A Markov chain approach is developed to model polarized mid-to long-wave infrared radiative transfer in an optically anisotropic medium. Such a medium contains oriented non-spherical particles with azimuthal randomness. Our model considers variations of temperature, pressure, gas concentration, and particle size distribution in the vertical dimension of the medium and resolves the total and polarized radiation in twodimensional angular space. It also accounts for emission, scattering, and absorption of the medium, as well as directional and polarized surface emission and reflection. Illustrative simulations are performed using MODIS infrared bands centered at 9.73, 11.03, and 12.02 mu m and several standard model atmospheres containing oriented dust or ice spheroids. The results are compared to those obtained for spherical droplets. Our preliminary numerical results demonstrate that while infrared brightness temperature contains information about particle amount, size, and layer height, adding multi-angle and spectro-polarimetry provides further remote sensing sensitivity to type, orientation, and morphology of the non-spherical particles. When reliable a priori information on the atmospheric physical temperature and absorbing gas profiles is available, infrared multi-angle polarimetry is a promising tool to fill the gap of shortwave and microwave remote sensing by resolving micro-meter scale particle properties to which shortwave and microwave frequencies have less sensitivity. Our simulation also reveals that solar radiation exerts a pronounced influence on the top-of-atmosphere brightness temperature when the wavelength approaches the short-wavelength end of the mid-wave infrared (approximate to 3-4 mu m).

There is a need to quickly convert aerosol microphysical properties into optical properties for global modeling, data assimilation, and remote sensing applications. This is generally accomplished through look-up tables (LUTs) of aerosol mass extinction coefficients (MEC), mass absorption coefficients (MAC), asymmetry parameters, normalized phase functions, etc. Unfortunately, many scientists are using outdated LUTs that are based upon measurements and computational techniques first published by Shettle and Fenn (1979) and later updated by Hess et al. (1998). Thus, the computations in common use are still largely based upon Mie theory and in situ information that has not been updated during this century.The Table of Aerosol Optics (TAO) is an open relational database (under construction) that expands upon existing LUTs by including recent measurements and new computational techniques for non-spherical particles (https://science.larc.nasa.gov/mira-wg/topics/tao/). The ‘open’ aspect of TAO is important, since the measurements and techniques of today will undoubtedly yield to different values in the future. This open architecture allows specialists to add new tables and gain exposure for their work and benefits modelers and remote sensing scientists by giving them easy access to computations that utilize the latest techniques. Quality is controlled by requiring methods to be peer-reviewed in the scientific literature.Thus far, we have computed mass extinction coefficients, mass absorption coefficients, lidar ratios, etc., at 73 wavelengths ranging from 0.25-40 µm for black carbon (BC), brown carbon (BrC), non-absorbing organic carbon, and mineral dust. For mineral dust, we use hexahedra shapes and mineral mixtures of montmorillonite, illite, hematite, and goethite. The illite volume fraction varies from 0 to 59% to capture the range of real refractive indices found in AERONET climatologies; the sum of the hematite and goethite mass fractions are ~2%. Additional mixtures will be added as appropriate.We have also computed optical properties for 22 size distributions of bare aggregated BC using the Multi-Sphere T-Matrix (MSTM) code (https://github.com/dmckwski/MSTM) at several remote sensing wavelengths. Our MSTM computations use aggregates of 20-nm spherules with particle-cluster growth. We obtained mass absorption coefficients (MACs) of 7.2-7.5 m2/g at a mid-visible wavelength (532 nm) when the BC fractal dimension was fixed at Df = 1.8 (i.e., fresh BC), consistent with values commonly recommended in literature reviews.We will present the TAO vision and example results for several aerosol types. TAO is part of the Models, In situ, and Remote sensing of Aerosols (MIRA) working group. MIRA seeks to build collaboration, consistency, and openness amongst the aerosol disciplines. We seek community feedback from aerosol scientists regarding the construction and content of TAO, especially in this early phase. Check out the MIRA webpage at https://science.larc.nasa.gov/mira-wg/ and subscribe to our mailing list at https://espo.nasa.gov/lists/listinfo/mira.Hess et al. (1998): Optical properties of aerosols and clouds: The software package OPAC, BAMS, 79, 831–844.Shettle and Fenn (1979): Tech. Rep. AFGL-TR-790214, Air Force Geophysics Laboratory, 1979.

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.

Abstract. Improvements in air quality and Earth’s climate predictions require improvements of the aerosol speciation in chemical transport models, using observational constraints. Aerosol speciation (e.g., organic aerosols, black carbon, sulfate, nitrate, ammonium, dust or sea salt) is typically determined using in situ instrumentation. Continuous, routine surface network aerosol composition measurements are not uniformly widespread over the globe. Satellites, on the other hand, can provide a maximum coverage of the horizontal and vertical atmosphere but observe aerosol optical properties (and not aerosol speciation) based on remote sensing instrumentation. Combinations of satellite-derived aerosol optical properties can inform on air mass aerosol types (AMTs e.g., clean marine, dust, polluted continental). However, these AMTs are subjectively defined, might often be misclassified and are hard to relate to the critical parameters that need to be refined in models. In this paper, we derive AMTs that are more directly related to sources and hence to speciation. They are defined, characterized, and derived using simultaneous in situ gas-phase, chemical and optical instruments on the same aircraft during the Study of Emissions and Atmospheric Composition, Clouds, and Climate Coupling by Regional Surveys (SEAC4RS, US, summer of 2013). First, we prescribe well-informed AMTs that display distinct aerosol chemical and optical signatures to act as a training AMT dataset. These in situ observations reduce the errors and ambiguities in the selection of the AMT training dataset. We also investigate the relative skill of various combinations of aerosol optical properties to define AMTs and how much these optical properties can capture dominant aerosol speciation. We find distinct optical signatures for biomass burning (from agricultural or wildfires), biogenic and dust-influence AMTs. Useful aerosol optical properties to characterize these signatures are the extinction angstrom exponent (EAE), the single scattering albedo, the difference of single scattering albedo in two wavelengths, the absorption coefficient, the absorption angstrom exponent (AAE), and the real part of the refractive index (RRI). We find that all four AMTs studied when prescribed using mostly airborne in situ gas measurements, can be successfully extracted from at least three combinations of airborne in situ aerosol optical properties (e.g., EAE, AAE and RRI) over the US during SEAC4RS. However, we find that the optically based classifications for BB from agricultural fires and polluted dust include a large percentage of misclassifications that limit the usefulness of results relating to those classes. The technique and results presented in this study are suitable to develop a representative, robust and diverse source-based AMT database. This database could then be used for widespread retrievals of AMTs using existing and future remote sensing suborbital instruments/networks. Ultimately, it has the potential to provide a much broader observational aerosol data set to evaluate chemical transport and air quality models than is currently available by direct in situ measurements. This study illustrates how essential it is to explore existing airborne datasets to bridge chemical and optical signatures of different AMTs, before the implementation of future spaceborne missions (e.g., the next generation of Earth Observing System (EOS) satellites addressing Aerosol, Cloud, Convection and Precipitation (ACCP) designated observables).

Cirrus clouds are important to the radiation energy budget due to their temporal duration and >50% global coverage.1 The variety of ice crystal shapes and sizes in a cirrus cloud create challenges differentiating radiation insulated by the Earth's atmosphere from that reflected back to space. The optical thickness of these clouds is often too thin to be sensed using any current passive satellite radiometers. Sensitivity studies in the UV have shown that the angle of linear polarization (AoLP) of solar radiation backscattered from thin cirrus clouds and thin liquid water clouds is rotated.2 Pust and Shaw also demonstrated subvisual clouds detection in degree of linear polarization (DoLP) and AoLP.3 An Ultraviolet Stokes Imaging Polarimeter (ULTRASIP) was designed and developed for optically thin clouds and sky observations in the 360 nm - 450 nm range.4 ULTRASIP is a time modulated polarimeter rotating a wire-grid polarizer in front of a 16-bit, water-cooled, back-illuminated CCD sensor. Polarized light scattering models will be compared in the visible and the UV to motivate measurements in this waveband.5

Advanced inversion Multi-term approach utilizing multiple a priori constraints is proposed. The approach is used as a base for the first unified algorithm GRASP that is applicable to diverse remote sensing observations and retrieving a variety of atmospheric properties. The utilization of GRASP for diverse remote sensing observations is demonstrated.

An optimization algorithm is developed to retrieve the vertical profiles of aerosol concentration, refractive index and size distribution, spherical particle fraction, as well as a set of ocean surface reflection properties. The retrieval uses a combined set of lidar and polarimeter measurements. Our inversion includes using 1) a hybrid radiative transfer (RT) model that combines the computational strengths of the Markov-chain and adding-doubling approaches in modeling polarized RT in vertically inhomogeneous and homogeneous media, respectively; 2) a bio-optical model that represents the water-leaving radiance as a function of chlorophyll-a concentration for open ocean; 3) the constraints regarding the smooth variations of several aerosol properties along altitude; and 4) an optimization scheme. We tested the retrieval using 50 sets of coincident lidar and polarimetric data acquired by NASA Langley airborne HSRL-2 and GISS RSP respectively during the ORACLES field campaign. The retrieved vertical profiles of aerosol single scattering albedo (SSA) and size distribution are compared to the reference data measured by University of Hawaii’s HiGEAR instrumentation suite. At the vertical resolution of 315 m, the mean absolute difference (MAD) between retrieved and HiGEAR derived aerosol SSA is 0.028. And the MADs between retrieved and HiGEAR effective radius of aerosol size distribution are 0.012 and 0.377 micron for fine and coarse aerosols, respectively. The retrieved aerosol optical depth (AOD) above aircraft are compared to NASA Ames 4-STAR measurement. The MADs are found to be 0.010, 0.006, and 0.004 for AOD at 355, 532 and 1,064 nm, respectively.

Abstract The Dark‐target (DT) aerosol algorithm retrieves spectral Aerosol Optical Depth (AOD) and other aerosol properties from Moderate‐resolution Imaging Spectrometer (MODIS) reflectance observations. Over the ocean, the DT algorithm is known to contain scattering‐angle‐dependent biases in its retrievals of AOD, Angstrom Exponent (AE), and Fine Mode Fraction (FMF) for dust aerosols. Following a two‐step strategy to improve the DT retrieval of dust over ocean, for which the first step is to identify dusty pixels (reported in “Part 1”), in this “Part 2,” we report on construction of a new dust model lookup table (LUT) and the strategy for applying it within the existing DT algorithm. In particular, we evaluate different characterizations of dust optical properties from a variety of frameworks and databases, and compare them with the current DT retrieval assumptions. Substituting the standard operational LUT with a spheroid dust model with identified dusty pixels shows significant improvement when compared with collocated AERONET‐identified dusty pixels. Specifically, the application of the new dust model to dusty pixels reduces their AOD bias from 0.06 to 0.02 while improving the fraction of retrievals within expected error from 64% to 82%. At the same time, the overall bias in AE is reduced from 0.13 to 0.06, and the scattering‐angle‐dependent AE bias is largely eliminated. In testing on two full months of data (April and July), the new retrieval will reduce the monthly mean AOD by up to 0.1 and 0.2 in the north Atlantic and Arabian seas, respectively. The average AE and FMF are also reduced in these dust heavy regions.

We have developed a method for evaluating the fidelity of the Aerosol Robotic Network (AERONET) retrieval algorithms by mimicking atmospheric extinction and radiance measurements in a laboratory experiment. This enables radiometric retrievals that use the same sampling volumes, relative humidities, and particle size ranges as observed by other in situ instrumentation in the experiment. We use three Cavity Attenuated Phase Shift (CAPS) monitors for extinction and University of Maryland Baltimore County’s (UMBC) three-wavelength Polarized Imaging Nephelometer (PI-Neph) for angular scattering measurements. We subsample the PI-Neph radiance measurements to angles that correspond to AERONET almucantar scans, with simulated solar zenith angles ranging from 50 ∘ to 77 ∘ . These measurements are then used as input to the Generalized Retrieval of Aerosol and Surface Properties (GRASP) algorithm, which retrieves size distributions, complex refractive indices, single-scatter albedos, and bistatic LiDAR ratios for the in situ samples. We obtained retrievals with residuals less than 8% for about 90 samples. Samples were alternately dried or humidified, and size distributions were limited to diameters of less than 1.0 or 2.5 μ m by using a cyclone. The single-scatter albedo at 532 nm for these samples ranged from 0.59 to 1.00 when computed with CAPS extinction and Particle Soot Absorption Photometer (PSAP) absorption measurements. The GRASP retrieval provided single-scatter albedos that are highly correlated with the in situ single-scatter albedos, and the correlation coefficients ranged from 0.916 to 0.976, depending upon the simulated solar zenith angle. The GRASP single-scatter albedos exhibited an average absolute bias of +0.023–0.026 with respect to the extinction and absorption measurements for the entire dataset. We also compared the GRASP size distributions to aerodynamic particle size measurements, using densities and aerodynamic shape factors that produce extinctions consistent with our CAPS measurements. The GRASP effective radii are highly correlated (R = 0.80) and biased under the corrected aerodynamic effective radii by 1.3% (for a simulated solar zenith angle of θ ∘ = 50 ∘ ); the effective variance indicated a correlation of R = 0.51 and a relative bias of 280%. Finally, our apparatus was not capable of measuring backscatter LiDAR ratios, so we measured bistatic LiDAR ratios at a scattering angle of 173 degrees. The GRASP bistatic LiDAR ratios had correlations of 0.71 to 0.86 (depending upon simulated θ ∘ ) with respect to in situ measurements, positive relative biases of 2–10%, and average absolute biases of 1.8–7.9 sr.

The research frontiers of radiative transfer (RT) in coupled atmosphere-ocean systems are explored to enable new science and specifically to support the upcoming Plankton, Aerosol, Cloud ocean Ecosystem (PACE) satellite mission. Given (i) the multitude of atmospheric and oceanic constituents at any given moment that each exhibits a large variety of physical and chemical properties and (ii) the diversity of light-matter interactions (scattering, absorption, and emission), tackling all outstanding RT aspects related to interpreting and/or simulating light reflected by atmosphere-ocean systems becomes impossible. Instead, we focus on both theoretical and experimental studies of RT topics important to the science threshold and goal questions of the PACE mission and the measurement capabilities of its instruments. We differentiate between (a) forward (FWD) RT studies that focus mainly on sensitivity to influencing variables and/or simulating data sets, and (b) inverse (INV) RT studies that also involve the retrieval of atmosphere and ocean parameters. Our topics cover (1) the ocean (i.e., water body): absorption and elastic/inelastic scattering by pure water (FWD RT) and models for scattering and absorption by particulates (FWD RT and INV RT); (2) the air-water interface: variations in ocean surface refractive index (INV RT) and in whitecap reflectance (INV RT); (3) the atmosphere: polarimetric and/or hyperspectral remote sensing of aerosols (INV RT) and of gases (FWD RT); and (4) atmosphere-ocean systems: benchmark comparisons, impact of the Earth's sphericity and adjacency effects on space-borne observations, and scattering in the ultraviolet regime (FWD RT). We provide for each topic a summary of past relevant (heritage) work, followed by a discussion (for unresolved questions) and RT updates.

Goddard Space Flight Center, Greenbelt, MD, USA Universities Space Research Association (USRA), Columbia, MD, USA University of Maryland, Baltimore County, Baltimore, MD, USA Laboratoire d’Optique Atmosphérique, UMR8518, CNRS Université de Lille 1, Villeneuve d’Ascq, France GRASP-SAS, Remote Sensing Developments, Université de Lille, Villeneuve d’Ascq, 59655, France RT Solutions, Cambridge, MA 02138, USA

Polarimetry is one of the most promising types of remote sensing for improved characterization of atmospheric aerosol. Indeed, aerosol particles constitute a highly variable atmospheric component characterized by a large number of parameters describing particle sizes, morphologies (including shape and internal structure), absorption and scattering properties, amounts, horizontal and vertical distribution, etc. Reliable monitoring of all these parameters is very challenging, and therefore the aerosol effects on climate and environment are considered to be among the most uncertain factors in climate and environmental research. In this regard, observations that provide both the angular distribution of the scattered atmospheric radiation as well as its polarization state at multiple wavelengths covering the UV-SWIR spectral range carry substantial implicit information on the atmospheric composition. Therefore, high expectations in improving aerosol characterization are associated with detailed passive photopolarimetric observations. The critical need to use space-borne polarimetry for global accurate monitoring of detailed aerosol properties was first articulated in the late 1980s and early 1990s. By now, several orbital instruments have already provided polarization observations from space, and a number of advanced missions are scheduled for launch in the coming years by international and national space agencies. The first and most extensive record of polarimetric imagery was provided by POLDER-I, POLDER-II, and POLDER/PARASOL multi-angle multi-spectral polarization sensors. Polarimetric observations with the POLDER-like design intended for collecting extensive multi-angular multi-spectral measurements will be provided by several instruments, such as the MAI/TG-2, CAPI/TanSat, and DPC/GF-5 sensors recently launched by the Chinese Space Agency. Instruments such as the 3MI/MetOp-SG, MAIA, SpexOne and HARP2 on PACE, POSP, SMAC, PCF, DPC-Lidar, ScanPol and MSIP/Aerosol-UA, MAP/Copernicus CO2 Monitoring, etc. are planned to be launched by different space agencies in the coming decade. The concepts of these future instruments, their technical designs, and the accompanying algorithm development have been tested intensively and analyzed using diverse airborne prototypes. Certain polarimetric capabilities have also been implemented in such satellite sensors as GOME-2/MetOp and SGLI/GCOM-C. A number of aerosol retrieval products have been developed based on the available measurements and successfully used for different scientific applications. However, the completeness and accuracy of aerosol data operationally derived from polarimetry do not yet appear to have reached the accuracy levels implied by theoretical sensitivity studies that analyzed the potential information content of satellite polarimetry. As a result, the dataset provided by MODIS is still most frequently used by the scientific community, yet this sensor has neither polarimetric nor multi-angular capabilities. Admittedly polarimetric multi-angular observations are highly complex and have extra sensitivities to aerosol particle morphology, vertical variability of aerosol properties, polarization of surface reflectance, etc. As such, they necessitate state-of-the-art forward modeling based on first-principles physics which remains rare, and conventional retrieval approaches based on look-up tables turn out to be unsuitable to fully exploit the information implicit in the measurements. Several new-generation retrieval approaches have recently been proposed to address these challenges. These methods use improved forward modeling of atmospheric (polarized) radiances and implement a search in the continuous space of solutions using rigorous statistically optimized inversions. Such techniques provide more accurate retrievals of the main aerosol parameters such as aerosol optical thickness and yield additional parameters such as aerosol absorption. However, the operational implementation of advanced retrieval approaches generally requires a significant extra effort, and the forward-modeling part of such retrievals still needs to be substantially improved. Ground-based passive polarimetric measurements have also been evolving over the past decade. Although polarimetry helps improve aerosol characterization, especially of the fine aerosol mode, the operators of major observational networks such as AERONET remain reluctant to include polarimetric measurements as part of routine retrievals owing to their high complexity and notable increase in effort required to acquire and interpret polarization data. In addition to remote-sensing observations, polarimetric characteristics of aerosol scattering have been measured in situ as well as in the laboratory using polar nephelometers. Such measurements constitute direct observations of single scattering with no contributions from multiple scattering effects and therefore provide unique data for the validation of aerosol optical models and retrieval concepts. This article overviews the above-mentioned polarimetric observations, their history and expected developments, and the state of resulting aerosol products. It also discusses the main achievements and challenges in the exploitation of polarimetry for the improved characterization of atmospheric aerosols. (C) 2018 The Authors. Published by Elsevier Ltd.

Aerosol models, composed of size distribution, complex refractive index, and spherical fraction, are derived from a new synergistic retrieval of airborne in situ angular scattering measurements made by the Polarized Imaging Nephelometer and absorption measurements from the Particle Soot Absorption Photometer. The data utilized include phase function (F-11), degree of polarization (-F-12/F-11), and absorption coefficient (beta(abs)) measured at low relative humidities during the Studies of Emissions and Atmospheric Composition, Clouds, and Climate Coupling by Regional Surveys (SEAC(4)RS) and Deep Convection Clouds and Chemistry (DC3) field campaigns. The Generalized Retrieval of Aerosol and Surface Properties (GRASP) is applied to these measurements to obtain summaries of particle properties that are optically consistent with the original measurements. A classification scheme is then used to categorize the corresponding retrieval results. Inversions performed on the DC3 measurements indicate the presence of a significant amount of dust-like aerosol in the inflow of storms sampled during this campaign, with the quantity of dust present depending strongly on the underlying surface features. In the SEAC(4)RS data, the retrieved size distributions were found to be remarkably similar among a range of aerosol types, including urban and industrial, biogenic, and biomass burning (BB) emissions. These aerosol types were found to have average fine mode volume median radii 0.155 <= r(vf) <= 0.163 mu m and lognormal standard deviations 0.32 <= sigma(f) <= 0.36. There were, however, consistent differences between the angular scattering patterns of the BB samples and the other particle types. The GRASP retrieval predominantly attributed these differences to elevated real and imaginary refractive indices in the BB samples (m(532nm) approximate to 1.55 + 0.007i) relative to the two other categories (m(532nm) approximate to 1.51 + 0.004i).