Lumbini isa world heritage site located in the southern plains region of Nepal, and is regarded as a potential site for evaluating transboundary air pollution due to its proximity to the border with India. In this study, 82 aerosol samples were collected between April 2013 and July 2014 to investigate the levels of particulate-bound mercury (PBM) and the corresponding seasonality, sources, and influencing factors. The PBM concentration in total suspended particulate (TSP) matter ranged from 6.8 pg m-3 to 351.7 pg m-3 (mean of 99.7 +/- 92.6 pg m-3), which exceeded the ranges reported for remote and rural sites worldwide. The Hg content (PBM/TSP) ranged from 68.2 ng g-1 to 1744.8 ng g-1 (mean of 446.9 +/- 312.7 ng g-1), indicating anthropogenic enrichment. The PBM levels were higher in the dry season (i.e., winter and the pre-monsoon period) than in the wet season (i.e., the monsoon period). In addition, the d202Hg signature indicated that waste/coal burning and traffic were the major sources of Hg in Lumbini during the pre-monsoon period. Meanwhile, precipitation occurring during photochemical processes in the atmosphere may have been responsible for the observed D199Hg values in the aerosol samples obtained during the monsoon period. The PBM concentration was influenced mostly by the resuspension of polluted dust during dry periods and crop residue burning during the post-monsoon period. The estimated PBM deposition flux at Lumbini was 15.7 lg m-2 yr-1. This study provides a reference dataset of atmospheric PBM over a year, which can be useful for understanding the geochemical cycling of Hg in this region of limited data. (c) 2021 China University of Geosciences (Beijing) and Peking University. Production and hosting by Elsevier B.V. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/ licenses/by-nc-nd/4.0/).

A comprehensive investigation of physical, optical, and chemical characteristics of columnar aerosols over two locations with distinct environmental settings in the Indo-Gangetic Plain (IGP) region, namely, Kanpur (urban and industrial area) and Gandhi College (rural area), is conducted using high-quality aerosol datasets obtained from ground-based Aerosol Robotic Network (AERONET) observations during the recent five year period (2015-2019). This study utilizes all the crucial columnar aerosol parameters necessary for accurately estimating aerosol radiative forcing. Quantification of contribution by different aerosol species originating from natural and anthropogenic sources to the total aerosol optical depth (AOD) and single scattering albedo (SSA) is important to understand the specific mechanisms that influence the aerosol composition, thereby reducing the uncertainty in aerosol radiative forcing. For the first time, two highly spatially resolved models' (Modern-Era Retrospective Analysis for Research and Applications-2 (MERRA-2) and Copernicus Atmosphere Monitoring Service (CAMS)) simulated absorbingspecies-wise (black carbon (BC), dust, and brown carbon (BrC)) AOD, and absorption AOD (AAOD) are compared and contrasted against the AERONET observations over the IGP region in a systematic manner. MERRA-2 AODs are mostly lower, whereas CAMS AODs are consistently higher than the AERONET AODs. A comparison of collocated time and space observations with models clearly suggests that improvements in emission inventories on a seasonal scale are essential. MERRA-2 SSA is noted lower than the AERONET SSA during the winter season due to overestimation in BC AOD. During winter in >70% of MERRA-2 simulated SSA the difference is higher than +/- 0.03 (the uncertainty range of AERONET SSA) whereas during pre-monsoon and monsoon seasons >60% of MERRA-2 SSA lies within the uncertainty range of AERONET SSA. Both models show a gradient in AODDust decreasing from west to east in the IGP. However, observations do not often exhibit the gradient in dust, which is validated by air mass back trajectory analyses as air masses travel through different pathways to IGP and reverse the west to east gradient in AODDust. This quantitative and comparative collocated analysis of observed aerosol characteristics with models on a seasonal scale will enable a better estimation of aerosol radiative forcing, and can help improve aerosol processes and parameterizations in models.

The significant uncertainty associated with black carbon (BC) radiative forcing estimation is mainly due to discrepancies related to its mixing state. The in situ measurement-based understanding of absorption properties is limited to only a few locations worldwide, primarily as a result of the unavailability of sophisticated instrumentations for absorption enhancement (Eabs) measurements resulting from mixing with non-BC chemicals. Therefore, we have proposed an alternative approach for a more robust in situ measurement of absorption enhancement using a thermal-optical carbon analyzer. In the present study, the absorption spectra during different stages of thermal-optical carbon analysis were used to estimate the absorption coefficients of mixed and pure BC aerosols. Moreover, we have also explored the possibility of apportioning light absorption by the BC core and absorbing organics (brown carbon). The present method was applied on a few ground-based aerosol samples collected at two distinct Indo-Gangetic Plain (IGP) sampling stations. Eabs at 808 nm was observed to be approximately 1.2 at both of the sampling sites. Interestingly, the absorbing brown carbon chromophores showed a wide range of absorption in the ultraviolet to near-infrared wavelengths with minimum absorption at 635 nm. Thus, the present study suggests that the absorption of organics in near-infrared wavelengths cannot be neglected.

This study investigates the long-term (2003-2019) variations of high aerosol loading days and their radiative impacts over the western Indo-Gangetic Plain (IGP) and eastern IGP during pre-monsoon season (March-April-May-June). The Aerosol Optical Depth (AOD) climatology from MODIS (Terra and Aqua) and MERRA-2 reanalysis shows high aerosol burden across the IGP region during the pre-monsoon season. The high aerosol loading days are identified based on a standardized AOD anomaly approach, from MODIS and MERRA-2. The frequency of high aerosol loading days over the western IGP is roughly twice that of the total number of high aerosol loading days over the eastern IGP. The area-averaged percentage differences in AOD between high aerosol loading days and normal days over western IGP is always higher, about 6-8%, than eastern IGP from Terra, Aqua and MERRA-2. The natural (mainly dust) and anthropogenic aerosols (particularly sulfate, black carbon and organic carbon) are majorly contributed to total AOD over western IGP and eastern IGP. Furthermore, the MERRA-2 and ERA5 composite surface and 850 hPa wind anomalies show that strong westerly winds dominate, transporting dust aerosols from arid regions to the western IGP. On the other hand, weak prevailing winds and background pre-monsoonal cyclonic circulations over eastern IGP favor the accumulation of regionally emitted aerosols. During high aerosol loading days, the decrease in ventilation coefficient indicates the high aerosol burden (less dispersion) over both the regions, leading to the deterioration of air quality. The enhanced aerosol loading induced potential atmospheric radiative forcing (19.78 Wm(-2) over western IGP and 20.77 Wm(-2) over eastern IGP) during high aerosol loading days compared to normal days (11.12 Wm(-2) and 12.9 Wm(-2)).

Total suspended particles (TSP) were collected in Lumbini from April 2013 to March 2016 to better understand the characteristics of carbonaceous aerosol (CA) concentrations, compositions and sources and their light absorption properties in rural region of severe polluted Indo-Gangetic Plain (IGP). Extremely high TSP (203.9 +/- 109.6 mu g m(-3)), organic carbon (OC 32.1 +/- 21.7 mu g m(-3)), elemental carbon (EC 6.44 +/- 3.17 mu g m(-3)) concentrations were observed in Lumbini particularly during winter and post-monsoon seasons, reflecting the combined influences of emission sources and weather conditions. SO42- (7.34 +/- 4.39 mu g m(-3)) and Ca2+ (5.46 +/- 5.20 mu g m(-3)) were the most dominant anion and cation in TSP. These components were comparable to those observed in urban areas in South and East Asia but significantly higher than those in remote regions over the Himalayas and Tibetan Plateau, suggesting severe air pollution in the study region. Various combustion activities including industry, vehicle emission, and biomass burning are the main reasons for high pollutant concentrations. The variation of OC/EC ratio further suggested that biomass such as agro-residue burning contributed a lot for CA, particularly during the non-monsoon season. The average mass absorption cross- of EC (MAC(EC)) and water-soluble organic carbon (MAC(WSOC)) were 7.58 +/- 3.39 and 1.52 +/- 0.41 m(2) g(-1), respectively, indicating that CA in Lumbini was mainly affected by local emissions. Increased biomass burning decreased MAC(EC); whereas, it could result in high MAC(WSOC) during the non-monsoon season. Furthermore, dust is one important factor causing higher MAC(WSOC) during the pre-monsoon season.

The sub-daily variability of aerosols affects the estimates of daily mean aerosol loading. However, large spatial scale estimates of their climate effects are mostly based on snapshots from low orbit satellites that may bias the mean estimate for daily, monthly, or annual timescales. In this study, an attempt is made to estimate the magnitude of such bias based on ground and satellite-based datasets. Using ground-based measurements, we show an apparent asymmetry (of the order of 10-50%) in the sub-daily variability of aerosol loading over the Indian region. For the first time, it is reported that this sub-daily variability has a spatial pattern with an increasing amplitude toward the east of the subcontinent. We also find this variability in aerosol loading is well-captured by the satellites but with a lower amplitude. Our study shows that such differences could alter the annual surface radiative forcing estimates by more than similar to 15 W m(-2) over this region. We find that NASA's Modern-Era Retrospective analysis for Research and Applications version 2 (MERRA-2), a state-of-the-art model-based chemical reanalysis, is unable to capture these sub-daily variabilities. This implies that both model and satellite-based radiative forcing estimates for large spatial scales should improve aerosol sub-daily information/variabilities for obtaining reliable radiative forcing estimates.

The Indo Gangetic Plain (IGP), one of the most densely populated regions of the world, is a global hotspot of anthropogenic aerosol emissions. In the pre-monsoon season (March-May), the strong westerlies carry transported dust aerosols along with anthropogenic aerosols onto the Bay of Bengal (BoB). The outflow from IGP modulates the aerosol loading and the aerosol direct radiative forcing (ADRF) over the BoB. The quantification of the anthropogenic aerosol impact on the radiative forcing over the outflow region remains inadequate. The enforced shutdown amid the COVID-19 pandemic eased the anthropogenic activities across the country, which helped to examine the magnitude and variability of aerosol loading and subsequent changes in ADRF over IGP and the outflow region of the BoB. Wind trajectory analysis illustrates that the ADRF over the BoB is greater during the days when the winds originated from the IGP region (at the surface-54.2 +/- 6.4 Wm(-2), at the top of the atmosphere,-26.9 +/- 3.4 Wm(-2) and on the atmosphere, 27.0 +/- 3.1 Wm(-2)) compared to the seasonal average (-46.3 +/- 7.1 Wm(-2),-24.9 +/- 4.0 W m(-2) and 20.6 +/- 3.2 Wm(-2), respectively). This indicates that anthropogenic aerosols emission from IGP can contribute an additional 31% of the atmospheric ADRF over the IGP outflow region of the BoB. The reduced aerosol loading during the shutdown period resulted in a reduction of ADRF at the surface, at the top of the atmosphere, and on the atmosphere over the IGP outflow region of the BoB by 22.0 +/- 3.1%, 20.9 +/- 3.4% and 23.2 +/- 3.3%, respectively. This resultant 20-25% reduction in ADRF over the IGP outflow region of BOB matches well with 10-25% reduction in aerosol optical depth (AOD) over the IGP during the shutdown period showing a robust coupling between IGP aerosol emissions and ADRF over the BoB. (C) 2021 Elsevier B.V. All rights reserved.

Mercury (Hg) is among the most toxic metals possessing a major threat to human health and aquatic ecosystems over the globe. However, measurement of Hg concentrations and seasonal variability remain poorly understood over the IndoGangetic Plain (IGP) in northern India. In this study, we present one-year data of particulate-bound mercury (HgP) in aerosol samples (PM10) collected from Kanpur to understand seasonal variability and factors influencing concentration, as well as dry deposition flux. The HgP concentration exhibit a large temporal variability and ranged between 100 (on 14 June 2007) to 4340 pg m(-3) (on 4 March 2007) with an annual average concentration of HgP is 776 +/- 846 pg m(-3). The HgP concentrations and HgP/PM10 ratios showed a marked seasonality with the highest in winter (Dec-Feb) followed by post-monsoon (Oct-Nov) and summer (April-June) seasons. HgP and HgP/PM10 were positively correlated (r(2) = 0.77, p < 0.05, N = 58) during the sampling period and the estimated dry deposition flux of HgP was 104.7 mu g m(-2) y(-1). Although this study provides a comprehensive data set on HgP in an urban atmosphere of the IGP revealing high levels of HgP, measurement of gaseous Hg is needed for estimation of the total Hg budget. Therefore, future studies should focus on identification of different sources as well as emission characteristics of all forms of Hg (organic and inorganic forms) for better mitigation strategy to prevent health risks associated with toxic Hg in the region.

The tropospheric NO2 concentration from OMI AURA always shows high concentrations of NO2 at a few locations in India, one of the high concentrations of NO2 hotspots is associated with the locations of seven coal-fired Thermal Power plants (TPPs) in Singrauli. Emissions from TPPs are among the major sources of black carbon (BC) soot in the atmosphere. Knowledge of BC emissions from TPPs is important in characterizing regional carbonaceous particulate emissions, understanding the fog/haze/smog formation, evaluating regional climate forcing, modeling aerosol optical parameters and concentrations of black carbon, and evaluating human health. Furthermore, elevated BC concentrations, over the Indo-Gangetic Plain (IGP) and the Himalayan foothills, have emerged as an important subject to estimate the effects of deposition and atmospheric warming of BC on the accelerated melting of snow and glaciers in the Himalaya. For the first time, this study reports BC concentrations and aerosol optical parameters near dense coal-fired power plants and open cast coal mining adjacent to the east IGP. In-situ measurements were carried out in Singrauli (located in south-east IGP) at a fixed site about 10 km from power plants and in transit measurements in close proximity to the plants, for few days in the month of January and March 2013. At the fixed site, BC concentration up to the 95 mu gm(-3) is observed with strong diurnal variations. BC concentration shows two maxima peaks during early morning and evening hours. High BC concentrations are observed in close proximity to the coal-fired TPPs (>200 mu gm(-3)), compared to the outside domain of our study region. Co-located ground-based sunphotometer measurements of aerosol optical depth (AOD) show strong spatial variability at the fixed site, with AOD in the range 0.38-0.58, and the highest AOD in the range 0.7-0.95 near the TPPs in transit measurements (similar to the peak of BC concentrations). Additionally, the Angstrom exponent was found to be in the range 0.4-1.0 (maximum in the morning time) and highest in the proximity of TPPs (similar to 1.0), suggesting abundance of fine particulates, whereas there was low Angstrom exponent over the surrounding coal mining areas. Low Angstrom exponent is characterized by dust from the unpaved roads and nearby coal mining areas. MODIS derived daily AOD shows a good match with the MICROTOPS AOD. The CALIPSO derived subtypes of the aerosol plot shows that the aerosols over Singrauli region are mainly dust, polluted dust, and elevated smoke. The preliminary study for few days provides information about the BC concentrations and aerosol optical properties from Singrauli (one of the NO2 hotspot locations in India). This preliminary study suggests that long-term continuous monitoring of BC is needed to understand the BC concentrations and aerosol optical properties for better quantification and the estimation of the emission to evaluate radiative forcing in the region.

We present the systematic analysis of individual black carbon (BC) mixing state and its impact on radiative forcing from an urban Indian city, Kanpur, located in Indo-Gangetic Plain (IGP). Simultaneous measurements using Single Particle Soot Photometer (SP2), Photo-Acoustic Soot Spectrometer (PASS-3) and High-Resolution Time-of-Flight Aerosol Mass Spectrometer (AMS) were conducted from 8 January 2015 to 28 February 2015 at Kanpur. BC mass and number concentrations varied between 0.7 and 17 mu g/m(3) and 277-5866 #/cm(3) with a mean of 4.06 mu g/m3 and 1314 #/cm3, respectively. The diurnal variation of BC mass concentration showed a traffic hour peak during both the morning and late night. The mean fraction of thickly coated BC particles (fTC(Bc)) was found to be 61.6%, indicating that a large fraction of BC particles was internally mixed. The fTCBc increased after sunrise with a peak at about noontime, indicating that the formation of secondary organic aerosol under active photochemistry can enhance organic coating on a core of black carbon. High-resolution positive matrix factorization (HR-PMF) factors showed distinct characteristics with fTCBc. While primary organic aerosols like cooking organic aerosols (COA) and biomass burning organic aerosols (BBOA) were negatively correlated with fTCBc = -0.78 and -0.51, respectively), aged low volatile oxygenated organic aerosol (LVOOA) was forming a coating over BC (r = 0.6). Similar positive correlation of fTCBc with inorganic species like ammonium (r = 0.58) and nitrate (r = 0.47) further suggested that BC appears to be largely coated with LVOOA, ammonium, and nitrate. A positive correlation between the fTCBc and the mass absorption cross- at 781 nm (MAC(781)) was also observed (r = 0.58). Our results suggest that the observed fTCBc could amplify the MAC781 approximately by a factor of 1.8, which may catalyze the positive radiative forcing in the IGP.