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The Plankton, Aerosol, Clouds, ocean Ecosystem (PACE) mission presents new opportunities and new challenges in applying observations of two complementary multi-angle polarimeters for the space-based retrieval of global aerosol properties.Aerosol remote sensing from multi-angle radiometric-only observations enables aerosol characterization to a greater degree than single-view radiometers, as demonstrated by nearly two decades of heritage instruments. Adding polarimetry to the multi-angle observations allows for the retrieval of aerosol optical depth, Angstrom exponent,parameters of size distribution, measures of aerosol absorption, complex refractive index and degree of non-sphericity of the particles, as demonstrated by two independent retrieval algorithms applied to the heritage POLarization and Directionality of the Earth's Reflectance (POLDER) instrument. The reason why this detailed particle characterization is possible is because a multi-angle polarimeter measurement contains twice the number of Degrees of Freedom of Signal (DFS) compared to an observation from a single-view radiometer. The challenges of making use of this information content involve separating surface signal from atmospheric signal, especially when the surface is optically complex and especially in the ultraviolet portion of the spectrum where we show the necessity of polarization in making that separation. The path forward is likely to involve joint retrievalsthat will simultaneously retrieve aerosol and surface properties, although advances will berequired in radiative transfer modeling and in representing optically complex constituents in those models. Another challenge is in having the processing capability that can keep pace with the output of these instruments in an operational environment. Yet, preliminaryalgorithms applied to airborne multi-angle polarimeter observations offer encouraging results that demonstrate the advantages of these instruments to retrieve aerosol layer height, particle single scattering albedo, size distribution and spectral optical depth, and also show the necessity of polarization measurements, not just multi-angle radiometricmeasurements, to achieve these results.

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.

Passive ocean color images have provided a sustained synoptic view of the distribution of ocean optical properties and color and biogeochemical parameters for the past 20-plus years. These images have revolutionized our view of the ocean. Remote sensing of ocean color has relied on measurements of the radiance emerging at the top of the atmosphere, thus neglecting the polarization and the vertical components. Ocean color remote sensing utilizes the intensity and spectral variation of visible light scattered upward from beneath the ocean surface to derive concentrations of biogeochemical constituents and inherent optical properties within the ocean surface layer. However, these measurements have some limitations. Specifically, the measured property is a weighted-integrated value over a relatively shallow depth, it provides no information during the night and retrievals are compromised by clouds, absorbing aerosols, and low Sun zenithal angles. In addition, ocean color data provide limited information on the morphology and size distribution of marine particles. Major advances in our understanding of global ocean ecosystems will require measurements from new technologies, specifically lidar and polarimetry. These new techniques have been widely used for atmospheric applications but have not had as much as interest from the ocean color community. This is due to many factors including limited access to in-situ instruments and/or space-borne sensors and lack of attention in university courses and ocean science summer schools curricula. However, lidar and polarimetry technology will complement standard ocean color products by providing depth-resolved values of attenuation and scattering parameters and additional information about particle morphology and chemical composition. This review aims at presenting the basics of these techniques, examples of applications and at advocating for the development of in-situ and space-borne sensors. Recommendations are provided on actions that would foster the embrace of lidar and polarimetry as powerful remote sensing tools by the ocean science community.

The linear polarization of sunlight reflected by ocean surfaces in the shortwave infrared (SWIR), at geometries where specular reflection dominates the signal, is a direct function of the refractive index of the surface microlayer(SML). This simple physical concept is at the base of a novel technique presented in this study. We invert observations obtained by the airborne Research Scanning Polarimeter (RSP) in the sun glint region, where each pixel's radiance is dominated by the signal originating from the wave slopes oriented precisely to cause specular reflection. The SWIR wavelength ensures minimization of aerosol interference when radiance travels through the atmosphere; strong absorption by the water body then limits the penetration depth to the first micrometer or so, effectively probing the SML. The resulting Degree of Linear Polarization (DoLP) is then governed by the refractive index via the Fresnel law for the specfic pixel geometry, independently of the wind speed. The selected dataset concerns several field deployments from both low- and high-altitude aircraft, including total reflectance measurements with the sole purpose of accounting for the residual aerosol effect.Stable retrievals from transects above pure seawater yielded values of refractive index that match the values published in the literature within an accuracy of 5 x 10 [superscript 4]. Flying over the oil spill caused by the explosion of the Deepwater Horizon platform, detected variations were found compatible with the presence of an oil slick. The robustness of the results, guaranteedby the high RSP polarimetric accuracy (less than or equal to 0:2%), opens the possibility for remote-sensing detection of other entities that similarly affect the refractive index including whitecaps, microplastics, biological gels, seaweed and grass mats.

The ObseRvations of Aerosols above Clouds and their interactions (ORACLES) project is making a series of field deployments to the southeastern Atlantic with NASA ER-2 and P3 aircraft to acquire both detailed remote sensing observations and in situ measurements of the aerosols and clouds in that region. This area is home to one of the largest low-level cloud decks on Earth that is seasonally affected by vast plumes of smoke from biomass burning, which in effect provides a natural experiment testing the radiative and microphysical interactions between the smoke and the clouds. The downward solar radiation at the surface, or cloud top, is always reduced by the presence of smoke. However, whether the amount of sunlight reflected back out to space is increased, or decreased by the presence of smoke is sensitively dependent on the brightness of the clouds and the fraction of light that the smoke absorbs each time light hits a smoke particle. In this study we use data from the Research Scanning Polarimeter, an along track scanning instrument, that provides measurements of the Stokes parameters I, Q and U at 410, 470, 555, 670, 865, 960, 1590, 1880 and 2260 nm at 150 viewing angles over a range of +/- 60° from nadir for each contiguous sub-aircraft pixel (~ 300 m in size). A retrieval algorithm is applied to the data acquired with a table look up technique, similar to that of the operational POLDER algorithm, to provide a first guess of the complex refractive index, optical depth and size distribution of the smoke particles together with cloud droplet size and optical depth. A subsequent iterative fitting procedure, where the fact that the doubling/adding method allows the construction of the Green's function for the radiative transfer equation, is used to obtain an efficient and statistically optimal estimate of the aerosol and cloud retrieval parameters. These retrieval parameters are evaluated against in situ observations, when available, and the optical depth and intensive lidar variables that are measured by the High Spectral Resolution Lidar 2. Finally, the aerosol and cloud retrievals are used to evaluate the variations in top of the atmosphere, surface/cloud top shortwave radiative forcing and atmospheric absorption that are caused by variations in the smoke and clouds.

The physical and chemical properties of soil dust aerosol particles fundamentally affect their interaction with climate, including shortwave absorption and radiative forcing, nucleation of cloud droplets and ice crystals, heterogeneous formation of sulfates and nitrates on the surface of dust particles, and atmospheric processing of iron into bioavailable forms that increase the productivity of marine phytoplankton. Lidar measurements, such as extinction-to-backscatter, color and depolarization ratios, are frequently used to distinguish between aerosol types with different physical and chemical properties. The chemical composition of aerosol particles determines their complex refractive index, hence affecting their backscattering properties. Here we present a study on how dust aerosol backscattering and depolarization properties at wavelengths of 355, 532 and 1064 nm are related to size and complex refractive index, which varies with the mineral composition of the dust. Dust aerosols are represented by collections of spheroids with a range of prolate and oblate aspect ratios and their optical properties are obtained using T-matrix calculations. We find simple, systematic relationships between lidar observables and the dust size and complex refractive index that may aid the use of space-based or airborne lidars for direct retrieval of dust properties or for the evaluation of chemical transport models using forward simulated lidar variables. In addition, we present first results on the spatial variation of forward-simulated lidar variables based on a dust model that accounts for the atmospheric cycle of eight different mineral types plus internal mixtures of seven mineral types with iron oxides, which was recently implemented in the NASA GISS Earth System ModelE2.

In this study, we present a radiative transfer model, so-called OSOAA, that is able to predict the radiance and degree of polarization within the coupled atmosphere-ocean system in the presence of a rough sea surface. The OSOAA model solves the radiative transfer equation using the successive orders of scattering method. Comparisons with another operational radiative transfer model showed a satisfactory agreement within 0.8%. The OSOAA model has been designed with a graphical user interface to make it user friendly for the community. The radiance and degree of polarization are provided at any level, from the top of atmosphere to the ocean bottom. An application of the OSOAA model is carried out to quantify the directional variations of the water leaving reflectance and degree of polarization for phytoplankton and mineral-like dominated waters. The difference between the water leaving reflectance at a given geometry and that obtained for the nadir direction could reach 40%, thus questioning the Lambertian assumption of the sea surface that is used by inverse satellite algorithms dedicated to multi-angular sensors. It is shown as well that the directional features of the water leaving reflectance are weakly dependent on wind speed. The quantification of the directional variations of the water leaving reflectance obtained in this study should help to correctly exploit the satellite data that will be acquired by the current or forthcoming multi-angular satellite sensors.

We illustrate our methods on examples from the recent NASA's field campaigns POlarimeter Definition EXperiment (PODEX, based in Palmdale, California, January - February 2013) and Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS, based in Houston, Texas in August - September 2013). During these campaigns the RSP was onboard the NASA's long-range high-altitude ER-2 aircraft together with an array of other remote sensing instrumentation. Correlative sampling measurements from another aircraft were also available. The data obtained during these campaigns provides an excellent opportunity to study cloud properties in variety of locations and atmospheric conditions. We present examples of boundary layer cumulus and stratocumulus clouds, liquid altostratus clouds, and fogs. In the latter two cases the droplet size distribution derived from RFT analysis exhibited multiple modes corresponding to different cloud layers, as supported by the correlative lidar atmospheric profiles.

We report the results of high-accuracy controlled laboratory measurements of the Stokes reflection matrix for suspensions of submicrometer-sized latex particles in water and compare them with the results of a numerically exact computer solution of the vector radiative transfer equation (VRTE). The quantitative performance of the VRTE is monitored by increasing the volume packing density of the latex particles from 2 to 10. Our results indicate that the VRTE can be applied safely to random particulate media with packing densities up to 2. VRTE results for packing densities of the order of 5 should be taken with caution, whereas the polarized bidirectional reflectivity of suspensions with larger packing densities cannot be accurately predicted. We demonstrate that a simple modification of the phase matrix entering the VRTE based on the so-called static structure factor can be a promising remedy that deserves further examination.

Remote sensing of aerosol optical properties is difficult, but multi-angle, multi-spectral, polarimetric instruments have the potential to retrieve sufficient information about aerosols that they can be used to improve global climate models. However, the complexity of these instruments means that it is difficult to intuitively understand the relationship between instrument design and retrieval success. We apply a Bayesian statistical technique that relates instrument characteristics to the information contained in an observation. Using realistic simulations of fine size mode dominated spherical aerosols, we investigate three instrument designs. Two of these represent instruments currently in orbit: the Multiangle Imaging SpectroRadiometer (MISR) and the POLarization and Directionality of the Earths Reflectances (POLDER). The third is the Aerosol Polarimetry Sensor (APS), which failed to reach orbit during recent launch, but represents a viable design for future instruments. The results show fundamental differences between the three, and offer suggestions for future instrument design and the optimal retrieval strategy for current instruments. Generally, our results agree with previous validation efforts of POLDER and airborne prototypes of APS, but show that the MISR aerosol optical thickness uncertainty characterization is possibly underestimated.