An investigation of the high spectral resolution signatures and radiative forcing of tropospheric aerosol in the thermal infrared was conducted. To do so and to support advanced modeling of optical properties, a high spectral resolution library of atmospheric aerosol optical constants was developed. This library includes new optical constants of sulfate-nitrate-ammonium aqueous solutions and the collection of a broad range of existing optical constants for aerosol components, particularly mineral optical constants. The mineral optical constants were used to model and study infrared dust optical signatures as a function of composition, size, shape and mixing state. In particular, spherical and non-spherical optical models of dust particles were examined and compared to high spectral resolution laboratory extinction measurements. Then the performance of some of the most common effective medium approximations for internal mixtures was examined by modeling the optical constants of the newly determined sulfate-nitrate-ammonium mixtures. The optical signature analysis was applied to airborne and satellite high spectral resolution thermal infrared radiance data impacted by Saharan dust events. A new technique to retrieve dust microphysical properties from the dust spectral signature was developed and compared to a standard technique. The microphysics retrieved from this new technique and from a standard technique were then used to investigate the effects of dust on radiative forcing and cooling rates in the thermal IR.

Aerosol properties are highly variable in space and time which makes the aerosol study more complex. The sources and production mechanism of aerosols decide the properties of the aerosols. Aerosol radiative forcing is defined as the perturbation to the radiative fluxes of the earth atmosphere system caused by the aerosols. High uncertainty in the aerosol radiative forcing values exists today due to the lack of the exact chemical composition data of the aerosols everywhere. There are previous studies which have introduced methods to estimate ‘optical equivalent’ composition of aerosols using spectral aerosol optical depth measurements at the surface. The impact of aerosols on the solar radiative flux depends on its size distribution and composition. Hence, measurements of downward solar spectral fluxes at the surface can be used to infer ‘optically equivalent’ composition of aerosols. Measurements of downward solar spectral flux at Bangalore were made on clear days using a spectroradiometer. This data has been used to infer the aerosol composition following an iterative method with the help of the Santa Barbara DISORT Atmospheric Radiative Transfer (SBDART). Aerosols have been classified as water soluble, black carbon and three types of dust. Influence of the different aerosol types on spectral down welling irradiance at the surface have been simulated using Optical Properties of Aerosols and Clouds (OPAC) and SBDART models. The strong spectral dependence influence of water soluble aerosols and the dust aerosols on the spectral irradiance is shown. Aerosol composition was inferred following least square error minimization principle. This method can be used to estimate near-surface aerosol concentration if the vertical profile of aerosols is known a priori. This method also enables derivation of spectral single scattering albedo. The aerosol spectral radiative forcing has been estimated using downward spectral flux at the surface and compared with modeled fluxes. The contribution to the total forcing by the wavelength band 360 – 528 nm is around 60% of the total forcing. The wavelength band of 453-518 nm contributes maximum to the total forcing and it is seen that the shape of the spectral forcing is a major function of shape of the incoming solar spectrum. Aerosol spectral radiative forcing from observations of radiative fluxes agreed with modeled values when derived aerosol chemical composition was used as input. This study demonstrates that spectral flux measurements at the surface are useful to infer aerosol composition (which is optically equivalent) when and where the conventional chemical analysis is unavailable.

Aerosols affect the global radiation budget which plays an important role in determining the state of the Earth's climate. The heterogeneous distribution of aerosols and the variety in their properties results in high uncertainty in the understanding of aerosols. Aerosols affect the radiation by scattering and absorption (direct effect) or by modifying the cloud properties which in turn affects the radiation (indirect effect). The current work focuses only on the direct radiative effect of aerosols. The change in the top-of-atmosphere (TOA) reflected flux due to the perturbation of aerosols and their properties is called direct aerosol radiative forcing (ARFTOA). Estimation of ARFTOA using aerosol properties is done by solving the radiative transfer equation using a radiative transfer model. However, before using the radiative transfer model, it has to be validated with observations for consistency. This is done to check if the model is able to replicate values close to actual observations. The current work uses the Santa Barbara DISORT Atmospheric Radiative Transfer (SBDART) model. The output radiative fluxes from SBDART are validated by comparing with the Clouds and the Earth's Radiant Energy System (CERES) satellite data. Under clear-skies SBDART agreed with observed fluxes at TOA well within the error limits of satellite observations. In the shortwave solar spectrum (0.25-4 µm) radiation is affected by change in various aerosol properties and also by water vapour and other gas molecules. To study the effect of each of these molecules separately on the aerosol forcing at TOA, SBDART is used. ARFTOA is found to depend on the aerosol loading (aerosol optical depth – AOD), aerosol type (SSA) and the angular distribution of scattered radiation (asymmetry parameter). The role of water vapour relative to the aerosol layer height was also investigated and for different aerosol types and aerosol layer heights, it was found that water vapour can induce a change of ~4 Wm-2 in TOA flux. The relative importance of aerosol scattering versus absorption is evaluated through a parameter called single scattering albedo (SSA) which can be estimated from satellites. SSA defined as the ratio of scattering efficiency to total extinction efficiency, depends on the aerosol composition and wavelength. Aerosols with SSA close to 1 (sea-salt, sulphates) scatter the radiation and cool the atmosphere. Aerosols with SSA < 0.9 (black carbon, dust) absorb radiation and warm the atmosphere. Over high reflective surfaces a small change in SSA can change forcing from negative (cooling) to positive (warming). This makes SSA one of the most important and uncertain aerosol parameters. Currently, the SSA retrievals from the Ozone Monitoring Instrument (OMI) are highly sensitive to sub-pixel cloud contamination and change in aerosol height. Using the sensitivity of OMI to aerosol absorption and the superior cloud masking technique and accurate AOD retrieval of Moderate Resolution Imaging Spectroradiometer (MODIS), an algorithm to retrieve SSA (OMI-MODIS) was developed. The algorithm was performed over global oceans (60S-60N) from 2008-2012. The difference in SSA estimated by OMI-MODIS and that of OMI depended on the aerosol type and aerosol layer height. Aerosol layer height plays an important role in the UV spectrum due to the dominance of Rayleigh scattering. This was verified using SBDART which otherwise would not have been possible using just satellite observations. Both the algorithms were validated with cruise measurements over Arabian Sea and Bay of Bengal. It was seen that when absorbing aerosols (low SSA values) were present closer to the surface, OMI overestimated the value of SSA. On the other hand OMI-MODIS algorithm, which made no assumption on the aerosol type or height, was better constrained than OMI and hence was closer to the cruise measurement The presence of clouds results in a more complex interaction between aerosols and radiation. Aerosols present above clouds are responsible to most of the direct radiative effect in cloudy regions. The ARFTOA depends not only on the aerosol properties but also on the relative position of aerosols with clouds. When absorbing aerosols are present above clouds, the ARFTOA is highly influenced by the albedo of the underlying surface. Recent studies, over regions influenced by biomass burning aerosol, have shown that it is possible to define a ‘critical cloud fraction’ (CCF) at which the aerosol direct radiative forcing switch from a cooling to a warming effect. Similar analysis was done over BoB (6.5-21.5N; 82.5-97.5E) for the years 2008-2011. Aerosol properties were taken from satellite observations. Satellites cannot provide for aerosols present at different heights and hence SBDART was used to calculate the forcing due to aerosols present only above clouds. Unlike previous studies which reported a single value of CCF, over BoB it was found that CCF varied from 0.28 to 0.13 from post-monsoon to winter as a result of shift from less absorbing to moderately absorbing aerosol. This implies that in winter, the absorbing aerosols present above clouds cause warming of the atmosphere even at low cloud fractions leading to lower CCF. The use of multiple satellites in improving the retrieval of SSA has been presented in this thesis. The effect of aerosols present above clouds on the radiative forcing at TOA is shown to be different between Bay of Bengal and Atlantic Ocean. This was due to the change in SSA of aerosols during different seasons. The effect of aerosol height, aerosol type and water vapour on the TOA flux estimation is also studied using a radiative transfer model.