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Mitigation of carbonaceous aerosol emissions is expected to provide climate and health co-benefits. The accurate representation of carbonaceous aerosols in climate models is critical for reducing uncertainties in their climate feedback. In this regard, emission fluxes and aerosol life cycle processes are the two primary sources of uncertainties. Here, we demonstrate that the incorporation of a dynamic ageing scheme and emission estimates that are updated for the local sources improves the representation of carbonaceous aerosols over the Indian monsoon region in a regional climate model, RegCM, compared with its default configuration. The respective mean black carbon (BC) and organic carbon (OC) surface concentrations in 2010 are estimated to be 4.25 and 10.35 µg m−3 over the Indo-Gangetic Plain (IGP) in the augmented model. The BC column burden over the polluted IGP is found to be 2.47 mg m−2, 69.95 % higher than in the default model configuration and much closer to available observations. The anthropogenic aerosol optical depth (AOD) increases by more than 19 % over the IGP due to the model enhancement, also leading to a better agreement with observed AOD. The respective top-of-the-atmosphere, surface, and atmospheric anthropogenic aerosol short-wave radiative forcing are estimated at −0.3, −9.3, and 9.0 W m−2 over the IGP and −0.89, −5.33, and 4.44 W m−2 over Peninsular India (PI). Our results suggest that the combined effect of two modifications leads to maximum improvements in the model performance in regions where emissions play a dominant role.

Cloud condensation nuclei (CCN) are mediators of aerosol-cloud interactions (ACI), contributing to the largest uncertainties in the understandings of global climate change. We present a novel remote sensing-based algorithm that quantifies the vertically-resolved CCN number concentrations (NCCN) using aerosol optical properties measured by a multiwavelength lidar. The algorithm considers five distinct aerosol subtypes with bimodal size distributions. The inversion used the look-up tables developed in this study, based on the observations from the Aerosol Robotic Network to efficiently retrieve optimal particle size distributions from lidar measurements. The method derives dry aerosol optical properties by implementing hygroscopic enhancement factors to lidar measurements. The retrieved optically equivalent particle size distributions and aerosol type dependent particle composition are utilized to calculate critical diameter using the κ-Köhler theory and NCCN at six supersaturations ranging from 0.07 % to 1.0 %. Sensitivity analyses indicate that uncertainties in extinction coefficients and relative humidity greatly influence the retrieval error in NCCN. The potential of this algorithm is further evaluated by retrieving NCCN using airborne lidar from the NASA ORACLES campaign and validated against simultaneous measurements from the CCN counter. The independent validation with robust correlation demonstrates promising results. Furthermore, the NCCN has been retrieved for the first time using a proposed algorithm from spaceborne lidar - Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) - measurements. The application of this new capability demonstrates the potential for constructing a 3D CCN climatology at a global scale, which help to better quantify ACI effects and thus reduce the uncertainty in aerosol climate forcing.

Xenobiotic chemical emissions from the informal electronic waste recycling (EW) sector are emerging problem for developing countries, with scale and impacts that are yet to be evaluated. We report an intensive polyurethane foam disk passive air sampling study in four megacities in India to investigate atmospheric organic pollutants along five transects viz., EW, information technology (IT), industrial, residential, and dumpsites. Intraurban emission sources were estimated and attributed by trajectory modeling and positive matrix factorization (PMF). ∑(17)PCDD/Fs, ∑(25)PCBs, ∑(7)plasticizers, and ∑(15)PAHs concentrations ranged from 3.1 to 26 pg/m(3) (14 ± 7; Avg ± SD), 0.5–52 ng/m(3) (9 ± 12); 7.5–520 ng/m(3), (63 ± 107) and 6–33 ng/m(3) (17 ± 6), respectively. EW contributed 45% of total PCB concentrations in this study and was evidenced as a major factor by PMF. The dominance of dioxin-like PCBs (dl-PCBs), particularly PCB-126, reflects combustion as the possible primary emission source. PCDD/Fs, PCBs and plasticizers were consistently highest at EW transect, while PAHs were maximum in industrial transect followed by EW. Concentrations of marker plasticizers (DnBP and DEHP) released during EW activities were significantly higher (p < 0.05) in Bangalore than in other cities. Toxic equivalents (TEQs) due to dl-PCBs was maximum in the EW transect and PCB-126 was the major contributor. For both youth and adult, the highest estimated inhalation risks for dl-PCBs and plasticizers were seen at the EW transect in Bangalore, followed by Chennai and New Delhi.

Mitigation of carbonaceous aerosol emissions is expected to provide climate and health co-benefits. The accurate representation of carbonaceous aerosols in climate models is critical for reducing uncertainties in their climate feedbacks. In this regard, emission fluxes and aerosol life-cycle processes are the two primary sources of uncertainties. Here we demonstrate that incorporating a dynamic ageing scheme and emission estimates that are updated for the local sources improve the representation of carbonaceous aerosols over the Indian monsoon region in a regional climate model, RegCM, compared to its default configuration. The mean BC and OC surface concentrations in 2010 are estimated to be 4.25 and 10.35 μg m−3, respectively, over the Indo-Gangetic Plain (IGP), in the augmented model. The BC column burden over the polluted IGP is found to be 2.47 mg m−2, 69.95 % higher than in the default model configuration and much closer to available observations. The anthropogenic AOD increases by more than 19 % over the IGP due to the model enhancement, also leading to a better agreement with observed AOD. The top-of-the-atmosphere, surface, and atmospheric anthropogenic aerosol shortwave radiative forcing are estimated at −0.3, −9.3, and 9.0 W m−2, respectively, over the IGP and −0.89, −5.33, and 4.44 W m−2, respectively, over Peninsular India. Our results suggest that both the accurate estimates of emission fluxes and a better representation of aerosol processes are required to improve the aerosol life cycle representation in the climate model.

Satellite observations have revealed an enhanced aerosol layer near the tropopause over Asia during the summer monsoon, called the "Asian Tropopause Aerosol Layer" (ATAL). In this work, aerosol particles in the ATAL were collected with a balloon-borne impactor near the tropopause region over India, using extended-duration balloon flights, in summer 2017 and winter 2018. The chemical composition of these particles was further investigated by quantitative analysis using offline ion chromatography. Nitrate (NO3-) and nitrite (NO2-) were found to be the dominant ions in the collected aerosols with values ranging between 87 and 343 ng M-3 at STP (standard temperature and pressure) during the summer campaign. In contrast, sulfate (SO42-) levels were found to be above the detection limit (> 10 ng m(-3) at STP) only in winter. In addition, we determined the origin of the air masses sampled during the flights using the analysis of back trajectories as well as a convective proxy from cloud-top temperature fields derived from a geostationary satellite. The results obtained from this analysis were put into the context of large-scale transport and aerosol distribution using GEOS-Chem chemical transport model simulations. The first flight in summer 2017 which sampled an air mass within the Asian monsoon anticyclone (AMA), influenced by convection over Western China, was associated with particle size diameters from 0.05 to 0.15 pm. In contrast, the second flight sampled air masses at the edge of the AMA associated with a larger particle size radius (> 2 mu m) with a higher NO2- concentration. The sampled air masses in winter 2018 were likely affected by smoke from the Pacific Northwest fire event in Canada, which occurred 7 months before our campaign, associated with concentration enhancements of SO42- and Ca2+. Overall, our results suggest that nitrogen-containing particles represent a large fraction of cloud-free and in-cloud aerosols populating the ATAL, which is partially in agreement with the results from aircraft measurements during the StratoClim (Stratospheric and upper tropospheric processes for better climate predictions) campaign. The exact nature of those particles is still unknown, but their coincidences with subvisible cirrus clouds and their sizes suggest nitric acid trihydrate (NAT) as a possible candidate, as NAT has already been observed in the tropical upper troposphere and lower stratosphere in other studies. Furthermore, GEOS-Chem model simulations indicate that lightning NOx emissions could have significantly impacted the production of nitrate aerosols sampled during the summer of 2017., Atmospheric Chemistry and Physics, 22 (18), ISSN:1680-7375, ISSN:1680-7367

The COVID-19 pandemic resulted in changed emission regimes all over the world. India also imposed complete lockdown on all modes of travel and industrial activities for about 2 months from 25-March-2020 and later unlocked these activities in a phased manner. Here, we study signatures of emissions changes on levels of atmospheric trace gases and aerosols contributing to air pollution over multiple sites in India’s capital Delhi covering various lockdown and unlock phases using satellite data and in-situ observations. The resulting changes in the levels of these species were compared with respect to their average of 2015–2019 to attribute for year to year and seasonal changes. A clear impact of lockdown was observed for AOD, PM, NO2, CO, and SO2 as a result of emission changes, while changed precursor levels led to a change in O3 chemical regimes impacting its concentrations. A detailed analysis of FLEXPART trajectories revealed increased PM levels over Delhi in north-westerly air masses sourced to Punjab region all the way up to Pakistan. Changes in aerosols and NO2 were not only restricted to the surface but transcended the total tropospheric column. The maximum decrease in PM, NO2, CO, and SO2 was observed during the month of total lockdown in April. The lockdown impact varied with species e.g., PM10 and PM2.5 as well as locations even within the periphery of Delhi. While surface level aerosols and NO2 showed significant and almost similar changes, AOD showed much lower decrease than tropospheric column NO2.

Ambient PM10 (particulate matter with aerodynamic diameter ≤ 10 µm) samples were collected and characterized from July 2012 to August 2013 with the objective to evaluate the variation in elemental concentration and use the same as markers for source apportionment and health risk assessment for the first time over Bhubaneswar, India. The yearly average mass of PM10 was 82.28 µg/m3, which was ~ 37% higher than the national ambient air quality (NAAQ) standards. Maximum PM10 concentration was observed during winter season followed by post-monsoon, pre-monsoon, and monsoon months. Acid soluble components in the PM10 samples were analyzed using ICP-OES (inductive coupled plasma optical emission spectroscopy), and 19 different elements including heavy metals were determined. Enrichment factor analysis attributed the source to either crustal or non-crustal origin. Principal component analysis (PCA) revealed that crustal sources, industrial activities, and vehicular emissions were significant contributors to PM mass. The contribution of total average elemental concentration showed a seasonal variation with the lowest (11.96 µg/m3) and highest (17.77 µg/m3) during monsoon and winter, respectively, which is relatively less significant than the variation in total PM10 mass that ranged between 48.43 µg/m3 in monsoon and 138.24 µg/m3 during the winter season. This observation evidences the predominant contribution of local/regional emission sources to the metallic components in coarse PM10 mass, which is corroborated by the wind pattern studies carried out using polar plots and a Lagrangian Particle Dispersion Model (LPDM) FLEXPART. Further, carcinogenic and non-carcinogenic health risk assessments of the measured elements that find their way into the human body through different exposure pathways have been calculated using United State Environmental Protection Agency (USEPA) standards. The carcinogenic risk of most of the elements was insignificant. The potential risk assessment study revealed that regular exposure to heavy metals through the ingestion pathway caused detrimental health effects. These effects were observed to be more severe in children in comparison to adults.

Aerosol behavior over the Himalayas plays an important role in the regional climate of South Asia. Previous studies at high-altitude observatories have provided evidence of the impact of long-range transport of pollutants from the Indo-Gangetic Plain (IGP). However, little information exists for the valley areas in the high Himalayas where significant local anthropogenic emissions can act as additional sources of short-living climate forcers and pollutants. The valley areas host most economic activities based on agriculture, forestry, and pilgrimage during every summer season. We report here first measurements at a valley site at ~2600 m a.s.l. on the trek to the Gangotri glacier (Gaumukh), in the Western Himalayas, where local infrastructures for atmospheric measurements are absent. The study comprised short-term measurement of aerosols, chemical characterization, and estimation of aerosol radiative forcing (ARF) during the winter and summer periods (2015-2016). The particulate matter mass concentrations were observed to be higher than the permissible limit during the summer campaigns. We obtained clear evidence of the impact of local anthropogenic sources: particulate nitrate is associated with coarse aerosol particles, the black carbon (BC) mass fraction appears undiluted with respect to measurements performed in the lower Himalayas, and in winter, both BC and sulfate concentrations in the valley site are well above the background levels reported from literature studies for mountain peaks. Finally, high concentrations of trace metals such as copper point to anthropogenic activities, including combustion and agriculture. While most studies in the Himalayas have addressed pollution in the high Himalayas in terms of transport from IGP, our study provides clear evidence that local sources cannot be overlooked over the high-altitude Himalayas. The estimated direct clear-sky ARF was estimated to be in the range of -0.1 to +1.6 W m-2, with significant heating in the atmosphere over the high-altitude Himalayan study site. These results indicate the need to establish systematic aerosol monitoring activities in the high Himalayan valleys.

Satellite observations have revealed an enhanced aerosol layer near the tropopause over Asia during the summer monsoon, called the Asian Tropopause Aerosol Layer (ATAL). The chemical composition of the ATAL is investigated here using offline ionic analysis of aerosols collected with a balloon-borne impactor near the tropopause region over India onboard extended duration balloon flights in the summer of 2017 and winter 2018. We found NO3- and NO2- dominant among other ions with values ranging between 87-343 ng/m3 during the summer campaign. In contrast, SO4 levels were found above detection limit (>10 ng/m3) only in winter. In addition, we determined the origin of the air masses sampled during the flights through back trajectory analysis combined with convection. The results obtained therein were put into a context of large-scale transport and aerosol distribution with GEOS-Chem chemical transport model simulations. The first flight of summer 2017 sampled air mass within the Asian monsoon anticyclone (AMA), associated with smaller particle size found on stage 2 (particle size cut off > 0.15 microns) of the impactor, while the second flight sampled air mass at the edge of the AMA associated with larger particle size on stage 1 (particle size cut off between 2 and 0.5 microns). The sampled air masses in winter 2018 were affected by smoke from the Pacific Northwest fire event in Canada, which occurred 7 months prior to our campaign. Concentrations of SO42-, NH4+, and Ca2+ were enhanced. Overall, our results suggest that nitrogen- containing particles represent a large fraction of aerosols populating the ATAL in agreement with aircraft measurements during the StratoClim campaign. Furthermore, GEOS-chem model simulations suggest that lightning NOx emissions had a minimal impact on the production of nitrate aerosols sampled during the two flights.

Particle number size distributions in the diameter range of 5 nm–34 µm were measured in tropical southern India during the transition season from May (pre-monsoon) to June–July (monsoon). Averaged over the entire measurement period, the particle number size distributions were bimodal with a total particle number concentration of NTot = (4.5 ± 2.7) × 103 cm−3 (arithmetic mean ± standard deviation). The ratio of Aitken to accumulation mode particle number concentrations (NAit/NAcc) ranged from 1.06 to 2.07, increasing from May to June–July due to a pronounced decrease in the accumulation mode particles with the onset of the monsoon. Cloud condensation nuclei concentrations at 0.4% supersaturation (CCN0.4) were calculated under the assumption of an average continental hygroscopicity parameter of κ = 0.3. The calculated CCN0.4 concentrations are mostly sensitive to variations in NAcc and vary accordingly between the May and June–July. Using a cloud parcel model, we investigated the formation of cloud droplets using the measured average particle number size distributions, updraft velocities up to 20 m s−1, and initial aerosol particle number concentrations up to 25,000 cm−3. We found different regimes of CCN activation and cloud formation for the month of May (shifting from aerosol-limited regime to transitional regime) and for June–July (transitional regime), which was primarily due to the variability of particle number concentrations in the accumulation mode.

Sulphur dioxide is a toxic pollutant in the atmosphere emitted from natural sources and human activities. Normally, SO2 has a life-time of about 2 days in the atmosphere and is not transported to long distances from its source region. However, under favourable circumstances such as low humidity or high wind speed, it can travel intercontinental distances from the point of emission. In this article, we have analysed the surface mixing-ratio of SO2 measured over the time period from January 2010 to April 2012 at a rural region in south India. It is found that SO2 mixing-ratio is very low over this region with an annual mean value in the range of 0.21–0.24 ppbv. OMI satellite estimates an annual mean value of 0.5 Dobson Units (DU) over the same location and period. However, during January to May relatively higher concentrations of SO2 are observed, mainly coming from power plants located in southern and eastern India as indicated by higher SO2/NO2 ratios of greater than 0.5. In one instance, on June 20th, 2011, it is found that the OMI SO2 value was a factor of 13 higher than 2011 annual mean at Gadanki. Using the FLEXible PARTicle dispersion model (FLEXPART) and satellite data, it is found that the observed higher SO2 value on 20th June was due to intercontinental transport of SO2 from Nabro volcanic eruption. Using the FLEXPART model with ECLIPSE-v5 emission inventory, the observed seasonal variation of SO2 could be well reproduced; however, the mixing ratios are found to be overestimated. CAMS (Copernicus Atmosphere Monitoring Service) SO2 reanalysis values available through its implementation in the ECMWF Integrated Forecasting System are a factor of 7.8 higher than observations, possibly due to incorrect vertical profile used in the model.

Spectral properties of Black Carbon (BC) produced during the burning of different biofuels have been studied using a 7 channel Aethalometer (Magee Scientific, USA). Different biofuels used for household purpose in the rural regions were selected after a survey conducted in Gadanki, A.P. - a typical village in South India. Biofuels were burnt in a custom made burning chamber and BC produced has been allowed to mix with ambient air and measured using Aethalometer kept 4 meters away from the burning chamber. The observed absorption coefficient spectra have been characterized by fitting to a power-law equation. The power co-efficient (α) values found to be ranging from 1.2-2.1 for different biofuels. It has been observed that the α values are related to the speed of burning; fast burning biofuels shown low values, whereas slow burning biofuels have shown higher values.

The Stratospheric Sudden Warming (SSW) is one of the most spectacular phenomena in the atmosphere and has impacts on the Earth’s lower, middle, and upper atmospheres. In this study, two major SSW episodes associated with vortex displacement and vortex splitting that occurred in the years 1998 and 1999, respectively, are investigated for the first time over Mt. Abu using lidar observations. Analyses show that ground-based lidar and satellite observations from the Halogen occultation experiment (HALOE) on board the upper atmospheric research satellite (UARS) can capture the effect of SSW events. Lidar measurements are able to capture SSW warming and its decay very accurately. The impact of SSW is further investigated in the European Centre for Medium-Range Weather Forecasts (ECMWF) Interim-reanalysed potential vorticity. Moreover, a detailed study has been presented to understand the latitudinal variation of SSW warming and the associated mesospheric cooling over the Indian region. The results showe...

Sixteen-year (1998–2013) climatology of cirrus clouds and their macrophysical (base height, top height and geometrical thickness) and optical properties (cloud optical thickness) observed using a ground-based lidar over Gadanki (13.5° N, 79.2° E), India, is presented. The climatology obtained from the ground-based lidar is compared with the climatology obtained from 7 and a half years (June 2006–December 2013) of Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) observations. A very good agreement is found between the two climatologies in spite of their opposite viewing geometries and the differences in sampling frequencies. Nearly 50–55 % of cirrus clouds were found to possess geometrical thickness less than 2 km. Ground-based lidar is found to detect a higher number of sub-visible clouds than CALIOP which has implications for global warming studies as sub-visible cirrus clouds have significant positive radiative forcing. Cirrus clouds with mid-cloud temperatures between −50 to −70 °C have a mean geometrical thickness greater than 2 km in contrast to the earlier reported value of 1.7 km. Trend analyses reveal a statistically significant increase in the altitude of sub-visible cirrus clouds which is consistent with the recent climate model simulations. The mid-cloud altitude of sub-visible cirrus clouds is found to be increasing at the rate of 41 ± 21 m year−1. Statistically significant decrease in optical thickness of sub-visible and thick cirrus clouds is observed. Also, the fraction of sub-visible cirrus cloud is found to have increased by 9 % in the last 16 years (1998 to 2013). This increase is mainly compensated by a 7 % decrease in thin cirrus cloud fraction. This has implications for the temperature and water vapour budget in the tropical tropopause layer.

We describe and show results from a series of field campaigns that used balloonborne instruments launched from India and Saudi Arabia during the summers 2014–17 to study the nature, formation, and impacts of the Asian Tropopause Aerosol Layer (ATAL). The campaign goals were to i) characterize the optical, physical, and chemical properties of the ATAL; ii) assess its impacts on water vapor and ozone; and iii) understand the role of convection in its formation. To address these objectives, we launched 68 balloons from four locations, one in Saudi Arabia and three in India, with payload weights ranging from 1.5 to 50 kg. We measured meteorological parameters; ozone; water vapor; and aerosol backscatter, concentration, volatility, and composition in the upper troposphere and lower stratosphere (UTLS) region. We found peaks in aerosol concentrations of up to 25 cm–3 for radii > 94 nm, associated with a scattering ratio at 940 nm of ∼1.9 near the cold-point tropopause. During medium-duration balloon flights near the tropopause, we collected aerosols and found, after offline ion chromatography analysis, the dominant presence of nitrate ions with a concentration of about 100 ng m–3. Deep convection was found to influence aerosol loadings 1 km above the cold-point tropopause. The Balloon Measurements of the Asian Tropopause Aerosol Layer (BATAL) project will continue for the next 3–4 years, and the results gathered will be used to formulate a future National Aeronautics and Space Administration–Indian Space Research Organisation (NASA–ISRO) airborne campaign with NASA high-altitude aircraft.

Influence of potential vorticity (PV) intrusions at 13.5°N over and near Indian sector (50°E–90°E) on tropical upper tropospheric ozone mixing ratio (OMR) variations is demonstrated based on two case studies. Increase of ECMWF (European Centre for Medium-range Weather Forecasting) reanalysis (ERA)-interim OMR in the upper troposphere (200–500 hPa) is observed during the intrusion events consistently in both cases. The OMR also shows similar tongue like structure as PV and it even follows the spatial shift of the PV tongue. In addition, the enhancements in the upper tropospheric OMR during the intrusion events are confirmed using microwave limb sounder (MLS) ozone data at 216 hPa. It is suggested that the existence of strong downdrafts, associated with the ageostrophic circulation due to jet stream, which is inferred from longitude-height cross-section of ERA-interim vertical velocity could bring the ozone further down, though high PV tongue remains only at higher level (above 400 hPa). The importance of these results lies in demonstrating the role of PV intrusion events on the enhancement of tropical upper tropospheric ozone over Indian sector, where the impact of the PV intrusions is not well understood when compared to that over Pacific and Atlantic sectors.

Five years (2006–2010) of clouds and earth’s radiant energy system (CERES) and CloudSat data have been analyzed to examine the role of vertical structure of cloud microphysical properties on cloud radiative forcing (CRF) parameters at the top-of-the atmosphere over the Asian monsoon region during the summer monsoon season (June–September) and the Pacific warm pool region during April. Vertical profile of cloud properties (optical depth, cloud liquid water content and cloud ice water content) derived from CloudSat data has been used for the present analysis. Shortwave, longwave and net CRF derived from the CERES data have been used. The results suggest an imbalance between shortwave cloud radiative forcing and longwave cloud radiative forcing over the Asian monsoon region consistent with the results reported earlier. The present analysis suggests that over the Bay-of-Bengal (BoB), vertical profile of cloud microphysical properties determine more than 50 % of variance in CRF. However, over the Pacific warm pool region, cloud microphysical property profiles does not contribute significantly to variance in net CRF (

Ozone mass mixing ratio (OMMR) obtained from both European Centre for Medium Range Weather Forecasting (ECMWF) Reanalysis (ERA)-Interim and Sounding of Atmosphere by Broadband Emission Radiometry (SABER) instrument onboard Thermosphere, Ionosphere, Mesosphere Energetics and Dynamics (TIMED) satellite shows large values in the equatorial upper stratosphere during the occurrence of a major stratospheric sudden warming (SSW) in January 2013 preceded by a large reduction of planetary wave activity. However, surprisingly equatorial stratospheric temperature is found to decrease at pressure levels where the ozone mixing ratio is larger. The computed radiative heating rate using Santa Barbara DISORT Atmospheric Radiative Transfer (SBDART) model also shows positive heating rate indicating that the temperature should increase in response to the ozone accumulation over equator. In addition to radiative heating due to ozone, heating rate due to other dominant factors, namely, ascending motion and convergence of meridional heat flux, which could influence the thermal structure of the equatorial stratosphere, are estimated. It is found that the observed low temperature during SSW is mainly due to large upward motions. The estimated heating rates agree reasonably well with the observed heating rates at 10-8 hPa indicating the dominance of transport at lower stratosphere. The large discrepancy between the estimated and observed heating rates in the upper stratosphere may be due to the dominance of photochemistry.

In the present study, characteristics of tropical cirrus clouds observed during 1998–2013 using a ground-based lidar located at Gadanki (13.5°N, 79.2°E), India, are presented. Altitude occurrences of cirrus clouds as well as its top and base heights are estimated using the advanced mathematical tool, wavelet covariance transform (WCT). The association of observed cirrus cloud properties with the characteristics of tropical tropopause layer (TTL) is investigated using co-located radiosonde measurements available since 2006. In general, cirrus clouds occurred for about 44% of the total lidar observation time (6246 h). The most probable altitude at which cirrus clouds occurr is 14.5 km. The occurrence of cirrus clouds exhibited a strong seasonal dependence with maximum occurrence during monsoon season (76%) and minimum occurrence during winter season (33%) which is consistent with the results reported recently using space-based lidar measurements. Most of the time, cirrus top was located within the TTL (between cold point and convective outflow level) while cirrus base occurred near the convective outflow level. The geometrical thickness of the cirrus cloud is found to be higher during monsoon season compared to winter and there exists a weak inverse relation with TTL thickness. During the observation period the percentage occurrence of cirrus clouds near the tropopause showed an 8.4% increase at 70% confidence level. In the last 16 years, top and base heights of cirrus cloud increased by 0.56 km and 0.41 km, respectively.

Surface ozone is mainly produced by photochemical reactions involving various anthropogenic pollutants, whose emissions are increasing rapidly in India due to fast-growing anthropogenic activities. This study estimates the losses of wheat and rice crop yields using surface ozone observations from a group of 17 sites, for the first time, covering different parts of India. We used the mean ozone for 7 h during the day (M7) and accumulated ozone over a threshold of 40 ppbv (AOT40) metrics for the calculation of crop losses for the northern, eastern, western and southern regions of India. Our estimates show the highest annual loss of wheat (about 9 million ton) in the northern India, one of the most polluted regions in India, and that of rice (about 2.6 million ton) in the eastern region. The total all India annual loss of 4.0–14.2 million ton (4.2–15.0%) for wheat and 0.3–6.7 million ton (0.3–6.3%) for rice are estimated. The results show lower crop loss for rice than that of wheat mainly due to lower surface ozone levels during the cropping season after the Indian summer monsoon. These estimates based on a network of observation sites show lower losses than earlier estimates based on limited observations and much lower losses compared to global model estimates. However, these losses are slightly higher compared to a regional model estimate. Further, the results show large differences in the loss rates of both the two crops using the M7 and AOT40 metrics. This study also confirms that AOT40 cannot be fit with a linear relation over the Indian region and suggests for the need of new metrics that are based on factors suitable for this region.

We report first measurements of ultrafine particles from a semi-rural location, Gadanki, from tropical Southern India. Measurements of particle number size distributions in the diameter range of 5 nm–32 μm were performed during 2 May–31 July 2012. The mean number concentrations of nucleation (NNUC), Aitken (NAIT), accumulation (NACCU), and total particles (NTOT) at this site were (1.1 ± 0.9) × 103 cm−3, (2.2 ± 1.3) × 103 cm−3, (1.5 ± 1.2) × 103 cm−3 and (4.8 ± 2.4) × 103 cm−3, respectively, comparable to other rural to semi-rural locations globally and declined as the season progressed, perhaps due to wet removal of aerosols with onset of monsoon in early June. Particle bursts in the nucleation mode size range (5–25 nm), followed by a sustained growth in size were observed very rarely (only 5 out of 79 observation days) at this site, less frequently than at most other locations around the world during May–July. Most factors affecting new particle formation (NPF) were similar on NPF and nonNPF event days, such as condensation sink, relative humidity, temperature, wind speed and direction, and mixing layer height. Thus, the infrequent occurrence of NPF at our site appeared to be linked to lower precursor gas concentrations and weak gas-phase oxidation chemistry due to diminished solar radiation on persistently cloudy days with the onset of the monsoon in early June over this region. The derived particle growth rates (GR > 5 nm) and formation rates of 5 nm particles (J5) ranged from 2.2 to 4.7 nm h−1 and 0.4–2.4 cm−3 s−1, with a mean and standard deviation of 3.4 ± 0.9 nm h−1 and 1.2 ± 2.3 cm−3 s−1, respectively, comparable to previous investigations at rural to semi-rural locations. The observed behavior in aerosol and meteorological parameters on NPF and nonNPF event days appeared to be distinctive compared to other rural to urban locations across the globe. However, this distinct behavior is limited and restricted to this site and season of the year, and should therefore not be generalized over a larger spatio-temporal scale. This emphasizes the need for long-term aerosol and precursor measurements over this and other regions of India.

We have studied long-term changes in tropospheric NO2 over South India using ground-based observations, and GOME and OMI satellite data. We have found that unlike urban regions, the region between Eastern and Western Ghat mountain ranges experiences statistically significant decreasing trend. There are few ground-based observatories to verify satellite based trends for rural regions. However, using a past study and recent measurements we show a statistically significant decrease in NOX and O3 mixing ratio over a rural location (Gadanki; 13.48° N, 79.18° E) in South India. In the ground-based records of surface NOX, the concentration during 2010–11 is found to be lower by 0.9 ppbv which is nearly 60 % of the values observed during 1994–95. Small but statistically significant decrease in noon-time peak ozone concentration is also observed. Noon-time peak ozone concentration has decreased from 34 ± 13 ppbv during 1993–96 to 30 ± 15 ppbv during 2010–11. NOX mixing ratios are very low over Gadanki. In spite of low NOX values (0.5 to 2 ppbv during 2010–11), ozone mixing ratios are not significantly low compared to many cities with high NOX. The monthly mean ozone mixing ratio varies from 9 ppbv to 37 ppbv with high values during Spring and low values during late Summer. Using a box-model, we show that presence of VOCs is also very important in addition to NOX in determining ozone levels in rural environment and to explain its seasonal cycle.

In the present study we compare the MODIS (Moderate Resolution Imaging Spectroradiometer) derived aerosol optical depth (AOD) data with that obtained from operating sky-radiometer at a remote rural location in southern India (Gadanki, 13.45° N, 79.18° E) from April 2008 to March 2011. While the comparison between total (coarse mode + fine mode) AODs shows correlation coefficient (R) value of about 0.71 for Terra and 0.77 for Aqua, if one separates the AOD into fine and coarse mode, the comparison becomes very poor, particularly for fine mode with an R value of 0.44 for both Terra and Aqua. The coarse mode AOD derived from MODIS and sky-radiometer compare better with an R value of 0.74 for Terra and 0.66 for Aqua. The seasonal variation is also well captured by both ground-based and satellite measurements. It is shown that both the total AOD and fine mode AOD are significantly underestimated with slope of regression line 0.75 and 0.35 respectively, whereas the coarse mode AOD is overestimated with a slope value of 1.28 for Terra. Similar results are found for Aqua where the slope of the regression line for total AOD and fine mode AOD are 0.72 and 0.27 whereas 0.95 for coarse mode. The fine mode fraction derived from MODIS data is less than one-half of that derived from the sky-radiometer data. Based on these observations and comparison of single scattering albedo observed using sky-radiometer with that of MODIS aerosol models, we argue that the selection of aerosol types used in the MODIS retrieval algorithm may not be appropriate particularly in the case of southern India. Instead of selecting a moderately absorbing aerosol model (as being done currently in the MODIS retrieval) a more absorbing aerosol model could be a better fit for the fine mode aerosols, while reverse is true for the coarse mode aerosols, where instead of using "dust aerosols" which is relatively absorbing type, usage of coarse sea-salt particles which is less absorbing is more appropriate. However, not all the differences could be accounted based on aerosol model, other factors like errors in retrieval of surface reflectance may also be significant in causing underestimation of AOD by MODIS.

Aerosols play a very significant role in determining earth's climate, but to study their quantitative effect is a challenging task due to their high spatial and temporal variability. The data from MODIS on-board Terra satellite during 2001–2008 have been used to study the spatial and temporal variability of AOD and also to identify homogeneous aerosol regions over South India. In this study we found two distinct regions within the selected study region that are characterised by low and high coefficients of variation (COV) of AOD values. The region with low COV is characterised by high AOD and vice versa. The spatial correlation is found to be symmetric for in-land locations but skewed towards Bay of Bengal for coastal locations. The spatial correlation is found to be significant for a radial distance of 150 km from the region of interest.

Absorbing aerosols supplements the global warming caused by greenhouse gases. However, unlike greenhouse gases, the effect of absorbing aerosol on climate is not known with certainty owing to paucity of data. Also, uncertainty exists in quantifying the contributing factors whether it is biomass or fossil fuel burning. Based on the observations of absorption coefficient at seven wavelengths and aerosol optical depth (AOD) at five wavelengths carried out at Gadanki (13.5° N, 79.2° E), a remote village in peninsular India, from April to November 2008, as part of the "Study of Atmospheric Forcing and Responses (SAFAR)" pilot campaign we discuss seasonal variation of black carbon (BC) concentration and aerosol optical depth. Also, using spectral information we estimate the fraction of fossil-fuel and non-fossil fuel contributions to absorption coefficient and contributions of soot (Black Carbon), non-soot fine mode aerosols and coarse mode aerosols to AOD. BC concentration is found to be around 1000 ng/m3 during monsoon months (JJAS) and around 4000 ng/m3 during pre and post monsoon months. Non-fossil fuel sources contribute nearly 20% to absorption coefficient at 880 nm, which increases to 40% during morning and evening hours. Average AOD is found to be 0.38±0.15, with high values in May and low in September. Soot contributes nearly 10% to the AOD. This information is further used to estimate the clear sky aerosol direct radiative forcing. Top of the atmosphere aerosol radiative forcing varies between −4 to 0 W m−2, except for April when the forcing is positive. Surface level radiative forcing is between −10 to −20 W m−2. The net radiation absorbed within the atmosphere is in the range of 9 to 25 W m−2, of which soot contributes about 80 to 90%.

Study of Atmospheric Forcing and Responses (SAFAR) is a five year (2009–2014) research programme specifically to address the responses of the earth's atmosphere to both natural and anthropogenic forcings using a host of collocated instruments operational at the National Atmospheric Research Laboratory, Gadanki (13.5° N, 79.2° E), India from a unified viewpoint of studying the vertical coupling between the forcings and responses from surface layer to the ionosphere. As a prelude to the main program a pilot campaign was conducted at Gadanki during May–November 2008 using collocated observations from the MST radar, Rayleigh lidar, GPS balloonsonde, and instruments measuring aerosol, radiation and precipitation, and supporting satellite data. We show the importance of the large radiative heating caused by absorption of solar radiation by soot particles in the lower atmosphere, the observed high vertical winds in the convective updrafts extending up to tropopause, and the difficulty in simulating the same with existing models, the upward traveling waves in the middle atmosphere coupling the lower atmosphere with the upper atmosphere, their manifestation in the mesospheric temperature structure and inversion layers, the mesopause height extending up to 100 km, and the electro-dynamical coupling between mesosphere and the ionosphere which causes irregularities in the ionospheric F-region. The purpose of this communication is not only to share the knowledge that we gained from the SAFAR pilot campaign, but also to inform the international atmospheric science community about the SAFAR program as well as to extend our invitation to join in our journey.

We evaluated three emission inventories of black carbon (BC) using Lagrangian particle dispersion model simulations and BC observations from a rural site in Southern India (Gadanki; 13.48° N, 79.18° E) from 2008 to 2012. We found that 93 to 95% of the BC load at the observation site originated from emissions in India and the rest from the neighbouring countries and shipping. A substantial fraction (33 to 43%) of the BC was transported from Northern India. Wet deposition is found to play a minor role in reducing BC mass at the site because of its proximity to BC sources during rainy season and relatively short rainy season over western and northern parts of India. Seasonally, the highest BC concentration (approx. 3.3 μg m−3) is observed during winter, followed by spring (approx. 2.8 μg m−3). While the model reproduced well the seasonal cycle, the modelled BC concentrations are significantly lower than observed values, especially in spring. The model bias is correlated to fire radiative power – a proxy of open biomass burning activity. Using potential emission sensitivity maps derived using the model, we suggest that underestimation of BC mass in the model during spring is due to the underestimation of BC fluxes over Southern India (possibly from open-biomass-burning/forest-fires). The overall performance of the model simulations using three different emission inventories (SAFAR-India, ECLIPSE and RETRO) is similar, with ECLIPSE and SAFAR-India performing marginally better as both have about 30% higher emissions for India than RETRO. The ratio of observed to modelled annual mean BC concentration was estimated as 1.5 for SAFAR, 1.7 for ECLIPSE and 2.4 for RETRO.

Results from a variety of complementary aerosol measurements made as part of the Indian Space Research Organization-Geosphere Biosphere Program (ISRO-GBP) road campaign experiment conducted during Feb 2004 in the central Indian region are reported. An instrumented vehicle fitted with the Micro Pulse Lidar for aerosol vertical profile measurements, nephelometer for scattering and athelometer for absorption coefficients measurements, Microtops II sun-photometer for column aerosol optical depth, Quartz Crystal Microbalance for aerosol mass concentration and Grimm spectrometer for aerosol number concentration was used in the campaign. The synergy of results from these complementary measurements is reflected in the computed aerosol radiative forcing for the region. We show that the large spatial and temporal variations found in the aerosol characteristics over the northwest Indian region are caused mainly by the naturally produced dust particles. The variation in their concentration modulates the overall atmospheric radiative forcing over this region. We also show that apart from the large north to south gradient in aerosol forcing caused due to transport of aerosols from the continent to the Indian Ocean region and reported during INDOEX, there is also a positive gradient in aerosol forcing from west to east, from the Arabian Sea to the Bay of Bengal region. A considerable portion of particles produced from the Indian main land is flushed to the Bay of Bengal region before being transported to the Indian Ocean, causing this west to east gradient.

In the present study we have compared the MODIS (Moderate Resolution Imaging Spectroradiometer) derived aerosol optical depth (AOD) data with that obtained from operating sky-radiometer at a remote rural location in South India (Gadanki, 13.45° N, 79.18° E). While the comparison between total (coarse mode + fine mode) AOD shows R2 value of about 0.71 with a negligible bias of 0.01, if one separates the AOD into fine and coarse mode, the comparison becomes very poor, particularly for fine mode with an R2 value of 0.44. The coarse mode AOD derived from MODIS and sky-radiometer compare better with an R2 value of 0.74 and also the seasonal variation is well captured by both measurements. It is shown that the fine mode fraction derived from MODIS data is more than a factor of two smaller than that derived from the sky-radiometer data. Based on these observations we argue that the selection of aerosol types used in the MODIS retrieval algorithm are not appropriate particularly in the case of South India. Instead of selecting a moderately absorbing aerosol type (as being done currently in the MODIS retrieval) a more absorbing type aerosol is better suited for fine mode aerosols, while reverse is true for the coarse mode aerosols, where instead of using "dust aerosols" which is relatively more absorbing, usage of coarse sea-salt particles which is less absorbing is more appropriate.

[1] Information on ultraviolet (UV) radiative fluxes is needed for public safety, understanding biodiversity, and for chemical transport modeling. Space-based observations can provide homogeneous and systematic estimates of the UV flux over large regions. In the past, UV flux estimates have been made from polar orbiting satellites; such estimates lack information on diurnal variability that can result in significant errors in UV dose (diurnally integrated UV flux). An algorithm has been developed to estimate diurnally varying spectral UV flux at the surface based on information from geostationary satellites (cloud amount, surface albedo and aerosols) and from polar orbiting satellites (ozone). Algorithm evaluation is done by comparison with ground-based observations made between January 1998 and December 2000 over eighteen stations of the United States Department of Agriculture (USDA)'s UV monitoring network. A good agreement between ground-based observations and satellite estimates is found with a mean bias (satellite − ground) of +3.5% for all-sky (cloudy + clear) cases. A negative mean bias of the same magnitude is found for clear-sky cases. Root mean square (RMS) differences are 25% and 14% for all-sky and clear-sky cases, respectively. Using simulations, it is shown that when only one observation near noontime is used to estimate UV dose, errors in the range of −61% to 48% can result, depending on cloud conditions. The RMS difference is 9% and it increases to 13% when off-noon hour (±2 hrs) observations are used to estimate the UV flux over Queenstown, MD.

[1] We present results on various physical and optical properties of aerosols measured over Ahmedabad, an urban location in western India, from 2002 to 2005 and discuss their seasonal and interannual variabilities. Aerosol parameters which have been studied include AOD spectra, aerosol mass concentration, size distribution, BC concentration, wavelength dependency in absorption, scattering coefficient, single scattering albedo and their vertical distribution in the atmosphere. All data have been classified in terms of four major seasons, namely, dry, premonsoon, monsoon and postmonsoon. AODs show an increasing trend over the first half of the year, and this is more consistent at higher wavelengths. Variation of Angstrom parameter α shows dominance of smaller size particles during dry and postmonsoon seasons while increase in coarser particle concentration during premonsoon and monsoon seasons. PM10 mass concentration varied from low values close to 40 μg/m3 to highs of about 106 μg/m3. Size distribution patterns of near surface aerosols exhibited presence of three distinct modes, all of which could be fitted using three lognormal modes. Highest values of BC mass are obtained during postmonsoon (7.3 ± 3.7 μg/m3) while lowest values are measured during monsoon season (1.5 ± 0.8 μg/m3). Wavelength dependency of aerosol absorption shows signatures of presence of significant amount of absorbing aerosols produced from biofuel/biomass burning in the atmosphere. Single scattering albedo at 0.525 μm are found to be 0.73 ± 0.1, 0.84 ± 0.04, 0.81 ± 0.03 and 0.73 ± 0.08 during dry, premonsoon, monsoon and postmonsoon seasons, respectively. Vertical distributions of aerosol for dry and postmonsoon seasons are characterized by high values of extinction coefficients within first few hundred meters from the surface where we find a sharp decrease in the extinction values with increasing altitude. Vertical distribution of aerosols during monsoon season shows presence of a very thick and stable aerosol layer between 0.5 and 2.0 km, contributing significantly to the columnar AODs.

Use of a compact, low power commercial lidar onboard a small aircraft for aerosol studies is demonstrated. A Micro Pulse Lidar fitted upside down in a Beech Superking aircraft is used to measure the vertical distribution of aerosols in and around Hyderabad, an urban location in the central India. Two sorties were made, one on 17 February 2004 evening hours and the other on 18 February 2004 morning hours for a total flight duration of four hours. Three different algorithms, proposed by Klett (1985), Stephens et al. (2001) and Palm et al. (2002) for deriving the aerosol extinction coefficient profile from lidar data are studied and is shown that the results obtained from the three methods compare within 2%. The result obtained from the airborne lidar is shown more useful to study the aerosol distribution in the free troposphere than that obtained by using the same lidar from ground. Using standard radiative transfer model the aerosol radiative forcing is calculated and is shown that knowledge on the vertical distribution of aerosols is very important to get more realistic values than using model vertical profiles of aerosols. We show that for the same aerosol optical depth, single scattering albedo and asymmetry parameter but for different vertical profiles of aerosol extinction the computed forcing values differ with increasing altitude and improper selection of the vertical profile can even flip the sign of the forcing at tropopause level.

[1] Extensive measurements of various aerosol parameters including single scattering albedo (SSA) were made at various locations over the central Indian region during February 2004 to study their impact on the regional aerosol radiative forcing. An overall increase in the measured value of SSA is noticed (0.75 to 0.9) over the period of this campaign, indicating unequal changes in source strength or removal processes of absorbing and scattering types of aerosols. Diurnally averaged value of direct SW radiative forcing for the region is in the range of −15 to −40 W/m2 at the surface, about 15% lower compared to that over the Bay of Bengal region and 22% higher than over the Arabian Sea. TOA forcing is in the range of +0.7 to −11 W/m2, about 50% lower compared to both these regions. This results in a heating rate of nearly 0.8 K/day for the first 2km in the atmosphere.

[1] Simultaneous measurements of surface level aerosol mass concentrations, their size distribution, and aerosol optical depth (AOD) were made during a ship cruise study conducted over the Bay of Bengal (BoB) between 19 and 28 February 2003, when the prevailing surface level wind flow is predominantly from the continent toward the ocean, using a ten-stage QCM cascade impactor and Microtops Sun photometer. On all cruise days, air parcels at different altitude levels were coming either from west or from northwest directions, crossing a significant portion of the Indian subcontinent before finally reaching over BoB. Average value of surface level aerosol mass concentration is found to be around 50, 37, and 13 μg/m3 for coarse mode (>1 μm), accumulation mode (between 1 μm and 0.1 μm), and nucleation mode (

[1] Measurements on spectral dependence of aerosol light absorption and BC mass concentrations were made at various locations between Ahmedabad (23.03°N, 72.50°E) and Hyderabad (17.47°N, 78.45°E) during February 2004. Average concentration of BC was close to 2 μg/m3 which is about 2 to 5% of the total aerosol mass loading measured at the surface. Absorption Angstrom coefficient estimated using a relation of the form βabs(λ) = K.λ−α is found to vary between 1.2 to 2.0 at different locations. Our result shows an excess absorption of up to 30% in lower wavelengths below 880 nm. Deviation from λ−1 dependence, which is typical of BC from fossil fuel, shows that aerosol mixture contains other particles from biofuel/biomass or mineral dust. As there was no major biomass burning observed in the study region as well as no specific enhancement observed in the coarse size aerosols, we attribute the observed excess absorption to the biofuel combustion.

Rayleigh lidars at Gadanki (13.5° N, 79.2° E), a tropical site, and at Mt. Abu (24.5° N, 72.7° E), a subtropical site, in India were operated simultaneously during the months of March, April, and May 2004. Significant differences are found in the temperatures over both the locations. Higher temperature, ~10–20 K, in the altitude region of 40–65 km is found during March 2004 over Mt. Abu. The mean stratopause temperature during March 2004 is found ~284 K at an altitude of 48 km over Mt. Abu, which is 18 K higher than the observed stratopause temperature of ~266 K over Gadanki. During April and May 2004, the temperatures over Mt. Abu are higher in the entire altitude range of 30–70 km than over Gadanki. Lidar-observed temperatures, over both the locations, are compared with the temperatures observed by SABER (Sounding of the Atmosphere using Broadband Emission Radiometry; onboard TIMED (Thermosphere Ionosphere Mesosphere Energetics and Dynamics)) and HALOE (Halogen Occultation Experiment; onboard UARS (Upper Atmosphere Research Satellite)). It is found that the lidar-observed temperatures are in qualitative agreement with the temperature observed by satellites, though quantitatively there are significant differences. Wave types of fluctuations have been noted in the upper stratosphere and in the lower mesosphere over both the locations.