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Improving the accuracy of regional aerosol climate impact assessment calls for improvement in the accuracy of regional aerosol radiative effect (ARE) estimation. One of the most important means of achieving this is to use spatially homogeneous and temporally continuous datasets of critical aerosol properties, such as spectral aerosol optical depth (AOD) and single scattering albedo (SSA), which are the most important parameters for estimating aerosol radiative effects. However, observations do not provide the above; the space-borne observations though provide wide spatial coverage, are temporal snapshots and suffer from possible sensor degradation over extended periods. On the other hand, the ground-based measurements provide more accurate and temporally continuous data but are spatially near-point observations. Realizing the need for spatially homogeneous and temporally continuous datasets on one hand and the near non-existence of such data over the south Asian region (which is one of the regions where aerosols show large heterogeneity in most of their properties), construction of accurate gridded aerosol products by synthesizing the long-term space-borne and ground-based data has been taken up as an important objective of the South West Asian Aerosol Monsoon Interactions (SWAAMI), a joint Indo-UK field campaign, aiming at characterizing aerosol–monsoon links and their variabilities over the Indian region. In Part 1 of this two-part paper, we present spatially homogeneous gridded datasets of AOD and absorption aerosol optical depth (AAOD), generated for the first time over this region. These data products are developed by merging the highly accurate aerosol measurements from the dense networks of 44 (for AOD) and 34 (for AAOD) ground-based observatories of Aerosol Radiative Forcing over India NETwork (ARFINET) and AErosol RObotic NETwork (AERONET) spread across the Indian region, with satellite-retrieved AOD and AAOD, following statistical assimilation schemes. The satellite data used for AOD assimilation include AODs retrieved from MODerate Imaging Spectroradiometer (MODIS) and Multiangle Imaging SpectroRadiometer (MISR) over the same domain. For AAOD, the ground-based black carbon (BC) mass concentration measurements from the network of 34 ARFINET observatories and satellite-based (Kalpana-1, INSAT-3A) infrared (IR) radiance measurements are blended with gridded AAODs (500 nm, monthly mean) derived from Ozone Monitoring Instrument (OMI)-retrieved AAODs (at 354 and 388 nm). The details of the assimilation methods and the gridded datasets generated are presented in this paper. The merged gridded AOD and AAOD products thus generated are validated against the data from independent ground-based observatories, which were not used for the assimilation process but are representative of different subregions of the complex domain. This validation exercise revealed that the independent ground-based measurements are better confirmed by merged datasets than the respective satellite products. As ensured by assimilation techniques employed, the uncertainties in merged AODs and AAODs are significantly less than those in corresponding satellite products. These merged products also all exhibit important large-scale spatial and temporal features which are already reported for this region. Nonetheless, the merged AODs and AAODs are significantly different in magnitude from the respective satellite products. On the background of above-mentioned quality enhancements demonstrated by merged products, we have employed them for deriving the columnar SSA and analysed its spatiotemporal characteristics. The columnar SSA thus derived has demonstrated distinct seasonal variation over various representative subregions of the study domain. The uncertainties in the derived SSA are observed to be substantially less than those in OMI SSA. On the backdrop of these benefits, the merged datasets are employed for the estimation of regional aerosol radiative effects (direct), the results of which would be presented in a companion paper, Part 2 of this two-part paper. [ABSTRACT FROM AUTHOR]

Satellite-based aerosol optical depth (AOD) is columnar light extinction by aerosol absorption and scattering and has become the most important variable for the assessment of the spatiotemporal distribution of aerosols at a regional and global level. In this paper, we have used AOD observations of multiangle imaging spectroradiometer (MISR) from September 2002 to May 2017, moderate resolution imaging spectroradiometer (MODIS) from September 2002 to December 2020, and sea-viewing wide field-of-view sensor (SeaWiFS) from September 2002 to December 2010 over South Asia. We have observed the association of AOD with enhanced vegetation index (EVI) and meteorological variables (temperature (TEMP), wind speed (WS), and relative humidity (RH)) acquired from Giovanni during the period September 2002–December 2020. The satellite observations of Terra-, MISR-, and SeaWiFS-AOD were also compared with Aqua-AOD. The findings show that AOD in eastern Pakistan is higher than in the western Pakistan due to increase in population density and biomass burning. Mean annual peak AOD (˃ 0.7) has been observed over the IGB region because of the significant increase in economical, industrial, and agricultural activities while AOD of ˃ 0.6 is observed over Bangladesh. The lowest mean annual AOD of ˂ 0.3 is observed over northeastern Afghanistan, western Nepal, and Bhutan whereas the AOD of 0.3 is seen over Sri Lanka. The highest seasonal mean AOD of 0.8 has been seen over Bihar, India, and AOD of ~ 0.7 is observed over Bangladesh while the lowest AOD is observed over Afghanistan, Sri Lanka, Nepal, and Bhutan during the winter season. However, the mean AOD over eastern Pakistan is maximum in both monsoon and post-monsoon season but relatively low in pre-monsoon and winter. The highest positive seasonal AOD anomalies were observed over South Asia in winter season followed by post-monsoon, pre-monsoon, and least being monsoon. The higher mean AOD anomaly value is found to be 0.2 over eastern Pakistan and western India. In northeastern Pakistan and central India, AOD and RH are positively correlated (r ˃ 0.54) while negatively correlated over Afghanistan, southwestern region of Pakistan, eastern India, Nepal, Bhutan, and Bangladesh. AOD is negatively correlated (r = ~ − 0.3) with EVI over eastern Pakistan and western India. The highest correlation coefficient (r) obtained among Terra and Aqua is 0.97, MISR and Aqua is 0.93, and SeaWiFS and Aqua is 0.58 over South Asia. [ABSTRACT FROM AUTHOR]

Clear-sky, direct shortwave aerosol radiative forcing (ARF) has been estimated over the Indian region, for the first time employing multi-year (2009–2013) gridded, assimilated aerosol products, as an important part of the South West Asian Aerosol Monsoon Interactions (SWAAMI) which is a joint Indo-UK research field campaign focused at understanding the variabilities in atmospheric aerosols and their interactions with the Indian summer monsoon. The aerosol datasets have been constructed following statistical assimilation of concurrent data from a dense network of ground-based observatories and multi-satellite products, as described in Part 1 of this two-part paper. The ARF, thus estimated, is assessed for its superiority or otherwise over other ARF estimates based on satellite-retrieved aerosol products, over the Indian region, by comparing the radiative fluxes (upward) at the top of the atmosphere (TOA) estimated using assimilated and satellite products with spatiotemporally matched radiative flux values provided by CERES (Clouds and Earth's Radiant Energy System) single-scan footprint (SSF) product. This clearly demonstrated improved accuracy of the forcing estimates using the assimilated vis-à-vis satellite-based aerosol datasets at regional, subregional and seasonal scales. The regional distribution of diurnally averaged ARF estimates has revealed (a) significant differences from similar estimates made using currently available satellite data, not only in terms of magnitude but also the sign of TOA forcing; (b) the largest magnitudes of surface cooling and atmospheric warming over the Indo-Gangetic Plain (IGP) and arid regions from north-western India; and (c) negative TOA forcing over most parts of the Indian region, except for three subregions – the IGP, north-western India and eastern parts of peninsular India where the TOA forcing changes to positive during pre-monsoon season. Aerosol-induced atmospheric warming rates, estimated using the assimilated data, demonstrate substantial spatial heterogeneities (∼0.2 to 2.0 K d -1) over the study domain with the IGP demonstrating relatively stronger atmospheric heating rates (∼0.6 to 2.0 K d -1). There exists a strong seasonality as well, with atmospheric warming being highest during pre-monsoon and lowest during winter seasons. It is to be noted that the present ARF estimates demonstrate substantially smaller uncertainties than their satellite counterparts, which is a natural consequence of reduced uncertainties in assimilated vis-à-vis satellite aerosol properties. The results demonstrate the potential application of the assimilated datasets and ARF estimates for improving accuracies of climate impact assessments at regional and subregional scales. [ABSTRACT FROM AUTHOR]

The paper investigates the physical phenomena that govern raindrop size distribution and cloud characteristics across the diverse climatic regions of the Indian subcontinent. The study focuses on four locations, Kolkata, Bhopal, Desalpar, and Kavaratti Island, during the monsoon period from 2014 to 2016. It employs various techniques, encompassing ground-based measurements from disdrometers, space-borne observations from MODIS, along with the Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model, MEERA-2, and ERA-5 reanalysis outputs. The study found that there is a predominance of larger raindrops in Kolkata and Kavaratti Island during the monsoon season. This is due to the high atmospheric instability in these regions, which is expressed through convective available potential energy (CAPE). Locations with noticeable diurnal CAPE variations also exert influence over rainfall rates and the occurrence of raindrop sizes at different times throughout the day. Airflow patterns combined with anthropogenic activities affect aerosol levels in India. Bhopal and Desalpar have high dust levels during monsoon due to airflow from desert regions. In urban centers with significant anthropogenic activity, such as Kolkata and Bhopal, sulfate aerosols dominate, while Desalpar and Kavaratti Islands are characterized by a greater prevalence of sea salt aerosols. The dominance of different aerosol types impacted the cloud features, and, as a result, the occurrence of mean raindrop sizes at the four locations. The investigation also found that regions characterized by the predominance of larger raindrops during the monsoon season exhibit a lower cloud-effective radius normalized by the liquid water path. The variability of the raindrop size distribution impacts the empirical relationships between radar reflectivity (Z) and rain rate (R) , as well as between mass-weighted mean drop diameter (D m) and R , over the four locations. The study emphasizes the importance of considering varying Z-R relationships for accurate estimation of rain rates from radar reflectivity measurements in different climatic regions. • Varied rain microstructure observed over the different geographical locations of the Indian subcontinent. • Drop size occurrence probability is controlled by the prevailing CAPE. • CER/LWP ratio is inversely related to mean drop size. • The aerosol types influence the cloud features and as a result the prevailing DSD in a region. • The aerosol environment is controlled by the airflow pattern, geographical location, and anthropogenic activities. [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]

Evapotranspiration (ET) accounts for over half of the moisture source of Asian monsoon rainfall, which has been significantly altered by anthropogenic forcings. However, how individual anthropogenic forcing affects the ET over monsoonal Asia is still elusive. In this study, we found a significant decline in ET over the Asian monsoon region during the period of 1950–2014 in Coupled Model Intercomparison Project Phase 6 (CMIP6) models. The attribution analysis suggests that anthropogenic aerosol forcing is the primary cause of the weakening in ET in the historical simulation, while it is only partially compensated by the strengthening effect from GHGs, although GHGs are the dominant forcings for surface temperature increase. The physical mechanisms responsible for ET changes are different between aerosol and GHG forcings. The increase in aerosol emissions enhances the reflection and scattering of the downward solar radiation, which decreases the net surface irradiance for ET. GHGs, on the one hand, increase the moisture capability of the atmosphere and, thus, the ensuing rainfall; on the other hand, they increase the ascending motion over the Indian subcontinent, leading to an increase in rainfall. Both processes are beneficial for an ET increase. The results from this study suggest that future changes in the land–water cycle may mainly rely on the aerosol emission policy rather than the carbon reduction policy. [ABSTRACT FROM AUTHOR]

The large-scale convection during the Asian summer monsoon plays an important role in the rapid transport of boundary layer aerosols into the Asian summer monsoon anticyclone. Here, using the state-of-the-art ECHAM6–HAMMOZ aerosol-chemistry-climate model, we show that these aerosols are further transported to the Arctic along isentropic surfaces by the Brewer-Dobson-Circulation (BDC) during the monsoon season. Our model simulations show that East and South Asian anthropogenic emissions contribute significantly to the aerosol transported to the Arctic, which causes a higher negative net aerosol radiative forcing at the surface (dimming) of −0.09 ± 0.02 Wm−2 and −0.07 ± 0.02 Wm−2, respectively. Over the Arctic, the East Asian anthropogenic aerosols that include large amounts of sulfate cause a seasonal mean net radiative forcing at the top of the atmosphere (TOA) of −0.003 ± 0.001Wm−2 and a surface cooling of −0.56 K while the black carbon dominated aerosol from South Asia shows a positive TOA forcing of +0.004 ± 0.001Wm−2 with an only minor surface cooling of −0.043 K. Overall, the long-range transport of South Asian aerosols results in a notably warming throughout the atmospheric column but minimal temperature response at the Arctic surface. Conversely, East Asian aerosols cool the troposphere and heat the lower stratosphere in the Arctic. The Asian aerosol thus plays an ambivalent role, with the East Asian sources in particular having the potential to counteract the rapid rise in Arctic temperatures and the associated melting of snow and ice. [ABSTRACT FROM AUTHOR]

Aerosol particles with diameters larger than 40 nm were collected during the flight campaign StratoClim 2017 within the Asian tropopause aerosol layer (ATAL) of the 2017 monsoon anticyclone above the Indian subcontinent. A multi-impactor system was installed on board the aircraft M-55 Geophysica, which was operated from Kathmandu, Nepal. The size and chemical composition of more than 5000 refractory particles/inclusions of 17 selected particle samples from seven different flights were analyzed by use of scanning electron microscopy (SEM) and transmission electron microscopy (TEM) combined with energy dispersive X-ray (EDX) microanalysis. Based on chemical composition and morphology, the refractory particles were assigned to the following particle groups: extraterrestrial, silicates, Fe-rich, Al-rich, Hg-rich, other metals, C-rich, soot, Cl-rich, and Ca-rich. Most abundant particle groups within the refractory particles are silicates and C-rich (non-volatile organics). In samples taken above the tropopause, extraterrestrial particles are becoming increasingly important with rising altitude. The most frequent particle sources for the small (maximum in size distribution DP-max=120 nm) refractory particles carried into the ATAL are combustion processes at the ground (burning of fossil fuels/biomass burning) and the agitation of soil material. The refractory particles in the ATAL represent only a very small fraction (< 2 % by number for particles > 40 nm) of the total aerosol particles, which are dominated by species like ammonium, sulfate, nitrate, and volatile organics. During one flight, a large number of very small (DP-max=25 nm) cinnabar particles (HgS) were detected, which are supposed to originate from a ground source such as coal combustion or underground coal fires. [ABSTRACT FROM AUTHOR]

Dust loading in West and South Asia has been a major environmental issue due to its negative effects on air quality, food security, energy supply and public health, as well as on regional and global weather and climate. Yet a robust understanding of its recent changes and future projection remains unclear. On the basis of several high-quality remote sensing products, we detect a consistently decreasing trend of dust loading in West and South Asia over the last two decades. In contrast to previous studies emphasizing the role of local land use changes, here, we attribute the regional dust decline to the continuous intensification of Arctic amplification driven by anthropogenic global warming. Arctic amplification results in anomalous mid-latitude atmospheric circulation, particularly a deepened trough stretching from West Siberia to Northeast India, which inhibits both dust emissions and their downstream transports. Large ensemble climate model simulations further support the dominant role of greenhouse gases induced Arctic amplification in modulating dust loading over West and South Asia. Future projections under different emission scenarios imply potential adverse effects of carbon neutrality in leading to higher regional dust loading and thus highlight the importance of stronger anti-desertification counter-actions such as reforestation and irrigation management. [ABSTRACT FROM AUTHOR]

The Asian tropopause aerosol layer (ATAL) is present during the Asian summer monsoon season affecting the radiative balance of the atmosphere. However, the source regions and transport pathways of ATAL particles are still uncertain. Here, we investigate transport pathways from different regions at the model boundary layer (MBL) to the ATAL by combining two Lagrangian transport models (CLaMS, Chemical Lagrangian Model of the Stratosphere; MPTRAC, Massive-Parallel Trajectory Calculations) with balloon-borne measurements of the ATAL performed by the Compact Optical Backscatter Aerosol Detector (COBALD) above Nainital (India) in August 2016. Trajectories are initialised at the measured location of the ATAL and calculated 90 d backwards in time to investigate the relation between the measured, daily averaged, aerosol backscatter ratio and source regions at the MBL. Different simulation scenarios are performed to find differences and robust patterns when the reanalysis data (ERA5 or ERA-Interim), the trajectory model, the vertical coordinate (kinematic and diabatic approach) or the convective parameterisation are varied. The robust finding among all scenarios is that the largest continental air mass contributions originate from the Tibetan Plateau and the Indian subcontinent (mostly the Indo-Gangetic Plain), and the largest maritime air mass contributions in Asia come from the western Pacific (e.g. related to tropical cyclones). Additionally, all simulation scenarios indicate that the transport of maritime air from the tropical western Pacific to the region of the ATAL lowers the backscatter ratio (BSR) of the ATAL, while most scenarios indicate that the transport of polluted air from the Indo-Gangetic Plain increases the BSR. While the results corroborate key findings from previous ERA-Interim-based studies, they also highlight the variability in the contributions of different MBL regions to the ATAL depending on different simulation scenarios. [ABSTRACT FROM AUTHOR]

Emissions from South Asia (SA) represent a critical source of aerosols on the Tibetan Plateau (TP), and aerosols can significantly reduce the surface solar energy. To enhance the precision of aerosol forecasting and its radiative effects in SA and the TP, we employed a four-dimensional local ensemble transform Kalman filter (4D-LETKF) aerosol data assimilation (DA) system. This system was utilized to assimilate Himawari-8 aerosol optical thickness (AOT) into the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) to depict one SA air pollution outbreak event in spring 2018. Sensitivity tests for the assimilation system were conducted first to tune temporal localization lengths. Comparisons with independent Moderate Resolution Imaging Spectroradiometer (MODIS) and AErosol RObotic NETwork (AERONET) observations demonstrate that the AOT analysis and forecast fields have more reasonable diurnal variations by assimilating all the observations within a 12 h window, which are both better than assimilating the hourly observations in the current assimilation time slot. Assimilation of the entire window of observations with aerosol radiative effect activation significantly improves the prediction of downward solar radiation compared to the free-run experiment. The AOT assimilation with aerosol radiative effect activation led to a reduction in aerosol concentrations over SA, resulting in increased surface radiation, temperature, boundary layer height, and atmospheric instability. These changes facilitated air uplift, promoting aerosol transport from SA to the southeastern TP and leading to an increase in AOT in this region. [ABSTRACT FROM AUTHOR]

Anthropogenic aerosols play a major role for the Earth-Atmosphere system by influencing the Earth's radiative budget and climate. The effect of the perturbation induced by changes in anthropogenic aerosols on the Earth's energy balance is quantified in terms of the effective radiative forcing (ERF) which is the recommended metric for perturbations affecting the Earth's top-of-atmosphere energy budget since it is a better way to link this perturbation to subsequent global mean surface temperature change. In this work, the present-day ERF of anthropogenic aerosols is quantified using simulations from Earth system models (ESMs) participating in the Coupled Model Intercomparison Project Phase 6 (CMIP6). The ERFs of individual aerosol species, such as sulphates, organic carbon (OC), and black carbon (BC) are calculated along with the ERF due to all anthropogenic aerosols and the transient ERF over the historical period (1850–2014). Additionally, ERF is analyzed into three components: (a) ERFARI, representing aerosol-radiation interactions, (b) ERFACI, accounting for aerosol-cloud interactions, and (c) ERFALB, which is mainly due to the contribution of surface albedo changes caused by anthropogenic aerosols. Here, the total anthropogenic aerosol ERF (calculated using the piClim-aer experiment) is estimated to be -1.11 ± 0.26 W m-2, mostly due to the large contribution of ERFACI (-1.14 ± 0.33 W m-2), compared to ERFARI (-0.02 ± 0.20 W m-2) and ERFALB (0.05 ± 0.07 W m-2). The total ERF caused by sulphates (piClim-SO2) is estimated at -1.11 ± 0.31 W m-2, the OC ERF (piClim-OC) is -0.35 ± 0.21 W m-2, whereas the ERF exerted by BC (piClim-BC) is 0.19 ± 0.18 W m-2. On top of that, our analysis reveals that ERFACI clearly prevails over the largest part of the Earth except for the BC experiment where ERFARI prevails over land. By the end of the historical period (1995–2014), the global mean total aerosol ERF is estimated at -1.28 ± 0.37 W m-2 (calculated using the histSST experiment). We find that sulphates dominate both present-day and transient ERF spatial patterns at the top of the atmosphere, exerting a strongly negative ERF especially over industrialized regions of the Northern Hemisphere, such as North America, Europe, East and South Asia. Since the mid-1980s ERF has become less negative over Eastern North America and Western and Central Europe, while over East and South Asia there is a steady increase in ERF magnitude towards more negative values until 2014. [ABSTRACT FROM AUTHOR]

Abstract As an important part of the anthropogenic aerosol, Black Carbon (BC) aerosols in the atmospheric environment have strong impacts on climate change. Recently, most remote sensing studies on aerosol components detection are limited to the inversion of aerosol optical properties, integration of chemistry models or in situ observations. In this paper, an algorithm based on Effective Medium Approximations (EMA) and statistically optimized aerosol inversion algorithm was integrated for retrieving the surface mass concentration of BC aerosols from satellite signals. The sensitivity analyses for the developed forward model proved that the volume fraction of vertical BC is sensitive to the satellite observations and significantly improved especially over bright surface targets or under polluted atmospheric conditions. By updating the forward model and retrieved parameters of the statistically optimized inversion algorithm, three cases of high aerosol loading days were retrieved from Polarization and Anisotropy of Reflectance for Atmospheric Sciences Coupled with Observations from a LiDAR (PARASOL) measurements, which shows a significant ability of BC aerosol detection. Additionally, the validation and closure studies of BC concentration retrievals also indicates an encouraging consistency with correlation (R) of 0.71, mean bias of 3.55, and root-mean-square error (RMSE) of 3.75 when compared against the in-situ observations over South Asia. The accuracy of the retrievals also demonstrates different trends under different levels of aerosol loadings, which shows a higher accuracy in biomass burning seasons (R = 0.75, RMSE = 4.04, Bias = 3.27) while exaggerates the results in the case of clear conditions (R = 0.47, RMSE = 4.83, Bias = 4.00). Finally, the uncertainties of three assumptions, including proposing uniform vertical profile for BC, neglecting light-absorbing aerosols and using spherical EMA models were discussed in our manuscript. The maximum standard deviations caused by these uncertainties on low BC aerosol volume fractions (f BC < 1%) are 0.8%, 0.35% and 0.2% while these deviations will change to 0.25%, 0.05% and 1.5% respectively under higher BC fractions (f BC > 5%). This conclusion confirmed that the proposed algorithm for BC surface concentration retrieval extends the application of satellite remote sensing in monitoring the extreme biomass burning pollution. Highlights • Satellite based BC surface concentration retrieval algorithm was developed. • Detailed sensitivities of integral forward modules of EMA and RTM were proposed. • Global high aerosol loads cases and closure validation studies of BC were tested. • Detailed uncertainties of expected assumptions in retrieval were analyzed. [ABSTRACT FROM AUTHOR]

Light-absorbing Brown Carbon (BrC) aerosols partially offset the overall climate-cooling of aerosols. However, the evolution of BrC light-absorption during atmospheric transport is poorly constrained. Here, we utilize optical properties, ageing-diagnostic δ13C-BrC and transport time to deduce that the mass absorption cross-section (MACWS-BrC) is decreasing by ~50% during long-range oversea transport, resulting in a first-order bleaching rate of 0.24 day‒1 during the 3-day transit from continental East Asia to a south-east Yellow Sea receptor. A modern 14C signal points to a strong inverse correlation between BrC light-absorption and age of the source material. Combining this with results for South Asia reveals a striking agreement between these two major-emission regions of rapid photobleaching of BrC with a higher intrinsic absorptivity for BrC stemming from biomass burning. The consistency of bleaching parameters constrained independently for the outflows of both East and South Asia indicates that the weakening of BrC light absorption, thus primarily related to photochemical processes rather than sources, is likely a ubiquitous phenomenon. [ABSTRACT FROM AUTHOR]

Two relatively long‐term satellite aerosol products during 1983–2020 and 2000–2020 are employed to investigate interannual relationships between anomalous aerosol loadings over the Bay of Bengal (BoB) and Arabian Sea (AS) in the early summer and Asian monsoon rainfall anomalies. It is shown that increased aerosol loading (IAL) over the BoB is primarily attributed to an intensified upstream aerosol transport by anomalous subtropical westerly winds and coincides with local sea surface temperature (SST) cooling due to intensified prevailing wind and the aerosol dimming effect, and vice versa. A deficient rainfall in India tends to concur with a BoB IAL while excessive rainfall with an AS IAL in May and June. In June, a BoB IAL coincides with significantly deficient rainfall in the southwestern China‐Huaihe River Basin primarily linked to an anomalous cyclone off the coast of Southeast China. Meanwhile a related overturning of Walker Circulation is identified to be driven by the contrast of anomalous convective activity between the southeastern Indian‐BoB and the South China Sea‐Philippine Sea. An AS IAL is associated with air warming in North India due to an elevated aerosol semi‐direct effect and remote forcing that reinforces the meridional air temperature gradient. The IAL over the respective BoB and AS in June are both preceded by cold SST anomalies in the western Indian Ocean that can be traced back to the preceding winter, but the corresponding atmospheric circulations driving aerosol‐monsoon interactions differ distinctly. The above aerosol‐monsoon relationships are sustained primarily during 2000–2020 and vague during 1983–2020. Plain Language Summary: The year‐by‐year aerosol variations over the Bay of Bengal (BoB) and Arabian Sea (AS) in early spring and their relationship to the Asian summer monsoon rainfall anomalies are studied using satellite‐observed aerosol products. Increased aerosol loading (IAL) over the BoB is revealed to be accompanied by deficient rainfall in India and excessive rainfall in the northern South China Sea‐Philippine Sea (NSCSPS), driven by the changes in Walker Circulation primarily caused by the contrast of anomalous convective activity between the southeastern Indian‐BoB and the NSCSPS. An IAL over the AS tends to concur with excessive monsoon rainfall in India in May and June and is associated with air warming in northern South Asia partially due to the aerosol semi‐direct effect that reinforces the meridional air temperature gradient. The aerosol dimming effect associated with an IAL over the BoB and AS, along with the intensified prevailing westerly, might be responsible for the cooling of the local sea surface temperature (SST) in early spring and vice versa. The SST anomaly in the western Indian Ocean, which can be traced back to the preceding winter, plays an important role in driving the aforementioned associated changes in the atmospheric circulations and monsoon rainfall anomalies. Key Points: Anomalous aerosol loadings over the Bay of Bengal concur with an out‐of‐phase rainfall change in South and East Asia in early summerAerosol‐monsoon interaction over the Arabian Sea tends to modulate Indian rainfall by changing the meridional air temperature gradientSea surface temperature anomalies in Indian Ocean play an important role in stimulation of the aforementioned aerosol‐monsoon interaction [ABSTRACT FROM AUTHOR]

Daytime and nighttime PM10 samples were collected during summer (June) and winter (February) at a representative urban site in Mumbai, located on the western coast of Indian subcontinent. Samples were studied for molecular distribution of water-soluble dicarboxylic acids, oxoacids and dicarbonyls as well as total carbon (TC), water-soluble organic carbon (WSOC), inorganic ions along with specific markers (levoglucosan, K+) to better understand sources and formation processes of organic aerosols in Mumbai. The distribution of water-soluble organics was characterised by high abundance of oxalic acid (C2), followed by phthalic (Ph), terephthalic (tPh), azelaic (C9), malonic (C3), and succinic acids (C4). Positive correlations between C2, sulfate and glyoxal (ωC2) suggest secondary production of C2 predominantly via aqueous phase chemistry. C2 also showed positive correlation with K+ and levoglucosan indicating that biomass/biofuel burning is the potential source of diacids in the Mumbai aerosols. In addition, higher average contributions of total diacids to WSOC and OC in winter than in summer suggest that aerosols were aged i.e., photochemically well processed in winter in Mumbai. On the other hand, diurnal change in their ratios is observed with higher ratio in daytime samples than that of previous and succeeding nighttime samples, suggesting diacids are also influenced from local sources in both the seasons. This study demonstrates that biomass burning as well as biogenic sources are important sources influencing the distributions of aerosols in Mumbai. [ABSTRACT FROM AUTHOR]

Aerosols over the Tibetan Plateau (TP) play an important role in the regional and global climate change and ecological environment. The Second Tibetan Plateau Scientific Expedition and Research Program (STEP) carried out observation experiment at the Nam Co Station for Multisphere Observation and Research, Chinese Academy of Sciences (Nam Co Station, 30°46′N, 90°59′E, 4730 m) in the central TP from August 5 to September 11, 2020. This paper investigated the aerosol optical properties and its potential sources over Nam Co region. The main results are as follow: the average aerosol optical depth was 0.025 during the observation period; the average black carbon (BC) concentration and aerosol number concentration was 37 ng/m3 and 129 N/cm3, respectively; the diurnal variation and vertical distribution of aerosol were affected by the local meteorological elements. Frequent southerly winds during the summer monsoon led to a certain contribution of South Asia to the BC concentration in Nam Co region. And particles from the Taklimakan Desert led to dramatic increasing of aerosol number concentration over Nam Co region. The aerosol optical characteristics and influencing factors over the central TP were analyzed, which is beneficial to further study the influence of aerosols over the TP on regional and global weather and climate. • Optical properties of aerosol over Nam Co station were observed by the STEP of China. • Nam Co region was generally influenced by BC from South Asia, local pollution emissions and north particles. • The average of AOD, depolarization ratio and BC over Nam Co station was 0.026, 0.033 and 37 ng/m3, respectively. [ABSTRACT FROM AUTHOR]

Anthropogenic aerosols mask the climate warming caused by greenhouse gases (GHGs). In the absence of observational constraints, large uncertainties plague the estimates of this masking effect. Here we used the abrupt reduction in anthropogenic emissions observed during the COVID-19 societal slow-down to characterize the aerosol masking effect over South Asia. During this period, the aerosol loading decreased substantially and our observations reveal that the magnitude of this aerosol demasking corresponds to nearly three-fourths of the CO2-induced radiative forcing over South Asia. Concurrent measurements over the northern Indian Ocean unveiled a ~7% increase in the earth's surface-reaching solar radiation (surface brightening). Aerosol-induced atmospheric solar heating decreased by ~0.4 K d−1. Our results reveal that under clear sky conditions, anthropogenic emissions over South Asia lead to nearly 1.4 W m−2 heating at the top of the atmosphere during the period March–May. A complete phase-out of today's fossil fuel combustion to zero-emission renewables would result in rapid aerosol demasking, while the GHGs linger on. [ABSTRACT FROM AUTHOR]

Both South Asia and East Asia are the most polluted regions of the world. Unlike East Asia, the aerosol optical depth (AOD) over South Asia keeps increasing for all recent years, which calls for more attention. This study investigates the impacts of anthropogenic emissions over South Asia on the downstream regional climate during spring with the Community Earth System Model 2 (CESM2). The model results suggest that South Asian pollutants have significant impacts on East Asian spring climate, and the impacts could be even larger than locally emitted aerosols. Two possible dynamical pathways (i.e., the northern and the southern pathways) bridging South Asian aerosol forcing and East Asian climate are proposed, and both ways are associated with the black carbon (BC)-induced climate feedbacks surrounding the Tibetan Plateau (TP). The northern pathway is mainly due to the TP warming induced by the BC snow darkening effect (SDE), which significantly reduces the surface air temperature (SAT) over northern East Asia. BC-induced TP warming increases the meridional thermal gradient and accelerates the midlatitude jet stream, which favors the cold-air advection over northern East Asia. The southern pathway is associated with the BC "elevated heat pump" hypothesis, which mainly affects the precipitation in southern East Asia. BC from South Asia accumulates near the south slope of TP, inducing an abnormal ascending motion near the Bay of Bengal. A compensating anomalous sinking motion is then forced in South China, which suppresses the precipitation there. A primary observational analysis is also performed to verify both dynamical pathways. [ABSTRACT FROM AUTHOR]

Utilizing the well-calibrated, high-spectral-resolution equal-quality performance of daytime and nighttime (09:30 and 21:30 local solar Equator-crossing time (local solar ECT)) products of the Infrared Atmospheric Sounder Interferometer (IASI) from the Laboratoire de Météorologie Dynamique (LMD), this study investigates the day–night differences in dust aerosols over the global dust belt of North Africa, the Middle East, and Asia. Both daytime dust optical depth (DOD) and nighttime DOD at 10 µ m show high consistency with solar and lunar observations of coarse-mode aerosol optical depth (CAOD) from AErosol RObotic NETwork (AERONET) sites across the dust belt, with correlation coefficients of 0.8–0.9 for most sites. Both IASI DOD and dust layer height show a significant (95 % confidence level) day–night difference over the major dust sources within the dust belt. Daytime DOD over the central to northern Sahara, the central to eastern Arabian Peninsula, and the Taklamakan Desert is significantly higher than that of nighttime but lower than nighttime over the southern Sahel to the Guinea Coast and the western to central Indian subcontinent in the annual mean. The magnitude of the day–night differences in DOD is larger and more evident in boreal winter and spring than in other seasons. The positive day–night differences in DOD (i.e., higher daytime values than nighttime) over the central Sahara, the Middle East, and Asia are likely associated with greater dust emissions driven by higher dust uplift potential (DUP) and stronger wind speeds during daytime. Dust layer heights demonstrate negative day–night differences over dust source regions in the central Sahara, central Arabian Peninsula, and Taklamakan Desert and positive height differences in the southern Sahel to the Guinea Coast, southern parts of the Arabian Peninsula, and large parts of the Indian subcontinent. The higher dust layer height over the Guinea Coast and the Indian subcontinent during the daytime is associated with a deeper planetary boundary layer height and greater convective instability during daytime than nighttime, which promotes vertical transport and mixing of dust aerosols. The corresponding lower daytime DOD over the Sahel and the Indian subcontinent indicates a possible dilution of dust aerosols when they are transported to higher altitudes by convection where they are more susceptible to horizontal transport. Ground-based observations of dust show surface PM 10 concentration and CAOD exhibit a spatially varying diurnal cycle across the dust belt. CAOD and PM 10 concentrations generally peak in late morning and from late afternoon to midnight in the Sahel and in early afternoon and around early morning in the Middle East, the timings of which are largely consistent with the day–night differences in IASI DOD. It is also found that DOD from reanalysis products (e.g., Modern-Era Retrospective Analysis for Research and Applications, version 2 (MERRA-2) and ECMWF Atmospheric Composition Reanalysis 4 (EAC4)) failed to capture the day–night differences in IASI DOD in large parts of the dust belt except in small dust source hotspots over North Africa. [ABSTRACT FROM AUTHOR]

The Asian tropopause aerosol layer (ATAL) is a distinct feature during the Asian summer monsoon season with an impact on the regional radiative balance of the Earth's atmosphere. However, the source regions and the detailed transport pathways of ATAL particles are still uncertain. In this study, we investigate transport pathways from different regions at the model boundary (MB) to the ATAL using the two Lagrangian transport models CLaMS (Chemical Lagrangian Model of the Stratosphere) and MPTRAC (Massive-Parallel Trajectory Calculations), two reanalyses (ERA5 and ERA-Interim), and balloon-borne measurements of the ATAL performed by the Compact Optical Backscatter Aerosol Detector (COBALD) above Nainital (India) in August 2016. Trajectories are initialized at the location of the ATAL, as measured by COBALD in the Himalayas, and calculated 90 days backward in time to investigate the relation between the measured, daily averaged, aerosol backscatter ratio and different source regions at the MB. Nine source regions at the MB are distinguished, marking continental and maritime sources in the region of the Asian monsoon. Different simulation scenarios are performed, to find systematic differences as well as robust patterns, when the reanalysis data, the trajectory model, the vertical coordinate (kinematic and diabatic approach) or the convective parameterisation are varied. While there are many robust features, the simulation scenarios also show some considerable differences between the air mass contributions of different source regions at the MB in the region of the Asian monsoon. The contribution to all air parcels from the MB varied between 5 % and 40 % for the Indo-Gangetic plain, the contribution from the Tibetan Plateau varied between 30 % and 40 % and contributions from oceans varied between 14 % and 43 % for different scenarios. However, the robust finding among all scenarios is that the largest continental air mass contributions originate from the Tibetan plateau and the India subcontinent (mostly the Indo-Gangetic plain), and largest maritime air mass contributions in Asia come from the Western Pacific (e. g. related to tropical cyclones such as typhoons). Additionally, all simulation scenarios indicate that transport of maritime air from the Tropical Western Pacific to the region of the ATAL lowers the backscatter ratio (BSR) of the ATAL, while most scenarios indicate that transport of polluted air from the Indo-Gangetic plain increases the BSR. Therefore, while the results corroborate key findings from previous ERA-Interim based studies, they highlight the variability of the contributions of different MB regions to the ATAL depending on the meteorological input data, vertical velocities and in particular on the treatment of convection within the model calculations. [ABSTRACT FROM AUTHOR]

Lucknow is the capital of India's largest state, Uttar Pradesh, one of South Asia's most polluted urban cities. Tropospheric photochemistry relies on non-methane volatile organic compounds (NMVOCs), which are ozone and secondary organic aerosol precursors. Using the proton-transfer reaction time-of-flight mass spectrometer (PTR-ToF-MS) at an urban background site in Lucknow, the chemical characterisation of NMVOCs was performed in real time from December 2020 to May 2021. About ∼ 173 NMVOCs from m/z 31.018 to 197.216 were measured during the study period, including aromatics, non-aromatics, oxygenates, and nitrogen-containing compounds. The campaign daily mean concentrations of the NMVOCs were 125.5 ± 37.5 ppbv. The NMVOC daily average concentrations were about ∼ 30 % higher during the winter months (December–February) than in summer (March–May). The oxygenated volatile organic compounds and aromatics were the dominant VOC families, accounting for ∼ 57 %–80 % of the total NMVOC concentrations. Acetaldehyde, acetone, and acetic acid were the major NMVOC species, 5–15 times higher than the other species. An advanced multi-linear engine (ME-2) model was used to perform the NMVOC source apportionment using positive matrix factorisation (PMF). It resolves the five main sources contributing to these organic compounds in the atmosphere. They include traffic (23.5 %), two solid fuel combustion factors, SFC 1 (28.1 %) and SFC 2 (13.2 %), secondary volatile organic compounds (SVOCs) (18.6 %), and volatile chemical products (VCPs) (16.6 %). Aged and fresh emissions from solid fuel combustion (SFCs 1 and 2) were the dominant contributors to the total NMVOCs, and compounds related to these factors had a high secondary organic aerosol (SOA) formation potential. Interestingly, the traffic factor was the second-highest contributor to the total NMVOCs, and compounds related to this factor had a high ozone formation potential. Significant differences in the composition of the two solid fuel combustions indicate the influence of local emissions and transport of regional pollution to the city. The high temperature during summer leads to more volatilisation of oxygenated VOCs, related to the VCP factor. The study is the first attempt to highlight the sources of NMVOCs and their contribution to secondary pollutant (SOA and O 3) formation in the city of Lucknow during winter and summer. The insights from the study would help various stakeholders to manage primary and secondary pollutants within the city. [ABSTRACT FROM AUTHOR]

The inter-annual variability of aerosol over Indian region and its possible implications on the Indian summer monsoon is investigated using Aerosol Optical Depth (AOD) data from Moderate Resolution Imaging Spectrometer (MODIS) during the period 2001 to 2016. An attempt has been made to link the seasonal aerosol distribution over South Asia during spring and summer season to Indian Summer Monsoon Rainfall (ISMR) distribution. AOD derived from MODIS Terra observations shows large spatial inhomogeneity and characteristic variability with distinct temporal distributions. The pre-monsoon (spring) seasons (March-April-May; MAM) is characterized by high aerosol concentration over north-west part of India along with IGP region. During the south-west monsoon (summer) seasons (June-July-August-September; JJAS), wide area of high aerosol loading along Indo Gangetic plains extending from North Arabian sea through north-west India and up to Himalayan foothills. The regional rainfall distribution and its relationship with spatial and temporal aerosol distribution are then evaluated. Further, distinct variability in the aerosol distribution with respect to excess, deficit and normal monsoon years are analysed to understand the role of aerosols on the inter-annual variability of ISMR. Monthly aerosol distribution over Central India [CI;15° -25° N;75° -88° E] and Indo Gangetic plain [IGP;25°- 35°N;70°- 90° E] shows increased aerosol loading during deficit rainfall years and corresponding delay in the monthly rainfall peak. This study emphasises the active role of regional aerosol loading on regulating the inter-annual variability of regional Indian summer monsoon rainfall. [ABSTRACT FROM AUTHOR]

Known as the "third pole" and "water tower of Asia", the Tibetan Plateau (TP) is the home to the largest number of glaciers in the mid-latitudes and one of the most sensitive areas to global climate change due to its special geographical location and powerful thermodynamic effects. In recent years, the TP has been affected by exogenous pollutants and the concentrations of some pollutants have shown an increasing trend, especially light-absorbing aerosols (LAAs), when ice core records, ground- and aircraft-based field campaigns and satellite technology enabled synthesized monitoring. The enhanced warming of the vast majority of regions in TP, together with Arctic warming, and snow/ice decline, represents credible evidence of anthropogenic climate change. This paper provides a comprehensive review of studies on the sources, characteristics and climate impacts of LAAs over the TP. Adjacent to the two major emission sources of LAAs in East Asia and South Asia, the unique geographical location and climatic characteristics of the TP make it possible for TP LAAs to cause atmospheric warming and accelerated glacier melting, affecting the hydrological cycle in South Asia, East Asia and even the Northern Hemisphere, thus causing a series of serious environmental and social problems. LAAs, such as black carbon and dust, can strongly absorb solar radiation and and have significantly influence on climate change. Moreover, light-absorbing impurities (LAIs) on snow/ice can reduce the snow/ice albedo and further accelerate the snow/ice melting. Both LAAs and LAIs over the TP can induce thermodynamic feedback processes, cause significant warming of the TP and then lead to a strengthening of the early monsoon and affect the subsequent evolution of the monsoon. Many mechanisms have been proposed forth regarding how TP LAAs modulate the phase, intensity, and amplitude of the Asian climate system. A wide range of theoretical, observational, and modeling findings on TP LAAs and their climate impacts are synthesized, in which dust aerosols from drylands and black carbon from biomass burning are considered leading components. By coupling an integrated approach with state-of-the-art modeling, high temporal and fine spatial resolution remote sensing observations with increasing sampling over the TP will provide further insights into TP aerosols. • Light-absorbing aerosols warm the Tibetan Plateau, further influence climate system • The external input of light-absorbing aerosols over the Tibetan Plateau is dominant • Climate effects of light-absorbing aerosols or impurities in snow is divergent [ABSTRACT FROM AUTHOR]

Aircraft-borne in situ measurements of the chemical aerosol composition were conducted in the Asian tropopause aerosol layer (ATAL) over the Indian subcontinent in the summer of 2017, covering particle sizes below ∼3 µm. We have implemented a recently developed aerosol mass spectrometer, which adopts the laser desorption technique as well as the thermal desorption method for quantitative bulk information (i.e., a modified Aerodyne AMS), aboard the high-altitude research aircraft M-55 Geophysica. The instrument was deployed in July and August 2017 during the StratoClim EU campaign (Stratospheric and upper tropospheric processes for better Climate predictions) over Nepal, India, Bangladesh, and the Bay of Bengal, covering altitudes up to 20 kma.s.l. For particles with diameters between 10 nm and ∼3 µm , the vertical profiles of aerosol number densities from the eight research flights show significant enhancements in the altitude range of the ATAL. We observed enhancements in the mass concentrations of particulate nitrate, ammonium, and organics in a similar altitude range between approximately 13 and 18 km (corresponding to 360 and 410 K potential temperature). By means of the two aerosol mass spectrometry techniques, we show that the particles in the ATAL mainly consist of ammonium nitrate (AN) and organics. The single-particle analysis from laser desorption and ionization mass spectrometry revealed that a significant particle fraction (up to 70 % of all analyzed particles by number) within the ATAL results from the conversion of inorganic and organic gas-phase precursors, rather than from the uplift of primary particles from below. This can be inferred from the fact that the majority of the particles encountered in the ATAL consisted solely of secondary substances, namely an internal mixture of nitrate, ammonium, sulfate, and organic matter. These particles are externally mixed with particles containing primary components as well. The single-particle analysis suggests that the organic matter within the ATAL and in the lower stratosphere (even above 420 K) can partly be identified as organosulfates (OS), in particular glycolic acid sulfate, which are known as components indicative for secondary organic aerosol (SOA) formation. Additionally, the secondary particles are smaller in size compared to those containing primary components (mainly potassium, metals, and elemental carbon). The analysis of particulate organics with the thermal desorption method shows that the degree of oxidation for particles observed in the ATAL is consistent with expectations about secondary organics that were subject to photochemical processing and aging. We found that organic aerosol was less oxidized in lower regions of the ATAL (<380 K) compared to higher altitudes (here 390–420 K). These results suggest that particles formed in the lower ATAL are uplifted by prevailing diabatic heating processes and thereby subject to extensive oxidative aging. Thus, our observations are consistent with the concept of precursor gases being emitted from regional ground sources, subjected to rapid convective uplift, and followed by secondary particle formation and growth in the upper troposphere within the confinement of the Asian monsoon anticyclone (AMA). As a consequence, the chemical composition of these particles largely differs from the aerosol in the lower stratospheric background and the Junge layer. [ABSTRACT FROM AUTHOR]

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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]

This study investigates the seasonal climatology of the three-dimensional distribution and transport pathways of dust aerosols over West Asia (WA). Dust column loading over WA exhibits strong seasonality, with markedly high (weak) loading during summer (winter). The summer dust features over WA include the (i) dust reaching up to the 500 hPa level between the Red Sea (RS) and the west coast of the Indian subcontinent (IS); (ii) a slantwise advection of dust aerosols between 850 and 700 hPa levels over the Arabian Peninsula (AP) and Arabian Sea (AS); and (iii) a prominent mid-tropospheric zonal transport of AP dust toward the IS. Maximum column integrated horizontal dust mass flux (DMF) over WA is observed in summer. The intraday changes in the intensity and spatial spread of the DMF over the AP are mediated by the out-of-phase evolution of the surface winds and low-level Shamal jets. Furthermore, the diurnal changes in the strength of the inversion layers located above the monsoon boundary layer and associated wind shear regulate the spatial patterns and intensity of the DMF over the AS. The findings will support future studies aiming at quantifying the radiative effects of dust on the regional climate. [ABSTRACT FROM AUTHOR]

Atmospheric concentrations of South Asian anthropogenic aerosols and their transport play a key role in the regional hydrological cycle. Here, we use the ECHAM6-HAMMOZ chemistry–climate model to show the structure and implications of the transport pathways of these aerosols during spring (March–May). Our simulations indicate that large amounts of anthropogenic aerosols are transported from South Asia to the northern Indian Ocean and western Pacific. These aerosols are then lifted into the upper troposphere and lower stratosphere (UTLS) by the ascending branch of the Hadley circulation, where they enter the westerly jet. They are further transported to the Southern Hemisphere (∼15 –30 ∘ S) and downward (320–340 K) via westerly ducts over the tropical Atlantic (5 ∘ S–5 ∘ N, 10–40 ∘ W) and Pacific (5 ∘ S–5 ∘ N, 95–140 ∘ E). The carbonaceous aerosols are also transported to the Arctic, leading to local heating (0.08–0.3 K per month, an increase by 10 %–60 %). The presence of anthropogenic aerosols causes a negative radiative forcing (RF) at the top of the atmosphere (TOA) (- 0.90 ± 0.089 W m -2) and surface (- 5.87 ± 0.31 W m -2) and atmospheric warming (+ 4.96 ± 0.24 W m -2) over South Asia (60–90 ∘ E, 8–23 ∘ N), except over the Indo-Gangetic Plain (75–83 ∘ E, 23–30 ∘ N), where RF at the TOA is positive (+ 1.27 ± 0.16 W m -2) due to large concentrations of absorbing aerosols. The carbonaceous aerosols lead to in-atmospheric heating along the aerosol column extending from the boundary layer to the upper troposphere (0.1 to 0.4 K per month, increase by 4 %–60 %) and in the lower stratosphere at 40–90 ∘ N (0.02 to 0.3 K per month, increase by 10 %–60 %). The increase in tropospheric heating due to aerosols results in an increase in water vapor concentrations, which are then transported from the northern Indian Ocean–western Pacific to the UTLS over 45–45 ∘ N (increasing water vapor by 1 %–10 %). [ABSTRACT FROM AUTHOR]

Water‐soluble organic carbon (WSOC) is a substantial component of carbonaceous aerosols in South/East Asia. However, the poorly constrained sources, molecular compositions, and light absorption properties of WSOC over South/East Asian marine regions lead to large uncertainty in climate effects. Herein, we collected marine aerosol samples from South China Sea to the eastern Indian Ocean to investigate the sources, molecular compositions, and light absorption properties of WSOC. The δ13C of Marine‐influenced WSOC (−20.6 ± 1.4‰) was higher than those in Continent‐influenced (South Asia‐influenced: −24.4 ± 1.1‰ and Southeast Asia‐influenced: −22.7 ± 1.0‰, p < 0.01) regions. Additionally, combining with 5‐day back trajectories and the relationships of δ13C‐WSOC with chemical tracers (Cl−/Na+ and nonsea salt K+/K+), we found that the Marine‐influenced WSOC was mostly related to oceanic emissions, which was more enriched in saturated primary marine biological compounds with lower oxidation level. In contrast, the Continent‐influenced WSOC was significantly affected by C3 biomass burning and secondary organic aerosols formation, and it has a higher fraction of aromatic and highly oxidized compounds. Moreover, the high aromatic level of Continental‐influenced WSOC may result in high mass absorption efficiency at 365 nm (MAE365) but low absorption Ångström exponent (AAE) values. Taken together with previous WSOC light absorption properties studies, we found that the MAE365 of WSOC in urban, rural and background, and marine regions correlated well with AAE. However, the response and correlation coefficients of MAE365 to AAE were highest in urban regions, followed by rural and background and marine regions, which is likely associated with different aromatic compound contents. Therefore, in the future, more attention should be paid to the sources and atmospheric processes of condensed aromatic compounds. Key Points: The Continent‐influenced and Marine‐influenced WSOC were significantly affected by anthropogenic and oceanic emissions, respectivelyThe Continental‐influenced WSOC was more enriched in aromatic compounds, with stronger light absorption capacity than Marine‐influenced WSOCDifference in response and correlation coefficients of MAE365 to AAE in different regions may be related to varied aromatic compound contents [ABSTRACT FROM AUTHOR]

The direct perturbation of anthropogenic aerosols on Earth's energy balance [i.e., direct aerosol radiative forcing (DARF)] remains uncertain in climate models. These uncertainties critically depend on aerosol optical properties, primarily aerosol optical depth (AOD), single scattering albedo (SSA), and the asymmetry factor g. In this study, we investigate the intermodel spread of DARF across 14 global models within phase 6 of the Coupled Model Intercomparison Project (CMIP6), using unified radiative transfer calculation and aerosol optical parameter assumptions. The global mean DARF for clear sky in 2014 with respect to 1850 is estimated as 20.77 ± 0.52 W m-2 assuming an externally mixed state and 20.68 ± 0.53 W m-2 for an internally mixed state. We further conduct a quantitative analysis and find that globally, for the external mixing assumption, AOD is the dominant factor, whose intermodel spread results in 36% of the total DARF uncertainty. For the internal mixing assumption, SSA becomes the major factor, which also leads to 36% DARF uncertainty. The g parameter and aerosol vertical distribution combined contribute to ~30% of the DARF uncertainty. Regionally, DARF uncertainty is typically more sensitive to SSA where the absorbing aerosol fraction is high, such as South Asia and central Africa. Substantial differences between model-averaged and observed aerosol optical parameters are still noticed, with external mixing in general yielding closer agreement with observations. Our results highlight the importance of aerosol scattering and absorption properties in DARF estimation. [ABSTRACT FROM AUTHOR]

In the present work, the variability, trends and relationships of aerosol, cloud and rainfall are explored for three regions of the Indian subcontinent: the Indo-Gangetic Plain (IGP), central India (CI) and the North Indian Ocean (NIO). The investigated properties include the monthly averages of satellite retrievals for the aerosol optical depth (AOD), angstrom exponent (AE), aerosol index (AI), cloud effective radius (Re), cloud optical thickness (COT), cloud liquid water path (LWP) and rain rate (RR). Inter-annual and seasonal variability and long-term trends for these properties were analyzed over the regions selected. The analysis showed apparent regional and temporal variations in all seven parameters. Strong increases in aerosol properties over the IGP and CI regions over the last two decades have enabled the study of the response to cloud and rainfall properties. Further, aerosol–cloud–rain rate relationships during the summer monsoon were verified using linear fit analysis (using AOD [and AI], Re, LWP and RR) for the three regions, respectively. A negative relation between AOD and Re was seen over the three regions, whereas AOD and RR showed a negative relation over IGP and NIO. It was found that the AI property, which represents the aerosol number, is inversely correlated with Re but positively correlated with RR during the monsoon season over the IGP and CI. AI and LWP showed a negative relation for CI but a positive relation for IGP and NIO. We believe that this study will help in assessing regional and global climate impacts due to aerosols. [ABSTRACT FROM AUTHOR]

Anthropogenic secondary organic aerosol (ASOA), formed from anthropogenic emissions of organic compounds, constitutes a substantial fraction of the mass of submicron aerosol in populated areas around the world and contributes to poor air quality and premature mortality. However, the precursor sources of ASOA are poorly understood, and there are large uncertainties in the health benefits that might accrue from reducing anthropogenic organic emissions. We show that the production of ASOA in 11 urban areas on three continents is strongly correlated with the reactivity of specific anthropogenic volatile organic compounds. The differences in ASOA production across different cities can be explained by differences in the emissions of aromatics and intermediate- and semi-volatile organic compounds, indicating the importance of controlling these ASOA precursors. With an improved model representation of ASOA driven by the observations, we attribute 340 000 PM 2.5 -related premature deaths per year to ASOA, which is over an order of magnitude higher than prior studies. A sensitivity case with a more recently proposed model for attributing mortality to PM 2.5 (the Global Exposure Mortality Model) results in up to 900 000 deaths. A limitation of this study is the extrapolation from cities with detailed studies and regions where detailed emission inventories are available to other regions where uncertainties in emissions are larger. In addition to further development of institutional air quality management infrastructure, comprehensive air quality campaigns in the countries in South and Central America, Africa, South Asia, and the Middle East are needed for further progress in this area. [ABSTRACT FROM AUTHOR]

Regional climatic implications of aerosol black carbon (BC), which has a wide variety of anthropogenic sources in large abundance, are well recognized over South Asia. Significant uncertainties remain in its quantification due to a lack of sufficient information on the microphysical properties (its concentration, size, and mixing state with other aerosol components) that determine the absorption potential of BC. In particular, the information on the mixing state of BC is extremely sparse over this region. In this study, the first observations of the size distribution and mixing state of individual refractory black carbon (rBC) particles in the South Asian outflow to the south-eastern Arabian Sea and the northern and equatorial Indian Ocean regions are presented based on measurements using a single particle soot photometer (SP2) aboard the Integrated Campaign for Aerosols, gases, and Radiation Budget (ICARB-2018) ship during winter 2018 (16 January to 13 February). The results revealed significant spatial heterogeneity of BC characteristics. The highest rBC mass concentrations (∼938±293 ngm-3) with the highest relative coating thickness (RCT; the ratio of BC core to its coating diameters) of ∼2.16±0.19 are found over the south-east Arabian Sea (SEAS) region, which is in the proximity of the continental outflow. As we move to farther oceanic regions, though the mass concentrations decreased by nearly half (∼546±80 ngm-3), BC still remained thickly coated (RCT∼2.05±0.07). The air over the remote equatorial Indian Ocean, which received considerable marine air masses compared to the other regions, showed the lowest rBC mass concentrations (∼206±114 ngm-3) with a moderately thick coating (RCT∼1.73±0.16). Even over oceanic regions far from the landmass, regions that received the outflow from the more industrialized east coast/the Bay of Bengal had a thicker coating (∼104 nm) compared to regions that received outflow from the west coast and/or peninsular India (∼86 nm). Although different regions of the ocean depicted contrasting concentrations and mixing state parameters due to the varied extent and nature of the continental outflow as well as the atmospheric lifetime of air masses, the modal parameters of rBC mass–size distributions (mean mass median diameters ∼ 0.19–0.20 µm) were similar over all regions. The mean fraction of BC-containing particles (FBC) varied in the range of 0.08–0.12 (suggesting significant amounts of non-BC particles), whereas the bulk mixing ratio of coating mass to rBC mass was highest (8.31±2.40) over the outflow regions compared to the remote ocean (4.24±1.45), highlighting the role of outflow in providing condensable material for coatings on rBC. These parameters, along with the information on the size-resolved mixing state of BC cores, throw light on the role of sources and secondary processing of their complex mixtures for coatings on BC under highly polluted conditions. Examination of the non-refractory sub-micrometre aerosol chemical composition obtained using the aerosol chemical speciation monitor (ACSM) suggested that the overall aerosol system was sulfate-dominated over the far-oceanic regions. In contrast, organics were equally prominent adjacent to the coastal landmass. An association between the BC mixing state and aerosol chemical composition suggested that sulfate was the probable dominant coating material on rBC cores. [ABSTRACT FROM AUTHOR]

To better understand the aerosol properties over the Arctic, Antarctic and Tibetan Plateau (TP), the aerosol optical properties were investigated using 13 years of CALIPSO (Cloud–Aerosol Lidar and Infrared Pathfinder Satellite Observations) L3 data, and the back trajectories for air masses were also simulated using the Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model. The results show that the aerosol optical depth (AOD) has obvious spatial- and seasonal-variation characteristics, and the aerosol loading over Eurasia, Ross Sea and South Asia is relatively large. The annual-average AODs over the Arctic, Antarctic and TP are 0.046, 0.024 and 0.098, respectively. Seasonally, the AOD values are larger from late autumn to early spring in the Arctic, in winter and spring in the Antarctic, and in spring and summer over the TP. There are no significant temporal trends of AOD anomalies in the three study regions. Clean marine and dust-related aerosols are the dominant types over ocean and land, respectively, in both the Arctic and Antarctic, while dust-related aerosol types have greater occurrence frequency (OF) over the TP. The OF of dust-related and elevated smoke is large for a broad range of heights, indicating that they are likely transported aerosols, while other types of aerosols mainly occurred at heights below 2 km in the Antarctic and Arctic. The maximum OF of dust-related aerosols mainly occurs at 6 km altitude over the TP. The analysis of back trajectories of the air masses shows large differences among different regions and seasons. The Arctic region is more vulnerable to mid-latitude pollutants than the Antarctic region, especially in winter and spring, while the air masses in the TP are mainly from the Iranian Plateau, Tarim Basin and South Asia. [ABSTRACT FROM AUTHOR]

Aerosol is a critical trace component of the atmosphere. Many processes in the Earth's climate system are intimately related to aerosols via their direct and indirect radiative effects. Aerosol effects are not limited to these climatic aspects, however. They are also closely related to human health, photosynthesis, new energy, etc., which makes aerosol a central focus in many research fields. A fundamental requirement for improving our understanding of the diverse aerosol effects is to accumulate high-quality aerosol data by various measurement techniques. Sunphotometer remote sensing is one of the techniques that has been playing an increasingly important role in characterizing aerosols across the world. Much progress has been made on this aspect in China during the past decade, which is the work reviewed in this paper. Three sunphotometer networks have been established to provide high-quality observations of long-term aerosol optical properties across the country. Using this valuable dataset, our understanding of spatiotemporal variability and long-term trends of aerosol optical properties has been much improved. The radiative effects of aerosols both at the bottom and at the top of the atmosphere are comprehensively assessed. Substantial warming of the atmosphere by aerosol absorption is revealed. The long-range transport of dust from the Taklimakan Desert in Northwest China and anthropogenic aerosols from South Asia to the Tibetan Plateau is characterized based on ground-based and satellite remote sensing as well as model simulations. Effective methods to estimate chemical compositions from sunphotometer aerosol products are developed. Dozens of satellite and model aerosol products are validated, shedding new light on how to improve these products. These advances improve our understanding of the critical role played by aerosols in both the climate and environment. Finally, a perspective on future research is presented. • Development of ground-based sunphotometer networks in China is presented. • Advances in our understanding of aerosol optical properties and radiative effects are reviewed. • A perspective on possible directions for future research is discussed. [ABSTRACT FROM AUTHOR]

Environmental context: The export of various man-made pollutants from northern India has a large impact on aerosol formation processes, their transformations and regional environmental chemistry over tropical peninsular India. The quantitative source apportionment of organic aerosols performed in this study provides a better understanding of their sources and implications for climate and air-quality management policies in South Asia. This study highlights seasonal characteristics, sources, daytime (sea-breeze) and night-time (land-breeze) variations of carbonaceous and water-soluble ionic components in PM10 (<10 µm particulate matter) aerosols from the east coast (Chennai city) of tropical India. Elemental and organic carbon (EC and OC) were found to be higher in winter when air masses were delivered from the northern part of India covered by the Indo-Gangetic-Plains whereas lower concentrations were observed during summer and monsoon associated with marine air masses. Sea salts (Na+ and Cl–), dust (Ca2+ and Mg2+) and nitrates (NO3–) were found to be highest in monsoon, suggesting these species may be co-transported over the sampling site with marine air masses. Using air mass back-trajectory analysis, linear relationships between chemical species and specific mass ratios, we demonstrate that east coast urban aerosols are strongly influenced by aged anthropogenic sources including biomass burning in winter and post monsoon while aged marine emissions mixed with local pollutants (dust and vehicular) are important in monsoon and summer. Further, the mesoscale phenomenon was reflected in measured chemical constituents during the study period. Positive-matrix-factorisation (PMF) analysis confirmed that OC aerosols are largely attributable to chemically aged anthropogenic (53 % in the day and 39 % in the night) and combustion-derived (17 % and 39 %) sources in winter and sea salts mixed with dust and vehicular emissions (61 % and 52 %) during monsoon. These important insights about the sources and formation processes of organic aerosols will help in understanding the formation of atmospheric brown clouds over south Asia. Environmental context. The export of various man-made pollutants from northern India has a large impact on aerosol formation processes, their transformations and regional environmental chemistry over tropical peninsular India. The quantitative source apportionment of organic aerosols performed in this study provides a better understanding of their sources and implications for climate and air-quality management policies in South Asia. [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]

A large uncertainty exists today in quantifying the absorbing aerosol snow darkening effect (SnoDE) and its relative role compared to the direct radiative effect (DRE), especially at the regional scale. Using a regional climate model over an enlarged South Asia Coordinated Regional Climate Downscaling Experiment (CORDEX) domain, here we isolate these effects and examine their impacts on the dynamics of the Indian pre-monsoon and summer monsoon (ISM) circulation. Our results clearly indicate that the regional dynamics associated with the pre-monsoon and ISM are highly sensitive to both aerosol SnoDE and DRE, with the SnoDE dominating during the pre-monsoon, and the DRE during the ISM. During the pre-monsoon, the deposition of aerosols on the Himalayas and Tibetan Plateau (HTP) reduces the surface albedo, leading to an increase in absorption of solar radiation and accelerated snow melting. The associated increase in surface and tropospheric temperature draws dry air from central Asia towards northern India and along the Himalayan foothills, creating a low-level anti-cyclonic anomaly over eastern India and the Bay of Bengal. This limits the northward propagation of southwest winds and leads to a decrease in precipitation over the central and eastern parts of India during the pre-monsoon and across northern India in the following ISM. Conversely, an increase in precipitation during the ISM is due to the strengthening of southwest winds caused by large-scale convergence over the Arabian Peninsula. The shift of winds from central Asia towards northern India in the SnoDE and towards the Arabian Peninsula in DRE leads to contrasting effects and can possibly modulate the monsoon onset dates. The SnoDE, with a prevailing contribution from dust, leads to an increase in precipitation over the HTP, which is amplified during the ISM when DRE is also considered. Our study provides evidence that both these aerosol effects have substantial impacts on the pre-monsoon and ISM dynamics and hence need to be considered in climate model simulations over the region. [ABSTRACT FROM AUTHOR]

The contribution of individual aerosol species and greenhouse gases to precipitation changes during the South Asian summer monsoon is uncertain. Mechanisms driving responses to anthropogenic forcings need further characterization. We use an atmosphere‐only climate model to simulate the fast response of the summer monsoon to different anthropogenic aerosol types and to anthropogenic greenhouse gases. Without normalization, sulfate is the largest driver of precipitation change between 1850 and 2000, followed by black carbon and greenhouse gases. Normalized by radiative forcing, the most effective driver is black carbon. The precipitation and moisture budget responses to combinations of aerosol species perturbed together scale as a linear superposition of their individual responses. We use both a circulation‐based and moisture budget‐based argument to identify mechanisms of aerosol and greenhouse gas induced changes to precipitation and find that in all cases the dynamic contribution is the dominant driver to precipitation change in the monsoon region. Plain Language Summary: Small particles suspended in the atmosphere and emitted by human activities, known as atmospheric aerosols, contribute to changes in precipitation in South Asia, yet the exact importance of individual components is not well understood. Further, the impact of human‐caused greenhouse gas emissions is also uncertain. We use a computer model to simulate the monsoon and find that aerosols are the largest driver of precipitation change compared to greenhouse gases. We also breakdown the precipitation changes by their components and find that changes in atmospheric vertical and horizontal motion of air dominate over increases in moisture for explaining the total rainfall changes. These results help further understand the impact of climate change on precipitation in South Asia, which is important to the lives of billions of people. Key Points: Per unit radiative forcing, black carbon is the most effective driver of precipitation change during the South Asian summer monsoonAnomalous sinking and rising explain modeled precipitation responses to anthropogenic greenhouse gases and aerosolsThe dynamic component dominates the mean column‐integrated moisture flux convergence over the thermodynamic component [ABSTRACT FROM AUTHOR]

Emissions and long-range transport of mineral dust and combustion-related aerosol from burning fossil fuels and biomass vary from year to year, driven by the evolution of the economy and changes in meteorological conditions and environmental regulations. This study offers both satellite and model perspectives on the interannual variability and possible trends of combustion aerosol and dust in major continental outflow regions over the past 15 years (2003–2017). The decade-long record of aerosol optical depth (AOD, denoted as τ), separately for combustion aerosol (τc) and dust (τd), over global oceans is derived from the Collection 6 aerosol products of the Moderate Resolution Imaging Spectroradiometer (MODIS) onboard both Terra and Aqua. These MODIS Aqua datasets, complemented by aerosol source-tagged simulations using the Community Atmospheric Model version 5 (CAM5), are then analyzed to understand the interannual variability and potential trends of τc and τd in the major continental outflows. Both MODIS and CAM5 consistently yield a similar decreasing trend of -0.017 to -0.020 per decade for τc over the North Atlantic Ocean and the Mediterranean Sea that is attributable to reduced emissions from North America and Europe, respectively. On the contrary, both MODIS and CAM5 display an increasing trend of + 0.017 to + 0.036 per decade for τc over the tropical Indian Ocean, the Bay of Bengal, and the Arabian Sea, which reflects the influence of increased anthropogenic emissions from South Asia and the Middle East in the last 2 decades. Over the northwestern Pacific Ocean, which is often affected by East Asian emissions of pollution and dust, the MODIS retrievals show a decreasing trend of -0.021 per decade for τc and -0.012 per decade for τd , which is, however, not reproduced by the CAM5 model. In other outflow regions strongly influenced by biomass burning smoke or dust, both MODIS retrievals and CAM5 simulations show no statistically significant trends; the MODIS-observed interannual variability is usually larger than that of the CAM5 simulation. [ABSTRACT FROM AUTHOR]

The long-term temporal–spatial variations in the aerosol optical properties over the Tibetan Plateau (TP) and the potential long-range transport from surrounding areas to the TP were analyzed in this work, by using multiple years of sun photometer measurements (CE318) at five stations in the TP, satellite aerosol products from the Moderate Resolution Imaging Spectroradiometer (MODIS) and Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP), back-trajectory analysis from the Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) and model simulations from the Goddard Earth Observing System (GEOS)-Chem chemistry transport model. The results from the ground-based observations showed that the annual aerosol optical depth (AOD) at 440 nm at most TP sites increased in recent decades with trends of 0.001±0.003 yr -1 at Lhasa, 0.013±0.003 yr -1 at Mt_WLG, 0.002±0.002 yr -1 at NAM_CO and 0.000±0.002 yr -1 at QOMS_CAS. The increasing trend was also found for the aerosol extinction Ångström exponent (EAE) at most sites with the exception of the Mt_WLG site. Spatially, the AOD at 550 nm observed from MODIS showed negative trends at the northwest edge close to the Taklimakan Desert and to the east of the Qaidam Basin and slightly positive trends in most of the other areas of the TP. Different aerosol types and sources contributed to a polluted day (with CE318 AOD at 440 nm > 0.4) at the five sites on the TP: dust was the dominant aerosol type in Lhasa, Mt_WLG and Muztagh with sources in the Taklimakan Desert, but fine-aerosol pollution was dominant at NAM_CO and QOMS_CAS with transport from South Asia. A case of aerosol pollution at Lhasa, NAM_CO and QOMS_CAS during 28 April–3 May 2016 revealed that the smoke aerosols from South Asia were lifted up to 10 km and transported to the TP, while the dust from the Taklimakan Desert could climb the north slope of the TP and then be transported to the central TP. The long-range transport of aerosol thereby seriously impacted the aerosol loading over the TP. [ABSTRACT FROM AUTHOR]

Emissions of anthropogenic aerosols are expected to change drastically over the coming decades, with potentially significant climate implications. Using the most recent generation of harmonized emission scenarios, the Shared Socioeconomic Pathways (SSPs) as input to a global chemistry transport and radiative transfer model, we provide estimates of the projected future global and regional burdens and radiative forcing of anthropogenic aerosols under three contrasting pathways for air pollution levels: SSP1-1.9, SSP2-4.5 and SSP3-7.0. We find that the broader range of future air pollution emission trajectories spanned by the SSPs compared to previous scenarios translates into total aerosol forcing estimates in 2100 relative to 1750 ranging from -0.04 in SSP1-1.9 to -0.51 W m -2 in SSP3-7.0. Compared to our 1750–2015 estimate of -0.55 W m -2 , this shows that, depending on the success of air pollution policies and socioeconomic development over the coming decades, aerosol radiative forcing may weaken by nearly 95 % or remain close to the preindustrial to present-day level. In all three scenarios there is a positive forcing in 2100 relative to 2015, from 0.51 in SSP1-1.9 to 0.04 W m -2 in SSP3-7.0. Results also demonstrate significant differences across regions and scenarios, especially in South Asia and Africa. While rapid weakening of the negative aerosol forcing following effective air quality policies will unmask more of the greenhouse-gas-induced global warming, slow progress on mitigating air pollution will significantly enhance the atmospheric aerosol levels and risk to human health in these regions. In either case, the resulting impacts on regional and global climate can be significant. [ABSTRACT FROM AUTHOR]

The regional climate model RegCM 4.4 at 50 km resolution is used to conduct a sensitivity study over South Asia Coordinated Regional climate Downscaling Experiment domain during the period 1998–2002, in order to investigate the best cumulus convective precipitation scheme, planetary boundary layer (PBL) and land-surface scheme. The inferences obtained from 11 sensitivity experiments include the better performance of community land model version 4.5 (CLM 4.5) over biosphere–atmosphere transfer scheme, Tiedtke as cumulus convective precipitation scheme and University of Washington (UW) as PBL scheme. The simulation with these parameterization schemes well captures the monsoon precipitation pattern over India ~ 7 mm/day and North Eastern Region of India (NER) ~ 12 mm/day, which are comparable to observations with a significant correlation of R2 > 0.93. The observed temperatures are also well simulated by the model. Therefore, RegCM 4.4 with these parameterization schemes is further used to simulate the aerosol fields (aerosol optical depth, AOD and black carbon, BC) and aerosol direct radiative forcing (DRF) for the period 2011–2014 over the same domain with special emphasis on NER. The model captures the seasonality in AOD and BC over the Indian Subcontinent and NER. BC hotspots in the Indo-Gangetic Plain and China are well captured by the model. The observed to simulated BC ratio over Dibrugarh (located in NER) is found to be improved. The model underestimation is significant in the dry season when burning over the region is predominant, which has not been considered by the emission inventories properly. Simulated DRF is found to exhibit seasonality qualitatively as well as a North–South latitudinal gradient. [ABSTRACT FROM AUTHOR]

The role of anthropogenic aerosols in future projections (up to 2100) of summertime precipitation and precipitation extremes over the Asian monsoon region is investigated, by comparing two sets of the Community Earth System Model (CESM1) large ensemble simulations under the Representative Concentration Pathway 8.5 scenario (RCP8.5) and the corresponding scenario with aerosol fixed at 2005 levels (RCP8.5_FixA). The model is verified to be performing well in capturing present-day (1986–2005) climate and precipitation extremes. Our results suggest that the Asian monsoon region would become progressively warmer and wetter in the future under RCP8.5, while precipitation extremes will be significantly aggravated due to anthropogenic aerosol mitigation, particularly over East Asia. Specifically, aerosol reductions are found to shift the distribution of precipitation mean and extremes to larger values. For example, aerosol reductions would result in an increased likelihood of extreme precipitation (e.g. the maximum consecutive 5-day precipitation amount) and related disasters. Sensitivities of changes in precipitation mean and extremes to local warming from aerosol reductions are much larger than that from greenhouse gas increases. This is particularly important over East Asia in accordance with larger magnitudes of aerosol reductions compared to South Asia. Finally, by investigating the response of the climate system to aerosol changes, our findings demonstrate that aerosol induced precipitation changes would be dominated by aerosol–radiation–cloud forcing over northern East Asia and aerosol forcing induced large-scale circulation anomalies over southern East and South Asia. [ABSTRACT FROM AUTHOR]

Wet and dry periods within the South Asian summer monsoon season can have acute societal impacts. Recent studies have identified changes in daily rainfall characteristics of the monsoon, but the underlying causes are poorly understood. In particular, although the dominant role of anthropogenic aerosols in shaping historical changes in seasonal-mean monsoon rainfall has been documented, their influence on daily-scale rainfall remains unconstrained. Using an ensemble of single-forcing climate simulations, we find that anthropogenic aerosols have a stronger influence on late-twentieth century changes in the frequency of wet events, dry events and rainless days, compared with other climate forcings. We also investigate the role of aerosol-cloud interactions ("indirect effects") in the total aerosol response, and the contribution of aerosols emitted from South Asia versus from remote sources. Based on additional simulations with the GFDL-CM3 climate model, we find that the simulated aerosol response over South Asia is largely associated with aerosol-indirect effects. In addition, local aerosols suppress wet-event frequency and enhance dry-event frequency over eastern-central India, where increases in aerosol loading are the largest. Remote aerosols cause a north–south dipole pattern of change in mean rainfall over India and fewer rainless days over western India. However, the overall spatial response of South Asian rainfall characteristics to total aerosol forcing is substantially influenced by the combined non-linear climate response to local and remote aerosols. Together, our results suggest that understanding the influence of different aerosol emissions trajectories on the regional climate dynamics is critical for effective climate-risk management in this populated, vulnerable region. [ABSTRACT FROM AUTHOR]

Aerosols can act as cloud condensation nuclei and ice nuclei, resulting in changes in cloud droplet/particle number/size, and hence altering the radiation budget. This study investigates the interactions between aerosols and ice clouds by incorporating the latest ice clouds parameterization in an atmospheric general circulation model. The simulation shows a decrease in effective ice cloud crystal size corresponding to aerosol increase, referred to as the aerosol first indirect effect, which has not been comprehensively studied. Ice clouds with smaller particles reflect more shortwave radiation and absorb more infrared radiation, resulting in radiation change by 0.5–1.0 W/m2 at the top of the atmosphere (TOA). The TOA radiation field is also influenced by cloud cover change due to aerosol-induced circulation change. Such aerosol effects on precipitation highly depend on the existence of a deep convection system: interactions between aerosols and ice clouds create dipole precipitation anomalies in the Asian monsoon regions; while in West Africa, enhanced convections are constrained by anticyclone effects at high levels and little precipitation increase is found. We also conduct an experiment to assess interactions between aerosols and liquid clouds and compare the climatic effects with that due to ice clouds. Radiation and temperature changes generated by liquid clouds are normally 1–2 times larger than those generated by ice clouds. The radiation change has a closer relationship to liquid cloud droplet size than liquid cloud cover, in contrast with what we find for ice clouds. [ABSTRACT FROM AUTHOR]

Recent studies point to combined effects of changes in regional land-use, anthropogenic aerosol forcing and sea surface temperature (SST) gradient on declining trends in the South Asian monsoon (SAM). This study attempted disentangling the effects produced by changes in SST gradient from those by aerosol levels in an atmospheric general circulation model. Two pairs of transient ensemble simulations were made, for a 40-year period from 1971 to 2010, with evolving versus climatological SSTs and with anthropogenic aerosol emissions fixed at 1971 versus 2010, in each case with evolution of the other forcing element, as well as GHGs. Evolving SST was linked to a widespread feedback on increased surface temperature, reduced land-sea thermal contrast and a weakened Hadley circulation, with weakening of cross-equatorial transport of moisture transport towards South Asia. Increases in anthropogenic aerosol levels (1971 versus 2010), led to an intensification of drying in the peninsular Indian region, through several regional pathways. Aerosol forcing induced north-south asymmetries in temperature and sea-level pressure response, and a cyclonic circulation in the Bay of Bengal, leading to an easterly flow, which opposes the monsoon flow, suppressing moisture transport over peninsular India. Further, aerosol induced decreases in convection, vertically integrated moisture flux convergence, evaporation flux and cloud fraction, in the peninsular region, were spatially congruent with reduced convective and stratiform rainfall. Overall, evolution of SST acted through a weakening of cross-equatorial moisture flow, while increases in aerosol levels acted through suppression of Arabian Sea moisture transport, as well as, of convection and vertical moisture transport, to influence the suppression of SAM rainfall. [ABSTRACT FROM AUTHOR]

The direct radiative effect of absorbing aerosols consists of absorption-induced atmospheric heating together with scattering- and absorption-induced surface cooling. It is thus important to understand whether some of the reported climate impacts of anthropogenic absorbing aerosols are mainly due to the coexistence of these two opposite effects and to what extent the nonlinearity raised from such coexistence would become a critical factor. To answer these questions specifically regarding the South Asia summer monsoon with focus on aerosol-induced changes in monsoon onset, a set of century-long simulations using the Community Earth System Model, version 1.0.3 (CESM 1.0.3), of NCAR with fully coupled atmosphere and ocean components was conducted. Prescribed direct heating to the atmosphere and cooling to the surface were applied in the simulations over the Indian subcontinent, either alone or combined, during the aerosol-laden months of May and June. Over many places in the Indian subcontinent, the nonlinear effect dominates in the changes of subcloud layer moist static energy, precipitation, and monsoon onset. The surface cooling effect of aerosols appears to shift anomalous precipitative cooling away from the aerosol-forcing region and hence turn the negative feedback to aerosol-induced atmospheric heating into a positive feedback on the monsoon circulation through latent heat release over the Himalayan foothills. Moisture processes form the critical chain mediating local aerosol direct effects and onset changes in the monsoon system. [ABSTRACT FROM AUTHOR]