Recent emphasis on the prediction of temperature and concentration fields in the atmosphere has led to the investigation of accurate solution methods of the time-dependent conservation equations for mass, momentum, energy and species. Atmospheric radiation is the key component of this system. Therefore, atmospheric radiation models were developed in isolation from the climate models. The time-dependent multi-dimensional governing equations of atmospheric models must be solved in conjunction with the radiative transfer equation for accurate modeling of the atmosphere. In order to achieve this objective, a 1-D Radiative-Convective Model for Earth-Atmosphere System (RCM4EAS) was developed for clear and cloudy sky atmospheres. The radiative component of the code is Santa Barbara DISORT (Discrete Ordinate Radiative Transfer) Atmospheric Radiative Transfer (SBDART) integrated with exponential sum-fitting method as the radiative property estimation technique. The accuracy of SBDART was tested by comparing its predictions of radiative fluxes with those of Line-by-Line Radiative Transfer Model (LBLRTM) for 1-D longwave (3.33-100 &micro / m) clear sky atmosphere and a good agreement was obtained. A parametric study aiming at finding the optimum parameters to be used as input in SBDART regarding the wavelength increment and order of approximation was also carried out. Variable wavelength and eight streams were selected as optimum parameters for the accuracy and computational efficiency. The code was then coupled with a 1-D Radiative-Convective Model (RCM) to obtain the time dependent code, (RCM4EAS), which was applied to the investigation of the sensitivity of climate to changes in the CO2 concentration for clear and cloudy sky conditions. CO2 sensitivity analyses revealed that doubling the CO2 concentration in the earth&rsquo / s atmosphere from its present value (387 ppm) results in an increase in equilibrium surface temperature of 4.2 K in the clear sky atmosphere as opposed to 2.1 K in cloudy sky atmosphere with typical cloud physical parameters. It is worth noting that times required to reach equilibrium surface temperatures are approximately 2000 and 6000 days for clear and cloudy sky atmospheres, respectively and these temperature increases are calculated assuming that all the other parameters except CO2 concentration remain unchanged within these time periods. Therefore, it should be noted that these temperature increases reflect only the effect of CO2 doubling and excludes the effect of other forcings which might positively or negatively affect these temperature increases. Overall evaluation of the performance of the code developed in this thesis study indicates that it can be used with confidence in 1-D radiative-convective modeling of the earth-atmosphere systems.

The Arctic radiation climate is influenced substantially by anthropogenic and natural aerosols. There have been numerous studies devoted to understanding the radiative impacts of anthropogenic aerosols (e.g. those responsible for producing the Arctic haze phenomenon) and natural aerosols (e.g. dust and smoke) on the Arctic environment, but volcanic aerosols have received less attention. Volcanic eruptions occur frequently in the Arctic and have the capacity to be long duration, high intensity events, expelling large amounts of aerosol-sized ash and gases, which form aerosols once in the atmosphere. Additionally, volcanic eruptions deposit ash, which can alter the surface reflectivity, and remain to influence the radiation balance long after the eruptive plume has passed over and dissipated. The goal of this dissertation is to quantify the radiative effects of volcanic aerosols in the Arctic caused by volcanic plumes and deposits onto ice and snow covered surfaces. The shortwave, longwave, and net direct aerosol radiative forcing efficiencies and atmospheric heating/cooling rates caused by volcanic aerosol from the 2009 eruption of Mt. Redoubt were determined by performing radiative transfer modeling constrained by NASA A-Train satellite data. The optical properties of volcanic aerosol were calculated by introducing a compositionally resolved microphysical model developed for both ash and sulfates. Two compositions of volcanic aerosol were considered in order to examine a fresh, ash rich plume and an older, ash poor plume. The results indicate that environmental conditions, such as surface albedo and solar zenith angle, can influence the sign and the magnitude of the radiative forcing at the top of the atmosphere and at the surface. Environmental conditions can also influence the magnitude of the forcing in the aerosol layer. For instance, a fresh, thin plume with a high solar zenith angle over snow cools the surface and warms the top of the atmosphere, but the opposite effect is seen by the same layer over ocean. The layer over snow also warms more than the same plume over seawater. It was found that plume aging can alter the magnitude of the radiative forcing. For example, an aged plume over snow at a high solar zenith angle would warm the top of the atmosphere and layer by less than the fresh plume, while the aged plume cools the surface more. These results were compared with those reported for other aerosols typical to the Arctic environment (smoke from wildfires, Arctic haze, and dust) to demonstrate the importance of volcanic aerosols. It is found that the radiative impacts of volcanic aerosol plumes are comparable to those of other aerosol types, and those compositions rich in volcanic ash can have greater impacts than other aerosol types. Volcanic ash deposited onto ice and snow in the Arctic has the potential to perturb the regional radiation balance by altering the surface reflectivity. The areal extent and loading of ash deposits from the 2009 eruption of Mt. Redoubt were assessed using an Eulerian volcanic ash transport and dispersion model, Fall3D, combined with satellite and deposit observations. Because observations are often limited in remote Arctic regions, we devised a novel method for modeling ash deposit loading fields for the entire eruption based on best-fit parameters of a well-studied eruptive event. The model results were validated against NASA A-train satellite data and field measurements reported by the Alaska Volcano Observatory. Overall, good to moderate agreement was found. A total cumulative deposit area of 3.7 X 10^6 km2 was produced, and loadings ranged from ~7000 ± 3000 gm-2 near the vent to <0.1 ± 0.002 gm-2 on the outskirts of the deposits. Ash loading histories for total deposits showed that fallout ranged from ~5 – 17 hours. The deposit loading results suggest that ash from short duration events can produce regionally significant deposits hundreds of kilometers from the volcano, with the potential of significantly modifying albedo over wide regions of ice and snow covered terrain. The solar broadband albedo change, surface radiative forcing, and snowmelt rates associated with the ash deposited from the 2009 eruption of Mt. Redoubt were calculated using the loadings from Fall3D and the snow, ice, and aerosol radiative models. The optical properties of ash were calculated from Mie theory, based on size information recovered from the Fall3D model. Two sizes of snow were used in order to simulate a young and old snowpack. Deposited ash sizes agree well with field measurements. Only aerosol-sized ashes in deposits were considered for radiative modeling, because larger particles are minor in abundance and confined to areas very close to the vent. The results show concentrations of ash in snow range from ~ 6.9x10^4 – 1x10^8 ppb, with higher values closer to the vent and lowest at the edge of the deposits, and integrated solar albedo reductions of ~ 0 – 59% for new snow and ~ 0 – 85% for old snow. These albedo reductions are much larger than those typical for black carbon, but on the same order of magnitude as those reported for volcanic deposits in Antarctica. The daily mean surface shortwave forcings associated with ash deposits on snow ranged from 0 – 96 Wm-2 from the outmost deposits to the vent. There were no significantly accelerated snowmelts calculated for the outskirts of the deposits. However, for areas of higher ash loadings/concentrations, daily melt rates are significantly higher (~ 220 – 320%) because of volcanic ash deposits.

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.