Optical and Physical Properties of Atmospheric Aerosols over the Bay of Bengal during ICARB

Simultaneous and collocated measurements of total and hemispherical backscattering coefficients (σ and β, respectively) at three wavelengths, mass size distributions, and columnar spectral aerosol optical depth (AOD) were made onboard an extensive cruise experiment covering, for the first time, the entire Bay of Bengal (BoB) and northern Indian Ocean. The results are synthesized to understand the optical properties of aerosols in the marine atmospheric boundary layer and their dependence on the size distribution. The observations revealed distinct spatial and spectral variations of all the aerosol parameters over the BoB and the presence of strong latitudinal gradients. The size distributions varied spatially, with the majority of accumulation modes decreasing from north to south. The scattering coefficient decreased from very high values (resembling those reported for continental/urban locations) in the northern BoB to very low values seen over near-pristine environments in the southeastern BoB. The average mass scattering efficiency of BoB aerosols was found to be 2.66 ± 0.1 m2 g−1 at 550 nm. The spectral dependence of columnar AOD deviated significantly from that of the scattering coefficients in the northern BoB, implying vertical heterogeneity in the aerosol type in that region. However, a more homogeneous scenario was observed in the southern BoB. Simultaneous lidar and in situ measurements onboard an aircraft over the ocean revealed the presence of elevated aerosol layers of enhanced extinction at altitudes of 1 to 3 km with an offshore extent of a few hundred kilometers. Back-trajectory analyses showed these layers to be associated with advection from west Asia and western India. The large spatial variations and vertical heterogeneity in aerosol properties, revealed by the present study, need to be included in the regional radiative forcing over the Bay of Bengal.

Atmospheric chemistry and climate

Atmospheric chemistry is a branch of atmospheric science where major focus is the composition of the Earth's atmosphere. Knowledge of atmospheric composition is essential due to its interaction with (solar and terrestrial) radiation and interactions of atmospheric species (gaseous and particulate matter) with living organisms. Since atmospheric chemistry covers a vast range of topics, in this article the focus is on the chemistry of atmospheric aerosols with special emphasis on the Indian region. I present a review of the current state of knowledge of aerosol chemistry in India and propose future directions.

Spatial and vertical heterogeneities in aerosol properties over oceanic regions around India: Implications for radiative forcing

The influence of atmospheric aerosols on Earth's radiation budget and hence climate, though well recognized and extensively investigated in recent years, remains largely uncertain mainly because of the large spatio-temporal heterogeneity and the lack of data with adequate resolution. To characterize this diversity, a major multi-platform field campaign ICARB (Integrated Campaign for Aerosols, gases and Radiation Budget) was carried out during the pre-monsoon period of 2006 over the Indian landmass and surrounding oceans, which was the biggest such campaign ever conducted over this region. Based on the extensive and concurrent measurements of the optical and physical properties of atmospheric aerosols during ICARB, the spatial distribution of aerosol radiative forcing was estimated over the entire Bay of Bengal (BoB), northern Indian Ocean and Arabian Sea (AS) as well as large spatial variations within these regions. Besides being considerably lower than the mean values reported earlier for this region, our studies have revealed large differences in the forcing components between the BoB and the AS. While the regionally averaged aerosol-induced atmospheric forcing efficiency was 31 +/- 6 W m(-2) tau(-1) for the BoB, it was only similar to 18 +/- 7 W m(-2) tau(-1) for the AS. Airborne measurements revealed the presence of strong, elevated aerosol layers even over the oceans, leading to vertical structures in the atmospheric forcing, resulting in significant warming in the lower troposphere. These observations suggest serious climate implications and raise issues ranging from the impact of aerosols on vertical thermal structure of the atmospheric and hence cloud formation processes to monsoon circulation.

Aerosol radiative forcing over land: effect of surface and cloud reflection

It is now clearly understood that atmospheric aerosols have a significant impact on climate due to their important role in modifying the incoming solar and outgoing infrared radiation. The question of whether aerosol cools (negative forcing) or warms (positive forcing) the planet depends on the relative dominance of absorbing aerosols. Recent investigations over the tropical Indian Ocean have shown that, irrespective of the comparatively small percentage contribution in optical depth (similar to11%), soot has an important role in the overall radiative forcing. However, when the amount of absorbing aerosols such as soot are significant, aerosol optical depth and chemical composition are not the only determinants of aerosol climate effects, but the altitude of the aerosol layer and the altitude and type of clouds are also important. In this paper, the aerosol forcing in the presence of clouds and the effect of different surface types (ocean, soil, vegetation, and different combinations of soil and vegetation) are examined based on model simulations, demonstrating that aerosol forcing changes sign from negative (cooling) to positive (warming) when reflection from below (either due to land or clouds) is high.

Meridional gradients in aerosol vertical distribution over Indian Mainland: Observations and model simulations

Multi-year observations from the network of ground-based observatories (ARFINET), established under the project `Aerosol Radiative Forcing over India' (ARFI) of Indian Space Research Organization and space-borne lidar `Cloud Aerosol Lidar with Orthogonal Polarization' (CALIOP) along with simulations from the chemical transport model `Goddard Chemistry Aerosol Radiation and Transport' (GOCART), are used to characterize the vertical distribution of atmospheric aerosols over the Indian landmass and its spatial structure. While the vertical distribution of aerosol extinction showed higher values close to the surface followed by a gradual decrease at increasing altitudes, a strong meridional increase is observed in the vertical spread of aerosols across the Indian region in all seasons. It emerges that the strong thermal convections cause deepening of the atmospheric boundary layer, which although reduces the aerosol concentration at lower altitudes, enhances the concentration at higher elevations by pumping up more aerosols from below and also helping the lofted particles to reach higher levels in the atmosphere. Aerosol depolarization ratios derived from CALIPSO as well as the GOCART simulations indicate the dominance of mineral dust aerosols during spring and summer and anthropogenic aerosols in winter. During summer monsoon, though heavy rainfall associated with the Indian monsoon removes large amounts of aerosols, the prevailing southwesterly winds advect more marine aerosols over to landmass (from the adjoining oceans) leading to increase in aerosol loading at lower altitudes than in spring. During spring and summer months, aerosol loading is found to be significant, even at altitudes as high as 4 km, and this is proposed to have significant impacts on the regional climate systems such as Indian monsoon. (C) 2015 Elsevier Ltd. All rights reserved.

Satellite-derived direct radiative effect of aerosols dependent on cloud cover

Aerosols from biomass burning can alter the radiative balance of the Earth by reflecting and absorbing solar radiation(1). Whether aerosols exert a net cooling or a net warming effect will depend on the aerosol type and the albedo of the underlying surface(2). Here, we use a satellite-based approach to quantify the direct, top-of-atmosphere radiative effect of aerosol layers advected over the partly cloudy boundary layer of the southeastern Atlantic Ocean during July-October of 2006 and 2007. We show that the warming effect of aerosols increases with underlying cloud coverage. This relationship is nearly linear, making it possible to define a critical cloud fraction at which the aerosols switch from exerting a net cooling to a net warming effect. For this region and time period, the critical cloud fraction is about 0.4, and is strongly sensitive to the amount of solar radiation the aerosols absorb and the albedo of the underlying clouds. We estimate that the regional-mean warming effect of aerosols is three times higher when large-scale spatial covariation between cloud cover and aerosols is taken into account. These results demonstrate the importance of cloud prediction for the accurate quantification of aerosol direct effects.

Vertical distribution of aerosols over the east coast of India inferred from airborne LIDAR measurements

The information on altitude distribution of aerosols in the atmosphere is essential in assessing the impact of aerosol warming on thermal structure and stability of the atmosphere.In addition, aerosol altitude distribution is needed to address complex problems such as the radiative interaction of aerosols in the presence of clouds. With this objective,an extensive, multi-institutional and multi-platform field experiment (ICARB-Integrated Campaign for Aerosols, gases and Radiation Budget) was carried out under the Geosphere Biosphere Programme of the Indian Space Research Organization (ISRO-GBP) over continental India and adjoining oceans during March to May 2006. Here, we present airborne LIDAR measurements carried out over the east Coast of the India during the ICARB field campaign. An increase in aerosol extinction (scattering + absorption) was observed from the surface upwards with a maximum around 2 to 4 km. Aerosol extinction at higher atmospheric layers (>2 km) was two to three times larger compared to that of the surface. A large fraction (75-85%) of aerosol column optical depth was contributed by aerosols located above 1 km. The aerosol layer heights (defined in this paper as the height at which the gradient in extinction coefficient changes sign) showed a gradual decrease with an increase in the offshore distance. A large fraction (60-75%) of aerosol was found located above clouds indicating enhanced aerosol absorption above clouds. Our study implies that a detailed statistical evaluation of the temporal frequency and spatial extent of elevated aerosol layers is necessary to assess their significance to the climate. This is feasible using data from space-borne lidars such as CALIPSO,which fly in formation with other satellites like MODIS AQUA and MISR, as part of the A-Train constellation.

A study on the variations of optical and physical properties of aerosols over a tropical semi-arid station during grassland fire

The present paper records the results of a case study on the impact of an extensive grassland fire on the physical and optical properties of aerosols at a semi-arid station in southern India for the first time from ground based measurements using a MICROTOPS-II sunphotometer, an aethalometer and a quartz crystal microbalance impactor (QCM). Observations revealed a substantial increase in aerosol optical depth (AOD) at all wavelengths during burning days compared to normal days. High AOD values observed at shorter wavelengths suggest the dominance of accumulation mode particle loading over the study area. Daily mean aerosol size spectra shows, most of the time, power-law distribution. To characterize AOD, the Angstrom parameters (i.e., alpha and beta) were used. Wavelength exponent (1.38) and turbidity coefficient (0.21) are high during burning days compared to normal days, thereby suggesting an increase in accumulation mode particle loading. Aerosol size distribution suggested dominance of accumulation mode particle loading during burning days compared to normal days. A significant positive correlation was observed between AOD at 500 mn and water vapour and negative correlation between AOD at 500 nm and wind speed for burning and non-burning days. Diurnal variations of black carbon (BC) aerosol mass concentrations increased by a factor of similar to 2 in the morning and afternoon hours during burning period compared to normal days.

Optical, radiative, and source characteristics of aerosols at Minicoy, a remote island in the southern Arabian Sea

Extensive measurements of aerosol radiative and microphysical properties were made at an island location, Minicoy (8.3 degrees N, 73.04 degrees E) in the southern Arabian Sea. A large variability in aerosol characteristics associated with changes in air mass and precipitation characteristics was observed. Six distinct transport pathways were identified on the basis of cluster analysis. The Indo-Gangetic Plain, along with the northern Arabian Sea and west Asia (NWA), was identified to be the region having the highest potential for aerosol mass loading at the island. This estimate is based on the concentration weighted trajectory as well as cluster analysis. Dust transport from the NWA region was found to make a substantial contribution to the supermicron mass fraction. The black carbon mass mixing ratios observed were the lowest compared to previous measurements over this region. Consequently, the atmospheric radiative forcing efficiency was low and was in the range 10-28 W m(-2).

Dust aerosols over India and adjacent continents retrieved using METEOSAT infrared radiance Part II: quantification of wind dependence and estimation of radiative forcing

Long-range transport of continental dust makes these particles a significant constituent even at locations far from their sources. It is important to study the temporal variations in dust loading over desert regions and the role of meteorology, in order to assess its radiative impact. In this paper, infrared radiance (10.5-12.5 mu m), acquired by the METEOSAT-5 satellite (similar to 5-km resolution) during 1999 and 2003 was used to quantify wind dependence of dust aerosols and to estimate the radiative forcing. Our analysis shows that the frequency of occurrence of dust events was higher during 2003 compared to 1999. Since the dust production function depends mainly on the surface wind speed over regions which are dry and without vegetation, the role of surface wind on IDDI was examined in detail. It was found that an increase of IDDI with wind speed was nearly linear and the rate of increase in IDDI with surface wind was higher during 2003 compared to 1999. It was also observed that over the Indian desert, when wind speed was the highest during monsoon months (June to August), the dust production rate was lower because of higher soil moisture (due to monsoon rainfall). Over the Arabian deserts, when the wind speed is the highest during June to August, the dust production rate is also highest, as soil moisture is lowest during this season. Even though nothing can be said precisely on the reason why 2003 had a greater number of dust events, examination of monthly mean soil moisture at source regions indicates that the occurrence of high winds simultaneous with high soil moisture could be the reason for the decreased dust production efficiency in 1999. It appears that the deserts of Northwest India are more efficient dust sources compared to the deserts of Saudi Arabia and Northeast Africa (excluding Sahara). The radiative impact of dust over various source regions is estimated, and the regionally and annually averaged top of the atmosphere dust radiative forcing (short wave, clear-sky and over land) over the entire study region (0-35 degrees N; 30 degrees-100 degrees E) was in the range of -0.9 to +4.5 W m(-2). The corresponding values at the surface were in the range of -10 to -25 W m(-2). Our studies demonstrate that neglecting the diurnal variation of dust can cause errors in the estimation of long wave dust forcing by as much as 50 to 100%, and nighttime retrieval of dust can significantly reduce the uncertainties. A method to retrieve dust aerosols during nighttime is proposed. The regionally and annually averaged long wave dust radiative forcing was +3.4 +/- 1.6 W m(-2).

Retrieval of dust aerosols during night: improved assessment of long wave dust radiative forcing over Afro-Asian regions

Several investigators in the past have used the radiance depression (with respect to clear-sky infrared radiance), resulting from the presence of mineral dust aerosols in the atmosphere, as an index of dust aerosol load in the atmosphere during local noon. Here, we have used a modified approach to retrieve dust index during night since assessment of diurnal average infrared dust forcing essentially requires information on dust aerosols during night. For this purpose, we used infrared radiance (10.5-12.5 mu m), acquired from the METEOSAT-5 satellite (similar to 5 km resolution). We found that the `dust index' algorithm, valid for daytime, will no longer hold during the night because dust is then hotter than the theoretical dust-free reference. Hence we followed a `minimum reference' approach instead of a conventional `maximum reference' approach. A detailed analysis suggests that the maximum dust load occurs during the daytime. Over the desert regions of India and Africa, maximum change in dust load is as much as a factor of four between day and night and factor of two variations are commonly observed. By realizing the consequent impact on long wave dust forcing, sensitivity studies were carried out, which indicate that utilizing day time data for estimating the diurnally averaged long-wave dust radiative forcing results in significant errors (as much as 50 to 70%). Annually and regionally averaged long wave dust radiative forcing (which account for the diurnal variation of dust) at the top of the atmosphere over Afro-Asian region is 2.6 +/- 1.8 W m(-2), which is 30 to 50% lower than those reported earlier. Our studies indicate that neglecting diurnal variation of dust while assessing its radiative impact leads to an overestimation of dust radiative forcing, which in turn result in underestimation of the radiative impact of anthropogenic aerosols.

Radiative effects of aerosols at an urban location in southern India: Observations versus model

The radiative impact of aerosols is one of the largest sources of uncertainty in estimating anthropogenic climate perturbations. Here we have used independent ground-based radiometer measurements made simultaneously with comprehensive measurements of aerosol microphysical and optical properties at a highly populated urban site, Bangalore (13.02 degrees N, 77.6 degrees E) in southern India during a dedicated campaign during winter of 2004 and summer and pre-monsoon season of 2005. We have also used longer term measurements carried out at this site to present general features of aerosols over this region. The aerosol radiative impact assessments were made from direct measurements of ground reaching irradiance as well as by incorporating measured aerosol properties into a radiative transfer model. Large discrepancies were observed between measured and modeled (using radiative transfer models, which employed measured aerosol properties) radiative impacts. It appears that the presence of elevated aerosol layers and (or) inappropriate description of aerosol state of mixing are (is) responsible for the discrepancies. On a monthly scale reduction of surface irradiance due to the presence of aerosols (estimated using radiative flux measurements) varies from 30 to 65 W m(-2). The lowest values in surface radiative impact were observed during June when there is large reduction in aerosol as a consequence of monsoon rainfall. Large increase in aerosol-induced surface radiative impact was observed from winter to summer. Our investigations re-iterate the inadequacy of aerosol measurements at the surface alone and importance of representing column properties (using vertical profiles) accurately in order to assess aerosol-induced climate changes accurately. (C) 2010 Elsevier Ltd. All rights reserved.

Dependence of climate forcing and response on the altitude of black carbon aerosols

Black carbon aerosols absorb solar radiation and decrease planetary albedo, and thus can contribute to climate warming. In this paper, the dependence of equilibrium climate response on the altitude of black carbon is explored using an atmospheric general circulation model coupled to a mixed layer ocean model. The simulations model aerosol direct and semi-direct effects, but not indirect effects. Aerosol concentrations are prescribed and not interactive. It is shown that climate response of black carbon is highly dependent on the altitude of the aerosol. As the altitude of black carbon increases, surface temperatures decrease; black carbon near the surface causes surface warming, whereas black carbon near the tropopause and in the stratosphere causes surface cooling. This cooling occurs despite increasing planetary absorption of sunlight (i.e. decreasing planetary albedo). We find that the trend in surface air temperature response versus the altitude of black carbon is consistent with our calculations of radiative forcing after the troposphere, stratosphere, and land surface have undergone rapid adjustment, calculated as ``regressed'' radiative forcing. The variation in climate response from black carbon at different altitudes occurs largely from different fast climate responses; temperature dependent feedbacks are not statistically distinguishable. Impacts of black carbon at various altitudes on the hydrological cycle are also discussed; black carbon in the lowest atmospheric layer increases precipitation despite reductions in solar radiation reaching the surface, whereas black carbon at higher altitudes decreases precipitation.