximum global cooling) and one with the maximum technically feasible reductions. The temperature response is calculated for four latitude response bands (90–28 ∘ S, 28 ∘ S–28 ∘ N, 28–60 ∘ N, and 60–90 ∘ N) by using existing absolute regional temperature change potential (ARTP) values for four emission regions: Europe, East Asia, shipping, and the rest of the world. By 2050, we find that global surface temperature can be reduced by -0.3±0.08 ∘ C with climate-optimal mitigation of SLCFs relative to a baseline scenario and as much as -0.7 ∘ C in the Arctic. Cutting CH4 and black carbon (BC) emissions contributes the most. The net global cooling could offset warming equal to approximately 15 years of current global CO2 emissions. On the other hand, mitigation of other SLCFs (e.g., SO2) leads to warming. If SLCFs are mitigated heavily, we find a net warming of about 0.1 ∘ C, but when uncertainties are included a slight cooling is also possible. In the climate optimal scenario, the largest contributions to cooling come from the energy, domestic, waste, and transportation sectors. In the maximum technically feasible mitigation scenario, emission changes from the industry, energy, and shipping sectors will cause warming. Some measures, such as those in the agriculture waste burning, domestic, transport, and industry sectors, have large impacts on the Arctic, especially by cutting BC emissions in winter in areas near the Arctic. [ABSTRACT FROM AUTHOR]

Mineral dust particles play an important role in the Earth system, imposing a variety of effects on air quality, climate, human health, and economy. Accurate forecasts of dust events are highly desirable to provide an early warning and inform the decision-making process. East Asia is one of the largest dust sources in the world. This study applies and evaluates four widely used regional air quality models to simulate dust storms in northeastern China. Three dust schemes in the Weather Research and Forecasting model with Chemistry (WRF-Chem) (version 3.9.1), two schemes in both CHIMERE (version 2017r4) and CMAQ (version 5.2.1), and one scheme in CAMx (version 6.50) were applied to a dust event during 4–6 May 2015 in northeastern China. Most of these models were able to capture this dust event with the exception of CAMx, which has no dust source map covering the study area; hence, another dust source mask map was introduced to replace the default one for the subsequent simulation. Although these models reproduced the spatial pattern of the dust plume, there were large discrepancies between predicted and observed PM 10 concentrations in each model. In general, CHIMERE had relatively better performance among all simulations with default configurations. After parameter tuning, WRF-Chem with the Air Force Weather Agency (AFWA) scheme using a seasonal dust source map from Ginoux et al. (2012) showed the best performance, followed by WRF-Chem with the UOC_Shao2004 scheme, CHIMERE, and CMAQ. The performance of CAMx had significantly improved by substituting the default dust map and removing the friction velocity limitation. This study suggested that the dust source maps should be carefully selected on a regional scale or replaced with a new one constructed with local data. Moreover, further study and measurement of sandblasting efficiency of different soil types and locations should be conducted to improve the accuracy of estimated vertical dust fluxes in air quality models. [ABSTRACT FROM AUTHOR]

Numerous studies have reported that ambient air pollution, which has both local and long-range sources, causes adverse impacts on the environment and human health. Previous studies have investigated the impacts of transboundary air pollution (TAP) in East Asia, albeit primarily through analyses of episodic events. In addition, it is useful to better understand the spatiotemporal variations in TAP and the resultant impact on the environment and human health. This study aimed at assessing and quantifying the air quality impacts in Japan and South Korea due to local emissions and TAP from sources in East Asia - one of the most polluted regions in the world. We applied state-of-the-science atmospheric models to simulate air quality in East Asia and then analyzed the air quality and acid deposition impacts of both local emissions and TAP sources in Japan and South Korea. Our results show that ∼ 30 % of the annual average ambient PM 2.5 concentrations in Japan and South Korea in 2010 were contributed to by local emissions within each country, while the remaining ∼ 70 % were contributed to by TAP from other countries in the region. More detailed analyses also revealed that the local contribution was higher in the metropolises of Japan (∼ 40 %–79 %) and South Korea (∼ 31 %–55 %) and that minimal seasonal variations in surface PM 2.5 occurred in Japan, whereas there was a relatively large variation in South Korea in the winter. Further, among all five studied anthropogenic emission sectors of China, the industrial sector represented the greatest contributor to annual surface PM 2.5 concentrations in Japan and South Korea, followed by the residential and power generation sectors. Results also show that TAP's impact on acid deposition (SO42- and NO3-) was larger than TAP's impact on PM 2.5 concentrations (accounting for over 80 % of the total deposition), and that seasonal variations in acid deposition were similar for both Japan and South Korea (i.e., higher in both the winter and summer). Finally, wet deposition had a greater impact on mixed forests in Japan and savannas in South Korea. Given these significant impacts of TAP in the region, it is paramount that cross-national efforts should be taken to mitigate air pollution problems across East Asia. [ABSTRACT FROM AUTHOR]

Aerosols in the middle and upper troposphere have a long enough lifetime for trans-Pacific transport from East Asia to North America to influence air quality on the west coast of the United States (US). Here, we conduct quasi-global simulations (180 ∘ W–180 ∘ E and 70 ∘ S–75 ∘ N) from 2010 to 2014 using an updated version of WRF-Chem (Weather Research and Forecasting model fully coupled with chemistry) to analyze the spatiotemporal characteristics and source contributions of trans-Pacific aerosol transport. We find that trans-Pacific total aerosols have a maximum mass concentration (about 15 µ g m -3) in the boreal spring with a peak between 3 and 4 km above the surface around 40 ∘ N. Sea salt and dust dominate the total aerosol mass concentration below 1 km and above 4 km, respectively. About 80.8 Tg of total aerosols (48.7 Tg of dust) are exported annually from East Asia, of which 26.7 Tg of aerosols (13.4 Tg of dust) reach the west coast of the US. Dust contributions from four desert regions in the Northern Hemisphere are analyzed using a tracer-tagging technique. About 4.9, 3.9, and 4.5 Tg year -1 of dust aerosol emitted from north Africa, the Middle East and central Asia, and East Asia, respectively, can be transported to the west coast of the US. The trans-Pacific aerosols dominate the column-integrated aerosol mass (∼65.5 %) and number concentration (∼80 %) over western North America. Radiation budget analysis shows that the inflow aerosols could contribute about 86.4 % (-2.91 W m -2) at the surface, 85.5 % (+1.36 W m -2) in the atmosphere, and 87.1 % (-1.55 W m -2) at the top of atmosphere to total aerosol radiative effect over western North America. However, near the surface in central and eastern North America, aerosols are mainly derived from local emissions, and the radiative effect of imported aerosols decreases rapidly. This study motivates further investigations of the potential impacts of trans-Pacific aerosols from East Asia on regional air quality and the hydrological cycle in North America. [ABSTRACT FROM AUTHOR]

To improve poor air quality in Asia and inform effective emission-reduction strategies, it is vital to understand the contributions of different pollution sources and their associated human health burdens. In this study, we use the WRF-Chem regional atmospheric model to explore the air quality and human health benefits of eliminating emissions from six different anthropogenic sectors (transport, industry, shipping, electricity generation, residential combustion, and open biomass burning) over South and East Asia in 2014. We evaluate WRF-Chem against measurements from air quality monitoring stations across the region and find the model captures the spatial distribution and magnitude of PM 2.5 (particulate matter with an aerodynamic diameter of no greater than 2.5 µ m). We find that eliminating emissions from residential energy use, industry, or open biomass burning yields the largest reductions in population-weighted PM 2.5 concentrations across the region. The largest human health benefit is achieved by eliminating either residential or industrial emissions, averting 467 000 (95 % uncertainty interval (95UI): 409 000–542 000) or 283 000 (95UI: 226 000–358 000) annual premature mortalities, respectively, in India, China, and South-east Asia, with fire prevention averting 28 000 (95UI: 24 000–32 000) annual premature mortalities across the region. We compare our results to previous sector-specific emission studies. Across these studies, residential emissions are the dominant cause of particulate pollution in India, with a multi-model mean contribution of 42 % to population-weighted annual mean PM 2.5. Residential and industrial emissions cause the dominant contributions in China, with multi-model mean contributions of 29 % for both sectors to population-weighted annual mean PM 2.5. Future work should focus on identifying the most effective options within the residential, industrial, and open biomass-burning emission sectors to improve air quality across South and East Asia. [ABSTRACT FROM AUTHOR]

A total of 14 chemical transport models (CTMs) participated in the first topic of the Model Inter-Comparison Study for Asia (MICS-Asia) phase III. These model results are compared with each other and an extensive set of measurements, aiming to evaluate the current CTMs' ability in simulating aerosol concentrations, to document the similarities and differences among model performance, and to reveal the characteristics of aerosol components in large cities over East Asia. In general, these CTMs can well reproduce the spatial–temporal distributions of aerosols in East Asia during the year 2010. The multi-model ensemble mean (MMEM) shows better performance than most single-model predictions, with correlation coefficients (between MMEM and measurements) ranging from 0.65 (nitrate, NO3-) to 0.83 (PM 2.5). The concentrations of black carbon (BC), sulfate (SO42-), and PM 10 are underestimated by MMEM, with normalized mean biases (NMBs) of -17.0 %, - 19.1 %, and - 32.6 %, respectively. Positive biases are simulated for NO3- (NMB = 4.9 %), ammonium (NH4+) (NMB = 14.0 %), and PM 2.5 (NMB = 4.4 %). In comparison with the statistics calculated from MICS-Asia phase II, frequent updates of chemical mechanisms in CTMs during recent years make the intermodel variability of simulated aerosol concentrations smaller, and better performance can be found in reproducing the temporal variations of observations. However, a large variation (about a factor of 2) in the ratios of SNA (sulfate, nitrate, and ammonium) to PM 2.5 is calculated among participant models. A more intense secondary formation of SO42- is simulated by Community Multi-scale Air Quality (CMAQ) models, because of the higher SOR (sulfur oxidation ratio) than other models (0.51 versus 0.39). The NOR (nitric oxidation ratio) calculated by all CTMs has larger values (∼0.20) than the observations, indicating that overmuch NO3- is simulated by current models. NH3 -limited condition (the mole ratio of ammonium to sulfate and nitrate is smaller than 1) can be successfully reproduced by all participant models, which indicates that a small reduction in ammonia may improve the air quality. A large coefficient of variation (CV > 1.0) is calculated for simulated coarse particles, especially over arid and semi-arid regions, which means that current CTMs have difficulty producing similar dust emissions by using different dust schemes. According to the simulation results of MMEM in six large Asian cities, different air-pollution control plans should be taken due to their different major air pollutants in different seasons. The MICS-Asia project gives an opportunity to discuss the similarities and differences of simulation results among CTMs in East Asian applications. In order to acquire a better understanding of aerosol properties and their impacts, more experiments should be designed to reduce the diversities among air quality models. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

The Community Multiscale Air Quality (CMAQ) model has been further developed in terms of simulating natural wind-blown dust in this study, with a series of modifications aimed at improving the model's capability to predict the emission, transport, and chemical reactions of dust. The default parameterization of initial threshold friction velocity constants are revised to correct the double counting of the impact of soil moisture in CMAQ by the reanalysis of field experiment data; source-dependent speciation profiles for dust emission are derived based on local measurements for the Gobi and Taklamakan deserts in East Asia; and dust heterogeneous chemistry is also implemented. The improved dust module in the CMAQ is applied over East Asia for March and April from 2006 to 2010. The model evaluation result shows that the simulation bias of PM10 and aerosol optical depth (AOD) is reduced, respectively, from -55.42 and -31.97% by the original CMAQ to -16.05 and -22.1% by the revised CMAQ. Comparison with observations at the nearby Gobi stations of Duolun and Yulin indicates that applying a source-dependent profile helps reduce simulation bias for trace metals. Implementing heterogeneous chemistry also results in better agreement with observations for sulfur dioxide (SO2), sulfate (SO2- 4 ), nitric acid (HNO3), nitrous oxides (NOx). The investigation of a severe dust storm episode from 19 to 21 March 2010 suggests that the revised CMAQ is capable of capturing the spatial distribution and temporal variation of dust. The model evaluation also indicates potential uncertainty within the excessive soil moisture used by meteorological simulation. The mass contribution of fine-mode particles in dust emission may be underestimated by 50%. The revised CMAQ model provides a useful tool for future studies to investigate the emission, transport, and impact of wind-blown dust over East Asia and elsewhere. [ABSTRACT FROM AUTHOR]-3). The investigation of a severe dust storm episode from 19 to 21 March 2010 suggests that the revised CMAQ is capable of capturing the spatial distribution and temporal variation of dust. The model evaluation also indicates potential uncertainty within the excessive soil moisture used by meteorological simulation. The mass contribution of fine-mode particles in dust emission may be underestimated by 50%. The revised CMAQ model provides a useful tool for future studies to investigate the emission, transport, and impact of wind-blown dust over East Asia and elsewhere. [ABSTRACT FROM AUTHOR]

Mixing of Asian mineral dust with anthropogenic pollutants allows pollutants (e.g. sulfate and nitrate) to be transported over longer distances (e.g. to the northern Pacific, even to North America) along with dust particles. This mixing therefore affects the atmospheric and oceanic environment at local, regional and even continental scales. In this study, we used a three-dimensional regional chemical transport model (Nested Air Quality Predicting Modeling System, NAQPMS) to examine the degree of mixing between Asian mineral dust and anthropogenic pollutants in a superduststorm event during 19-22 March 2010. Influences of the mixing processes on regional atmospheric environmental and oceanic biogeochemical cycles were also investigated. A comparison with measurements showed that the model reproduced well the trajectory of long-range dust transport, the vertical dust profile, the chemical evolution of dust particles. We found that along-path mixing processes during the long-range transport of Asian dust led to increasingly polluted particles. As a result, ~60% of the sulfate and 7095 % of the nitrate in the downwind regions was derived from active mixing processes of minerals with pollutants sourced from the North China Plain and enhanced by transport over South China. This mixing had a significant impact on the regional-scale atmospheric composition and oceanic biogeochemical cycle. Surface HNO, SO2 and O3 were decreased by up to 90%, 40% and 30%, respectively, due to the heterogeneous reactions on dust particles. Fe solubility rose from ~0.5% in the Gobi region to ~3-5% in the northwestern Pacific, resulting from oxidization of SO2 on dust particles. Total Fe(II) deposition in the ocean region of East Asia reached 327 tons during the 4-day dust event, created a calculated primary productivity of ~520 mgC m-2 d-1 in the Kuril Islands, which can support almost 100% of the observed mean marine primary productivity in spring in this region (526 mgC m-2 d-1). [ABSTRACT FROM AUTHOR]

This study employs the regional Community Multiscale Air Quality (CMAQ) model to examine seasonal and diurnal variations of boundary layer ozone (O3) over East Asia. We evaluate the response of model simulations of boundary layer O3 to the choice of chemical mechanisms, meteorological fields, boundary conditions, and model resolutions. Data obtained from surface stations, aircraft measurements, and satellites are used to advance understanding of O3 chemistry and mechanisms over East Asia and evaluate how well the model represents the observed features. Satellite measurements and model simulations of summertime rainfall are used to assess the impact of the Asian monsoon on O3 production. Our results suggest that summertime O3 over Central Eastern China is highly sensitive to cloud cover and monsoonal rainfall over this region. Thus, accurate simulation of the East Asia summer monsoon is critical to model analysis of atmospheric chemistry over China. Examination of hourly summertime O3 mixing ratios from sites in Japan confirms the important role of diurnal boundary layer fluctuations in controlling ground-level O3. By comparing five different model configurations with observations at six sites, the specific mechanisms responsible for model behavior are identified and discussed. In particular, vertical mixing, urban chemistry, and dry deposition depending on boundary layer height strongly affect model ability to capture observed behavior. Central Eastern China appears to be the most sensitive region in our study to the choice of chemical mechanisms. Evaluation with TRACE-P aircraft measurements reveals that neither the CB4 nor the SAPRC99 mechanisms consistently capture observed behavior of key photochemical oxidants in springtime. However, our analysis finds that SAPRC99 performs somewhat better in simulating mixing ratios of H2O2 (hydrogen peroxide) and PAN (peroxyacetyl nitrate) at flight altitudes below 1 km. The high level of uncertainty associated with O3 production in Central Eastern China poses a major problem for regional air quality management. This highly polluted, densely populated region would greatly benefit from comprehensive air quality monitoring and the development of model chemical mechanisms appropriate to this unique atmospheric environment. [ABSTRACT FROM AUTHOR]