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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]

South Asian air pollutants exert substantial effect on the climate and environment change over the Tibetan Plateau (TP). This paper investigates the trans-boundary transport of PM 10 , PM 2.5 , and O 3 from South Asia to the TP via WRF-Chem sensitive analysis. It is found that PM 10 , PM 2.5 , and O 3 over South Asia are mainly sourced from anthropogenic sources. South Asian emissions contribute up to 54% of PM 10 (PM 2.5) in the TP in the pre-monsoon season. For O 3 , the highest contribution of 18.13% is in the monsoon season, while the lowest contribution of 8.67% is in the winter season. To evaluate the respective contributions of anthropogenic and biomass burning emissions in South Asia to PM 10 , PM 2.5 , and O 3 in the TP, anthropogenic and biomass burning emissions in South Asia are considered separately. The results show that the largest percentage contribution of PM 10 (PM 2.5) from South Asian anthropogenic emissions to PM 10 (PM 2.5) in the TP with value of 35.86% (37.77%) occurs in winter, while the lowest percentage contribution of 16.52% (16.77%) appears in the monsoon season. For O 3 , the largest contribution of 17.74% from South Asian anthropogenic emissions appears in the monsoon season, whereas the lowest contribution of 8.59% occurs in winter. Compared to the anthropogenic emissions, the biomass burning emissions in South Asia have a relative less contribution to PM 10 , PM 2.5 , and O 3 in the TP. The largest contribution of PM 10 (PM 2.5) from South Asian biomass burning emissions to PM 10 (PM 2.5) in the TP is 20.04% (18.37%) in the pre-monsoon season. Conversely, the lowest contribution of 0.58% (0.53) appears in the monsoon season. O 3 from South Asian biomass burning emissions contributes <1% to O 3 in the TP in each season, implying that the biomass burning emissions in South Asia have little effect on O 3 in the TP. This study is of great significance to the ecological environment protection for the TP. • Contributions of South Asian emissions to PM 10 , PM 2.5 , and O 3 in the TP are quantified. • Anthropogenic emissions in South Asia have a larger contribution to PM 10 , PM 2.5 , and O 3 in the TP. • O 3 from South Asian biomass burning emissions contributes <1% to O 3 in the Tibetan Plateau. [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]

Over the past few decades, the tropospheric ozone precursor anthropogenic emissions: nitrogen oxides (NOx) and reactive carbon (RC) from mid-latitude regions have been decreasing, and those from Asia and tropical regions have been increasing, leading to an equatorward emission redistribution. In this study, we quantify the contributions of various sources of NOx and RC emissions to tropospheric ozone using a source attribution technique during the 2000–2018 period in a global chemistry transport model: CAM4-Chem. We tag the ozone molecules with the source of their NOx or RC precursor emission in two separate simulations, one for each of NOx and RC. These tags include various natural (biogenic, biomass burning, lightning and methane), and regional anthropogenic (North American, European, East Asian, South Asian etc.) precursor emission sources. We simulate ~336 Tg O3 with an increasing trend of 0.91 Tg O3/yr (0.28 %/yr), largely contributed (and trend driven) by anthropogenic NOx emissions and methane. The ozone production efficiency of regional anthropogenic NOx emissions increases significantly when emissions decrease (Europe, North American and Russia-Belarus-Ukraine region's emissions) and decreases significantly when emissions increase (South Asian, Middle Eastern, International Shipping etc.). Tropical regions, despite smaller emissions, contribute more to tropospheric ozone burden compared to emissions from higher latitudes, consistent with previous work, due to large convection at the tropics thereby lifting O3 and its precursor NOx molecules into the free troposphere where ozone's lifetime is longer. We contrast the contribution to tropospheric ozone burden with that of the contribution to the global surface ozone. We simulate a smaller relative contribution from tropical regions to the global mean surface ozone compared to their contribution to the tropospheric ozone burden. The global population-weighted mean ozone (related to ozone exposure) is much larger compared to surface mean, mainly due to large anthropogenic emissions from densely populated regions: East Asia, South Asia, and other tropical regions, and a substantial contribution from international ship NOx emissions. The increasing trends in anthropogenic emissions from these regions are the main drivers of increasing global population-weighted mean ozone. [ABSTRACT FROM AUTHOR]

This study estimates the radiative forcing by biomass burning and dust aerosols over the Indian subcontinent, with emphasis on the Indo-Gangetic Plains (IGP) during the period from January 2021 to April 2021, based on multiple satellite and reanalysis datasets. In this respect, we used retrievals from the Moderate Resolution Spectroradiometer (MODIS) and the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) system, as well as reanalysis data from the Goddard Earth Observing System, version 5 (GEOS-5), the Modern-Era Retrospective analysis for Research and Applications, version 2 (MERRA-2), the Copernicus Atmosphere Monitoring Service (CAMS), and ERA-Interim. According to the MERRA-2 and the CAMS, the highest black carbon (BC) concentrations in January 2021 were 7–8 µg m−3, which were significantly lower than measurements performed in main cities along the IGP, such as Patiala, Delhi, and Kanpur. The meteorological data analysis accompanied by the CALIPSO lidar measurements showed that the vertical distribution of total attenuated backscatter (TAB) could reach altitudes of up to ~4–5 km and could be transported over the central Himalayan region. The spatial-averaged daily aerosol radiative forcing (ARF) values over the Indian subcontinent from January 2021 to April 2021 were found to range from −51.40 to −6.08 W m−2 (mean of −22.02 ± 9.19 W m−2), while on a monthly basis, the ARF values varied widely, from −146.24 to −1.63 W m−2 (mean of −45.56 ± 22.85 W m−2) over different parts of the study region. Furthermore, the spatial-averaged daily BC radiative forcing ranged from −2.23 to −0.35 (−1.01 ± 0.40 W m−2), while it varied from −15.29 to −0.31 W m−2 (−2.46 ± 2.32 W m−2) over different regions of southern Asia, indicating a rather small contribution to the total aerosol radiative effect and a large presence of highly scattering aerosols. Our findings highlight the importance of growing biomass burning, in light of recent climate change and the rapid decline in air quality over North India and the Indian Ocean. [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]

Devising effective national-level climate action plans needs a more detailed understanding of the regional distribution of sources and sinks of greenhouse gases. Due to insufficient observations and modelling capabilities, India's current carbon source-sink estimates are uncertain. This study uses a high-resolution transport model to examine the potential of CO2 observations over India for inverse estimation of regional carbon fluxes. We make use of four different sites in India that vary in measurement technique, frequency and spatial representation. These observations exhibit substantial seasonal (7.5 to 9.2 ppm) and intra-seasonal (2 to 12 ppm) variability. Our modelling approach, a high-resolution Weather Research and Forecasting Model combined with Stochastic Time Inverted Lagrangian Transport (WRF-STILT) model, performs better in simulating seasonal (R2 = 0.50 to 0.96) and diurnal (R2 = 0.96) variability of observed CO2 than the current generation global models analysed in the study. Representation of local flux variability like biomass burning in the model needs further refinement, depending on the site location. During the agricultural season, crop biospheric uptake in the Indo-Gangetic Plain region significantly modulates the CO2 variability in the northern Indian stations. Depending on the region and time of the year, the anthropogenic and biospheric emission components contribute differently to CO2 variability. The choice of emission inventory in the modelling framework alone leads to significant biases in simulations (5 to 10 ppm), endorsing the need for accounting emission fluxes, especially for non-background sites. By implementing a high-resolution model, our results emphasise that observations from Indian sites can be useful in deducing carbon flux information at regional (Nainital) and sub-urban to urban (Mohali, Shadnagar, Nagpur) scales. On accounting for observed variability, the global carbon data assimilation system can thus benefit from the measurements from the Indian subcontinent. [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]

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]

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]

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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]

Based on source-specific saccharide tracers, the characteristics of biomass burning (BB) and biogenic emissions of saccharides were investigated in three rural sites at Lincang, which is 65 % covered with forest in the southwest border of China. The total saccharides accounted for 8.4 ± 2.7 % of organic carbon (OC) and 1.6 ± 0.6 % of PM 2.5. The measured anhydrosugars accounted for 48.5 % of total saccharides, among which levoglucosan was the most dominant species. The high level of levoglucosan was both attributed to the local BB activities and biomass combustion smoke transported from the neighboring regions of Southeast Asia (Myanmar) and the northern Indian subcontinent. The measured mono- or disaccharides and sugar alcohols accounted for 24.9 ± 8.3 % and 26.6 ± 9.9 % of the total saccharides, respectively, and both proved to be mostly emitted by direct biogenic volatilization from plant material or surface soils rather than byproducts of polysaccharide breakdown during BB processes. Five sources of saccharides were resolved by non-negative matrix factorization (NMF) analysis, including BB, soil microbiota, plant senescence, airborne pollen, and plant detritus with contributions of 34.0 %, 16.0 %, 21.0 %, 23.7 %, and 5.3 %, respectively. The results provide information on the magnitude of levoglucosan and contributions of BB, as well as the characteristic of biogenic saccharides, at the remote sites of southwest China, which can be further applied to regional source apportionment models and global climate models. [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]

Open burning of crop residue is an important source of air pollution which is poorly characterized in South Asia. Currently, the gridded inventory reported by Global Fire Emissions Database for biomass burning including open burning of crop residue are of coarse resolution (0.25° × 0.25°), and may not be appropriate for a simulation for Nepal. This study develops a comprehensive high resolution (1 km × 1 km) gridded model-ready emissions inventory for Nepal to understand the spatial characteristics of air pollutant emissions from open burning. We estimate the national air pollutant emissions from crop residue burned between the years 2003 and 2017. The best available data on agricultural production, residue consumption patterns, agricultural burning parameters and emission factors were derived from secondary sources. The Monte Carlo method was used to estimate uncertainties. The mass of crop residue burned in 2016/17 was 2908 Gg (61–139%), which was 22% of the dry matter generated that year. By multiplying the burned crop residue mass by emission factors, the air pollutant emissions were estimated as 4140 for CO 2 (56–144%), 154 for CO (4–196%), 6.5 for CH 4 (7–193%), 1.2 for SO 2 (60–140%), 24.5 for PM 2.5 (30–170%), 8.6 for OC (38–162%), 2.2 for BC (-1-201%), 7 for NO x (54–146%), 22.5 for NMVOC (8–192%) and 2.7 for NH 3 (3–197%) in unit of Gg yr−1. More than 80% of air pollutants were generated during the months of February to May from the open burning of crop residue. The findings of this paper indicate that substantial reduction in open field burning would dramatically improve air quality in both the Terai region and other parts of Nepal and help reduce negative health impacts associated with the open burning of residue such as premature deaths, respiratory disease, and cardiovascular disease. GHGs, PM and traditional air pollutants increased from 2003 to 2017. • Highest emission flux is more in the Terai region followed by Hills and Mountain. • Highest emissions occurred in the month of April and zero from July to September. • Agricultural residue burning leads to severe health impact and regional warming. • Raising livestock could be potential mitigation measures to reduce open burning. [ABSTRACT FROM AUTHOR]

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

In complex atmospheric emission environments such as urban agglomerates, multiple sources control the ambient chemical composition driving air quality and regional climate. In contrast to pristine sites, where reliance on single or a few chemical tracers is often adequate for resolving pollution plumes and source influences, the comprehensive chemical fingerprinting of sources using non-methane hydrocarbons (NMHCs) and the identification of suitable tracer molecules and emission ratios becomes necessary. Here, we characterise and present chemical fingerprints of some major urban and agricultural emission sources active in South Asia, such as paddy stubble burning, garbage burning, idling vehicular exhaust and evaporative fuel emissions. A total of 121 whole air samples were actively collected from the different emission sources in passivated air sampling steel canisters and then analysed for 49 NMHCs (22 alkanes, 16 aromatics, 10 alkenes and one alkyne) using thermal desorption gas chromatography flame ionisation detection. Several new insights were obtained. Propane was found to be present in paddy stubble fire emissions (8 %), and therefore, for an environment impacted by crop residue fires, the use of propane as a fugitive liquefied petroleum gas (LPG) emission tracer must be done with caution. Propene was found to be ∼ 1.6 times greater (by weight) than ethene in smouldering paddy fires. Compositional differences were observed between evaporative emissions of domestic LPG and commercial LPG, which are used in South Asia. While the domestic LPG vapours had more propane (40 ± 6 %) than n -butane (19 ± 2 %), the converse was true for commercial LPG vapours (7 ± 6 % and 37 ± 4 %, respectively). Isoprene was identified as a new tracer for distinguishing paddy stubble and garbage burning in the absence of isoprene emissions at night from biogenic sources. Analyses of source-specific inter-NMHC molar ratios revealed that toluene/benzene ratios can be used to distinguish among paddy stubble fire emissions in the flaming (0.38 ± 0.11) and smouldering stages (1.40 ± 0.10), garbage burning flaming (0.26 ± 0.07) and smouldering emissions (0.59 ± 0.16), and traffic emissions (3.54 ± 0.21), whereas i -pentane / n -pentane can be used to distinguish biomass burning emissions (0.06–1.46) from the petrol-dominated traffic and fossil fuel emissions (2.83–4.13). i -butane / n -butane ratios were similar (0.20–0.30) for many sources and could be used as a tracer for photochemical ageing. In agreement with previous studies, i -pentane, propane and acetylene were identified as suitable chemical tracers for petrol vehicular and evaporative emissions, LPG evaporative and vehicular emissions and flaming-stage biomass fires, respectively. The secondary pollutant formation potential and human health impact of the sources was also assessed in terms of their hydroxyl radical (OH) reactivity (s -1), ozone formation potential (OFP; gO 3 /gNMHC) and fractional benzene, toluene, ethylbenzene and xylenes (BTEX) content. Petrol vehicular emissions, paddy stubble fires and garbage fires were found to have a higher pollution potential (at ≥95 % confidence interval) relative to the other sources studied in this work. Thus, many results of this study provide a new foundational framework for quantitative source apportionment studies in complex emission environments. [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]

Here we present results from an evaluation of model simulations from the International Hemispheric Transport of Air Pollution Phase II (HTAPII) and Chemistry Climate Model Initiative (CCMI) model inter-comparison projects against a comprehensive series of ground-based, aircraft and satellite observations of ozone mixing ratios made at various locations across India. The study focuses on the recent past (observations from 2008 to 2013, models from 2009–2010) as this is most pertinent to understanding the health impacts of ozone. To our understanding this is the most comprehensive evaluation of these models' simulations of ozone across the Indian subcontinent to date. This study highlights some significant successes and challenges that the models face in representing the oxidative chemistry of the region. The multi-model range in area-weighted surface ozone over the Indian subcontinent is 37.26–56.11 ppb, whilst the population-weighted range is 41.38–57.5 ppb. When compared against surface observations from the Modelling Atmospheric Pollution and Networking (MAPAN) network of eight semi-urban monitoring sites spread across India, we find that the models tend to simulate higher ozone than that which is observed. However, observations of NOx and CO tend to be much higher than modelled mixing ratios, suggesting that the underlying emissions used in the models do not characterise these regions accurately and/or that the resolution of the models is not adequate to simulate the photo-chemical environment of these surface observations. Empirical orthogonal function (EOF) analysis is used in order to identify the extent to which the models agree with regards to the spatio-temporal distribution of the tropospheric ozone column, derived using OMI-MLS observations. We show that whilst the models agree with the spatial pattern of the first EOF of observed tropospheric ozone column, most of the models simulate a peak in the first EOF seasonal cycle represented by principle component 1, which is later than the observed peak. This suggests a widespread systematic bias in the timing of emissions or some other unknown seasonal process. In addition to evaluating modelled ozone mixing ratios, we explore modelled emissions of NOx , CO, volatile organic compounds (VOCs) and the ozone response to the emissions. We find a high degree of variation in emissions from non-anthropogenic sources (e.g. lightning NOx and biomass burning CO) between models. Total emissions of NOx and CO over India vary more between different models in the same model intercomparison project (MIP) than the same model used in different MIPs, making it impossible to diagnose whether differences in modelled ozone are due to emissions or model processes. We therefore recommend targeted experiments to pinpoint the exact causes of discrepancies between modelled and observed ozone and ozone precursors for this region. To this end, a higher density of long-term monitoring sites measuring not only ozone but also ozone precursors including speciated VOCs, located in more rural regions of the Indian subcontinent, would enable improvements in assessing the biases in models run at the resolution found in HTAPII and CCMI. [ABSTRACT FROM AUTHOR]

The source and sinks of carbon dioxide (CO2) and methane (CH4) due to anthropogenic and natural biospheric activities were estimated for the South Asian region (Bangladesh, Bhutan, India, Nepal, Pakistan and Sri Lanka). Flux estimates were based on top-down methods that use inversions of atmospheric data, and bottom-up methods that use field observations, satellite data, and terrestrial ecosystem models. Based on atmospheric CO2 inversions, the net biospheric CO2 flux in South Asia (equivalent to the Net Biome Productivity, NBP) was a sink, estimated at -104±150 TgCyr-1 during 2007-2008. Based on the bottom-up approach, the net biospheric CO2 flux is estimated to be -191±193 TgCyr -1 during the period of 2000-2009. This last net flux results from the following flux components: (1) the Net Ecosystem Productivity, NEP (net primary production minus heterotrophic respiration) of -220±186 TgCyr -1 (2) the annual net carbon flux from land-use change of -14±50 TgCyr -1, which resulted from a sink of -16 TgCyr -1 due to the establishment of tree plantations and wood harvest, and a source of 2 TgCyr -1 due to the expansion of croplands; (3) the riverine export flux from terrestrial ecosystems to the coastal oceans of +42.9 TgCyr -1; and (4) the net CO2 emission due to biomass burning of +44.1±13.7 TgCyr -1. Including the emissions from the combustion of fossil fuels of 444 TgCyr -1 for the 2000s, we estimate a net CO2 land--atmosphere flux of 297 TgCyr -1. In addition to CO2, a fraction of the sequestered carbon in terrestrial ecosystems is released to the atmosphere as CH4. Based on bottom-up and top-down estimates, and chemistry-transport modeling, we estimate that 37±3.7 TgC-CH4 yr -1 were released to atmosphere from South Asia during the 2000s. Taking all CO2 and CH4 fluxes together, our best estimate of the net land--atmosphere CO2-equivalent flux is a net source of 334 TgCyr-1 for the South Asian region during the 2000s. If CH4 emissions are weighted by radiative forcing of molecular CH4, the total CO2-equivalent flux increases to 1148 TgCyr -1 suggesting there is great potential of reducing CH4 emissions for stabilizing greenhouse gases concentrations. [ABSTRACT FROM AUTHOR]

We measured black carbon (BC) with a seven-wavelength aethalometer (AE-31) at the Nam Co Lake (NCL), the hinterland of the Tibetan Plateau (TP) from May 2015 to April 2016. The daily average concentration of BC was 145 ± 85 ng m−3, increasing by 50% since 2006. The seasonal variation of BC shows higher concentrations in spring and summer and lower concentrations in autumn and winter, dominated by the adjacent sources and meteorological conditions. The diurnal variation of BC showed that its concentrations peaked at 9:00–16:00 (UTC + 8), significantly related to local human activities (e.g., animal-manure burning and nearby traffic due to the tourism industry). The concentration-weighted trajectory (CWT) analysis showed that the long-distance transport of BC from South Asia could also be a potential contributor to BC at the NCL, as well as the biomass burning by the surrounding residents. The analyses of the absorption coefficient and absorption Ångström exponent show the consistency of sourcing the BC at the NCL. We suggest here that urgent measures should be taken to protect the atmospheric environment at the NCL, considering the fast-increasing concentrations of BC as an indicator of fuel combustion. [ABSTRACT FROM AUTHOR]

The influence of local meteorology and convection activities on the vertical distribution of carbon monoxide (CO) over Chennai in southern India was investigated by analysing the measurements of ozone aboard airbus in-service aircraft observations during the years 2012–2013. The seasonal variation of CO in the free troposphere was observed to be different and less pronounced than that in the planetary boundary layer (PBL). The near surface mixing ratio of CO was the highest ( 190 ± 68 ppbv ) during winter, while enhanced values ( 117 ± 11 ppbv ) in the free troposphere were observed during post-monsoon. The mixing ratios were the lowest throughout the troposphere during the monsoon. In the PBL, the mixing ratios of CO showed a decline with an increase in wind speed and were the highest ( > 200 ppbv ) under stagnant conditions ( 1 - 2 m s - 1 ) during winter. The higher CO in the lower free troposphere during the pre-monsoon period is attributed to the stronger biomass burning emissions. In the middle–upper troposphere, higher levels of CO during post-monsoon are due to the enhanced vertical mixing of regional emissions associated with weaker wind shears and frequent convection activities. Overall, the contrasting effects of stronger CO emissions can be observed in winter/pre-monsoon, while the efficient vertical mixing during the monsoon/post-monsoon season governs the observed seasonality of CO. The model for ozone and related chemical tracers, version 4 (MOZART-4) provides a reasonable representation of the convection effect on the CO mixing ratio. This study highlights a need to conduct more observations, especially of aircraft-borne instruments, to understand the effects of regional-scale emissions and dynamics in the middle–upper tropospheric chemistry over South Asia. [ABSTRACT FROM AUTHOR]