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Effects of the El Niño–Southern Oscillation (ENSO) on the interannual variability in spring aerosols over East Asia are investigated using the Modern Era Retrospective analysis for Research and Applications Version 2 (MERRA-2) reanalysis aerosol data. Results show that the ENSO has a crucial effect on the spring aerosols over mainland South East Asia, southern China, and the ocean south of Japan. The above-normal (below-normal) aerosols are found over these regions during the ensuing spring of El Niño (La Niña). In contrast to the local aerosol diffusion in winter, the ENSO affects East Asian aerosols in the following spring mainly via the modulation of upstream aerosol generation and transport processes. The underlying physical mechanism is that during the ensuing spring of El Niño (La Niña), the dry (wet) air and reduced (enhanced) precipitation are beneficial for the increase (reduction) in biomass burning activities over northern mainland South East Asia, resulting in more (fewer) carbonaceous aerosol emissions. On the other hand, the anomalous anticyclone (cyclone) over the north-western Pacific (WNP) associated with El Niño (La Niña) enhances (weakens) the low-level south-westerly wind from northern mainland South East Asia to southern Japan, which transports more (less) carbonaceous aerosol downstream. Anomalous precipitation plays a role in reducing aerosols over the source region, but its washout effect over the downstream region is limited. The ENSO's impact on the ensuing spring aerosols is mainly attributed to the eastern Pacific ENSO rather than the central Pacific ENSO. [ABSTRACT FROM AUTHOR]

Bromoform is the major by-product from chlorination of cooling water in coastal power plants. The number of power plants in East and Southeast Asian economies has increased rapidly, exceeding mean global growth. Bottom-up estimates of bromoform emissions based on few measurements appear to under-represent the industrial sources of bromoform from East Asia. Using oceanic Lagrangian analyses, we assess the amount of bromoform produced from power plant cooling-water treatment in East and Southeast Asia. The spread of bromoform is simulated as passive particles that are advected using the three-dimensional velocity fields over the years 2005/2006 from the high-resolution NEMO-ORCA0083 ocean general circulation model. Simulations are run for three scenarios with varying initial bromoform concentrations based on the range of bromoform measurements in cooling-water discharge. Comparing the modelled anthropogenic bromoform to in situ observations in the surface ocean and atmosphere, the two lower scenarios show the best agreement, suggesting initial bromoform concentrations in cooling water to be around 20–60 µgL-1. Based on these two scenarios, the model produces elevated bromoform in coastal waters of East Asia with average concentrations of 23 and 68 pmolL-1 and maximum values in the Yellow Sea, Sea of Japan and East China Sea. The industrially produced bromoform is quickly emitted into the atmosphere with average air–sea flux of 3.1 and 9.1 nmolm-2h-1 , respectively. Atmospheric abundances of anthropogenic bromoform are derived from simulations with the Lagrangian particle dispersion model FLEXPART based on ERA-Interim wind fields in 2016. In the marine boundary layer of East Asia, the FLEXPART simulations show mean anthropogenic bromoform mixing ratios of 0.4–1.3 ppt , which are 2–6 times larger compared to the climatological bromoform estimate. During boreal winter, the simulations show that some part of the anthropogenic bromoform is transported by the northeasterly winter monsoon towards the tropical regions, whereas during boreal summer anthropogenic bromoform is confined to the Northern Hemisphere subtropics. Convective events in the tropics entrain an additional 0.04–0.05 ppt of anthropogenic bromoform into the stratosphere, averaged over tropical Southeast Asia. In our simulations, only about 10 % of anthropogenic bromoform is outgassed from power plants located in the tropics south of 20 ∘ N, so that only a small fraction of the anthropogenic bromoform reaches the stratosphere. We conclude that bromoform from cooling-water treatment in East Asia is a significant source of atmospheric bromine and might be responsible for annual emissions of 100–300 Mmol of Br in this region. These anthropogenic bromoform sources from industrial water treatment might be a missing factor in global flux estimates of organic bromine. While the current emissions of industrial bromoform provide a significant contribution to regional tropospheric budgets, they provide only a minor contribution to the stratospheric bromine budget of 0.24–0.30 ppt of Br. [ABSTRACT FROM AUTHOR]

Asian dust is an important source of atmospheric ice-nucleating particles (INPs). However, the freezing activity of airborne Asian dust, especially its sensitivity to particle size, is poorly understood. In this study we report the first INP measurement of size-resolved airborne mineral dust collected during East Asian dust events. The measured total INP concentrations in the immersion mode ranged from 10 -2 to 10 2 L -1 in dust events at temperatures between -25 and -5 ∘ C. The average contributions of heat-sensitive INPs at three temperatures, -10 , -15 , and -20 ∘ C, were 81±12 %, 70±15 %, and 38±21 %, respectively, suggesting that proteinaceous biological materials have a substantial effect on the ice nucleation properties of Asian airborne mineral dust at high temperatures. The dust particles which originated from China's northwest deserts are more efficient INPs compared to those from northern regions. In general, there was no significant difference in the ice nucleation properties between East Asian dust particles and other regions in the world. An explicit size dependence of both INP concentration and surface ice-active-site density was observed. The nucleation efficiency of dust particles increased with increasing particle size, while the INP concentration first increased rapidly and then leveled, due to the significant decrease in the number concentration of larger particles. A new set of parameterizations for INP activity based on size-resolved nucleation properties of Asian mineral dust particles were developed over an extended temperature range (-35 to -6 ∘ C). These size-dependent parameterizations require only particle size distribution as input and can be easily applied in models. [ABSTRACT FROM AUTHOR]

Aromatics contribute a significant fraction to organic compounds in the troposphere and are mainly emitted by anthropogenic activities and biomass burning. Their oxidation in lab experiments is known to lead to the formation of ozone and aerosol precursors. However, their overall impact on tropospheric composition is uncertain as it depends on transport, multiphase chemistry, and removal processes of the oxidation intermediates. Representation of aromatics in global atmospheric models has been either neglected or highly simplified. Here, we present an assessment of their impact on gas-phase chemistry, using the general circulation model EMAC (ECHAM5/MESSy Atmospheric Chemistry). We employ a comprehensive kinetic model to represent the oxidation of the following monocyclic aromatics: benzene, toluene, xylenes, phenol, styrene, ethylbenzene, trimethylbenzenes, benzaldehyde, and lumped higher aromatics that contain more than nine C atoms. Significant regional changes are identified for several species. For instance, glyoxal increases by 130 % in Europe and 260 % in East Asia, respectively. Large increases in HCHO are also predicted in these regions. In general, the influence of aromatics is particularly evident in areas with high concentrations of NOx , with increases up to 12 % in O3 and 17 % in OH. On a global scale, the estimated net changes of trace gas levels are minor when aromatic compounds are included in our model. For instance, the tropospheric burden of CO increases by about 6 %, while the burdens of OH , O3 , and NOx (NO+NO2) decrease between 3 % and 9 %. The global mean changes are small, partially because of compensating effects between high- and low- NOx regions. The largest change is predicted for the important aerosol precursor glyoxal, which increases globally by 36 %. In contrast to other studies, the net change in tropospheric ozone is predicted to be negative, -3 % globally. This change is larger in the Northern Hemisphere where global models usually show positive biases. We find that the reaction with phenoxy radicals is a significant loss for ozone, on the order of 200–300 Tg yr -1 , which is similar to the estimated ozone loss due to bromine chemistry. Although the net global impact of aromatics is limited, our results indicate that aromatics can strongly influence tropospheric chemistry on a regional scale, most significantly in East Asia. An analysis of the main model uncertainties related to oxidation and emissions suggests that the impact of aromatics may even be significantly larger. [ABSTRACT FROM AUTHOR]

The Cloud-Aerosol Transport System (CATS) lidar, on board the International Space Station (ISS), provides a new opportunity for studying aerosol vertical distributions, especially the diurnal variations, from space observations. In this study, we investigate the seasonal variations and diurnal cycles in the vertical aerosol extinction coefficients (AECs) over East Asia by taking advantage of 32 months of continuous and uniform aerosol measurements from the CATS lidar. Over the Tibetan Plateau, a belt of AECs at approximately 6 km between 30 and 38 ∘ N persistently exists in all seasons with an obvious seasonal variation. In summer, the aerosols at 6 km are identified as a mixture of both anthropogenic aerosols transported from India and coarse dust particles from Asian dust sources. In addition, the high AECs up to 8 km in summer over the Tibetan Plateau are caused by smoke aerosols from thermal dynamic processes. In fall and winter, the northern slope of the plateau is continuously influenced by both dust aerosols and polluted aerosols transported upslope from cities located at lower elevations in northwestern Asia. The diurnal variation in AECs in North China is mainly related to the diurnal variations in the transported dust and local polluted aerosols. Below 2 km , the AEC profiles in North China at 06:00 and 12:00 CST (China standard time) are significantly higher than those at 00:00 and 18:00 CST, reaching a maximum at midday. The aerosol vertical profiles over the Tarim Desert region in summer have obvious diurnal variations, and the AECs at 12:00 and 18:00 CST are significantly higher than those at 00:00 and 06:00 CST, which are induced by the strong diurnal variations in near-surface wind speeds. In addition, the peak in the AEC profiles has a significant seasonal variation, which is mainly determined by the boundary layer height. [ABSTRACT FROM AUTHOR]

Global coupled chemistry–climate models underestimate carbon monoxide (CO) in the Northern Hemisphere, exhibiting a pervasive negative bias against measurements peaking in late winter and early spring. While this bias has been commonly attributed to underestimation of direct anthropogenic and biomass burning emissions, chemical production and loss via OH reaction from emissions of anthropogenic and biogenic volatile organic compounds (VOCs) play an important role. Here we investigate the reasons for this underestimation using aircraft measurements taken in May and June 2016 from the Korea–United States Air Quality (KORUS-AQ) experiment in South Korea and the Air Chemistry Research in Asia (ARIAs) in the North China Plain (NCP). For reference, multispectral CO retrievals (V8J) from the Measurements of Pollution in the Troposphere (MOPITT) are jointly assimilated with meteorological observations using an ensemble adjustment Kalman filter (EAKF) within the global Community Atmosphere Model with Chemistry (CAM-Chem) and the Data Assimilation Research Testbed (DART). With regard to KORUS-AQ data, CO is underestimated by 42 % in the control run and by 12 % with the MOPITT assimilation run. The inversion suggests an underestimation of anthropogenic CO sources in many regions, by up to 80 % for northern China, with large increments over the Liaoning Province and the North China Plain (NCP). Yet, an often-overlooked aspect of these inversions is that correcting the underestimation in anthropogenic CO emissions also improves the comparison with observational O 3 datasets and observationally constrained box model simulations of OH and HO 2. Running a CAM-Chem simulation with the updated emissions of anthropogenic CO reduces the bias by 29 % for CO, 18 % for ozone, 11 % for HO 2 , and 27 % for OH. Longer-lived anthropogenic VOCs whose model errors are correlated with CO are also improved, while short-lived VOCs, including formaldehyde, are difficult to constrain solely by assimilating satellite retrievals of CO. During an anticyclonic episode, better simulation of O 3 , with an average underestimation of 5.5 ppbv, and a reduction in the bias of surface formaldehyde and oxygenated VOCs can be achieved by separately increasing by a factor of 2 the modeled biogenic emissions for the plant functional types found in Korea. Results also suggest that controlling VOC and CO emissions, in addition to widespread NO x controls, can improve ozone pollution over East Asia. [ABSTRACT FROM AUTHOR]

The Taklamakan desert is an important dust source for the global atmospheric dust budget and a cause of the dust weather in East Asia. The characterization of Taklamakan dust in the source region is still very limited. To fill this gap, the DAO (dust aerosol observation) was conducted in April 2019 in Kashi, China. The Kashi site is about 150 km from the western rim of the Taklamakan desert and is strongly impacted by desert dust aerosols, especially in spring time, i.e., April and May. According to sun–sky photometer measurements, the aerosol optical depth (at 500 nm) varied in the range of 0.07–4.70, and the Ångström exponent (between 440 and 870 nm) in the range of 0.0–0.8 in April 2019. In this study, we provide the first profiling of the 2α+3β+3δ parameters of Taklamakan dust based on a multiwavelength Mie–Raman polarization lidar. For Taklamakan dust, the Ångström exponent related to the extinction coefficient (EAE, between 355 and 532 nm) is about 0.01 ± 0.30, and the lidar ratio is found to be 45 ± 7 sr (51 ± 8–56 ± 8 sr) at 532 (355) nm. The particle linear depolarization ratios (PLDRs) are about 0.28–0.32 ± 0.07 at 355 nm, 0.36 ± 0.05 at 532 nm and 0.31 ± 0.05 at 1064 nm. Both lidar ratios and depolarization ratios are higher than the typical values of Central Asian dust in the literature. The difference is probably linked to the fact that observations in the DAO campaign were collected close to the dust source; therefore, there is a large fraction of coarse-mode and giant particles (radius >20 µ m) in the Taklamakan dust. Apart from dust, fine particles coming from local anthropogenic emissions and long-range transported aerosols are also non-negligible aerosol components. The signatures of pollution emerge when dust concentration decreases. The polluted dust (defined by PLDR 532≤0.30 and EAE 355-532≥0.20) is featured with reduced PLDRs and enhanced EAE 355-532 compared to Taklamakan dust. The mean PLDRs of polluted dust generally distributed in the range of 0.20–0.30. Due to the complexity of the nature of the involved pollutants and their mixing state with dust, the lidar ratios exhibit larger variabilities compared to those of dust. The study provides the first reference of novel characteristics of Taklamakan dust measured by Mie–Raman polarization lidar. The data could contribute to complementing the dust model and improving the accuracy of climate modeling. [ABSTRACT FROM AUTHOR]

Understanding the global distribution of atmospheric black carbon (BC) is essential for unveiling its climatic effect. However, there are still large uncertainties regarding the simulation of BC transport due to inadequate information about the removal process. We accessed the wet removal rate of BC in East Asia based on long-term measurements over the 2010–2016 period at three representative background sites (Baengnyeong and Gosan in South Korea and Noto in Japan). The average wet removal rate, represented by transport efficiency (TE), i.e., the fraction of undeposited BC particles during transport, was estimated to be 0.73 in East Asia from 2010 to 2016. According to the relationship between accumulated precipitation along trajectory and TE, the wet removal efficiency was lower in East and North China but higher in South Korea and Japan, implying the importance of the aging process and frequency of exposure to below- and in-cloud scavenging conditions during air mass transport. Moreover, the wet scavenging in winter and summer showed the highest and lowest efficiency, respectively, although the lowest removal efficiency in summer was primarily associated with a reduced BC aging process because the in-cloud scavenging condition was dominant. The average half-life and e -folding lifetime of BC were 2.8 and 7.1 d , respectively, which is similar to previous studies, but those values differed according to the geographical location and meteorological conditions of each site. Next, by comparing TE from the FLEXible PARTicle (FLEXPART) Lagrangian transport model (version 10.4), we diagnosed the scavenging coefficients (s -1) of the below- and in-cloud scavenging scheme implemented in FLEXPART. The overall median TE from FLEXPART (0.91) was overestimated compared to the measured value, implying the underestimation of wet scavenging coefficients in the model simulation. The median of the measured below-cloud scavenging coefficient showed a lower value than that calculated according to FLEXPART scheme by a factor of 1.7. On the other hand, the overall median of the calculated in-cloud scavenging coefficients from the FLEXPART scheme was highly underestimated by 1 order of magnitude, compared to the measured value. From an analysis of artificial neural networks, the convective available potential energy, which is well known as an indicator of vertical instability, should be considered in the in-cloud scavenging process to improve the representative regional difference in BC wet scavenging over East Asia. For the first time, this study suggests an effective and straightforward evaluation method for wet scavenging schemes (both below and in cloud), by introducing TE along with excluding effects from the inaccurate emission inventories. [ABSTRACT FROM AUTHOR]

Atmospheric black carbon (BC) in the Tibetan Plateau (TP) can largely impact regional and global climate. Still, studies on the inter-annual variation in atmospheric BC over the TP and associated variation in BC sources and controlling factors are rather limited. In this study, we characterize the variations in atmospheric BC over the TP surface layer through analysis of 20-year (1995–2014) simulations from a global chemical transport model, GEOS-Chem. The results show that surface BC concentrations over the TP vary largely in space and by season, reflecting complicated interplays of BC sources from different origins. Of all areas in the TP, surface BC concentrations are highest over the eastern and southern TP, where surface BC is susceptible to BC transport from East Asia and South Asia, respectively. Applying a backward-trajectory method that combines BC concentrations from GEOS-Chem and trajectories from the Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model, we assess the contributions of worldwide source regions to surface BC in the TP. We estimate that on the 20-year average, 77 % of surface BC in the TP comes from South Asia (43 %) and East Asia (35 %). Regarding seasonal variation in non-local influences, South Asia and East Asia are dominant source regions in winter and summer, respectively, in terms of the amount of BC imported. However, in terms of affected areas in the TP, South Asia is the dominant contributor throughout the year. Inter-annually, surface BC over the TP is largely modulated by atmospheric transport of BC from non-local regions year-round and by biomass burning in South Asia, mostly in spring. We find that the extremely strong biomass burning in South Asia in the spring of 1999 greatly enhanced surface BC concentrations in the TP (31 % relative to the climatology). We find that the strength of the Asian monsoon correlates significantly with the inter-annual variation in the amount of BC transported to the TP from non-local regions. In summer, a stronger East Asian summer monsoon and a stronger South Asian summer monsoon tend to, respectively, lead to more BC transport from central China and north-eastern South Asia to the TP. In winter, BC transport from central China is enhanced in years with a strong East Asian winter monsoon or a strong Siberian High. A stronger Siberian High can also bring more BC from northern South Asia to the TP. This study underscores the impacts of atmospheric transport and biomass burning on the inter-annual variation in surface BC over the TP. It reveals a close connection between the Asian monsoon and atmospheric transport of BC from non-local regions to the TP. [ABSTRACT FROM AUTHOR]

Cloud water acidity affects the atmospheric chemistry of sulfate and organic aerosol formation, halogen radical cycling, and trace metal speciation. Precipitation acidity including post-depositional inputs adversely affects soil and freshwater ecosystems. Here, we use the GEOS-Chem model of atmospheric chemistry to simulate the global distributions of cloud water and precipitation acidity as well as the total acid inputs to ecosystems from wet deposition. The model accounts for strong acids (H2SO4 , HNO3 , and HCl), weak acids (HCOOH, CH3COOH , CO2 , and SO2), and weak bases (NH3 as well as dust and sea salt aerosol alkalinity). We compile a global data set of cloud water pH measurements for comparison with the model. The global mean observed cloud water pH is 5.2±0.9 , compared to 5.0±0.8 in the model, with a range from 3 to 8 depending on the region. The lowest values are over East Asia, and the highest values are over deserts. Cloud water pH over East Asia is low because of large acid inputs (H2SO4 and HNO3), despite NH3 and dust neutralizing 70 % of these inputs. Cloud water pH is typically 4–5 over the US and Europe. Carboxylic acids account for less than 25 % of cloud water H+ in the Northern Hemisphere on an annual basis but 25 %–50 % in the Southern Hemisphere and over 50 % in the southern tropical continents, where they push the cloud water pH below 4.5. Anthropogenic emissions of SO2 and NOx (precursors of H2SO4 and HNO3) are decreasing at northern midlatitudes, but the effect on cloud water pH is strongly buffered by NH4+ and carboxylic acids. The global mean precipitation pH is 5.5 in GEOS-Chem, which is higher than the cloud water pH because of dilution and below-cloud scavenging of NH3 and dust. GEOS-Chem successfully reproduces the annual mean precipitation pH observations in North America, Europe, and eastern Asia. Carboxylic acids, which are undetected in routine observations due to biodegradation, lower the annual mean precipitation pH in these areas by 0.2 units. The acid wet deposition flux to terrestrial ecosystems taking into account the acidifying potential of NO3- and NH4+ in N-saturated ecosystems exceeds 50 meqm-2a-1 in East Asia and the Americas, which would affect sensitive ecosystems. NH4+ is the dominant acidifying species in wet deposition, contributing 41 % of the global acid flux to continents under N-saturated conditions. [ABSTRACT FROM AUTHOR]

In this work, we use Coupled Model Intercomparison Project Phase 6 (CMIP6) simulations from 10 Earth system models (ESMs) and general circulation models (GCMs) to study the fast climate responses on pre-industrial climate, due to present-day aerosols. All models carried out two sets of simulations: a control experiment with all forcings set to the year 1850 and a perturbation experiment with all forcings identical to the control, except for aerosols with precursor emissions set to the year 2014. In response to the pattern of all aerosols effective radiative forcing (ERF), the fast temperature responses are characterized by cooling over the continental areas, especially in the Northern Hemisphere, with the largest cooling over East Asia and India, sulfate being the dominant aerosol surface temperature driver for present-day emissions. In the Arctic there is a warming signal for winter in the ensemble mean of fast temperature responses, but the model-to-model variability is large, and it is presumably linked to aerosol-induced circulation changes. The largest fast precipitation responses are seen in the tropical belt regions, generally characterized by a reduction over continental regions and presumably a southward shift of the tropical rain belt. This is a characteristic and robust feature among most models in this study, associated with weakening of the monsoon systems around the globe (Asia, Africa and America) in response to hemispherically asymmetric cooling from a Northern Hemisphere aerosol perturbation, forcing possibly the Intertropical Convergence Zone (ITCZ) and tropical precipitation to shift away from the cooled hemisphere despite that aerosols' effects on temperature and precipitation are only partly realized in these simulations as the sea surface temperatures are kept fixed. An interesting feature in aerosol-induced circulation changes is a characteristic dipole pattern with intensification of the Icelandic Low and an anticyclonic anomaly over southeastern Europe, inducing warm air advection towards the northern polar latitudes in winter. [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]

Recent studies suggested significant impacts of boreal cryosphere changes on wintertime air stagnation and haze pollution extremes in China. However, the underlying mechanisms of such a teleconnection relationship remains unclear. Here we use the Whole Atmosphere Community Climate Model (WACCM) to investigate dynamic processes leading to atmospheric circulation and air stagnation responses to Arctic sea ice changes. We conduct four climate sensitivity experiments by perturbing sea ice concentrations (SIC) and corresponding sea surface temperature (SST) in autumn and early winter over the whole Arctic and three subregions in the climate model. The results indicate distinct responses in circulation patterns and regional ventilation to the region-specific Arctic changes, with the largest increase of both the probability (by 132 %) and the intensity (by 30 %) of monthly air stagnation extremes being found in the experiment driven by SIC and SST changes over the Pacific sector of the Arctic (the East Siberian and Chukchi seas). The increased air stagnation extremes are mainly driven by an amplified planetary-scale atmospheric teleconnection pattern that resembles the negative phase of the Eurasian (EU) pattern. Dynamical diagnostics suggest that convergence of transient eddy forcing in the vicinity of Scandinavia in winter is largely responsible for the amplification of the teleconnection pattern. Transient eddy vorticity fluxes dominate the transient eddy forcing and produce a barotropic anticyclonic anomaly near Scandinavia and wave train propagation across Eurasia to the downstream regions in East Asia. The piecewise potential vorticity inversion analysis reveals that this long-range atmospheric teleconnection of Arctic origin takes place primarily via the middle and upper troposphere. The anomalous ridge over East Asia in the middle and upper troposphere worsens regional ventilation conditions by weakening monsoon northwesterlies and enhancing temperature inversions near the surface, leading to more and stronger air stagnation and pollution extremes over eastern China in winter. Ensemble projections based on state-of-the-art climate models in the Coupled Model Intercomparison Project Phase 6 (CMIP6) corroborate this teleconnection relationship between high-latitude environmental changes and midlatitude weather extremes, though the tendency and magnitude vary considerably among each participating model. [ABSTRACT FROM AUTHOR]

To investigate the characteristics of atmospheric brown carbon (BrC) in the semiarid region of East Asia, PM 2.5 and size-resolved particles in the urban atmosphere of Xi'an, inland China, during the winter and summer of 2017 were collected and analyzed for optical properties and chemical compositions. Methanol extracts (MeOH extracts) were more light-absorbing than water extracts (H2O extracts) in the optical wavelength of 300–600 nm and well correlated with nitrophenols, polycyclic aromatic hydrocarbons (PAHs) and oxygenated PAHs (r>0.78). The light absorptions (abs λ=365nm) of H2O extracts and MeOH extracts in winter were 28±16 and 49±32 M m -1 , respectively, which are about 10 times higher than those in summer, mainly due to the enhanced emissions from biomass burning for house heating. Water-extracted BrC predominately occurred in the fine mode (< 2.1 µ m) during winter and summer, accounting for 81 % and 65 % of the total absorption of BrC, respectively. The light absorption and stable carbon isotope composition measurements showed an increasing ratio of abs λ=365nm -MeOH to abs λ=550nm -EC along with an enrichment of 13C in PM 2.5 during the haze development, indicating an accumulation of secondarily formed BrC (e.g., nitrophenols) in the aerosol aging process. Positive matrix factorization (PMF) analysis showed that biomass burning, fossil fuel combustion, secondary formation, and fugitive dust are the major sources of BrC in the city, accounting for 55 %, 19 %, 16 %, and 10 % of the total BrC of PM 2.5 , respectively. [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]

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. [ABSTRACT FROM AUTHOR]

Despite the significant progress in improving chemical transport models (CTMs), applications of these modeling endeavors are still subject to large and complex model uncertainty. The Model Inter-Comparison Study for Asia III (MICS-Asia III) has provided the opportunity to assess the capability and uncertainty of current CTMs in East Asian applications. In this study, we have evaluated the multi-model simulations of nitrogen dioxide (NO2), carbon monoxide (CO) and ammonia (NH3) over China under the framework of MICS-Asia III. A total of 13 modeling results, provided by several independent groups from different countries and regions, were used in this study. Most of these models used the same modeling domain with a horizontal resolution of 45 km and were driven by common emission inventories and meteorological inputs. New observations over the North China Plain (NCP) and Pearl River Delta (PRD) regions were also available in MICS-Asia III, allowing the model evaluations over highly industrialized regions. The evaluation results show that most models captured the monthly and spatial patterns of NO2 concentrations in the NCP region well, though NO2 levels were slightly underestimated. Relatively poor performance in NO2 simulations was found in the PRD region, with larger root-mean-square error and lower spatial correlation coefficients, which may be related to the coarse resolution or inappropriate spatial allocations of the emission inventories in the PRD region. All models significantly underpredicted CO concentrations in both the NCP and PRD regions, with annual mean concentrations that were 65.4 % and 61.4 % underestimated by the ensemble mean. Such large underestimations suggest that CO emissions might be underestimated in the current emission inventory. In contrast to the good skills for simulating the monthly variations in NO2 and CO concentrations, all models failed to reproduce the observed monthly variations in NH3 concentrations in the NCP region. Most models mismatched the observed peak in July and showed negative correlation coefficients with the observations, which may be closely related to the uncertainty in the monthly variations in NH3 emissions and the NH3 gas–aerosol partitioning. Finally, model intercomparisons have been conducted to quantify the impacts of model uncertainty on the simulations of these gases, which are shown to increase with the reactivity of species. Models contained more uncertainty in the NH3 simulations. This suggests that for some highly active and/or short-lived primary pollutants, like NH3 , model uncertainty can also take a great part in the forecast uncertainty in addition to the emission uncertainty. Based on these results, some recommendations are made for future studies. [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]

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]

Spatiotemporal variations of ozone (O3) and nitrogen oxide (NOx) mixing ratios from 14 state-of-the-art chemical transport models (CTMs) are intercompared and evaluated with O3 observations in East Asia, within the framework of the Model Inter-Comparison Study for Asia Phase III (MICS-Asia III). This study was designed to evaluate the capabilities and uncertainties of current CTMs simulations for Asia and to provide multi-model estimates of pollutant distributions. These models were run by 14 independent groups working in China, Japan, South Korea, the United States and other countries/regions. Compared with the previous phase of MICS-Asia (MICS-Asia II), the evaluation with observations was extended from 4 months to 1 full year across China and the western Pacific Rim. In general, model performance levels for O3 varied widely by region and season. Most models captured the key patterns of monthly and diurnal variation of surface O3 and its precursors in the North China Plain and western Pacific Rim but failed to do so for the Pearl River Delta. A significant overestimation of surface O3 was evident from May to September/October and from January to May over the North China Plain, the western Pacific Rim and the Pearl River Delta. Comparisons drawn from observations show that the considerable diversity in O3 photochemical production partly contributed to this overestimation and to high levels of inter-model variability in O3 for North China. In terms of O3 soundings, the ensemble average of models reproduced the vertical structure for the western Pacific, but overestimated O3 levels to below 800 hPa in the summer. In the industrialized Pearl River Delta, the ensemble average presented an overestimation for the lower troposphere and an underestimation for the middle troposphere. The ensemble average of 13 models for O3 did not always exhibit superior performance compared with certain individual models in contrast with its superior value for Europe. This finding suggests that the spread of ensemble-model values does not represent all of the uncertainties of O3 or that most MICS-Asia III models missed key processes. This study improved the performance of modeling O3 in March at Japanese sites compared with MICS-Asia II. However, it overpredicted surface O3 concentrations for western Japan in July, which was not found by MICS-Asia II. Major challenges still remain with regard to identifying the sources of bias in surface O3 over East Asia in CTMs. [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]

Tropospheric ozone in East Asia is influenced by the transport of ozone from foreign regions around the world. However, the magnitudes and variations in such influences remain unclear. This study was performed to investigate the influences using a global chemical transport model, GEOS-Chem, through the tagged ozone and emission perturbation simulations. The results show that foreign ozone is transported to East Asia (20–60 ∘ N, 95–150 ∘ E) mainly through the middle and upper troposphere. In East Asia, the influence of foreign ozone increases rapidly with altitude. In the middle and upper troposphere, the regional mean concentrations of foreign ozone range from 32 to 65 ppbv, being 0.8–4.8 times higher than its native counterpart (11–18 ppbv). Annually, ∼60 % of foreign ozone in the East Asian middle and upper troposphere comes from North America (5–13 ppbv) and Europe (5–7 ppbv), as well as from foreign oceanic regions (9–21 ppbv). Over the East Asian tropospheric columns, foreign ozone appears most in spring when ozone concentrations in the foreign regions are high and the westerlies are strong and least in summer when the South Asian High blocks eastward foreign ozone from reaching East Asia south of 35 ∘ N. At the East Asian surface, the annual mean of foreign ozone concentrations is ∼22.2 ppbv, which is comparable to its native counterpart of ∼20.4 ppbv. In the meantime, the annual mean of anthropogenic ozone concentrations from foreign regions is ∼4.7 ppbv, half of which comes from North America (1.3 ppbv) and Europe (1.0 ppbv). Seasonally, foreign ozone concentrations at the East Asian surface are highest in winter (27.1 ppbv) and lowest in summer (16.5 ppbv). This strong seasonality is largely modulated by the East Asian monsoon (EAM) via its influence on vertical motion. The large-scale subsidence prevailing during the East Asian winter monsoon (EAWM) favours the downdraft of foreign ozone to the surface, while widespread convection in the East Asian summer monsoon (EASM) blocks such transport. Interannually, the variation in foreign ozone at the East Asian surface is found to be closely related to the intensity of the EAM. Specifically, the stronger the EAWM is in a winter, the more ozone from North America and Europe reaches the East Asian surface because of the stronger subsidence behind the East Asian trough. In summer, ozone from South and South-east Asia is reduced in strong EASM years due to weakened south-westerly monsoon winds. This study suggests substantial foreign influences on ozone at the East Asian surface and in its tropospheric columns. It also underscores the importance of the EAM in the seasonal and interannual variations in foreign influences on surface ozone in East Asia. [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]

The East Asian winter monsoon (EAWM) is greatly influenced by many factors that can be classified as anthropogenic forcing and natural forcing. Here we explore the contribution of anthropogenic influence to the change in the EAWM over the past decades. Under all forcings observed during 1960–2013 (All-Hist run), the atmospheric general circulation model is able to reproduce the climatology and variability of the EAWM-related surface air temperature and 500 hPa geopotential height and shows a statistically significant decreasing EAWM intensity with a trend coefficient of ∼-0.04 yr -1 , which is close to the observed trend. By contrast, the simulation, which is driven by the same forcing as the All-Hist run but with the anthropogenic contribution to them removed, shows no decreasing trend in the EAWM intensity. By comparing the simulations under two different forcing scenarios, we further reveal that the responses of the EAWM to the anthropogenic forcing include a rise of 0.6 ∘ in surface air temperature over East Asia as well as weakening of the East Asian trough, which may result from the poleward expansion and intensification of the East Asian jet forced by the change in temperature gradient in the troposphere. Additionally, compared with the simulation without anthropogenic forcing, the frequency of strong (weak) EAWM occurrence is reduced (increased) by 45 % (from 0 to 10/7). These results indicate that the weakening of the EAWM during 1960–2013 may be mainly attributed to the anthropogenic influence. [ABSTRACT FROM AUTHOR]

In this study, a full description and comprehensive evaluation of a global–regional nested model, the Aerosol and Atmospheric Chemistry Model of the Institute of Atmospheric Physics (IAP-AACM), is presented for the first time. Not only are the global budgets and distribution explored, but comparisons of the nested simulation over China against multiple datasets are investigated, which benefit from access to Chinese air quality monitoring data from 2013 to the present and the "Model Inter-Comparison Study for Asia" project. The model results and analysis can help reduce uncertainties and aid with understanding model diversity with respect to assessing global and regional aerosol effects on climate and human health, especially over East Asia and areas affected by East Asia. For the global simulation, the 1-year simulation for 2014 shows that the IAP-AACM is within the range of other models. Overall, it reasonably reproduced spatial distributions and seasonal variations of trace gases and aerosols in both surface concentrations and column burdens (mostly within a factor of 2). The model captured spatial variation for carbon monoxide well with a slight underestimation over ocean, which implicates the uncertainty of the ocean source. The simulation also matched the seasonal cycle of ozone well except for the continents in the Northern Hemisphere, which was partly due to the lack of stratospheric–tropospheric exchange. For aerosols, the simulation of fine-mode particulate matter (PM 2.5) matched observations well. The simulation of primary aerosols (normalized mean biases, NMBs, are within ±0.64) is better than that of secondary aerosols (NMB values are greater than 1.0 in some regions). For the nested regional simulation, the IAP-AACM shows the superiority of higher-resolution simulation using the nested domain over East Asia. The model reproduced variation of sulfur dioxide (SO2), nitrogen dioxide (NO2), and PM 2.5 accurately in typical cities, with correlation coefficients (R) above 0.5 and NMBs within ±0.5. Compared with the global simulation, the nested simulation exhibits an improved ability to capture the high temporal and spatial variability over China. In particular, the R values for SO2 , NO2 and PM 2.5 are increased by ∼0.15 , ∼0.2 , and ∼0.25 respectively in the nested grid. Based on the evaluation and analysis, future model improvements are suggested. [ABSTRACT FROM AUTHOR]

Hong Kong, as one of the densely populated metropolises in East Asia, has been suffering from severe photochemical smog in the past decades, though the observed nitrogen oxides (NOx) and total volatile organic compounds (TVOCs) were significantly reduced. This study, based on the observation data in the autumns of 2007, 2013 and 2016, investigated the photochemical ozone (O3) formation and radical chemistry during the three sampling periods in Hong Kong with the aid of a photochemical box model incorporating the Master Chemical Mechanism (PBM–MCM). While the simulated locally produced O3 remained unchanged (p=0.73) from 2007 to 2013, the observed O3 increased (p < 0.05) at a rate of 1.78 ppbv yr -1 driven by the rise in regionally transported O3 (1.77±0.04 ppbv yr -1). Both the observed and locally produced O3 decreased (p < 0.05) from the VOC sampling days in 2013 to those in 2016 at a rate of -5.31±0.07 and -5.52±0.05 ppbv yr -1 , respectively. However, a leveling-off (p=0.32) was simulated for the regionally transported O3 during 2013–2016. The mitigation of autumn O3 pollution in this region was further confirmed by the continuous monitoring data, which have never been reported. Benefiting from the air pollution control measures taken in Hong Kong, the local O3 production rate decreased remarkably (p < 0.05) from 2007 to 2016, along with the lowering of the recycling rate of the hydroxyl radical (OH). Specifically, VOCs emitted from the source of liquefied petroleum gas (LPG) usage and gasoline evaporation decreased in this decade at a rate of -2.61±0.03 ppbv yr -1 , leading to a reduction of the O3 production rate from 0.51±0.11 ppbv h -1 in 2007 to 0.10±0.02 ppbv h -1 in 2016. In addition, solvent usage made decreasing contributions to both VOCs (rate =-2.29±0.03 ppbv yr -1) and local O3 production rate (1.22±0.17 and 0.14±0.05 ppbv h -1 in 2007 and 2016, respectively) in the same period. All the rates reported here were for the VOC sampling days in the three sampling campaigns. It is noteworthy that meteorological changes also play important roles in the inter-annual variations in the observed O3 and the simulated O3 production rates. Evaluations with more data in longer periods are therefore recommended. The analyses on the decadal changes of the local and regional photochemistry in Hong Kong in this study may be a reference for combating China's nationwide O3 pollution in near future. [ABSTRACT FROM AUTHOR]

Past studies have suggested that ozone in the troposphere has increased globally throughout much of the 20th century due to increases in anthropogenic emissions and transport. We show, by combining satellite measurements with a chemical transport model, that during the last four decades tropospheric ozone does indeed indicate increases that are global in nature, yet still highly regional. Satellite ozone measurements from Nimbus-7 and Earth Probe Total Ozone Mapping Spectrometer (TOMS) are merged with ozone measurements from the Aura Ozone Monitoring Instrument/Microwave Limb Sounder (OMI/MLS) to determine trends in tropospheric ozone for 1979–2016. Both TOMS (1979–2005) and OMI/MLS (2005–2016) depict large increases in tropospheric ozone from the Near East to India and East Asia and further eastward over the Pacific Ocean. The 38-year merged satellite record shows total net change over this region of about +6 to +7 Dobson units (DU) (i.e., ∼15 %–20 % of average background ozone), with the largest increase (∼4 DU) occurring during the 2005–2016 Aura period. The Global Modeling Initiative (GMI) chemical transport model with time-varying emissions is used to aid in the interpretation of tropospheric ozone trends for 1980–2016. The GMI simulation for the combined record also depicts the greatest increases of +6 to +7 DU over India and East Asia, very similar to the satellite measurements. In regions of significant increases in tropospheric column ozone (TCO) the trends are a factor of 2–2.5 larger for the Aura record when compared to the earlier TOMS record; for India and East Asia the trends in TCO for both GMI and satellite measurements are ∼+3 DU decade -1 or greater during 2005–2016 compared to about +1.2 to +1.4 DU decade -1 for 1979–2005. The GMI simulation and satellite data also reveal a tropospheric ozone increases in ∼+4 to +5 DU for the 38-year record over central Africa and the tropical Atlantic Ocean. Both the GMI simulation and satellite-measured tropospheric ozone during the latter Aura time period show increases of ∼+3 DU decade -1 over the N Atlantic and NE Pacific. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

We analyzed long-term fine- and coarse-mode synergetic observations of nitrate and related aerosols (SO42-, NO3-, NH4+, Na+, Ca2+) at Fukuoka (33.52° N, 130.47° E) from August 2014 to October 2015. A Goddard Earth Observing System chemical transport model (GEOS-Chem) including dust and sea salt acid uptake processes was used to assess the observed seasonal variation and the impact of long-range transport (LRT) from the Asian continent. For fine aerosols (fSO42-, fNO3-, and fNH4+), numerical results explained the seasonal changes, and a sensitivity analysis excluding Japanese domestic emissions clarified the LRT fraction at Fukuoka (85% for fSO42-, 47% for fNO3-, 73% for fNH4+). Observational data confirmed that coarse NO3- (cNO3-) made up the largest proportion (i.e., 40-55%) of the total nitrate (defined as the sum of fNO3-, cNO3-, and HNO3) during the winter, while HNO3 gas constituted approximately 40% of the total nitrate in summer and fNO3- peaked during the winter. Large-scale dust-nitrate (mainly cNO3-) outflow from China to Fukuoka was confirmed during all dust events that occurred between January and June. The modeled cNO3- was in good agreement with observations between July and November (mainly coming from sea salt NO3-). During the winter, however, the model underestimated cNO3- levels compared to the observed levels. The reason for this underestimation was examined statistically using multiple regression analysis (MRA). We used cNa+, nss-cCa2+, and cNH4+ as independent variables to describe the observed cNO3- levels; these variables were considered representative of sea salt cNO3-, dust cNO3-, and cNO3- accompanied by cNH4+), respectively. The MRA results explained the observed seasonal changes in dust cNO3- and indicated that the dust-acid uptake scheme reproduced the observed dust-nitrate levels even in winter. The annual average contributions of each component were 43% (sea salt cNO3-), 19% (dust cNO3-), and 38% (cNH4+ term). The MRA dust-cNO3- component had a high value during the dust season, and the sea salt component made a large contribution throughout the year. During the winter, cNH4+ term made a large contribution. The model did not include aerosol microphysical processes (such as condensation and coagulation between the fine anthropogenic aerosols NO3- and SO42- and coarse particles), and our results suggest that inclusion of aerosol microphysical processes is critical when studying observed cNO3- formation, especially in winter. [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]

We have found a stratospheric area of anomalously low annual cycle amplitude and specific dynamics in the stratosphere over the northeastern Pacific-eastern Asia coastal region. Using GPS radio occultation density profiles from the Formosat Satellite Mission 3/Constellation Observing System for Meteorology, Ionosphere, and Climate (FORMOSAT-3/COSMIC), we have discovered an internal gravity wave (IGW) activity and breaking hotspot in this region. Conditions supporting orographic wave sourcing and propagation were found. Other possible sources of wave activity in this region are listed. The reasons why this particular IGW activity hotspot was not discovered before as well as why the specific dynamics of this region have not been pointed out are discussed together with the weaknesses of using the mean potential energy as a wave activity proxy. Possible consequences of the specific dynamics in this region on the middle atmospheric dynamics and transport are outlined. [ABSTRACT FROM AUTHOR]

In order to optimize surface CO2 fluxes at grid scales, a regional surface CO2 flux inversion system (Carbon Flux Inversion system and Community Multi-scale Air Quality, CFI-CMAQ) has been developed by applying the ensemble Kalman filter (EnKF) to constrain the CO2 concentrations and applying the ensemble Kalman smoother (EnKS) to optimize the surface CO2 fluxes. The smoothing operator is associated with the atmospheric transport model to constitute a persistence dynamical model to forecast the surface CO2 flux scaling factors. In this implementation, the "signalto-noise" problem can be avoided; plus, any useful observed information achieved by the current assimilation cycle can be transferred into the next assimilation cycle. Thus, the surface CO2 fluxes can be optimized as a whole at the grid scale in CFI-CMAQ. The performance of CFI-CMAQ was quantitatively evaluated through a set of Observing System Simulation Experiments (OSSEs) by assimilating CO2 retrievals from GOSAT (Greenhouse Gases Observing Satellite). The results showed that the CO2 concentration assimilation using EnKF could constrain the CO2 concentration effectively, illustrating that the simultaneous assimilation of CO2 concentrations can provide convincing CO2 initial analysis fields for CO2 flux inversion. In addition, the CO2 flux optimization using EnKS demonstrated that CFI-CMAQ could, in general, reproduce true fluxes at grid scales with acceptable bias. Two further sets of numerical experiments were conducted to investigate the sensitivities of the inflation factor of scaling factors and the smoother window. The results showed that the ability of CFI-CMAQ to optimize CO2 fluxes greatly relied on the choice of the inflation factor. However, the smoother window had a slight influence on the optimized results. CFICMAQ performed very well even with a short lag-window (e.g. 3 days). [ABSTRACT FROM AUTHOR]

The morphology, microstructure, and composition of the submicron fraction of individual light-absorbing carbon (LAC) particles collected by research aircraft during the ACE-Asia (Asian Pacific Regional Aerosol Characterization Experiment) project above the Yellow Sea at altitudes of 120, 450 and 1500m are investigated by transmission electron microscopy (TEM), and energy dispersive X-ray spectroscopy (EDS). Two types of carbonaceous particles, small spherule soot with graphitic spherules and amorphous carbonaceous spheres (brown carbon), are found at all altitudes in high concentration. For soot particles, emphasis of the study is on the component subparticles (spherules). The nanoscopic structures of the small spherule soot show no significant difference at three altitudes although the size distribution of primary spherules showed that 70% of the total volume lies in the ranges 30-50, 50-85 and 30-50 nm, respectively. For the amorphous carbonaceous spheres, 70% of the total volume from three altitudes lies in the range 200-350, 160-470 and 150-320 nm, respectively. Within the size fraction studied (submicron, with most particles in the range 50 to 500 nm) the number concentration ratios of the amorphous carbonaceous spheres to primary spherules in soot at altitudes of 120, 450 and 1500m are about 1, 1.5 and 10, respectively and their volume ratios are about 260, 50 and 1400. Lower relative concentrations of large spherule soot with intermediate graphitic structure were observed at 120 m. Also, low relative number concentrations of carbon cenospheres were observed at 120 and 1500 m. A key result of the study is that in vertically stratified outflow from East Asia, the character of LAC may have strong variance with altitude thus resulting in optical characteristics that vary with altitude. Also, apparent "aging" of LAC deduced from samples at multiple ground stations may instead reflect differences in the original carbon aerosols. [ABSTRACT FROM AUTHOR]

The response of East Asian Summer Monsoon (EASM) precipitation to long term changes in regional anthropogenic aerosols (sulphate and black carbon) is explored in an atmospheric general circulation model, the atmospheric component of the UK High-Resolution Global Environment Model v1.2 (HiGAM). Separately, sulphur dioxide (SO2) and black carbon (BC) emissions in 1950 and 2000 over East Asia are used to drive model simulations, while emissions are kept constant at year 2000 level outside this region. The response of the EASM is examined by comparing simulations driven by aerosol emissions representative of 1950 and 2000. The aerosol radiative effects are also determined using an off-line radiative transfer model. During June, July and August, the EASM was not significantly changed as either SO2 or BC emissions increased from 1950 to 2000 levels. However, in September, precipitation is significantly decreased by 26.4% for sulphate aerosol and 14.6% for black carbon when emissions are at the 2000 level. Over 80% of the decrease is attributed to changes in convective precipitation. The cooler land surface temperature over China in September (0.8 °C for sulphate and 0.5 °C for black carbon) due to increased aerosols reduces the surface thermal contrast that supports the EASM circulation. However, mechanisms causing the surface temperature decrease in September are different between sulphate and BC experiments. In the sulphate experiment, the sulphate direct and the 1st indirect radiative effects contribute to the surface cooling. In the BC experiment, the BC direct effect is the main driver of the surface cooling, however, a decrease in low cloud cover due to the increased heating by BC absorption partially counteracts the direct effect. This results in a weaker land surface temperature response to BC changes than to sulphate changes. The resulting precipitation response is also weaker, and the responses of the monsoon circulation are different for sulphate and black carbon experiments. This study demonstrates a mechanism that links regional aerosol emission changes to the precipitation changes of the EASM, and it could be applied to help understand the future changes in EASM precipitation in CMIP5 simulations. [ABSTRACT FROM AUTHOR]

We use satellite observations of aerosol optical depth (AOD) from the Moderate Resolution Imaging Spectrometer (MODIS) together with the GEOS-Chem global chemical transport model to contrast export of aerosols from East Asia and North America during 2004-2010. The GEOS-Chem model reproduces the spatial distribution and temporal variations of Asian aerosol outflow generally well, although a low bias (-30 %) is found in the model fine mode AOD, particularly during summer. We use the model to identify 244 aerosol pollution export events from E. Asia and 251 export events from N. America over our 7-year study period. When these events are composited by season, we find that the AOD in the outflow is enhanced by 50-100% relative to seasonal mean values. The composite Asian plume splits into one branch going poleward to the Arctic in 3-4 days, with the other crossing the Pacific Ocean in 6-8 days. A fraction of the aerosols is trapped in the subtropical Pacific High during spring and summer. The N. American plume travels to the northeast Atlantic, reaching Europe after 4-5 days. Part of the composite plume turns anticyclonically in the Azores High, where it slowly decays. Both the Asian and N. American export events are favored by a dipole structure in sea-level pressure anomalies, associated with midlatitude cyclone activity over the respective source regions. This dipole structure during outflow events is a strong feature for all seasons except summer, when convection becomes more important. The observed AOD in the E. Asian outflow exhibits stronger seasonality, with a spring maximum, than the N. American outflow, with a broad spring/summer maximum. The large spring AOD in the Asian outflow is the result of enhanced sulfate and dust aerosol concentrations, but is also due to a larger export efficiency of sulfate and SO2 from the Asian boundary layer relative to the N. American boundary layer. While the N. American sulfate outflow is mostly found in the lower troposphere (1-3 km altitude), the Asian sulfate outflow occurs at higher altitudes (2-6 km). In the Asian outflow 42-59% of the sulfate column is present above 2 km altitude, with only 24-35% in the N. American outflow. We link this to the factor of 2-5 lower precipitation in the warm conveyor belts (WCB) of midlatitude cyclones over E. Asia compared to N. America. This relative lack of precipitation makes Asian WCB very efficient for injecting aerosols in the middle troposphere. [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]

To evaluate the impact of biomass burning from Southeast Asia to East Asia, this study conducted numerical simulations during NASA's 2006 Biomass-burning Aerosols in South-East Asia: Smoke Impact Assessment (BASE-ASIA). Two typical episode periods (27--28 March and 13--14 April) were examined. Two emission inventories, FLAMBE and GFED, were used in the simulations. The influences during two episodes in the source region (Southeast Asia) contributed to the surface CO, O3 and PM2.5 concentrations as high as 400 ppbv, 20 ppbv and 80 µgm-3, respectively. The perturbations with and without biomass burning of the above three species during the intense episodes were in the range of 10 to 60 %, 10 to 20% and 30 to 70 %, respectively. The impact due to long-range transport could spread over the southeastern parts of East Asia and could reach about 160 to 360 ppbv, 8 to 18 ppbv and 8 to 64 µgm-3 on CO, O3 and PM2.5, respectively; the percentage impact could reach 20 to 50% on CO, 10 to 30% on O3, and as high as 70% on PM2.5. In March, the impact of biomass burning mainly concentrated in Southeast Asia and southern China, while in April the impact becomes slightly broader and even could go up to the Yangtze River Delta region. Two cross-sections at 15° N and 20° N were used to compare the vertical flux of biomass burning. In the source region (Southeast Asia), CO, O3 and PM2.5 concentrations had a strong upward transport from surface to high altitudes. The eastward transport becomes strong from 2 to 8 km in the free troposphere. The subsidence process during the long-range transport contributed 60 to 70 %, 20 to 50 %, and 80% on CO, O3 and PM2.5, respectively to surface in the downwind area. The study reveals the significant impact of Southeastern Asia biomass burning on the air quality in both local and downwind areas, particularly during biomass burning episodes. This modeling study might provide constraints of lower limit. An additional study is underway for an active biomass burning year to obtain an upper limit and climate effects. [ABSTRACT FROM AUTHOR]

The 14C-free fossil carbon added to atmospheric CO2 by combustion dilutes the atmospheric 14C/C ratio (Δ14C), potentially providing a means to verify fossil CO2 emissions calculated using economic inventories. However, sources of 14C from nuclear power generation and spent fuel reprocessing can counteract this dilution and may bias 14C/C-based estimates of fossil fuel-derived CO2 if these nuclear influences are not correctly accounted for. Previous studies have examined nuclear influences on local scales, but the potential for continental-scale influences on Δ14C has not yet been explored. We estimate annual 14C emissions from each nuclear site in the world and conduct an Eulerian transport modeling study to investigate the continental-scale, steady-state gradients of Δ14C caused by nuclear activities and fossil fuel combustion. Over large regions of Europe, North America and East Asia, nuclear enrichment may offset at least 20% of the fossil fuel dilution in Δ14C, corresponding to potential biases of more than -0.25 ppm in the CO2 attributed to fossil fuel emissions, larger than the bias from plant and soil respiration in some areas. Model grid cells including high 14C-release reactors or fuel reprocessing sites showed much larger nuclear enrichment, despite the coarse model resolution of 1.8° x 1.8°. The recent growth of nuclear 14C emissions increased the potential nuclear bias over 1985-2005, suggesting that changing nuclear activities may complicate the use of Δ14C observations to identify trends in fossil fuel emissions. The magnitude of the potential nuclear bias is largely independent of the choice of reference station in the context of continental-scale Eulerian transport and inversion studies, but could potentially be reduced by an appropriate choice of reference station in the context of local-scale assessments. [ABSTRACT FROM AUTHOR]

To more accurately estimate direct radiative forcing (DRF) by aerosols, and better investigate particulate pollution over East Asia, precise calculations of the optical properties of aerosols, such as aerosol optical depth (AOD), single scattering albedo (SSA) and aerosol extinction coefficient (σext), are of primary importance. The aerosol optical properties over East Asia were investigated in this study, based on US EPA Models-3/CMAQ v4.5.1 model simulations. The CMAQ model simulations in this study were improved in several ways compared to those in a previous study (Song et al., 2008). Although the details of the improvements were described in the manuscript, the following points should be emphasized: (1) two data assimilation techniques were employed for producing more accurate AOD products and meteorological fields over East Asia; (2) updated/ upgraded emission inventories were used in the CMAQ model simulations with a fine grid resolution of 30x30 km²; and (3) the 4-D particulate composition calculated from the CMAQ model simulations was converted into 3-D or 4-D aerosol optical products, using the Malm and Hand (2007) algorithm with significant further modifications. The results from the CMAQ model simulations (without assimilation) showed great improvements compared to those from a previous study. For example, in terms of the regression coefficients (R), R values were increased from 0.48-0.68 (previous study) to 0.62-0.79 (this study). The monthly-averaged CMAQ-simulated single scattering albedo (SSA) also agreed well with the AERONET SSA, with the exceptions of the Hong Kong and Taipei sites, where the air qualities were strongly influenced by active biomass burning events from January to April. There were also excellent matches between the vertical profiles of the CMAQ-simulated σext and LIDAR-retrieved σext. It was also found that the contributions of (NH4)2SO4 during summer, NH4NO3 during winter, sea-salt particles during winter and dust particles during spring to the total AOD were large over East Asia. In particular, the largest contribution of NH4NO3 to the total AOD was found over East Asia during winter. Therefore, it was suggested that this contribution of NH4NO3 should not be neglected. In order to produce more accurate AOD products, the CMAQ-simulated AODs were further assimilated with the MODIS-retrieved AODs. Both of the assimilated and AERONET AODs were better correlated with each other than the CMAQ-simulated and AERONET AODs. The obvious benefits from this study would be that with these improved aerosol optical properties, the particulate pollution (e.g. AOD can be served as a proxy to PM2.5 or PM10) and DRF by aerosols over East Asia can be more satisfactorily investigated in future. [ABSTRACT FROM AUTHOR]

On a research flight on 10 July 2008, the German research aircraft Falcon sampled an air mass with unusually high carbon monoxide (CO), peroxyacetyl nitrate (PAN) and water vapour (H2O) mixing ratios in the Arctic lowermost stratosphere. The air mass was encountered twice at an altitude of 11.3 km, ~800m above the dynamical tropopause. In-situ measurements of ozone, NO, and NOy indicate that this layer was a mixed air mass containing both air from the troposphere and stratosphere. Backward trajectory and Lagrangian particle dispersion model analysis suggest that the Falcon sampled the top of a polluted air mass originating from the coastal regions of East Asia. The anthropogenic pollution plume experienced strong uplift in a warm conveyor belt (WCB) located over the Russian east-coast. Subsequently the Asian air mass was transported across the North Pole into the sampling area, elevating the local tropopause by up to ~3 km. Mixing with surrounding Arctic stratospheric air most likely took place during the horizontal transport when the tropospheric streamer was stretched into long and narrow filaments. The mechanism illustrated in this study possibly presents an important pathway to transport pollution into the polar tropopause region. [ABSTRACT FROM AUTHOR]

Understanding the exchange processes between the atmospheric boundary layer and the free troposphere is crucial for estimating hemispheric transport of air pollution. Most studies of hemispheric air pollution transport have taken a large-scale perspective using global chemical transport models with fairly coarse spatial and temporal resolutions. In support of United Nations Task Force on Hemispheric Transport of Air Pollution (TF HTAP; www.htap. org), this study employs two high-resolution atmospheric chemistry models (WRF-Chem and CMAQ; 36×36 km) driven with chemical boundary conditions from a global model (MOZART; 1.9×1.9°) to examine the role of finescale transport and chemistry processes in controlling pollution export and import over the Asian continent in spring (March 2001). Our analysis indicates the importance of rapid venting through deep convection that develops along the leading edge of frontal system convergence bands, which are not adequately resolved in either of two global models compared with TRACE-P aircraft observations during a frontal event. Both regional model simulations and observations show that frontal outflows of CO, O3 and PAN can extend to the upper troposphere (6-9 km). Pollution plumes in the global MOZART model are typically diluted and insufficiently lofted to higher altitudes where they can undergo more efficient transport in stronger winds. We use sensitivity simulations that perturb chemical boundary conditions in the CMAQ regional model to estimate that the O3 production over East Asia (EA) driven by PAN decomposition contributes 20% of the spatial averaged total O3 response to European (EU) emission perturbations in March, and occasionally contributes approximately 50% of the total O3 response in subsiding plumes at mountain observatories (at approximately 2 km altitude). The response to decomposing PAN of EU origin is strongly affected by the O3 formation chemical regimes, which vary with the model chemical mechanism and NOx/VOC emissions. Our highresolution models demonstrate a large spatial variability (by up to a factor of 6) in the response of local O3 to 20% reductions in EU anthropogenic O3 precursor emissions. The response in the highly populated Asian megacities is 40- 50% lower in our high-resolution models than the global model, suggesting that the source-receptor relationships inferred from the global coarse-resolution models likely overestimate health impacts associated with intercontinental O3 transport. Our results highlight the important roles of rapid convective transport, orographic forcing, urban photochemistry and heterogeneous boundary layer processes in controlling intercontinental transport; these processes may not be well resolved in the large-scale models. [ABSTRACT FROM AUTHOR]

A global model of aerosol microphysics is used to simulate a large East Asian dust storm during the ACE-Asia experiment. We use the model together with size resolved measurements of aerosol number concentration and composition to examine how dust modified the production of sulfate aerosol and the particle size distribution in East Asian outflow. Simulated size distributions and mass concentrations of dust, sub- and super-micron sulfate agree well with observations from the C-130 aircraft. Modeled mass concentrations of fine sulfate (Dp<1.3 μm) decrease by ~10% due to uptake of sulfur species onto super-micron dust. We estimate that dust enhanced the mass concentration of coarse sulfate (Dp>1.0 μm) by more than an order of magnitude, but total sulfate concentrations increase by less than 2% because decreases in fine sulfate have a compensating effect. Our analysis shows that the sulfate associated with dust can be explained largely by the uptake of H2SO4 rather than reaction of SO2 on the dust surface, which we assume is suppressed once the particles are coated in sulfate. We suggest that many previous model investigations significantly overestimated SO2 oxidation on East Asian dust, possibly due to the neglect of surface saturation effects. We extend previous model experiments by examining how dust modified existing particle concentrations in Asian outflow. Total particle concentrations (condensation nuclei, CN) modeled in the dust-pollution plume are reduced by up to 20%, but we predict that dust led to less than 10% depletion in particles large enough to act as cloud condensation nuclei (CCN). Our analysis suggests that E. Asian dust storms have only a minor impact on sulfate particles present at climate-relevant sizes. [ABSTRACT FROM AUTHOR]

Size-segregated (9 stages) n-alkanes, polycyclic aromatic hydrocarbons (PAHs) and hopanes in the urban (Baoji city in inland China), mountain (Mt. Tai in east coastal China) and marine (Okinawa Island, Japan) atmospheres over East Asia were studied using a GC/MS technique. Ambient concentrations of n-alkanes (1698±568 ngm-3 in winter and 487±145 ngm-3 in spring), PAHs (536±80 and 161±39 ngm-3), and hopanes (65±24 and 20±2.4 ngm-3) in the urban air are 1-2 orders of magnitude higher than those in the mountain aerosols and 2-3 orders of magnitude higher than those in the marine samples. Mass ratios of nalkanes, PAHs and hopanes clearly demonstrate coal-burning emissions as their major source. Size distributions of fossil fuel derived n-alkane, PAHs and hopanes were found to be unimodal in most cases, peaking at 0.7-1.1μm size. In contrast, plant wax derived n-alkanes presented a bimodal distribution with two peaks at the sizes of 0.7-1.1μm and >4.7μm in the summer mountain and spring marine samples. Among the three types of samples, geometric mean diameter (GMD) of the organics in fine mode (<2.1μm) was found to be smallest (av. 0.63μm in spring) for the urban samples and largest (1.01μm) for the marine samples, whereas the GMD in coarse mode (≥2.1μm) was found to be smallest (3.48μm) for the marine aerosols and largest (4.04μm) for the urban aerosols. The fine mode GMDs of the urban and mountain samples were larger in winter than in spring and summer. Moreover, GMDs of 3- and 4-ring PAHs were larger than those of 5- and 6-ring PAHs in the three types of atmospheres. Such differences in GMDs can be interpreted by the repartitioning of organic compounds and the coagulation and hygroscopic growth of particles during a long-range transport from the inland continent to the marine area, as well as the difference in their sources among the three regions. [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]

The ICTP regional climate model (RegCM3) coupled with a desert dust aerosol model is used to simulate the net radiative forcing (short-wave and long-wave) and related climate effects of dust aerosols over East Asia. Two sets of experiments are completed and intercompared, one without (Exp. 1) and one with (Exp. 2) the radiative effects of dust aerosols. The experiments encompass the main dust producing months, February through May, for 10 years (1997-2006), and the simulation results are evaluated against ground station and satellite data. The model captures the basic observed climatology over the area of interest. The spatial and temporal variations of near surface concentration, mass load, optical depth and emission of dust aerosols from the main source regions are reproduced by model. The main model deficiency is an overestimate of dust amounts over the source regions and an underestimate downwind of these source areas, which indicates an underestimate of dust dispersal. Over the desert source regions, the net TOA radiative forcing is positive, while it is small over the other regions as a result of high surface albedo values which reduce the shortwave radiative forcing. The net surface radiative fluxes are decreased by dust and this causes a surface cooling locally up to -1°C. The inclusion of net (short-wave and long-wave) dust radiative forcing leads to a reduction of dust emission in the East Asia source regions, which is mainly caused by an increase in local stability and a corresponding decrease in dust lifting. Our results indicate that dust effects should be included in the assessment of climate change over East Asia. [ABSTRACT FROM AUTHOR]

In this study, NO2 columns from the US EPA Models-3/CMAQ model simulations carried out using the 2001 ACE-ASIA (Asia Pacific Regional Aerosol Characterization Experiment) emission inventory over East Asia were compared with the GOME-derived NO2 columns. There were large discrepancies between the CMAQ-predicted and GOME-derived NO2 columns in the fall and winter seasons. In particular, while the CMAQ-predicted NO2 columns produced larger values than the GOME-derived NO2 columns over South Korea for all four seasons, the CMAQ-predicted NO2 columns produced smaller values than the GOME-derived NO2 columns over North China for all seasons with the exception of summer (summer anomaly). It is believed that there might be some error in the NOx emission estimates as well as uncertainty in the NOx chemical loss rates over North China and South Korea. Regarding the latter, this study further focused on the biogenic VOC (BVOC) emissions that were strongly coupled with NOx chemistry during summer in East Asia. This study also investigated whether the CMAQ-modeled NO2/NOx ratios with the possibly overestimated isoprene emissions were higher than those with reduced isoprene emissions. Although changes in both the NOx chemical loss rates and NO2/NOx ratios from CMAQ-modeling with the different isoprene emissions affected the CMAQ-modeled NO2 levels, the effects were found to be limited, mainly due to the low absolute levels of NO2 in summer. Seasonal variations of the NOx emission fluxes over East Asia were further investigated by a set of sensitivity runs of the CMAQ model. Although the results still exhibited the summer anomaly possibly due to the uncertainties in both NOx-related chemistry in the CMAQ model and the GOME measurements, it is believed that consideration of both the seasonal variations in NOx emissions and the correct BVOC emissions in East Asia are critical. Overall, it is estimated that the NOx emissions are underestimated by ∼57.3% in North China and overestimated by ∼46.1% in South Korea over an entire year. In order to confirm the uncertainty in NOx emissions, the NOx emissions over South Korea and China were further investigated using the ACEASIA, REAS (Regional Emission inventory in ASia), and CAPSS (Clean Air Policy Support System) emission inventories. The comparison between the CMAQ-calculated and GOME-derived NO2 columns indicated that both the ACEASIA and REAS inventories have some uncertainty in NOx emissions over North China and South Korea, which can also lead to some errors in modeling the formation of ozone and secondary aerosols in South Korea and North China. [ABSTRACT FROM AUTHOR]

The impact of the East Asia monsoon on the seasonal behavior of O3 in the boundary layer of Eastern China and the west Pacific region was analyzed for 2004-2006 by means of full-year nested chemical transport model simulations and continuous observational data obtained from three inland mountain sites in central and eastern China and three oceanic sites in the west Pacific region. The basic common features of O3 seasonal behaviors over all the monitoring sites are the pre- and post-monsoon peaks with a summer trough. Such bimodal seasonal patterns of O3 are predominant over the region with strong summer monsoon penetration, and become weaker or even disappear outside the monsoon region. The seasonal/geographical distribution of the pre-defined monsoon index indicated that the East Asia summer monsoon is responsible for the bimodal seasonal O3 pattern, and also partly account for the differences in the O3 seasonal variations between the inland mountain and oceanic sites. Over the inland mountain sites, the O3 concentration increased gradually from the beginning of the year, reached a maximum in June, decreased rapidly to the summer valley in July or August, and then peaked in September or October, thereafter decreased gradually again. Over the oceanic sites, O3 abundance showed a similar increasing trend beginning in January, but then decreased gradually from the end of March, followed by a wide trough with the minimum in July and August and a small peak in October or November. A sensitivity analysis performed by setting China-emission to zero revealed that the chemically produced O3 from China-emission contributed substantially to the O3 abundance, particularly the pre- and post-monsoon O3 peaks, over China mainland. We found that China-emission contributed more than 40% to total boundary layer O3 during summertime (60-70% in July) and accounted for about 40 ppb of each peak value over the inland region if without considering the effect of the nonlinear chemical productions. In contrast, over the oceanic region in the high monsoon index zone, the contribution of China-emission to total boundary layer O3 was always less than 20% (<10 ppb), and less than 10% in summer. [ABSTRACT FROM AUTHOR]

Simultaneous ground-based measurements of ozone (O3) and carbon monoxide (CO) were conducted in March 2005 as part of the East Asian Regional Experiment (EAREX) 2005 under the umbrella of the Atmospheric Brown Clouds (ABC) project. Multiple air quality monitoring networks were integrated by performing intercomparison of individual calibration standards and measurement techniques to ensure comparability of ambient measurements, along with providing consistently high time-resolution measurements of O3 and CO at the surface sites in East Asia. Ambient data collected from eight surface stations were compared with simulation results obtained by a regional chemistry transport model to infer recent changes in CO emissions from East Asia. Our inverse estimates of the CO emissions from China up to 2005 suggested an increase of 16% since 2001, in good agreement with the recent MOPITT satellite observations and the bottom-up estimates up to 2006. The O3 enhancement relative to CO in continental pollution plumes traversed in the boundary layer were examined as a function of transport time from the Asian continent to the western Pacific Ocean. The observed ΔO3/ΔCO ratios show increasing tendency during eastward transport events due likely to enroute photochemical O3 formation, suggesting that East Asia is an important O3 source region during spring. [ABSTRACT FROM AUTHOR]