Search

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

Reliable attribution of Asian summer monsoon variations to aerosol forcing is critical to reducing uncertainties in future projections of regional water availability, which is of utmost importance for risk management and adaptation planning in this densely populated region. Yet, simulating the monsoon remains a challenge for climate models that suffer from long-standing biases, undermining their reliability in attributing anthropogenically forced changes. We analyze a suite of climate model experiments to identify a link between model biases and monsoon responses to Asian aerosols and associated physical mechanisms, including the role of large-scale circulation changes. The aerosol impact on monsoon precipitation and circulation is strongly influenced by a model's ability to simulate the spatio-temporal variability in the climatological monsoon winds, clouds, and precipitation across Asia, which modulates the magnitude and efficacy of aerosol–cloud–precipitation interactions, an important component of the total aerosol response. There is a strong interplay between South Asia and East Asia monsoon precipitation biases and their relative predominance in driving the overall monsoon response. We found a striking contrast between the early- and late-summer aerosol-driven changes ascribable to opposite signs and seasonal evolution of the biases in the two regions. A realistic simulation of the evolution of the large-scale atmospheric circulation is crucial to realize the full extent of the aerosol impact over Asia. These findings provide important implications for better understanding and constraining the diversity and inconsistencies of model responses to aerosol changes over Asia in historical simulations and future projections. [ABSTRACT FROM AUTHOR]

Anthropogenic emissions of aerosols and precursor gases have changed significantly in the past few decades around the world. In this study, the Explicit Aerosol Source Tagging (EAST) system is merged into the Energy Exascale Earth System Model version 1 (E3SMv1) to quantify the variations in anthropogenic aerosol concentrations, source contributions, and their subsequent radiative impact in four major emission regions across the globe during 1850–1980, 1980–2010, and 2010–2017. In North America and Europe, changes in anthropogenic PM2.5 were mainly caused by changes in emissions from local energy and industrial sectors. The local industrial sector caused the largest increase in PM2.5 in East Asia during 1980–2010 and decrease during 2010–2017. In South Asia, the increase in energy-related emissions dominated the rise in PM2.5 levels during 1980–2017. During 1850–1980, the increases in emissions from North America contributed to the increase in the European PM2.5 burden by 1.7 mgm-2 and the sources from the Europe were also responsible for the PM2.5 burden increase in East Asia and South Asia by about 1.0 mgm-2. During 1980–2010, East Asia contributed to an increase of 0.4–0.6 mgm-2 in the PM2.5 burden in North America and Europe, while South Asia contributed about 0.3 mgm-2. During 2010–2017, the contributions from East Asia to the PM2.5 burdens in the North America, Europe, and South Asia declined by 0.3–0.6 mgm-2 due to the clean air actions in China, while the contributions from South Asia still increased due to the continuous increase in emissions in South Asia. The historical changes in aerosols had an impact on effective radiative forcing through aerosol–radiation interactions (ERFari). During 1980–2010, a decline in North American aerosols resulted in a positive ERFari change (warming effect) in Europe and a decline in aerosols in Europe caused a warming effect in Russia and northern China. The changes in ERFari from the increase and decrease in aerosols in China during 1980–2010 and 2010–2017, respectively, are comparable in magnitude. The continuous aerosol increases in South Asia from 1980 to 2017 resulted in negative ERFari (cooling) changes in South Asia, Southeast Asia, and southern China. [ABSTRACT FROM AUTHOR]

Organic aerosols from marine sources over the western Pacific Ocean of East Asia were investigated using an online coupled regional chemistry–climate model RIEMS-Chem for the entire year 2014. Model evaluation against a wide variety of observations from research cruises and in situ measurements demonstrated a good skill of the model in simulating temporal variation and spatial distribution of particulate matter with aerodynamic diameter less than 2.5 and 10 µm (PM 2.5 and PM 10), black carbon (BC), organic carbon (OC), sodium, and aerosol optical depth (AOD) in the marine atmosphere. The inclusion of marine organic aerosols improved model performance on OC concentration by reducing model biases of up to 20 %. The regional and annual mean near-surface marine organic aerosol (MOA) concentration was estimated to be 0.27 µgm-3 , with the maximum in spring and the minimum in winter, and contributed 26 % of the total organic aerosol concentration on average over the western Pacific. Marine primary organic aerosol (MPOA) accounted for the majority of marine organic aerosol (MOA) mass, and the MPOA concentration exhibited the maximum in autumn and the minimum in summer, whereas marine secondary organic aerosol (MSOA) was approximately 1–2 orders of magnitude lower than MPOA, having a distinct summer maximum and a winter minimum. MOA induced a direct radiative effect (DRE MOA) of - 0.27 Wm-2 and an indirect radiative effect (IRE MOA) of - 0.66 Wm-2 at the top of the atmosphere (TOA) in terms of annual and oceanic average over the western Pacific, with the highest seasonal mean IRE MOA up to - 0.94 Wm-2 in spring. IRE MOA was stronger than, but in a similar magnitude to, the IRE due to sea salt aerosol on average, and it was approximately 9 % of the IRE due to anthropogenic aerosols in terms of annual mean over the western Pacific. This ratio increased to 19 % in the northern parts of the western Pacific in autumn. This study reveals an important role of MOA in perturbing cloud properties and shortwave radiation fluxes in the western Pacific of East Asia. [ABSTRACT FROM AUTHOR]

Trace metals in aerosol particles impact Earth's radiative budget, human health, and ocean biogeochemistry. Semi-continuous measurements of the elemental composition of fine-mode (PM 2.5) aerosols were conducted using an automated X-ray fluorescence analyzer on a remote island of Japan during the spring of 2018. Temporal variations in mass concentrations of geochemically important elements for this period, such as Pb, Cu, Si, Fe, and Mn, and their relationships with the emission tracers, carbon monoxide (CO) and black carbon (BC), were reported. The Integrated Massively Parallel Atmospheric Chemical Transport (IMPACT) model was used to evaluate the source apportionment of these components and was evaluated in terms of emissions and wet removal processes. Pb and Cu originated mainly from anthropogenic sources (98 % and 93 % on average, respectively) over the East Asian continent. Positive correlations of Pb and Cu with BC and CO and the similarity of their concentration-weighted trajectories indicated that the emission sources of these metals share the region where the large CO (and BC) emission sources are located and that CO can be regarded as a tracer of continental anthropogenic emissions. The air masses with minimized impacts of the wet removal during transport were extracted to elucidate the "top-down" emission ratio of Pb and Cu to CO, which were, for the first time, evaluated as 152.7 and 63.1 µg g -1 , respectively, during the spring of 2018 in the East Asian outflow. The analysis of the tagged tracer simulations by the IMPACT model confirmed that BC and Si could be used as tracers for anthropogenic and dust emissions, respectively, during the observation period. The source apportionment of Fe and Mn in PM 2.5 aerosols was conducted using Si and BC tracers, which revealed that the anthropogenic contribution was 17 % and 44 % on average, respectively. Based on the air mass origins of Fe and Mn, their anthropogenic fraction varied from 2 % to 29 % and 9 % to 68 %, respectively, during the high-PM 2.5 -concentration periods. However, despite the non-dominant anthropogenic contributions of Fe, they could adversely affect human health and ocean biogeochemistry, owing to their higher water solubility. The modeled BC, Pb, Cu, and Fe were evaluated by separately diagnosing their emission and transport. Ratios of modeled to observed concentrations for these components were analyzed in terms of the accumulated precipitation along the transport from the East Asian continent. The current model simulations were found to overestimate the emissions (based on the Community Emissions Data System, CEDS v2021-02-05) of BC by 44 % and underestimate Cu by 45 %, anthropogenic Fe by 28 % in East Asia, and the wet deposition rates for BC and Pb. Overall, Cu in East Asia exhibited a different nature from BC and Pb in terms of emission sources and wet removal. [ABSTRACT FROM AUTHOR]

The atmospheric deposition of iron (Fe) promotes primary production in the surface ocean, which results in the enhanced uptake of carbon dioxide into surface seawater. Given that microorganisms in seawater utilize dissolved Fe (d-Fe) as a nutrient, the bioavailability of Fe in aerosol particles depends on its solubility. However, the factors controlling fractional Fe solubility (Fe sol %) in aerosol particles have not been fully understood. This study performed annual observations of the total and dissolved metal concentrations in size-fractionated (seven fractions) aerosol particles at Higashi-Hiroshima, Japan. The feasibility of the molar concentration ratio of d-Fe relative to dissolved Al ([d-Fe] / [d-Al]) as an indicator of sources of d-Fe in aerosol particles was investigated because this ratio is likely dependent on the emission sources of Fe (e.g., mineral dust, fly ash, and anthropogenic Fe oxides) and their dissolution processes (proton- and ligand-promoted dissolutions). Approximately 70 % of the total Fe in total suspended particulates (TSPs) was present in coarse aerosol particles, whereas about 70 % of d-Fe in TSPs was mainly found in fine aerosol particles. The average Fe sol % in fine aerosol particles (11.4 ± 7.0 %) was higher than that of coarse aerosol particles (2.19 ± 2.27 %). In addition, the average ratio of [d-Fe] / [d-Al] in coarse aerosol particles (0.408 ± 0.168) was lower than that in fine aerosol particles (1.15 ± 0.80). The range of [d-Fe] / [d-Al] ratios in the coarse aerosol particles (0.121–0.927) was similar to that obtained by proton-promoted dissolution of mineral dust (0.1–1.0), which indicates that the d-Fe in coarse aerosol particles was derived from mineral dust. The [d-Fe] / [d-Al] ratios of fine aerosol particles ranged from 0.386 to 4.67, and [d-Fe] / [d-Al] ratios greater than 1.50 cannot be explained by proton- and ligand-promoted dissolutions (1.00 < [d-Fe] / [d-Al] < 1.50). The [d-Fe] / [d-Al] ratio correlated with the enrichment factor of Fe in fine aerosol particles (r : 0.505), which indicates that anthropogenic Fe with a high [d-Fe] / [d-Al] ratio was the source of d-Fe in fine aerosol particles. The high [d-Fe] / [d-Al] ratio was attributed to anthropogenic Fe oxides emitted from high-temperature combustions. Finally, the fraction of anthropogenic Fe oxides to d-Fe in TSPs was calculated based on the [d-Fe] / [d-Al] ratio of aerosols and their emission source samples. As a result, the fraction of anthropogenic Fe oxides to d-Fe in TSPs varied from 1.48 % to 80.7 %. A high fraction was observed in summer when air masses originated from industrial regions in Japan. By contrast, approximately 10 % of d-Fe in the TSPs collected in spring and during Asian dust events was derived from anthropogenic Fe oxides when air masses were frequently transported from East Asia to the Pacific Ocean. Thus, mineral dust was the dominant source of d-Fe in Asian outflow to the Pacific Ocean. [ABSTRACT FROM AUTHOR]

We apply a local ensemble transform Kalman smoother (LETKS) in combination with the global aerosol–climate model ECHAM–HAM to estimate aerosol emissions from POLDER-3/PARASOL (POLarization and Directionality of the Earth's Reflectances) observations for the year 2006. We assimilate aerosol optical depth at 550 mnm (AOD550), the Ångström exponent at 550 and 865 nm (AE550–865), and single-scattering albedo at 550 nm (SSA550) in order to improve modeled aerosol mass, size and absorption simultaneously. The new global aerosol emissions increase to 1419 Tgyr-1 (+ 28 %) for dust, 1850 Tgyr-1 (+ 75 %) for sea salt, 215 Tgyr-1 (+ 143 %) for organic aerosol and 13.3 Tgyr-1 (+ 75 %) for black carbon, while the sulfur dioxide emissions increase to 198 Tgyr-1 (+ 42 %) and the total deposition of sulfates to 293 Tgyr-1 (+ 39 %). Organic and black carbon emissions are much higher than their prior values from bottom-up inventories, with a stronger increase in biomass burning sources (+ 193 % and + 90 %) than in anthropogenic sources (115 % and 70 %). The evaluation of the experiments with POLDER (assimilated) and AERONET as well as MODIS Dark Target (independent) observations shows a clear improvement compared with the ECHAM–HAM control run. Specifically based on AERONET, the global mean error in AOD550 improves from - 0.094 to - 0.006, while absorption aerosol optical depth at 550 nm (AAOD550) improves from - 0.009 to - 0.004 after the assimilation. A smaller improvement is also observed in the AE550–865 mean absolute error (from 0.428 to 0.393), with a considerably higher improvement over isolated island sites at the ocean. The new dust emissions are closer to the ensemble median of AEROCOM I, AEROCOM III and CMIP5 as well as some of the previous assimilation studies. The new sea salt emissions have become closer to the reported emissions from previous studies. Indications of a missing fraction of coarse dust and sea salt particles are discussed. The biomass burning changes (based on POLDER) can be used as alternative biomass burning scaling factors for the Global Fire Assimilation System (GFAS) inventory distinctively estimated for organic carbon (2.93) and black carbon (1.90) instead of the recommended scaling of 3.4 (Kaiser et al., 2012). The estimated emissions are highly sensitive to the relative humidity due to aerosol water uptake, especially in the case of sulfates. We found that ECHAM–HAM, like most of the global climate models (GCMs) that participated in AEROCOM and CMIP6, overestimated the relative humidity compared with ERA5 and as a result the water uptake by aerosols, assuming the kappa values are not underestimated. If we use the ERA5 relative humidity, sulfate emissions must be further increased, as modeled sulfate AOD is lowered. Specifically, over East Asia, the lower AOD can be attributed to the underestimated precipitation and the lack of simulated nitrates in the model. [ABSTRACT FROM AUTHOR]

As a natural aerosol with the largest emissions on land, dust has important impacts on the atmospheric environment and climate systems. Both the emissions and transport of dust aerosols are tightly connected to meteorological conditions and as a result are confronted with strong modulations by the changing climate. Here, we project the changes in the global dust emissions and loading by the end of the 21st century, using an ensemble of model outputs from the Coupled Model Intercomparison Project version 6 (CMIP6) under four Shared Socioeconomic Pathways (SSPs). Based on the validations against site-level observations, we select 9 out of 14 models and estimate an ensemble global dust emissions of 2566 ± 1996 Tga-1 (1 Tg = 10 12 g) for the present day, in which 68 % is dry deposited and 31 % is wet deposited. Compared to 2005–2014, global dust emissions show varied responses, with a reduction of - 5.6 ± 503 Tga-1 under the SSP3–7.0 scenario but increased emissions up to 60.7 ± 542 Tga-1 under the SSP5–8.5 scenario at 2090–2099. For all scenarios, the most significant increase in the dust emissions appears in North Africa (0.6 %–5.6 %) due to the combined effects of reduced precipitation but strengthened surface wind. In contrast, all scenarios show decreased emissions in the Taklimakan and Gobi deserts (- 0.8 % to - 11.9 %) because of the increased precipitation but decreased wind speed on a regional scale. The dust loading shows uniform increases over North Africa (1.6 %–13.5 %) and the downwind Atlantic, following the increased emissions but decreases over East Asia (- 1.3 % to - 10.5 %), and the downwind Pacific, partly due to enhanced local precipitation that promotes wet deposition. In total, global dust loading will increase by 2.0 %–12.5 % at the end of the 21st century under different climate scenarios, suggesting a likelihood of strengthened radiative and climatic perturbations by dust aerosols in a warmer climate. [ABSTRACT FROM AUTHOR]

The national and global restrictions in response to the COVID-19 pandemic led to a sudden, albeit temporary, emission reduction of many greenhouse gases (GHGs) and anthropogenic aerosols, whose near-term climate impact were previously found to be negligible when focusing on global- and/or annual-mean scales. Our study aims to investigate the monthly scale coupled climate-and-circulation response to regional, COVID-19-related aerosol emission reductions, using the output from 10 Earth system models participating in the Covid model intercomparison project (CovidMIP). We focus on January–February and March–May 2020, which represent the seasons of largest emission changes in sulfate (SO2) and black carbon (BC). During January–February (JF), a marked decrease in aerosol emissions over eastern China, the main emission region, resulted in a lower aerosol burden, leading to an increase in surface downwelling radiation and ensuing surface warming. Regional sea-level pressure and circulation adjustments drive a precipitation increase over the Maritime Continent, embedded in a negative Pacific Decadal Oscillation (PDO)- and/or El Niño–Southern Oscillation (ENSO)-like response over the Pacific, in turn associated with a northwestward displacement and zonal shrinking of the Indo-Pacific Walker cell. Remote climate anomalies across the Northern Hemisphere, including a weakening of the Siberian High and Aleutian Low, as well as anomalous temperature patterns in the northern mid-latitudes, arise primarily as a result of stationary Rossby wave trains generated over East Asia. The anomalous climate pattern and driving dynamical mechanism reverse polarity between JF and MAM (March–May) 2020, which is shown to be consistent with an underlying shift of the dominant region of SO2 emission reduction from eastern China in JF to India in MAM. Our findings highlight the prominent role of large-scale dynamical adjustments in generating a hemispheric-wide aerosol climate imprint even on short timescales, which are largely consistent with longer-term (decadal) trends. Furthermore, our analysis shows the sensitivity of the climate response to the geographical location of the aerosol emission region, even after relatively small, but abrupt, emission changes. Scientific advances in understanding the climate impact of regional aerosol perturbations, especially the rapidly evolving emissions over China and India, are critically needed to reduce current uncertainties in near-future climate projections and to develop scientifically informed hazard mitigation and adaptation policies. [ABSTRACT FROM AUTHOR]

With high emissions of aerosols and the known world's "Third Pole" of the Tibet Plateau (TP) in East Asia, knowledge on the energy budget over this region has been widely concerned. This study first attempts to estimate the present-day land energy balance over East Asia by combining surface and satellite observations as well as the atmospheric reanalysis and Coupled Model Intercomparison Project Phase 6 (CMIP6) simulations. Compared to the global land budget, a substantially larger fraction of atmospheric shortwave radiation of 5.2 % is reflected, highly associated with the higher aerosol loadings and more clouds over East Asian land. While a slightly smaller fraction of atmospheric shortwave absorption of 0.6 % is unexpectedly estimated, possibly related to the lower water vapor content effects due to the thinner air over the TP to overcompensate for the aerosol and cloud effects over East Asian land. The weaker greenhouse effect and fewer low clouds due to the TP are very likely the causes of the smaller fraction of East Asian land surface downward longwave radiation. Hence, high aerosol loadings, clouds, and the TP over East Asia play vital roles in the shortwave budgets, while the TP is responsible for the longwave budgets during this regional energy budget assessment. The further obtained cloud radiative effects suggest that the presence of clouds results in a larger cooling effect on the climate system over East Asian land than that over the globe. This study provides a perspective to understand fully the roles of potential factors in influencing the different energy budget assessments over regions. [ABSTRACT FROM AUTHOR]

This study examines the role played by aerosols which act as cloud condensation nuclei (CCN) in the development of clouds and precipitation in two metropolitan areas in East Asia that have experienced substantial increases in aerosol concentrations over the last decades. These two areas are the Seoul and Beijing areas and the examination was done by performing simulations using the Advanced Research Weather Research and Forecasting model as a cloud system resolving model. The CCN are advected from the continent to the Seoul area and this increases aerosol concentrations in the Seoul area. These increased CCN concentrations induce the enhancement of condensation that in turn induces the enhancement of deposition and precipitation amount in a system of less deep convective clouds as compared to those in the Beijing area. In a system of deeper clouds in the Beijing area, increasing CCN concentrations also enhance condensation but reduce deposition. This leads to negligible CCN-induced changes in the precipitation amount. Also, in the system there is a competition for convective energy among clouds with different condensation and updrafts. This competition results in different responses to increasing CCN concentrations among different types of precipitation, which are light, medium and heavy precipitation in the Beijing area. The CCN-induced changes in freezing play a negligible role in CCN-precipitation interactions as compared to the role played by CCN-induced changes in condensation and deposition in both areas. [ABSTRACT FROM AUTHOR]

We used the EMEP MSC-W (European Monitoring and Evaluation Programme Meteorological Synthesizing Centre – West) model version 4.34 coupled with WRF (Weather Research and Forecasting) model version 4.2.2 meteorology to undertake a present-day (2015) global and regional quantification of the concentrations, deposition, budgets, and lifetimes of atmospheric reactive N (N r) and S (S r) species. These are quantities that cannot be derived from measurements alone. In areas with high levels of reduced N r (RDN = NH 3+ NH 4+), oxidized N r (OXN = NO x+ HNO 3+ HONO + N 2 O 5 + NO 3-+ "Other OXN" species), and oxidized S r (OXS = SO 2+ SO 42-), RDN is predominantly in the form of NH 3 (NH 4+ typically <20 %), OXN has majority gaseous species composition, and OXS predominantly comprises SO 42- except near major SO 2 sources. Most continental regions are now "ammonia rich", more so than previously, which indicates that, although reducing NH 3 emissions will decrease the RDN concentration, decreasing these emissions will have little effect on mitigating secondary inorganic aerosol (SIA). South Asia is the most ammonia-rich region. Coastal areas around East Asia, northern Europe, and the north-eastern United States are "nitrate rich" where NH 4 NO 3 formation is limited by NH 3. These locations experience transport of OXN from the adjacent continent and/or direct shipping emissions of NO x , but NH 3 concentrations are lower. The least populated continental areas and most marine areas are "sulfate rich". Deposition of OXN (57.9 TgN yr -1 , 51 %) and RDN (55.5 TgN yr -1 , 49 %) contribute almost equally to total nitrogen deposition. OXS deposition is 50.5 TgS yr -1. Globally, wet and dry deposition contribute similarly to RDN deposition; for OXN and OXS, wet deposition contributes slightly more. Dry deposition of NH 3 is the largest contributor to RDN deposition in most regions except for the Rest of Asia area and marine sectors where NH 3 emissions are small and RDN deposition is mainly determined by the transport and rainout of NH 4+ (rather than rainout of gaseous NH 3). Thus, reductions in NH 3 would efficiently reduce the deposition of RDN in most continental regions. The two largest contributors to OXN deposition in all regions are HNO 3 and coarse NO 3- (via both wet and dry deposition). The deposition of fine NO 3- is only important over East Asia. The tropospheric burden of RDN is 0.75 TgN, of which NH 3 and NH 4+ comprise 32 % (0.24 TgN; lifetime of 1.6 d) and 68 % (0.51 TgN; lifetime of 8.9 d) respectively. The lifetime of RDN (4.9–5.2 d) is shorter than that of OXN (7.6–7.7 d), which is consistent with a total OXN burden (1.20 TgN) almost double that of RDN. The tropospheric burden of OXS is 0.78 TgS with a lifetime of 5.6–5.9 d. Total nitrate burden is 0.58 TgN with fine NO 3- only constituting 10 % of this total, although fine NO 3- dominates in eastern China, Europe, and eastern North America. It is important to account for contributions of coarse nitrate to global nitrate budgets. Lifetimes of RDN, OXN, and OXS species vary by a factor of 4 across different continental regions. In East Asia, lifetimes for RDN (2.9–3.0 d), OXN (3.9–4.5 d), and OXS (3.4–3.7 d) are short, whereas lifetimes in the Rest of Asia and Africa regions are about twice as long. South Asia is the largest net exporter of RDN (2.21 TgN yr -1 , 29 % of its annual emission), followed by the Euro_Medi region. Despite having the largest RDN emissions and deposition, East Asia has only small net export and is therefore largely responsible for its own RDN pollution. Africa is the largest net exporter of OXN (1.92 TgN yr -1 , 22 %), followed by Euro_Medi (1.61 TgN yr -1 , 26 %). Considerable marine anthropogenic N r and S r pollution is revealed by the large net import of RDN, OXN, and OXS to these areas. Our work demonstrates the substantial regional variation in N r and S r budgets and the need for modelling to simulate the chemical and meteorological linkages underpinning atmospheric responses to precursor emissions. [ABSTRACT FROM AUTHOR]

The Asian summer monsoon is an effective pathway for aerosol particles and precursors from the planetary boundary layer over Central, South, and East Asia into the upper troposphere and lower stratosphere. An enhancement of aerosol particles within the Asian monsoon anticyclone (AMA), called the Asian tropopause aerosol layer (ATAL), has been observed by satellites. We discuss airborne in situ and remote sensing observations of aerosol microphysical properties conducted during the 2017 StratoClim field campaign within the AMA region. The aerosol particle measurements aboard the high-altitude research aircraft M55 Geophysica (maximum altitude reached of ∼20.5 km) were conducted with a modified ultra-high-sensitivity aerosol spectrometer – airborne (UHSAS-A; particle diameter detection range of 65 nm to 1 µm), the COndensation PArticle counting System (COPAS, detecting total concentrations of submicrometer-sized particles), and the New Ice eXpEriment – Cloud and Aerosol Spectrometer with Detection of POLarization (NIXE-CAS-DPOL). In the COPAS and UHSAS-A vertical particle mixing ratio (PMR) profiles and the size distribution profiles (for number, surface area, and volume concentration), the ATAL is evident as a distinct layer between ∼370 and 420 K potential temperature (Θ). Within the ATAL, the maximum detected PMRs (from the median profiles) were ∼700 mg-1 for particle diameters between 65 nm and 1 µm (UHSAS-A) and higher than 2500 mg-1 for diameters larger than 10 nm (COPAS). These values are up to 2 times higher than those previously found at similar altitudes in other tropical locations. The difference between the PMR profiles measured by the UHSAS-A and the COPAS indicate that the region below the ATAL at Θ levels from 350 to 370 K is influenced by the nucleation of aerosol particles (diameter <65 nm). We provide detailed analyses of the vertical distribution of the aerosol particle size distributions and the PMR and compare these with previous tropical and extratropical measurements. The backscatter ratio (BR) was calculated based on the aerosol particle size distributions measured in situ. The resulting data set was compared with the vertical profiles of the BR detected by the multiwavelength aerosol scatterometer (MAS) and an airborne miniature aerosol lidar (MAL) aboard the M55 Geophysica and by the satellite-borne Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP). The data of all four methods largely agree with one another, showing enhanced BR values in the altitude range of the ATAL (between ∼15 and 18.5 km) with a maximum at 17.5 km altitude. By means of the AMA-centered equivalent latitude calculated from meteorological reanalysis data, it is shown that such enhanced values of the BR larger than 1.1 could only be observed within the confinement of the AMA. [ABSTRACT FROM AUTHOR]

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]

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]

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]

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]

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]

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]

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]

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 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]

CUACE/Dust, an operational mesoscale sand and dust storm (SDS) forecasting system for East Asia, has been developed by online coupling a dust aerosol emission scheme and dust aerosol microphysics onto a regional meteorological model with improved advection and diffusion schemes and a detailed Northeast Asia soil erosion database. With improved initial dust aerosol conditions through a 3-DVar data assimilation system, CUACE/Dust successfully forecasted most of the 31 SDS processes in East Asia. A detailed comparison of the model predictions for the 8-12 March SDS process with surface network observations and lidar measurements revealed a robust forecasting ability of the system. The time series of the operationally forecasted dust concentrations for a number of representative stations for the whole spring 2006 (1 March-31 May) were evaluated against surface PM10 monitoring data, showing a good agreement in terms of the SDS timing and magnitudes at and near the source regions where dust aerosols dominate. For the operational forecasts of spring 2006 in East Asia, a TS (threat score) system evaluated the performance of CUACE/Dust against all available observations and rendered a spring averaged TS value of 0.31 for FT1 (24 h forecasts), 0.23 for FT2 (48 h forecasts) and 0.21 for FT3 (72 h forecasts). [ABSTRACT FROM AUTHOR]