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The optical and radiative properties of dust particles in solar and thermal infrared regions are investigated. Dust particles are assumed to be spheres and spheroids for a comparison aimed at understanding the nonsphericity effect of these particles on the radiation at the top of a dusty atmosphere. The classical Lorenz–Mie theory is employed to compute the optical properties of spherical dust particles. To compute the single-scattering properties of spheroidal dust particles, a combination of the T-matrix method and an approximate method is used in the present study. In the approximate method, applicable to large particles, the geometric optics method is applied to the computation of the scattering phase matrix. A combination of the solution from the geometric optics method and the contribution of the so-called edge effect is used to compute the extinction efficiency of a spheroidal particle whose absorption efficiency is computed by adding the so-called above- and below-edge effect (a term from the well-known complex angular momentum theory) to the geometric optics result. Numerical results show that the results from the T-matrix method and the present approximate approach converge at a size parameter of 50 for computing the integrated scattering properties (i.e., the extinction efficiency, single-scattering albedo, and asymmetry factor). Additionally, the phase functions computed from the two methods are quite similar for size parameters larger than 40 although some considerable differences may still be noticed for other phase matrix elements. Furthermore, the effect of surface roughness on the single-scattering properties of spheroidal particles is discussed. The present radiative transfer simulations illustrate the nonsphericity effect of dust particles is significant at short wavelengths, however, not at the thermal infrared wavelengths.

For a sparse, disordered, plane-parallel particulate medium, we analyze quantitatively the effects of particle microphysical properties on the values of the linear and circular backscattering polarization ratios. Using numerically exact T-matrix and vector radiative-transfer codes, we performed computations for the following models: (1) a semi-infinite homogeneous layer composed of randomly oriented, polydisperse oblate spheroids with the real part of the refractive index equal to 1.2, 1.4 and 1.6 and the imaginary part of the refractive index equal to 0 and 0.01; (2) a semi-infinite homogeneous layer composed of randomly oriented, polydisperse, oblate circular cylinders with the refractive index 1.4; (3) finite homogeneous layers of various optical thickness composed of randomly oriented, polydisperse, oblate spheroids with the refractive index 1.55. Our computations demonstrate that the values of the polarization ratios depend substantially on particle shape, real and imaginary parts of the particle refractive index, particle size relative to the wavelength, illumination geometry and optical thickness.

A number of passive satellite instruments have been used to develop global climatologies of terrestrial tropospheric aerosols by analyzing the properties of sunlight reflected by the atmosphere–surface system. The outcome of these efforts are several climatologies which all purport to represent the same aerosol characteristics such as optical thickness and size. However, the quantitative differences between these climatologies have been found to far exceed the corresponding individual uncertainty claims. The magnitude of these differences is alarming and necessitates a detailed critical assessment and integrated analysis that would go far beyond simple intercomparisons of various satellite products and comparisons of satellite aerosol optical thickness results with ground-based sun-photometer data. This paper outlines the framework for a global long-term satellite climatology of aerosol properties based on a consistent combination of previous, current, and near-future satellite retrievals. We also discuss potential future strategies for deriving a much improved aerosol climatology from Earth-orbiting satellites.

The T-matrix method is among the most versatile, efficient, and widely used theoretical techniques for the numerically exact computation of electromagnetic scattering by homogeneous and composite particles, clusters of particles, discrete random media, and particles in the vicinity of an interface separating two half-spaces with different refractive indices. This paper presents an update to the comprehensive database of T-matrix publications compiled by us previously and includes the publications that appeared since 2007. It also lists several earlier publications not included in the original database.

We use the superposition T-matrix method to compute the scattering matrix elements and optical cross-sections for a variety of complex soot and soot-containing aggregate particles in random orientation at a visible wavelength 0.628 μm. It is shown that random variations in the geometrical configuration of monomers in a soot cluster for fixed fractal dimension and prefactor, monomer size, and number of monomers have a rather weak effect on scattering and absorption, at least in the visible part of the spectrum. Thus, the electromagnetic scattering and absorption characteristics of a single cluster realization are sufficient to represent the mean values obtained by averaging over many realizations of the “equivalent” clusters generated for the same fractal parameters. However, the results for the soot clusters differ fundamentally from those calculated for the volume-equivalent soot sphere and for the corresponding external mixture of soot monomers, assuming that there are no electromagnetic interactions between the monomers. We also compute and analyze the scattering and absorption properties of aerosols formed by semi-external aggregation of larger ammonium sulfate, silica, or dust particles with soot clusters as well as semi-external aggregates consisting of several components with different sizes and refractive indices. Depending on its chemical composition and size, the larger particle that is in touch with a soot cluster can strongly influence, or even dominate, the overall optical characteristics of the aggregate. Aggregation can result in stronger extinction, absorption, and scattering cross-sections relative to those computed for the corresponding external mixture. Possibly owing to mutual shadowing, the optical cross-sections of multi-component aggregates are smaller than those of their externally mixed counterparts, but by no more than ∼20%. Implications of our study for analyses of remote sensing observations and atmospheric radiation balance computations are discussed.

We use the superposition T-matrix method to solve the Maxwell equations and compute electromagnetic scattering characteristics of a 3D volume filled with densely packed, randomly distributed, wavelength-sized spherical particles. Our numerically exact data provide, for the first time, a direct demonstration of the onset and evolution of coherent backscattering with increasing number of particles and prove unequivocally that weak localization of electromagnetic waves can survive even in densely packed particulate media.

The NASA Glory mission is intended to facilitate and improve upon long-term monitoring of two key forcings influencing global climate. One of the mission's principal objectives is to determine the global distribution of detailed aerosol and cloud properties with unprecedented accuracy, thereby facilitating the quantification of the aerosol direct and indirect radiative forcings. The other is to continue the 28-yr record of satellite-based measurements of total solar irradiance from which the effect of solar variability on the Earth's climate is quantified. These objectives will be met by flying two state-of-the-art science instruments on an Earth-orbiting platform. Based on a proven technique demonstrated with an aircraft-based prototype, the Aerosol Polarimetry Sensor (APS) will collect accurate multiangle photopolarimetric measurements of the Earth along the satellite ground track within a wide spectral range extending from the visible to the shortwave infrared. The Total Irradiance Monitor (TIM) is an improved version of an instrument currently flying on the Solar Radiation and Climate Experiment (SORCE) and will provide accurate and precise measurements of spectrally integrated sunlight illuminating the Earth. Because Glory is expected to fly as part of the A-Train constellation of Earth-orbiting spacecraft, the APS data will also be used to improve retrievals of aerosol climate forcing parameters and global aerosol assessments with other A-Train instruments. In this paper, we detail the scientific rationale and objectives of the Glory mission, explain how these scientific objectives dictate the specific measurement strategy, describe how the measurement strategy will be implemented by the APS and TIM, and briefly outline the overall structure of the mission. It is expected that the Glory results will be used extensively by members of the climate, solar, atmospheric, oceanic, and environmental research communities as well as in education and outreach activities.

We employ the numerically exact superposition T-matrix method to perform extensive computations of elec nottromagnetic scattering by a volume of discrete random medium densely filled with increasingly absorbing as well as non-absorbing particles. Our numerical data demonstrate that increasing absorption diminishes and nearly extinguishes certain optical effects such as depolarization and coherent backscattering and increases the angular width of coherent backscattering patterns. This result corroborates the multiple-scattering origin of such effects and further demonstrates the heuristic value of the concept of multiple scattering even in application to densely packed particulate media.

Soot aggregates (SAs)-fractal clusters of small, spherical carbonaceous monomers-modulate the incoming visible solar radiation and contribute significantly to climate forcing. Experimentalists and climate modelers typically assume a spherical morphology for SAs when computing their optical properties, causing significant errors. Here, we calculate the optical properties of freshly-generated (fractal dimension Df = 1.8) and aged (Df = 2.6) SAs at 550 nm wavelength using the numerically-exact superposition T-Matrix method. These properties were expressed as functions of equivalent aerosol diameters as measured by contemporary aerosol instruments. This work improves upon previous efforts wherein SA optical properties were computed as a function of monomer number, rendering them unusable in practical applications. Future research will address the sensitivity of variation in refractive index, fractal prefactor, and monomer overlap of SAs on the reported empirical relationships.

Small particles forming clouds of interstellar and circumstellar dust, regolith surfaces of many solar system bodies, and cometary atmospheres have a strong and often controlling effect on many ambient physical and chemical processes. Similarly, aerosol and cloud particles exert a strong influence on the regional and global climates of the Earth, other planets of the solar system, and exoplanets. Therefore, detailed and accurate knowledge of physical and chemical characteristics of such particles has the utmost scientific importance.

We revisit the optical theorem relevant to the far-field electromagnetic scattering by an arbitrary particle. We compute both the Poynting vector and the energy density of the total field and demonstrate once again that, despite a recent claim to the contrary, the extinction is caused by the interference of the incident and the forward-scattered field. However, caution must be exercised when one describes electromagnetic scattering using a formalism based on the coherency dyad since this approach may lead to unphysical artifacts.

In this study, we model single-scattering properties of small cirrus crystals using mixtures of polydisperse, randomly oriented spheroids and cylinders with varying aspect ratios and with a refractive index representative of water ice at a wavelength of 1.88 μm. The Stokes scattering matrix elements averaged over wide shape distributions of spheroids and cylinders are compared with those computed for polydisperse surface-equivalent spheres. The shape-averaged phase function for a mixture of oblate and prolate spheroids is smooth, featureless, and nearly flat at side-scattering angles and closely resembles those typically measured for cirrus. Compared with the ensemble-averaged phase function for spheroids, that for a shape distribution of cylinders shows a relatively deeper minimum at side-scattering angles. This may indicate that light scattering from realistic cirrus crystals can be better represented by a shape mixture of ice spheroids. Interestingly, the single-scattering properties of shape-averaged oblate and prolate cylinders are very similar to those of compact cylinders with a diameter-to-length ratio of unity. The differences in the optical cross sections, single-scattering albedo, and asymmetry parameter between the spherical and the nonspherical particles studied appear to be relatively small. This may suggest that for a given optical thickness, the influence of particle shape on the radiative forcing caused by a cloud composed of small ice crystals can be negligible.

This tutorial paper provides a general overview of the hierarchy of problems involving electromagnetic scattering by particles and clarifies the place of the radiative transfer theory and the theory of coherent backscattering in the context of classical electromagnetics. The self-consistent microphysical approach to radiative transfer is compared with the traditional phenomenological treatment.

The volume integral equation formalism is used to derive and analyze specific criteria of applicability of the far-field approximation in electromagnetic scattering by a finite three-dimensional object. In the case of wavelength-sized and larger objects, this analysis leads to a natural subdivision of the entire external space into a near-field zone, a transition zone, and a far-field zone. It is demonstrated that the general criteria of far-field scattering are consistent with the theory and practice of T-matrix computations.

We analyze theoretically the effect of particle nonsphericity on the backscattering enhancement factor ζ hp in the helicity-preserving channel. Using numerically exact T-matrix and vector radiative-transfer codes, we have performed computations for optically semi-infinite homogeneous layers composed of polydisperse, randomly oriented oblate spheroids with the real part of the refractive index equal to 1.2, 1.4, and 1.6, the imaginary part of the refractive index equal to 0 and 0.01, various values of the equal-surface-area-sphere effective size parameter, and aspect ratios 1 ⩽ ɛ ⩽ 2 . Our computations demonstrate that whereas for spheres ζ hp ≡ 2 , for spheroids the helicity-preserving enhancement factor can deviate quite significantly from the value 2. The magnitude of this deviation varies substantially with particle microphysical parameters and illumination geometry.

We tested the applicability of three rigorous radiative transfer computational approaches, namely, the discrete ordinates radiative transfer (DISORT) method, the adding–doubling approach, and an efficient computational technique based on Ambartsumian's nonlinear integral equation for computing the bidirectional reflectance of a semi-infinite layer. It was found that each of these three models, in a combination with the truncation of the forward peak of the bulk scattering phase functions of ice particles, can be used to simulate the bidirectional reflectance of a semi-infinite snow layer with appropriate accuracy. Furthermore, we investigate the sensitivity of the bidirectional reflectance of a homogeneous and optically infinite snow layer to ice crystal habit and effective particle size. It is shown that the bidirectional reflectance is not sensitive to the particle effective size in the visible spectrum. The sensitivity of the bidirectional reflectance in the near-infrared spectrum to the particle effective size increases with the increase of the incident wavelength. The sensitivity of the bidirectional reflectance to the effective particle size and shape is attributed fundamentally to the sensitivity of the single-scattering properties to particle size and shape. For a specific ice crystal habit, the truncated phase function used in the radiative transfer computations is not sensitive to particle effective size. Thus, the single-scattering albedo is primarily responsible for the sensitivity of the bidirectional reflectance to particle size, particularly, at a near-infrared wavelength.

Finite-difference time domain (FDTD) solutions are first compared with the corresponding T-matrix results for light scattering by circular cylinders with specific orientations. The FDTD method is then utilized to study the scattering properties of horizontally oriented hexagonal ice plates at two wavelengths, 0.55 and 12 μm. The phase functions of horizontally oriented ice plates deviate substantially from their counterparts obtained for randomly oriented particles. Furthermore, we compute the phase functions of horizontally oriented ice crystal columns by using the FDTD method along with two schemes for averaging over the particle orientations. It is shown that the phase functions of hexagonal ice columns with horizontal orientations are not sensitive to the rotation about the principal axes of the particles. Moreover, hexagonal ice crystals and circular cylindrical ice particles have similar optical properties, particularly, at a strongly absorbing wavelength, if the two particle geometries have the same length and aspect ratio defined as the ratio of the radius or semi-width of the cross section of a particle to its length. The phase functions for the two particle geometries are slightly different in the case of weakly absorbing plates with large aspect ratios. However, the solutions for circular cylinders agree well with their counterparts for hexagonal columns.

Monthly mean aerosol optical depth (AOD) over ocean is compared from a total of 9 aerosol retrievals during a 40 months period. Comparisons of AOD have been made both for the entire period and sub periods. We identify regions where there is large disagreement and good agreement between the aerosol satellite retrievals. Significant differences in AOD have been identified in most of the oceanic regions. Several analyses are performed including spatial correlation between the retrievals as well as comparison with AERONET data. During the 40 months period studied there have been several major aerosol field campaigns as well as events of high aerosol content. It is studied how the aerosol retrievals compare during such circumstances. The differences found in this study are larger than found in a previous study where 5 aerosol retrievals over an 8 months period were compared. Part of the differences can be explained by limitations and deficiencies in some of the aerosol retrievals. In particular, results in coastal regions are promising especially for aerosol retrievals from satellite instruments particularly suited for aerosol research. In depth analyses explaining the differences between AOD obtained in different retrievals are clearly needed. We limit this study to identifying differences and similarities and indicating possible sources that affect the quality of the retrievals. This is a necessary first step towards understanding the differences and improving the retrievals.

The lidar backscatter cross sections of aluminum-oxide rocket exhaust particles are sensitive to slight deviations from their nominal spherical shape. We have therefore determined the distribution of particle shapes usingautomated image analysis of scanning electron microscope particle photographs. These shape statistics were used in conjunction with T-matrix calculations for nonspherical particles to estimate the backscatter properties of representative rocket exhaust particles. For the range of particle sizes and nonsphericities e relevant to exhaust plumes, both the backscatter intensity and depolarization scale approximately with the product of nonsphericity e times the particle radius (er). This correlation allows us to formulate a simple model for both the backscatter intensity and the depolarization of typical Al 2 O 3 rocket exhaust particles. This model is applied to a recent particle collection from the exhaust plume of a Titan-IVA rocket obtained from the NASA WB-57F high-altitude research aircraft at an altitude of 19 km.

The extensive set of measurements performed during the Chesapeake Lighthouse and Aircraft Measurements for Satellites (CLAMS) experiment provides a unique opportunity to evaluate aerosol retrievals over the ocean from multiangle, multispectral photometric, and polarimetric remote sensing observations by the airborne Research Scanning Polarimeter (RSP) instrument.Previous studies have shown the feasibility of retrieving particle size distributions and real refractive indices from such observations for visible wavelengths without prior knowledge of the ocean color. This work evaluates the fidelity of the aerosol retrievals using RSP measurements during the CLAMS experiment against aerosol properties derived from in situ measurements, sky radiance observations, and sun-photometer measurements, and further extends the scope of the RSP retrievals by using a priori information about the ocean color to constrain the aerosol absorption and vertical distribution.It is shown that the fine component of the aerosol observed on 17 July 2001 consisted predominantly of dirty sulfatelike particles with an extinction optical thickness of several tenths in the visible, an effective radius of 0.15 ± 0.025 μm and a single scattering albedo of 0.91 ± 0.03 at 550 nm. Analyses of the ocean color and sky radiance observations favor the lower boundary of aerosol single scattering albedo, while in situ measurements favor its upper boundary. Both analyses support the polarimetric retrievals of fine-aerosol effective radius and the consequent spectral variation in extinction optical depth. The estimated vertical distribution of this aerosol component depends on assumptions regarding the water-leaving radiances and is consistent with the top of the aerosol layer being close to the aircraft height (3500 m), with the bottom of the layer being between 2.7 km and the surface. The aerosol observed on 17 July 2001 also contained coarse-mode particles. Comparison of RSP data with sky radiance and in situ measurements suggests that this component consists of nonspherical particles with an effective radius in excess of 1 μm, and with the extinction optical depth being much less than one-tenth at 550 nm.

The influence of the assumed shape of aerosols on the estimates of the refractive index and size of particles (based on the data of ground-based spectropolarimetric measurements) is investigated for Jupiter’s cloud layer. In the present analysis, we supposed the atmospheric particles to be chaotically oriented spheroids and cylinders with a gamma size distribution. Their single-scattering characteristics were calculated with the T-matrix method, and the intensity and degree of linear polarization of the radiation reflected by the center of the planetary disk were found by solving the vector radiative-transfer equation with consideration for multiple scattering in a plane-parallel atmosphere. We considered a spectral interval from 0.423 to 0.798 µm and phase angles α from 0° to 11°. It has been shown that, if we use the optical characteristics of aerosols found within the frames of a spherical model (Mishchenko, 1990a), the models with the nonspherical particles considered here cannot fit the observational data. The refractive index and the sizes of spheroidal and cylindrical particles were estimated from a comparison of the data of measurements and calculations, and the simplest models for the Jovian cloud layer structure have been considered. We have concluded that the optical parameters of cloud particles (specifically, the refractive index) cannot be reliably estimated only on the basis of measurements made in a narrow range of phase angles.

This review paper outlines the rationale for long-term monitoring of the global distribution of natural and anthropogenic aerosols and clouds with specificity, accuracy, and coverage necessary for a reliable quantification of the direct and indirect aerosol effects on climate. We discuss the hierarchy of passive instruments suitable for aerosol remote sensing and give examples of aerosol retrievals obtained with instruments representing the low and the high end of this hierarchy.

In this paper we study potential errors in the retrieved values of the cloud particle refractive index and size that may result from the neglect of nonsphericity in analyses of ground-based spectropolarimetric observations of Jupiter. Using T -matrix and vector radiative-transfer codes, we have carried out numerous computations in the spectral range from 0.423 to 0.798 μm for a plane-parallel model atmosphere comprising polydisperse ensembles of randomly oriented oblate and prolate spheroids with sizes comparable to the wavelength. The particle models were specified by a gamma size distribution with varying values of the effective radius and effective variance and by a varying refractive index. Two models of the Jovian atmosphere were considered: (i) a homogeneous semi-infinite layer composed of gas and cloud particles; and (ii) a two-layered medium with a layer of pure gas on top of a semi-infinite homogeneous layer composed of gas and cloud particles. Good agreement between ground-based observational data of the brightness and the degree of linear polarization for the center of the Jovian disk and model computations was found for the following combinations of the real part of the refractive index m R , the effective radius r eff , and the effective variance v eff : m R = 1.45 , r eff = 0.35 μ m , v eff = 0.40 for oblate spheroids with an axial ratio of a / b = 1.3 ; m R = 1.50 , r eff = 0.35 μ m , v eff = 0.30 for prolate spheroids with a / b = 1 / 1.3 ; m R = 1.52 , r eff = 0.40 μ m , v eff = 0.35 for oblate spheroids with a / b = 1.5 , and m R = 1.54 , r eff = 0.90 μ m , v eff = 0.30 for prolate spheroids with a / b = 1 / 1.5 . These values (especially the real part of the refractive index) differ quite significantly from those retrieved previously for the model of spherical cloud particles and emphasize nonuniqueness of remote-sensing retrievals based on the ground-based data alone.

The paper presents validation results for the aerosol optical thickness derived by applying a two-channel retrieval algorithm to Advanced Very High Resolution Radiometer (AVHRR) radiance data. The satellite retrievals are compared with ship-borne sun-photometer results. The comparison of spatial and temporal statistics of the AVHRR results and the ship measurements shows a strong correlation. The satellite retrieval results obtained with the original algorithm for a wavelength of 0.55 μ m are systematically higher than the sun-photometer measurements in the cases of low aerosol loads. The ensemble averaged satellite-retrieved optical thickness overestimates the ensemble averaged sun-photometer data by about 11% with a random error of about 0.04. Increasing the diffuse component of the ocean surface reflectance from 0.002 to 0.004 in the AVHRR algorithm produces a better match, with the ensemble-averaged AVHRR-retrieved optical thickness differing by only about 3.6% from the sun-photometer truth and having a small offset of 0.03.

We present an update on the status of the global climatology of the aerosol column optical thickness and Angstrom exponent derived from channel-1 and -2 radiances of the Advanced Very High Resolution Radiometer (AVHRR) in the framework of the Global Aerosol Climatology Project (GACP). The latest version of the climatology covers the period from July 1983 to September 2001 and is based on an adjusted value of the diffuse component of the ocean reflectance as derived from extensive comparisons with ship sun-photometer data. We use the updated GACP climatology and Stratospheric Aerosol and Gas Experiment (SAGE) data to analyze how stratospheric aerosols from major volcanic eruptions can affect the GACP aerosol product. One possible retrieval strategy based on the AVHRR channel-1 and -2 data alone is to infer both the stratospheric and the tropospheric aerosol optical thickness while assuming fixed microphysical models for both aerosol components. The second approach is to use the SAGE stratospheric aerosol data in order to constrain the AVHRR retrieval algorithm. We demonstrate that the second approach yields a consistent long-term record of the tropospheric aerosol optical thickness and Angstrom exponent. Preliminary comparisons of the GACP aerosol product with MODerate resolution Imaging Spectrometer (MODIS) and Multiangle Imaging Spectro-Radiometer aerosol retrievals show reasonable agreement, the GACP global monthly optical thickness being lower than the MODIS one by approximately 0.03. Larger differences are observed on a regional scale. Comparisons of the GACP and MODIS Angstrom exponent records are less conclusive and require further analysis.

The superposition T -matrix method is used to compute the scattering of unpolarized light by semi-external aerosol mixtures in the form of polydisperse, randomly oriented two-particle clusters with touching components. The results are compared with those for composition-equivalent external aerosol mixtures, in which the components are widely separated and scatter light in isolation from each other. It is concluded that aggregation is likely to have a relatively weak effect on scattering and radiative properties of two-component tropospheric aerosols and can be replaced by the much simpler external-mixture model in remote sensing studies and atmospheric radiation balance computations.

We discuss the rationale for long-term monitoring of the global distribution of natural and anthropogenic aerosols (black carbon, sulfates, mineral aerosols, etc.) and clouds with specificity, accuracy, and coverage sufficient for a reliable quantification of the direct and indirect aerosol effects on climate, the anthropogenic component of these effects, and the long-term change of these effects caused by natural and anthropogenic factors. This discussion is followed by the formulation of specific scientific objectives of the Aerosol Polarimetry Sensor component of the National Aeronautics and Space Administration's Glory Project established within the framework of the US Climate Change Research Initiative.

We consider the problem of backscattering of light by a layer of discrete random medium illuminated by an obliquely incident plane electromagnetic wave. The multiply scattered reflected radiation is assumed to consist of incoherent and coherent parts, the coherent part being caused by the interference of multiply scattered waves. Formulas describing the characteristics of the reflected radiation are derived assuming that the scattering particles are spherical. The formula for the incoherent contribution reproduces the standard vector radiative transfer equation. The interference contribution is expressed in terms of a system of Fredholm integral equations with kernels containing Bessel functions. The special case of the backscattering direction is considered in detail. It is shown that the angular width of the backscattering interference peak depends on the polar angle of the incident wave and on the azimuth angle of the reflection direction.

Starting from first principles, we present a detailed analysis of the concept of single scattering of light by a small volume element filled with sparsely and randomly positioned particles. We first derive the formulas of the far-field single-scattering approximation, which treats the volume element as a single scatterer, and discuss its range of applicability, using for illustration exact T-matrix results for randomly oriented two-sphere clusters. Our second approach is to treat the volume element as a small cloud of particles and apply the so-called first-order-scattering approximation. We demonstrate that although the two approaches are based on somewhat different sets of assumptions, they give essentially the same result for the electromagnetic response of a sufficiently distant polarization-sensitive detector.

This paper compares and combines the results of laboratory measurements of the Stokes scattering matrix for nonspherical quartz aerosols at a visible wavelength in the scattering angle range 5–173° and the results of Lorenz–Mie computations for projected-area-equivalent spheres with the refractive index of quartz. A synthetic normalized phase function is constructed based on the laboratory data and the assumption that the diffraction forward-scattering peak is the same for spherical and nonspherical projected-area-equivalent particles. The experimental scattering matrix for the nonspherical quartz particles is poorly represented by the Lorenz–Mie results for most scattering angles. However, the asymmetry parameters for the synthetic phase function and for the equivalent spherical particles are similar.

The backscattering of light by quasi-horizontally oriented hexagonal ice plates is investigated because of its pertinence to lidar measurements of cirrus clouds. For oriented ice crystals, the commonly used geometric optics ray-tracing method is not applicable to the computation of the scattered field in certain scattering directions, in particular, the backscattering direction, because of the singularity problem inherent to the ray-tracing technique. In this study, we solve for the electric field due to scattering by quasi-horizontally oriented ice plates using an approach based on the electromagnetic wave theory. We simplify the analysis by ignoring the effect of the plate's side faces on the internal field inside the particle. This is a reasonable approximation when the ratio of the particle diameter to its thickness is large. This approximation is also valid if the tilt of the particle's symmetric axis from zenith is small and the size parameter is large. The present numerical results indicate that very strong oscillations in the backscattering cross section occur with the variation of size parameter. Furthermore, the bulk backscattering intensity has been calculated by including the effect of a particle size distribution and the random tilt of particle symmetric axis within a small angular region, for example, 2°. A strong dependence is found between the lidar backscattering cross section and the degree of the random tilt of the particles. A combination of the present method with the T-matrix method, which works well for particles having small and moderate size parameters, may provide a more complete picture of the lidar backscattering by quasi-horizontally oriented ice plates.

The paper describes and discusses long-term global retrievals of aerosol properties from channel-1 and -2 Advanced Very High-Resolution Radiometer (AVHRR) radiances. We reconfirm the previously reached conclusion that the nonsphericity of dust-like and dry sea salt aerosols can lead to very large errors in the retrieved optical thickness if one mistakenly applies the scattering model for spherical particles. Comparisons of single-scattering albedo and A ngstrom exponent values retrieved from the AVHRR data and those measured in situ at Sable Island indicate that the currently adopted value 0.003 can be a reasonable choice for the imaginary part of the aerosol refractive index in the global satellite retrievals. Several unexpected features in the long-term satellite record indicate a serious problem with post-launch calibration of channel-2 radiances from the NOAA-11 spacecraft. We solve this problem by using a simple re-calibration procedure removing the observed artifacts and derive a global climatology of aerosol optical thickness and size over the oceans for the period extending from July 1983 to December 1999. The global monthly mean optical thickness and A ngstrom exponent of tropospheric aerosols show no significant trends over the entire period and oscillate around the average values 0.145 and 0.75, respectively. The Northern Hemisphere mean optical thickness systematically exceeds that averaged over the Southern Hemisphere. The AVHRR retrieval results during the period affected by the Mt. Pinatubo eruption are consistent with the retrievals of the stratospheric aerosol optical thickness based on Stratospheric Aerosol and Gas Experiment Data (SAGE). Time series of the aerosol optical thickness and A ngstrom exponent derived for four separate geographic regions exhibit varying degrees of seasonal variability controlled by local meteorological events and/or anthropogenic activities.

The distribution and properties of atmospheric aerosols on a global scale are not well known in terms of determination of their effects on climate. This mostly is due to extreme variability of aerosol concentrations, properties, sources, and types. Aerosol climate impact is comparable to the effect of greenhouse gases, but its influence is more difficult to measure, especially with respect to aerosol microphysical properties and the evaluation of anthropogenic aerosol effect. There are many satellite missions studying aerosol distribution in the terrestrial atmosphere, such as MISR/Terra, OMI/Aura, AVHHR, MODIS/Terra and Aqua, CALIOP/CALIPSO. To improve the quality of data and climate models, and to reduce aerosol climate forcing uncertainties, several new missions are planned. The gap in orbital instruments for studying aerosol microphysics has arisen after the Glory mission failed during launch in 2011. In this review paper, we describe several planned aerosol space missions, including the Ukrainian project Aerosol-UA that obtains data using a multi-channel scanning polarimeter and wide-angle polarimetric camera. The project is designed for remote sensing of the aerosol microphysics and cloud properties on a global scale.

A comprehensive set of monthly mean aerosol optical thickness (AOT) data from coastal and island AErosol RObotic NETwork (AERONET) stations is used to evaluate Global Aerosol Climatology Project (GACP) retrievals for the period 1995–2009 during which contemporaneous GACP and AERONET data were available. To put the GACP performance in broader perspective, we also compare AERONET and MODerate resolution Imaging Spectroradiometer (MODIS) Aqua level-2 data for 2003–2009 using the same methodology. We find that a large mismatch in geographic coverage exists between the satellite and ground-based datasets, with very limited AERONET coverage of open-ocean areas. This is especially true of GACP because of the smaller number of AERONET stations at the early stages of the network development. Monthly mean AOTs from the two over-the-ocean satellite datasets are well-correlated with the ground-based values, the correlation coefficients being 0.81–0.85 for GACP and 0.74–0.79 for MODIS. Regression analyses demonstrate that the GACP mean AOTs are approximately 17%–27% lower than the AERONET values on average, while the MODIS mean AOTs are 5%–25% higher. The regression coefficients are highly dependent on the weighting assumptions (e.g., on the measure of aerosol variability) as well as on the set of AERONET stations used for comparison. Comparison of over-the-land and over-the-ocean MODIS monthly mean AOTs in the vicinity of coastal AERONET stations reveals a significant bias. This may indicate that aerosol amounts in coastal locations can differ significantly from those in adjacent open-ocean areas. Furthermore, the color of coastal waters and peculiarities of coastline meteorological conditions may introduce biases in the GACP AOT retrievals. We conclude that the GACP and MODIS over-the-ocean retrieval algorithms show similar ranges of discrepancy when compared to available coastal and island AERONET stations. The factors mentioned above may limit the performance of the validation procedure and cause us to caution against a direct extrapolation of the presented validation results to the entirety of the GACP dataset.

Sunlight illuminating the Earth's atmosphere is scattered by gas molecules and suspended particles, giving rise to blue skies, white clouds, and optical displays such as rainbows and halos. By scattering and absorbing the shortwave solar radiation and the longwave radiation emitted by the underlying surface, cloud and aerosol particles strongly affect the radiation budget of the terrestrial climate system. As a consequence of the dependence of scattering characteristics on particle size, morphology, and composition, scattered light can be remarkably rich in information on particle properties and thus provides a sensitive tool for remote retrievals of macro- and microphysical parameters of clouds and aerosols.

Scattering and absorption characteristics of water cloud droplets containing black carbon (BC) inclusions are calculated at a visible wavelength of by a combination of ray-tracing and Monte Carlo techniques. In addition, Lorenz–Mie calculations are performed assuming that the same amount of BC particles are mixed with water droplets externally. The results show that it is unlikely under normal conditions that BC aerosols can modify scattering and absorption properties of cloud droplets in any significant way except for geographical locations very close to major sources of BC. The differences in the single-scattering co-albedo and asymmetry parameter between BC-fraction-equivalent internal and external mixtures are negligibly small for normal black carbon loadings, which makes possible the use of the much simpler external mixing model in radiative transfer modeling irrespective of the actual form of mixing. For a fixed amount of BC internally mixed with cloud droplets, the absorption is maximal when the effective radius of the BC inclusions is about 0.05–.

Babinet’s principle is widely used to compute the diffraction by a particle. However, the diffraction by a 3-D object is not totally the same as that simulated with Babinet’s principle. This letter uses a surface integral equation to exactly formulate the diffraction by an arbitrary particle and illustrates the condition for the applicability of Babinet’s principle. The present results may serve to close the debate on the diffraction formalism.

Described is an improved algorithm that uses channel 1 and 2 radiances of the Advanced Very High Resolution Radiometer (AVHRR) to retrieve the aerosol optical thickness and Angstrom exponent over the ocean. Specifically discussed are recent changes in the algorithm as well as the results of a sensitivity study analyzing the effect of several sources of retrieval errors not addressed previously. Uncertainties in the AVHRR radiance calibration (particularly in the deep-space count value) may be among the major factors potentially limiting the retrieval accuracy. A change by one digital count may lead to a 50% change in the aerosol optical thickness and a change of 0.4 in the Angstrom exponent. On the other hand, the performance of two-channel algorithms weakly depends on a specific choice of the aerosol size distribution function with less than 10% changes in the optical thickness resulting from replacing a power law with a bimodal modified lognormal distribution. The updated algorithm is applied t...

We use a recent computer implementation of the first-principles theory of electromagnetic scattering to compute far-field extinction by a spherical particle embedded in an absorbing unbounded host. Our results show that the suppressing effect of increasing absorption inside the host medium on the ripple structure of the extinction efficiency factor as a function of the size parameter is similar to the well-known effect of increasing absorption inside a particle embedded in a nonabsorbing host. However, the accompanying effects on the interference structure of the extinction efficiency curves are diametrically opposite. As a result, sufficiently large absorption inside the host medium can cause negative particulate extinction. We offer a simple physical explanation of the phenomenon of negative extinction consistent with the interpretation of the interference structure as being the result of interference of the field transmitted by the particle and the diffracted field due to an incomplete wavefront resulting from the blockage of the incident plane wave by the particle's geometrical projection.

The influence of the shape of dust aerosol particles in the Martian atmosphere on the imaginary part of the refractive index ni as derived from photometric observations during the period of the highest activity of the dust storm in 1971 was studied and exemplified for particles of spherical and oblate spheroidal shape. A similar analysis was performed for mean particle radii r0 and optical thicknesses τ0 of the dust layer estimated from polarization observations for periods of high atmospheric transparency. It was demonstrated that the values obtained for these optical parameters are affected by the adopted aerosol shape. Namely, the values of ni, r0, and τ0 found for spheroidal particles proved to be nearly twice as large as those for spheres. However, they are still much less than the available estimates of these parameters inferred, in particular, from interpreting space experiments. The reason for this difference needs further investigation.

We use the recently extended superposition T-matrix method to calculate scattering and absorption properties of micrometer-sized water droplets contaminated by black carbon. Our numerically exact results reveal that, depending on the mode of soot-water mixing, the soot specific absorption can vary by a factor exceeding 6.5. The specific absorption is maximized when the soot material is quasi-uniformly distributed throughout the droplet interior in the form of numerous small monomers. The range of mixing scenarios captured by our computations implies a wide range of remote sensing and radiation budget implications of the presence of black carbon in liquid-water clouds. We show that the popular Maxwell-Garnett effective-medium approximation can be used to calculate the optical cross sections, single-scattering albedo, and asymmetry parameter for the quasi-uniform mixing scenario, but is likely to fail in application to other mixing scenarios and in computations of the elements of the scattering matrix.