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.

Chemical composition of aerosols is of great concern in the Arctic because of its great influence on climate. In this communication, we report the physico-chemical properties of size-separated aerosol data archived at Gruvebadet lab in Ny-& Aring;lesund (78.55 degrees S, 11.55 degrees E) as a part of the Indian Arctic Mission over the station "Himadri" in 2010. The results reveal that the mass-size distribution (MSD) of aerosol composition exhibits tri-modal distribution with coarse-mode (62%), fine-mode (32%) and weak nucleation-mode (6%) indicating dominance of natural sources over the study region. MSD of chemical components showed a significant contribution to coarse-mode particles for Ca2+ ,Mg2+ ,Na+ and Cl -; fine-mode particles for SO42 -, NO3 -, NH4 + and K + . The marine sources contributed maximum for SO 42- (89%) and Mg2+ (44%) in the coarse fraction, and in the fine fraction, 31% to SO 42- and 86% to Mg2+. Non-marine sources were major contributors (80 to 95%) in both mode fractions for Ca2 + and K + . The estimated aerosol radiative forcing in the atmosphere of similar to 3.21 W/m2 could be attributed to the loading of black carbon aerosols (62%) over the site. The backward trajectories show air masses from Canada and Greenland travelling from 6000 m elevation, bringing the pollutants to Ny-& Aring;lesund and lower altitudes; the oceanic region within Arctic circle contributes more.

The variability and trend of ozone (O3) in the Upper troposphere and Lower Stratosphere (UTLS) over the Asian region needs to be accurately quantified. Ozone in the UTLS radiatively heats this region and cools the upper parts of the stratosphere. This results in an impact on relative humidity, static stability in the UTLS region and tropical tropopause temperature. A major challenge for understanding ozone chemistry in the UTLS is sparse observations and thus the representation of precursor gases in model emission inventories. Here, we evaluate ozonesonde measurements during August 2016 at Nainital, in the Himalayas, against ozone from multiple reanalyses and the ECHAM6-HAMMOZ model. We find that compared to measurements both reanalyses and ECHAM6-HAMMOZ control simulation overestimate ozone mixing ratios in the troposphere (20 ppb) and in the UTLS (55 ppb). We performed sensitivity simulations using the ECHAM6-HAMMOZ model for a 50% reduction in the emission of (1) NOx and (2) VOCs. The model simulations with NOX reduction agree better with the ozonesonde observations in the lower troposphere and in the UTLS. Thus, neither reanalyses nor ECHAM6-HAMMOZ results can reproduce observed O3 over the South Asian region. For a better representation of O3 in the ECHAM6-HAMMOZ model, NOX emission should be reduced by 50% in the emission inventory. A larger number of observations of ozone and precursor gases over the South Asian region would improve the assessment of ozone chemistry in models.

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 %).

In this study, we investigate the temporal variations in columnar aerosol pollutants and their possible association with the simultaneously measured black carbon (BC) aerosol mass concentration and associated biomass burning (BB) over urban (Delhi) and rural (Panchgaon) sites during the lockdown phases of the COVID-19 pandemic. We also show the impact of lockdown measures on boundary layer ozone and its primary precursors, NO 2 , and water vapor (H 2 O), potent greenhouse gases that destroy protective ozone. For this purpose, we used multiple datasets, namely, black carbon (BC) aerosol mass concentration and biomass burning (BB) aerosols using an aethalometer at Amity University Haryana (AUH), Panchgaon, India, and satellite retrievals from NASA’s MODIS and OMI at both the stations. The analysis was conducted during the pre-lockdown period (1–25 March), lockdown 1st phase (25 March–14 April), lockdown 2nd phase (15 April–3 May), lockdown 3rd phase (4–17 May), lockdown 4th phase (18–31 May), and post-lockdown (1–30 June) period in 2020. Our diagnostic analysis shows a substantial reduction in AOD (Delhi: −20% to −80%, Panchgaon: −20% to −80%) and NO 2 (Delhi: −10% to −42.03%, Panchgaon −10% to −46.54%) in comparison with climatology (2010–2019) during all four phases of lockdown. The reduction in AOD is attributed to lockdown measures and less transport of dust from west Asia than climatology. Despite a reduction in NO 2, there is an increase in the ozone amount (Delhi: 1% to 8% and Panchgaon: 1% to 10%) during lockdown I, II, and III phases. The observed enhancement in ozone may be resultant from the complex photochemical processes that involve the presence of NO 2 , CO, volatile organic compounds (VOCs), and water vapor. The reduction in AOD and NO 2 and enhancement in ozone are stronger at the rural site, Panchgaon than that at the urban site, Delhi.

Accumulation of water vapor in the upper troposphere/lower stratosphere (UT/LS) over the Asian continent is a recognized feature during the boreal summer monsoon. While there has been a debate on the role of monsoon convective intensities on the UT/LS water vapor accumulations, there are ambiguities with regard to the effects of organized monsoon convection on the spatial distribution of water vapor. We provide insights into this aspect using high precision balloon measurements of water vapor from a high-elevation site Nainital (29.4° N, 79.5° E), India, located in the Himalayan foothills and satellite retrievals of water vapor from the Microwave Limb Sounder (MLS). We also use precipitation estimates from the Tropical Rainfall Measuring Mission (TRMM) satellite (i.e., merged product 3B42 and precipitation radar 3A25 estimates of rain rate and rain type viz convective/stratiform), reanalysis circulation data, as well as numerical model simulations. We first evaluate the MLS estimates of water vapor mixing ratios with in situ high precision hygrometer balloon observations over Nainital. It is seen from our analyses of the MLS data that the LS water vapor distribution is closely linked to the organization of the South Asian monsoon convection and its influence on the UT/LS circulation. This link between LS water vapor distribution and organized monsoon convection is also captured in the in situ observations on 3 August 2016. It is evidenced that periods of organized summer monsoon convective activity over the Indian subcontinent and Bay of Bengal promote divergence of water vapor flux in the UT/LS; additionally the Tibetan anticyclonic circulation causes widespread distribution of the UT/LS water vapor. In addition to the effects of Asian monsoon convection, we also note that global climate drivers such as El Niño-Southern Oscillation (ENSO), Brewer–Dobson circulation (BDC), and Quasi-Biennial Oscillation (QBO) can contribute to nearly 38% of the UT/LS water vapor variability over the Asian monsoon region. The main result of our study indicates that widespread spatial distribution and accumulation of water vapor in the LS (about 80% of total accumulation between May and August months) tend to co-occur with organized monsoon convection, intensified divergence of water vapor flux in the UT/LS and intensified Tibetan anticyclone. On the other hand, the circulation response and LS water vapor distribution to pre-monsoon localized deep convection tend to have a limited spatial scale confined to Southeast Asia. Results from model experiments suggest that the UT/LS circulation pattern to organized monsoon convection has resemblance to stationary Rossby waves forced by organized latent heating, with the westward extending response larger by about 15° longitudes as compared to that of the pre-monsoon localized deep convection.

The Magee Scientific Model AE33 Next Generation Aethalometer, installed at Amity University Haryana (AUH), Panchgaon (rural station) has been operated round-the-clock and obtained highresolution (1-5 Minutes) observations of Black Carbon (BC) mass concentration at seven different sensing wavelengths (ranging from UV to NIR). For each observation, contribution from Biomass Burning (BB, in percent) to the BC has also been recorded. These measurements have been analyzed to segregate different sources, responsible for BC at this rural station. The results reveal that the major contributor is 'traffic' (fossil-fuel diesel emissions), followed by 'biomass smoke', wood-burning activities. The diurnal variation in BC and associated BB over this study area reveals a significant maximum around 0900 h and minimum around 1600 h. These maximum and minimum concentrations are attributed to transport activities during morning and ascending of local atmospheric boundary-layer height. The results also exhibit a strong affinity between BC mass concentration and coincident CO2 and PM2.5 mass concentrations. Synchronous BC measurements have also been organized over two more locations, namely, Bhopal (urban station) and Mahabaleshwar (high-altitude station). The black carbon aerosol transport through long-range air mass back-trajectories is explained.

The AErosol RObotic NETwork (AERONET) is the most developed ground-based network for aerosol remote sensing and has been playing a significant role not only in monitoring air quality for protecting human health but also in assessing the radiative budget of our planet Earth. In this paper, we report the direct-Sun and inversion products, comprising of spectral variation of aerosol optical depth (AOD), associated Ångström exponent (AE), fine- and coarse-mode aerosol fractions, aerosol size distribution (ASD), refractive index (RI), asymmetry parameter (AP), single scattering albedo (SSA), aerosol radiative forcing (ARF) and columnar concentration of gas constituents such as water vapor (H2O), obtained from a Cimel Sun–sky radiometer, functioning in Pune, India, under the AERONET program since October 2004. These long-term measurements carried out from 2005 to 2015 could serve as an urban aerosol optical long-term average or climatology. The AOD long-term variations at all wavelengths, considered in the study, exhibited an increasing trend, implying year-to-year enhancement in aerosol loading. The mean seasonal variations in AOD from cloud-free days indicated greater values during the monsoon season, revealing dominance of hygroscopic aerosol particles over the station. Contribution by different aerosol types to AOD has also been deduced and discussed, and dominance of a mixed type of aerosols (44.85 %) found, followed by combination of biomass burning and urban industrial aerosols (22.57 %) compared to other types of aerosols during the study period. The long-term datasets, derived aerosol and trace gas products play a significant role in understanding aerosol climate forcing, trends and evaluation of regional air pollution and validation of aerosol transport models over the study region.

The South Asian summer monsoon is associated with a large-scale anticyclonic circulation in the upper troposphere and lower stratosphere (UTLS), which confines the air mass inside. During boreal summer, the confinement of this air mass leads to an accumulation of aerosol between about 13 and 18 km (360 and 440 K potential temperature); this accumulation of aerosol constitutes the Asian Tropopause Aerosol Layer (ATAL). We present balloon-borne aerosol backscatter measurements of the ATAL performed by the Compact Optical Backscatter Aerosol Detector (COBALD) instrument in Nainital in northern India in August 2016, and compare these with COBALD measurements in the post-monsoon time in November 2016. The measurements demonstrate a strong variability of the ATAL's altitude, vertical extent, aerosol backscatter intensity and cirrus cloud occurrence frequency. Such a variability cannot be deduced from climatological means of the ATAL as they are derived from satellite measurements. To explain this observed variability we performed a Lagrangian back-trajectory analysis using the Chemical Lagrangian Model of the Stratosphere (CLaMS). We identify the transport pathways as well as the source regions of air parcels contributing to the ATAL over Nainital in August 2016. Our analysis reveals a variety of factors contributing to the observed day-to-day variability of the ATAL: continental convection, tropical cyclones (maritime convection), dynamics of the anticyclone and stratospheric intrusions. Thus, the air in the ATAL is a mixture of air masses coming from different atmospheric altitude layers. In addition, contributions from the model boundary layer originate in different geographic source regions. The location of the strongest updraft along the backward trajectories reveals a cluster of strong upward transport at the southern edge of the Himalayan foothills. From the top of the convective outflow level (about 13 km; 360 K) the air parcels ascend slowly to ATAL altitudes within a large-scale upward spiral driven by the diabatic heating in the anticyclonic flow of the South Asian summer monsoon at UTLS altitudes. Cases with a strong ATAL typically show boundary layer contributions from the Tibetan Plateau, the foothills of the Himalayas and other continental regions below the Asian monsoon. Weaker ATAL cases show higher contributions from the maritime boundary layer, often related to tropical cyclones, indicating a mixing of clean maritime and polluted continental air. On the one hand increasing anthropogenic emissions in the future are expected due to the strong growth of Asian economies; on the other hand the implementation of new emission control measures (in particular in China) has reduced the anthropogenic emissions of some pollutants contributing to the ATAL substantially. It needs to be monitored in the future whether the thickness and intensity of the ATAL will further increase, which will likely impact the surface climate.

Black carbon (BC) mass concentration observations were carried out using Aethalometer (AE-33) at an urban site Pune and at a high altitude forest site Mahabaleshwar during April 2018 to February 2019. The annual averaged BC mass concentration over Pune was observed to be ~2.8 times higher than Mahabaleshwar. Daily, seasonal and diurnal variations of BC over these two different environments were compared. The effect of meteorological parameters on the BC was also evaluated. Planetary boundary layer (PBL) plays a pivotal role in diluting the atmospheric pollutant BC during daytime at Pune, whereas, contribution of combustion sources mostly dominated over PBL dilution at Mahabaleshwar. Higher wind speed regime also tends to dilute the atmosphere whereas higher BC concentration was observed during RH condition depicting the significance of low dispersion under these conditions. The contribution of different sources namely biomass burning (BB) and fossil fuel (FF), wavelength dependent source apportionment study was also evaluated. Traffic emission contributed 72%–75% of the BC loading at Mahabaleshwar, whereas at Pune it was estimated to be 82%–94% during all the seasons indicating BB contributed more at Mahabaleshwar. Cluster analysis and concentration weighted trajectory (CWT) analysis were also performed to visualize the importance of regional transport for both the locations. The study confers the significance of regional transport in addition to local emissions over both the sites.

The Asian summer monsoon anticyclone (ASMA) is a major meteorological system of the upper troposphere-lower stratosphere (UTLS) during boreal summer. It is known to contain enhanced tropospheric trace gases and aerosols, due to rapid lifting from the boundary layer by deep convection and subsequent horizontal confinement. Given its dynamical structure, the ASMA represents an efficient pathway for the transport of pollutants to the global stratosphere. A detailed understanding of the thermal structure and processes in the ASMA requires accurate in situ measurements. Within the StratoClim project we performed state-of-the-art balloon-borne measurements of temperature, water vapor, ozone and aerosol backscatter from two stations on the southern slopes of the Himalayas. In total, 63 balloon soundings were conducted during two extensive monsoon-season campaigns, in August 2016 in Nainital, India (29.4 degrees N, 79.5 degrees E), and in July-August 2017 in Dhulikhel, Nepal (27.6 degrees N, 85.5 degrees E); one shorter post-monsoon campaign was also carried out in November 2016 in Nainital. These measurements provide unprecedented insights into the UTLS thermal structure, the vertical distributions of water vapor, ozone and aerosols, cirrus cloud properties and interannual variability in the ASMA. Here we provide an overview of all of the data collected during the three campaign periods, with focus on the UTLS region and the monsoon season. We analyze the vertical structure of the ASMA in terms of significant levels and layers, identified from the temperature and potential temperature lapse rates and Lagrangian backward trajectories, which provides a framework for relating the measurements to local thermodynamic properties and the large-scale anticyclonic flow. Both the monsoon-season campaigns show evidence of deep convection and confinement extending up to 1.5-2 km above the cold-point tropopause (CPT), yielding a body of air with high water vapor and low ozone which is prone to being lifted further and mixed into the free stratosphere. Enhanced aerosol backscatter also reveals the signature of the Asian tropopause aerosol layer (ATAL) over the same region of altitudes. The Dhulikhel 2017 campaign was characterized by a 5 K colder CPT on average than in Nainital 2016 and a local water vapor maximum in the confined lower stratosphere, about 1 km above the CPT. Data assessment and modeling studies are currently ongoing with the aim of fully exploring this dataset and its implications with respect to stratospheric moistening via the ASMA system and related processes.

The effect of aerosols on cloud droplet number concentration and droplet effective radius is investigated from ground-based measurements over a high-altitude site where clouds pass over the surface. First aerosol indirect effect (AIE) estimates were made using (i) relative changes in cloud droplet number concentration (AIEn) and (ii) relative changes in droplet effective radius (AIEs) with relative changes in aerosol for different cloud liquid water contents (LWCs). AIE estimates from two different methods reveal that there is systematic overestimation in AIEn as compared to that of AIEs. Aerosol indirect effects (AIEn and AIEs) and dispersion effect (DE) at different LWC regimes ranging from 0.05 to 0.50 g m−3 were estimated. The analysis demonstrates that there is overestimation of AIEn as compared to AIEs, which is mainly due to DE. Aerosol effects on spectral dispersion in droplet size distribution play an important role in altering Twomey's cooling effect and thereby changes in climate. This study shows that the higher DE in the medium LWC regime offsets the AIE by 30 %.

The space-time variability of aerosol inhomogeneities provides unique information on atmospheric behavior needed for climate and environmental research and operational programs. An additional indirect forcing from aerosols results from their involvement in nucleation and growth of cloud droplets, reducing droplet size and thereby potentially influencing cloud albedo. These studies have particular significance over tropics where the convective and dynamical processes associated with high-altitude thunderstorms greatly affect the vertical distributions of aerosols and pre-cursor gases. As the anthropogenic share of the total aerosol loading is quite substantial over many parts of the world, it is essential to monitor the aerosol features systematically over longer time scales. Such observations are very important for understanding the coupling processes that exist between physico-chemical, radiative, dynamical and biological phenomena in the Earth's environment, and provide valuable input information for modeling and simulation studies of climate and air quality. The multi-year aerosol number density data acquired during October 1986-September 2000 with a computer-controlled lidar at the Indian Institute of Tropical Meteorology (IITM), Pune, an urban station in India have been utilized to investigate (i) climate variability, (ii) cloud macro-physical parameters and (iii) environmental pollution. The results reveal a long-term trend in aerosol loading, single and multiple layer clouds with low cloud-base during the south-west monsoon months, and high pollution potential during winter late evenings. The trends in aerosol loading and air quality are found to be changing from year to year depending upon meteorological parameters (precipitation in particular). Some of these parameters have also been compared with co-located complementary facilities such as solar radiometers. In order to enlarge the scope of these studies, a dual polarization micro pulse lidar (DPMPL) has been installed at IITM recently to investigate the cloud composition, and aerosol-cloud-climate interactions. The initial results obtained from this state-of-the-art lidar system showed interesting features in the time evolution of nocturnal (stable) boundary layer which have strong bearing on air pollution potential over the experimental station. The complete details of the lidar systems used in the above studies together with discussion of salient results are presented in this paper.