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Intensity and polarization of light scattered by size distributions of randomly oriented nonspherical particles

Calculations of light scattering by small particles are important in many diverse fields of science and engineering. In many cases of practical interest, scattering particles are nonspherical and are distributed over sizes and orientations. However, accurate light scattering computations for ensembles of nonspherical particles are difficult and time-consuming, and the literature in which such calculations are reported is rather scarce. In this paper, the T-matrix approach, as extended recently to randomly oriented particles, is used to calculate rigorously light scattering by size distributions of randomly oriented axially symmetric particles. To model the variation of particle sizes in real ensembles, we use a power law distribution typical of some terrestrial aerosols. Contour plots of intensity and degree of linear polarization for polydisperse prolate and oblate spheroids of different aspect ratios and effective equivalent-sphere size parameters from 0 to 10 are calculated and compared with calculations for equivalent spheres. The angular scattering behavior of nonspherical polydispersions is found to be greatly different from that of spheres, while the scattering properties of oblate and prolate spheroids of the same aspect ratio are similar. With increasing particle size, both intensity and polarization become more shape-dependent. In general, nonspherical particles are stronger side scatterers and weaker backscatterers than equivalent spheres. With increasing aspect ratio of nonspherical particles polarization tends to be predominantly positive. Possible effects of particle nonsphericity on optical remote sensing of atmospheric aerosols are discussed.

Mishchenko, M. I.↗

Lidar multiple scattering: Dependence on atmospheric parameters

Backscatter lidars are very useful tools in gaining information about the atmosphere. Inversion of backscatter signals can be used to retrieve the spatial distribution of clouds and aerosols, e.g., vertical extensions of clouds and aerosol layers, detection of 'subvisible' cirrus, etc., very accurately compared to passive radiometers. To retrieve extinction coefficient profiles, in general, the so-called lidar equation is solved. This equation describes a laser pulse which propagates through an atmosphere with transmission exp(- integral of sigma(z')dz'), which is scattered singly under 180 degrees towards a receiver, and which is attenuated on its way back again by exp(- integral of sigma(z')dz'). For inversion, further information on optical properties of the scatterers are required (extinction to backscatter ratio). However, it is evident that, at least for optically thick clouds and/or large receiver's field-of-views, this approach may be erroneous because of multiply scattered photons. Several studies were performed to simulate multiple scattering in case of collimated beams or pulses including Monte Carlo, transport, and diffusion theory. Unfortunately, most of the approaches require an enormous amount of computer time. Thus, it is meaningful to elaborate approximate methods, and one such method is discussed. Our method is based on Bissonnett (1988). We have improved the numerical simulation of limited field-of-view detectors, and compared the results to Monte Carlo calculations and an exact model of Altmann (1989).

Wiegner, Matthias↗

Studies of optical and chemical properties of aged and fresh biomass burning absorbing aerosols for climate models

Particulate emissions from burning fuels from sub-Saharan Africa is currently poorly characterized. With increasing population and industrialization, emissions are expected to grow. Optical methods for measuring light absorption in the ultraviolet (UV) and visible (vis) regions of the spectrum are crucial for understanding the optical properties of BB aerosols (Bond and Bergstrom, 2006; Lack and Cappa, 2010; Moschos et al., 2021). One such instrument is the dual-spot AE33 model aethalometer is a common filter-based instrument that can be used to measure aerosol absorption properties (Hansen et al., 1984). This instrument has many figures of merit; however, the method's limitations include potential biases from scattering within the filter material, multiple scattering effects of the particles, filter loading (i.e. particle shadowing), and the need for wavelength-specific correction factors (Cλ), which depend on accurate intercomparison with other in situ techniques (Bond et al., 1999; Collaud Coen et al., 2010). This work aims to: 1. Optically characterize BB aerosol generated from African fuel 2. Correct the aethalometer at multiple wavelengths 3. Parametrize these correction factors. 4. Combusting the same fuels with two difference tube furnace systems assess the general applicability of this flexible means of producing BB aerosol. This was accomplished by conducting laboratory studies at Los Alamos National Laboratory (LANL) and North Carolina A&T State University (NCA&T), where aethalometer measurements were compared to in situ optical measurements. Mass cross sections of BB aerosol from these under-studied fuels will be determined along with their wavelength dependence.

09 BIOMASS FUELS↗

AROTEL Temperature Retrievals Within PSC's Using Raman Scattering

NASA Goddard Space Flight Center's Airborne Raman Ozone Temperature Lidar (AROTEL) made temperature retrievals within Polar Stratospheric Clouds (PSCs) on several flights during the SAGE III Ozone Loss and Validation Experiment (SOLVE) campaign. The location of the PSCs was confirmed using simultaneously acquired data from the NASA Langley Aerosol lidar. Retrievals were made on flight dates 991207, 991210 and 000127 from just above the aircraft to 25 kilometers geometric altitude. Raman temperature retrievals are, to first order, insensitive to Mie interference because the Raman signals are red shifted by 2331 cm(exp -1) from the initial laser wavelength. Backscattering from clouds and aerosols is consequently not observed by the detector; however, extinction does impact the measurement and limits retrievals to optically thin clouds. Comparisons between retrievals employing Rayleigh and Raman scattering show the Raman temperatures to be significantly warmer than those employing Rayleigh scattering. Uncertainties are a function of altitude: at 25 km they were approximately 3 K. Temperature profiles could not be retrieved for optically thick clouds.

Burris, John↗

Mineral Dust Optical Properties for Remote Sensing and Global Modeling: A Review

Dust plays a key role in many Earth system processes and is ubiquitous in the Martian atmosphere. Various intensive field campaigns, laboratory analyses, space-based remote sensing missions, and global modeling efforts aim to characterize dust optical properties. This is a bountiful time for dust scientists, and yet the interpretation of retrievals and comparison to models remains complicated by various conflicting assumptions that are part of each algorithm. For example, the conversion of satellite radiance measurements into products like aerosol optical depth for model evaluation depends upon aerosol properties like particle size and shape that are often prescribed and not part of the retrieval. Conversely, the model calculation of aerosol optical depth often uses different assumptions. The goal of this review is to first document algorithmic assumptions by various satellite retrieval products and models, and identify where there is consistency and where there are differences. In general, the differences documented in this paper reflect uncertainties resulting from incomplete observational characterization of dust aerosols and limitations in our understanding. Second, we note what observations might reduce uncertainties in our knowledge and bring greater consistency to retrievals and models, allowing for a more rigorous and harmonious comparison. The lack of comprehensive and realistic shape models for dust is an outstanding issue, such that closure between forward modeling from particle refractive index, shape, and size and observed optical properties cannot be achieved. Limitations in the computational methods that must be applied to model scattering from complex shapes also makes accurate optical modeling for dust challenging. Field observations indicate the persistence of coarse and giant dust particles at higher altitudes and farther downwind from their source than previously expected. Remote sensing retrieval algorithms based on observations at visible wavelengths have limited sensitivity to these particles and generally do not consider them, although a recent product based on longwave radiances is encouraging. Current measurements of the refractive index of bulk dust and fundamental dust minerology components such as hematite vary widely, inhibiting attempts to represent the variability in dust optical properties and forcing, as expected from different major dust source regions on Earth that have varying mineralogical composition. Some remote sensing retrieval algorithms allow for limited refractive index variability in their inversion solutions through mixing with other fine mode aerosol models, or optimizing the single scattering albedo, but Earth system models surveyed for this paper assume a globally uniform, size-invariant refractive index. Although no Martian dust samples have yet been returned to Earth, remote sensing observations indicate that Martian dust is globally homogenous in composition, and a single spectral refractive index assumption has been widely adopted to represent Martian dust. The lack of comprehensive, statistically representative measurements of dust particle microphysical properties (size distribution, morphology, complex index of refraction spectra, internal structure heterogeneity), and the resulting optical properties, limits our ability to verify the fidelity of these assumptions. A chain of measurements is needed, ranging from characterizing individual dust mineralogy components (e.g., pure hematite and goethite) to in situ sampling of complex atmospheric aerosol mixtures. Such results could be applied to both remote sensing retrievals that characterize the optical properties of the total aerosol burden in the atmosphere from total radiance measurements, and to global models that represent the total aerosol burden in the atmosphere by building it up from the balance of individual aerosol sources and sinks.

Aeolian dust↗

Single and multiple scattering contributions to circumsolar radiation

The contributions to the angular distribution of the almucantar radiance in the forward direction due to multiple scattering are compared to those due to single scattering. The contributions have been calculated by a computer code employing the Gauss-Seidel iterative approach to the solution of the radiative transfer equation for a plane parallel atmosphere composed of air molecules, aerosol particles, and ozone. The code is similar to that of Dave (1972) except in the construction of the source matrix. In the near-forward direction the multiple scattering contributions are significant for optical depths of the order of 0.4. The shape of the angular distribution of almucantar radiance to 10 degrees is less sensitive to multiple scattering.

Box, M. A.↗

CALIPSO Detection of an Asian Tropopause Aerosol Layer

The first four years of the CALIPSO lidar measurements have revealed the existence of an aerosol layer at the tropopause level associated with the Asian monsoon season in June, July and August. This Asian Tropopause Aerosol Layer (ATAL) extends geographically from Eastern Mediterranean (down to North Africa) to Western China (down to Thailand), and vertically from 13 to 18 km. The Scattering Ratio inferred from CALIPSO shows values between 1.10. 1.15 on average with associated depolarization ratio of less than 5%. The Gaussian distribution of the points indicates that the mean value is statistically driven by an enhancement of the background aerosol level and not by episodic events such as a volcanic eruption or cloud contamination. Further satellite observations of aerosols and gases as well as field campaigns are urgently needed to characterize this layer, which is likely to be a significant source of non-volcanic aerosols for the global upper troposphere with a potential impact on its radiative and chemical balance

Vemier, J.-P.↗

Effects of aerosols and surface shadowing on bidirectional reflectance measurements of deserts

Desert surfaces are probably one of the most stable of the Earth's natural targets for remote sensing. The bidirectional reflectance properties of the Saudi Arabian desert was investigated during the Summer Monsoon Experiment (Summer Monex). A comparison of high-altitude with near-surface measurements of the White Sands desert showed significant differences. These discrepancies have been attributed to forward scattering of the dust-laden atmosphere prevalent during Summer Monex. This paper is concerned in general with modeling the effects of atmospheric aerosols and surface shadowing on the remote sensing of bidirectional reflectance factors of desert targets, and in particular with comparing the results of these models with flight results. Although it is possible to approximate the latter, it is felt that a surface reflectance model with a smaller specular component would have permitted using a more realistic set of atmospheric conditions in the simulations.

Bowker, David E.↗

Aerosol Retrievals over the Ocean using Channel 1 and 2 AVHRR Data: A Sensitivity Analysis and Preliminary Results

This paper outlines the methodology of interpreting channel 1 and 2 AVHRR radiance data over the oceans and describes a detailed analysis of the sensitivity of monthly averages of retrieved aerosol parameters to the assumptions made in different retrieval algorithms. The analysis is based on using real AVHRR data and exploiting accurate numerical techniques for computing single and multiple scattering and spectral absorption of light in the vertically inhomogeneous atmosphere-ocean system. We show that two-channel algorithms can be expected to provide significantly more accurate and less biased retrievals of the aerosol optical thickness than one-channel algorithms and that imperfect cloud screening and calibration uncertainties are by far the largest sources of errors in the retrieved aerosol parameters. Both underestimating and overestimating aerosol absorption as well as the potentially strong variability of the real part of the aerosol refractive index may lead to regional and/or seasonal biases in optical thickness retrievals. The Angstrom exponent appears to be the most invariant aerosol size characteristic and should be retrieved along with optical thickness as the second aerosol parameter.

Mishchenko, Michael I.↗

Forwardscattering corrections for optical extinction measurements in aerosol media. I - Monodispersions

A parametric investigation of forwardscattering corrections applicable to experimentally determined optical extinction coefficients in homogeneous aerosol media is discussed for the case of monodispersion. Assuming forwardscattering to be a single-scattering phenomenon, corrections are made by two methods: one employing the exact Mie theory, the other employing the approximate Rayleigh diffraction formula. The corrections are evaluated as functions of particle size, the real and imaginary parts of the complex refractive index, and the half-angle of the detector view cone.

Deepak, A.↗

Lidar Observations of the Optical Properties and 3-Dimensional Structure of Cirrus Clouds

The scientific research conducted under this grant have been reported in a series of journal articles, dissertations, and conference proceedings. This report consists of a compilation of these publications in the following areas: development and operation of a High Spectral Resolution Lidar, cloud physics and cloud formation, mesoscale observations of cloud phenomena, ground-based and satellite cloud cover observations, impact of volcanic aerosols on cloud formation, visible and infrared radiative relationships as measured by satellites and lidar, and scattering cross sections.

Eloranta, E. W.↗

EMIRS Observations of the Aphelion-Season Mars Atmosphere

Thermal infrared spectra taken by the Emirates Mars Infrared Spectrometer (EMIRS) on-board the Emirates Mars Mission (EMM) spacecraft are well suited for the retrieval of surface temperatures, the atmospheric temperature profile from the surface to ∼40 km, and the column abundance of dust aerosols, water ice clouds, and water vapor. A constrained linear inversion retrieval routine that includes multiple scattering has been developed and optimized for this purpose. Here, we present a brief overview of the retrieval algorithm and first atmospheric science results from observations taken by EMIRS over the first Earth year of EMM Science Phase operations. These retrievals show extensive water ice clouds, typical for the aphelion season of these observations, and the expected north polar summer maximum and subsequent equatorward transport of water vapor is well documented. An unusually strong and early regional dust storm and its associated thermal response were also observed.

Michael D. Smith↗

Cloud and aerosol optical depths

An airborne Sun photometer was used to measure optical depths in clear atmospheres between the appearances of broken stratus clouds, and the optical depths in the vicinity of smokes. Results show that (human) activities can alter the chemical and optical properties of background atmospheres to affect their spectral optical depths. Effects of water vapor adsorption on aerosol optical depths are apparent, based on data of the water vapor absorption band centered around 940 nm. Smoke optical depths show increases above the background atmosphere by up to two orders of magnitude. When the total optical depths measured through clouds were corrected for molecular scattering and gaseous absorption by subtracting the total optical depths measured through the background atmosphere, the resultant values are lower than those of the background aerosol at short wavelengths. The spectral dependence of these cloud optical depths is neutral, however, in contrast to that of the background aerosol or the molecular atmosphere.

Pueschel, R. F.↗

Surface Reflectance of Mars Observed by CRISM-MRO: 1. Multi-angle Approach for Retrieval of Surface Reflectance from CRISM Observations (mars-reco)

This article addresses the correction for aerosol effects in near-simultaneous multiangle observations acquired by the Compact Reconnaissance Imaging Spectrometer for Mars (CRISM) aboard the Mars Reconnaissance Orbiter. In the targeted mode, CRISM senses the surface of Mars using 11 viewing angles, which allow it to provide unique information on the scattering properties of surface materials. In order to retrieve these data, however, appropriate strategies must be used to compensate the signal sensed by CRISM for aerosol contribution. This correction is particularly challenging as the photometric curve of these suspended particles is often correlated with the also anisotropic photometric curve of materials at the surface. This article puts forward an innovative radiative transfer based method named Multi-angle Approach for Retrieval of Surface Reflectance from CRISM Observations (MARS-ReCO). The proposed method retrieves photometric curves of surface materials in reflectance units after removing aerosol contribution. MARS-ReCO represents a substantial improvement regarding previous techniques as it takes into consideration the anisotropy of the surface, thus providing more realistic surface products. Furthermore, MARS-ReCO is fast and provides error bars on the retrieved surface reflectance. The validity and accuracy of MARS-ReCO is explored in a sensitivity analysis based on realistic synthetic data. According to experiments, MARS-ReCO provides accurate results (up to 10 reflectance error) under favorable acquisition conditions. In the companion article, photometric properties of Martian materials are retrieved using MARS-ReCO and validated using in situ measurements acquired during the Mars Exploration Rovers mission.

CRISM/MRO↗

Dust Optical Properties Over North Africa and Arabian Peninsula Derived from the AERONET Dataset

Dust optical properties over North Africa and the Arabian Peninsula are extracted from the quality assured multi-year datasets obtained at 14 sites of the Aerosol Robotic Network (AERONET). We select the data with (a) large aerosol optical depth (AOD >= 0.4 at 440 nm) and (b) small Angstrom exponent (A(sub ext)<= 0.2) for retaining high accuracy and reducing interference of non-dust aerosols. The result indicates that the major fraction of high aerosol optical depth days are dominated by dust over these sites even though it varies depending on location and time. We have found that the annual mean and standard deviation of single scattering albedo, asymmetry parameter, real refractive index, and imaginary refractive index for Saharan and Arabian desert dust is 0.944 +/- 0.005, 0.752 +/- 0.014, 1.498 +/- 0.032, and 0.0024 +/- 0.0034 at 550 nm wavelength, respectively. Dust aerosol selected by this method is less absorbing than the previously reported values over these sites. The weaker absorption of dust from this study is consistent with the studies using remote sensing techniques from satellite. These results can help to constrain uncertainties in estimating global dust shortwave radiative forcing.

Kim, D.↗

Estimating mass-absorption cross-section of ambient black carbon aerosols: theoretical, empirical, and machine learning models

The mass-absorption cross-section of black carbon (MAC BC ) is an essential parameter to link the atmospheric concentration of black carbon (BC) with its radiative forcing. When a direct calculation of MAC BC based on observations of aerosol light absorption and BC mass concentration is impossible, we rely on modeling and simulations to estimate MAC BC , but currently, there is no consensus model that can be relied on for accurate predictions across all atmospheric environments when BC particles have different coating thicknesses. Here, we applied five MAC BC prediction models (including three light scattering theories, an empirical model based on observations of particle mass concentrations, and a machine learning model developed in our previous work) to aerosols from three Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) field campaigns. While many studies have found that increasing the complexity of the models helps to constrain biases of the estimated MAC BC , our effort is to evaluate the models based on the criteria of simplicity and accuracy. We find that our machine learning model (support vector machine for regression, SVM) generally performs well across all DOE ARM field campaign data, while the accuracy of core-shell Mie theory depends on the bias correction algorithm applied to filter-based light absorption data. Generally, the empirical model for internally-mixed particles that we considered tends to over-predict MAC BC , while Mie theory for externally-mixed particles tends to under-predict MAC BC . An examination of the influence of coating material on BC cores suggests that the performance of our current SVM model is degraded when the BC is thickly-coated (e.g., it has undergone aging and mixing with other materials in the atmosphere).

54 ENVIRONMENTAL SCIENCES↗

The Calipso Version 4.5 Stratospheric Aerosol Subtyping Algorithm

The accurate classification of aerosol types injected into the stratosphere is important to properly characterize their chemical and radiative impacts within the Earth climate system. The updated stratospheric aerosol subtyping algorithm used in the version 4.5 (V4.5) release of the Cloud Aerosol Lidar with Orthogonal Polarization (CALIOP) level 2 data products now delivers more comprehensive and accurate classifications than its predecessor. The original algorithm identified four aerosol subtypes for layers detected above the tropopause: volcanic ash, smoke, sulfate/other, and polar stratospheric aerosol (PSA). In the revised algorithm, sulfates are separately identified as a distinct, homogeneous subtype, and the diffuse, weakly scattering layers previously assigned to the sulfate/other class are recategorized as a fifth “unclassified” subtype. By making two structural changes to the algorithm and revising two thresholds, the V4.5 algorithm improves the ability to discriminate between volcanic ash and smoke from pyrocumulonimbus injections, improves the fidelity of the sulfate subtype, and more accurately reflects the uncertainties inherent in the classification process. The 532 nm lidar ratio for volcanic ash was also revised to a value more consistent with the current state of knowledge. This paper briefly reviews the previous version of the algorithm (V4.1 and V4.2) then fully details the rationale and impact of the V4.5 changes on subtype classification frequency for specific events where the dominant aerosol type is known based on the literature. Classification accuracy is best for volcanic ash due to its characteristically high depolarization ratio. Smoke layers in the stratosphere are also classified with reasonable accuracy, though during the daytime a substantial fraction are misclassified as ash. It is also possible for mixtures of ash and sulfate to be misclassified as smoke. The V4.5 sulfate subtype accuracy is less than that for ash or smoke, with sulfates being misclassified as smoke about one-third of the time. However, because exceptionally tenuous layers are now assigned to the unclassified subtype and the revised algorithm levies more stringent criteria for identifying an aerosol as sulfate, it is more likely that layers labeled as this subtype are in fact sulfate compared to those assigned the sulfate/other classification in the previous data release.

Jason L Tackett↗

El Chichon aerosols in the stratosphere: Analyses of lidar data and calculations of radiation budget

Lidar observation at Fukuoka has provided over four years the data of ElChichon aerosols in the stratosphere. Analyses of the data show that an enormous amount of volcanic aerosols has continuously decreased since the beginning of 1983 with significant fluctuations. These fluctuations reveal themselves as a seasonal variation of aerosol content with a maximum in winter-spring and a minimum in summer. The vertical structure of the aerosol layer also shows the seasonal variation. Although the height of a peak around 18 km in the vertical profile of scattering ratio show littel variation, the higher second peak appears frequently from late fall and the lower third peak from late winter to late spring just as two and more tropopauses appear in these periods. The mechanism which causes the seasonal variation will be discussed in terms of the transport by the atmoshperic circulation and the removal through the tropopause gap. Radiation budget in the atmosphere was calculated taking into account the large amount of aerosols observed in the early stages of the El Chichon event. The heating rate of the atmosphere is more than 1 K in the bottom region of the stratosphere even in the nighttime. The possible effect of the volcanic aerosols on the other geophysical phenomena will be discussed using the calculated values of the heating rate.

Fujiwara, M.↗