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This research has been supported by the H2020 Marie Sklodowska-Curie Actions (grant no. 778349), the Spanish Ministry of Economy and Competitiveness (RTI2018101154.A.I00), and by the Russian Science Foundation (project 2117-00114, entitled Development of lidar retrieval algorithms)., This work focuses on the characterization of vertically resolved aerosol hygroscopicity properties and their direct radiative effects through a unique combination of ground-based and airborne remote sensing measurements during the Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) 2011 field campaign in the Baltimore-Washington DC metropolitan area. To that end, we combined aerosol measurements from a multiwavelength Raman lidar located at NASA Goddard Space Flight Center and the airborne NASA Langley High Spectral Resolution Lidar-1 (HSRL-1) lidar system. In situ measurements aboard the P-3B airplane and ground-based Aerosol Robotic Network - Distributed Regional Aerosol Gridded Observational Network (AERONET-DRAGON) served to validate and complement quantifications of aerosol hygroscopicity from lidar measurements and also to extend the study both temporally and spatially. The focus here is on 22 and 29 July 2011, which were very humid days and characterized by a stable atmosphere and increasing relative humidity with height in the planetary boundary layer (PBL). Combined lidar and radiosonde (temperature and water vapor mixing ratio) measurements allowed the retrieval of the Hanel hygroscopic growth factor which agreed with that obtained from airborne in situ measurements and also explained the significant increase of extinction and backscattering with height. Airborne measurements also confirmed aerosol hygroscopicity throughout the entire day in the PBL and identified sulfates and water-soluble organic carbon as the main species of aerosol particles. The combined Raman and HSRL-1 measurements permitted the inversion for aerosol microphysical properties revealing an increase of particle radius with altitude consistent with hygroscopic growth. Aerosol hygroscopicity pattern served as a possible explanation of aerosol optical depth increases during the day, particularly for fine-mode particles. Lidar measurements were used as input to the libRadtran radiative transfer code to obtain vertically resolved aerosol radiative effects and heating rates under dry and humid conditions, and the results reveal that aerosol hygroscopicity is responsible for larger cooling effects in the shortwave range (7-10 W m(-2) depending on aerosol load) near the ground, while heating rates produced a warming of 0.12 K d(-1) near the top of PBL where aerosol hygroscopic growth was highest., H2020 Marie Sklodowska-Curie Actions 778349, Spanish Ministry of Economy and Competitiveness RTI2018101154.A.I00, Russian Science Foundation (RSF) 2117-00114

NASA's Plankton, Aerosol, Cloud, ocean Ecosystem (PACE) mission, scheduled for launch in the timeframe of 2023, will carry a hyperspectral scanning radiometer named the Ocean Color Instrument (OCI) and two multi-angle polarimeters (MAPs): the UMBC Hyper-Angular Rainbow Polarimeter (HARP2) and the SRON Spectro-Polarimeter for Planetary EXploration one (SPEXone). The MAP measurements contain rich information on the microphysical properties of aerosols and hydrosols and therefore can be used to retrieve accurate aerosol properties for complex atmosphere and ocean systems. Most polarimetric aerosol retrieval algorithms utilize vector radiative transfer models iteratively in an optimization approach, which leads to high computational costs that limit their usage in the operational processing of large data volumes acquired by the MAP imagers. In this work, we propose a deep neural network (NN) forward model to represent the radiative transfer simulation of coupled atmosphere and ocean systems for applications to the HARP2 instrument and its predecessors. Through the evaluation of synthetic datasets for AirHARP (airborne version of HARP2), the NN model achieves a numerical accuracy smaller than the instrument uncertainties, with a running time of 0.01 s in a single CPU core or 1 ms in a GPU. Using the NN as a forward model, we built an efficient joint aerosol and ocean color retrieval algorithm called FastMAPOL, evolved from the well-validated Multi-Angular Polarimetric Ocean coLor (MAPOL) algorithm. Retrievals of aerosol properties and water-leaving signals were conducted on both the synthetic data and the AirHARP field measurements from the Aerosol Characterization from Polarimeter and Lidar (ACEPOL) campaign in 2017. From the validation with the synthetic data and the collocated High Spectral Resolution Lidar (HSRL) aerosol products, we demonstrated that the aerosol microphysical properties and water-leaving signals can be retrieved efficiently and within acceptable error. Comparing to the retrieval speed using a conventional radiative transfer forward model, the computational acceleration is 103 times faster with CPU or 104 times with GPU processors. The FastMAPOL algorithm can be used to operationally process the large volume of polarimetric data acquired by PACE and other future Earth-observing satellite missions with similar capabilities.

In the southeast Atlantic, well-defined smoke plumes from Africa advect over marine boundary layer cloud decks; both are most extensive around September, when most of the smoke resides in the free troposphere. A framework is put forth for evaluating the performance of a range of global and regional atmospheric composition models against observations made during the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) airborne mission in September 2016. A strength of the comparison is a focus on the spatial distribution of a wider range of aerosol composition and optical properties than has been done previously. The sparse airborne observations are aggregated into approximately 2∘ grid boxes and into three vertical layers: 3–6 km, the layer from cloud top to 3 km, and the cloud-topped marine boundary layer. Simulated aerosol extensive properties suggest that the flight-day observations are reasonably representative of the regional monthly average, with systematic deviations of 30 % or less. Evaluation against observations indicates that all models have strengths and weaknesses, and there is no single model that is superior to all the others in all metrics evaluated. Whereas all six models typically place the top of the smoke layer within 0–500 m of the airborne lidar observations, the models tend to place the smoke layer bottom 300–1400 m lower than the observations. A spatial pattern emerges, in which most models underestimate the mean of most smoke quantities (black carbon, extinction, carbon monoxide) on the diagonal corridor between 16∘ S, 6∘ E, and 10∘ S, 0∘ E, in the 3–6 km layer, and overestimate them further south, closer to the coast, where less aerosol is present. Model representations of the above-cloud aerosol optical depth differ more widely. Most models overestimate the organic aerosol mass concentrations relative to those of black carbon, and with less skill, indicating model uncertainties in secondary organic aerosol processes. Regional-mean free-tropospheric model ambient single scattering albedos vary widely, between 0.83 and 0.93 compared with in situ dry measurements centered at 0.86, despite minimal impact of humidification on particulate scattering. The modeled ratios of the particulate extinction to the sum of the black carbon and organic aerosol mass concentrations (a mass extinction efficiency proxy) are typically too low and vary too little spatially, with significant inter-model differences. Most models overestimate the carbonaceous mass within the offshore boundary layer. Overall, the diversity in the model biases suggests that different model processes are responsible. The wide range of model optical properties requires further scrutiny because of their importance for radiative effect estimates.

In the fall of 2017, an airborne field campaign was conducted from the NASA Armstrong Flight Research Center in Palmdale, California, to advance the remote sensing of aerosols and clouds with multi-angle polarimeters (MAP) and lidars. The Aerosol Characterization from Polarimeter and Lidar (ACEPOL) campaign was jointly sponsored by NASA and the Netherlands Institute for Space Research (SRON). Six instruments were deployed on the ER-2 high-altitude aircraft. Four were MAPs: the Airborne Hyper Angular Rainbow Polarimeter (AirHARP), the Airborne Multiangle SpectroPolarimetric Imager (AirMSPI), the Airborne Spectrometer for Planetary EXploration (SPEX airborne), and the Research Scanning Polarimeter (RSP). The remainder were lidars, including the Cloud Physics Lidar (CPL) and the High Spectral Resolution Lidar 2 (HSRL-2). The southern California base of ACEPOL enabled observation of a wide variety of scene types, including urban, desert, forest, coastal ocean, and agricultural areas, with clear, cloudy, polluted, and pristine atmospheric conditions. Flights were performed in coordination with satellite overpasses and ground-based observations, including the Ground-based Multiangle SpectroPolarimetric Imager (GroundMSPI), sun photometers, and a surface reflectance spectrometer. ACEPOL is a resource for remote sensing communities as they prepare for the next generation of spaceborne MAP and lidar missions. Data are appropriate for algorithm development and testing, instrument intercomparison, and investigations of active and passive instrument data fusion. They are freely available to the public. The DOI for the primary database is https://doi.org/10.5067/SUBORBITAL/ACEPOL2017/DATA001 (ACEPOL Science Team, 2017), while for AirMSPI it is https://doi.org/10.5067/AIRCRAFT/AIRMSPI/ACEPOL/RADIANCE/ELLIPSOID_V006 and https://doi.org/10.5067/AIRCRAFT/AIRMSPI/ACEPOL/RADIANCE/TERRAIN_V006 (ACEPOL AirMSPI 75 Science Team, 2017a, b). GroundMSPI data are at https://doi.org/10.5067/GROUND/GROUNDMSPI/ACEPOL/RADIANCE_v009 (GroundMSPI Science Team, 2017). Table 3 lists further details of these archives. This paper describes ACEPOL for potential data users and also provides an outline of requirements for future field missions with similar objectives.

Satellite quantification of aerosol effects on clouds relies on aerosol optical depth (AOD) as a proxy for aerosol concentration or cloud condensation nuclei (CCN). However, the lack of error characterization of satellite-based results hampers their use for the evaluation and improvement of global climate models. We show that the use of AOD for assessing aerosol–cloud interactions (ACIs) is inadequate over vast oceanic areas in the subtropics. Instead, we postulate that a more physical approach that consists of matching vertically resolved aerosol data from the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) satellite at the cloud-layer height with Moderate Resolution Imaging Spectroradiometer (MODIS) Aqua cloud retrievals reduces uncertainties in satellite-based ACI estimates. Combined aerosol extinction coefficients (σ) below cloud top (σBC) from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) and cloud droplet number concentrations (Nd) from MODIS Aqua yield high correlations across a broad range of σBC values, with σBC quartile correlations ≥0.78. In contrast, CALIOP-based AOD yields correlations with MODIS Nd of 0.54–0.62 for the two lower AOD quartiles. Moreover, σBC explains 41 % of the spatial variance in MODIS Nd, whereas AOD only explains 17 %, primarily caused by the lack of spatial covariability in the eastern Pacific. Compared with σBC, near-surface σ weakly correlates in space with MODIS Nd, accounting for a 16 % variance. It is concluded that the linear regression calculated from ln(Nd)–ln(σBC) (the standard method for quantifying ACIs) is more physically meaningful than that derived from the Nd–AOD pair.

Determining the direct aerosol radiative effect (DARE) of absorbing aerosols above clouds from satellite observations alone is a challenging task, in part because the radiative signal of the aerosol layer is not easily untangled from that of the clouds below. In this study, we use aircraft measurements from the NASA ObseRvations of CLouds above Aerosols and their intEractionS (ORACLES) project in the southeastern Atlantic to derive it with as few assumptions as possible. This is accomplished by using spectral irradiance measurements (Solar Spectral Flux Radiometer, SSFR) and aerosol optical depth (AOD) retrievals (Spectrometer for Sky-Scanning, Sun-Tracking Atmospheric Research, 4STAR) during vertical profiles (spirals) that minimize the albedo variability of the underlying cloud field – thus isolating aerosol radiative effects from those of the cloud field below. For two representative cases, we retrieve spectral aerosol single scattering albedo (SSA) and the asymmetry parameter (g) from these profile measurements and calculate DARE given the albedo range measured by SSFR on horizontal legs above clouds. For mid-visible wavelengths, we find SSA values from 0.80 to 0.85 and a significant spectral dependence of g. As the cloud albedo increases, the aerosol increasingly warms the column. The transition from a cooling to a warming top-of-aerosol radiative effect occurs at an albedo value (critical albedo) just above 0.2 in the mid-visible wavelength range. In a companion paper, we use the techniques introduced here to generalize our findings to all 2016 and 2017 measurements and parameterize aerosol radiative effects.

The total effect of aerosols, both directly and on cloud properties, remains the biggest source of uncertainty in anthropogenic radiative forcing on the climate. Correct characterization of intensive aerosol optical properties, particularly in conditions where absorbing aerosol is present, is a crucial factor in quantifying these effects. The southeast Atlantic Ocean (SEA), with seasonal biomass burning smoke plumes overlying and mixing with a persistent stratocumulus cloud deck, offers an excellent natural laboratory to make the observations necessary to understand the complexities of aerosol–cloud–radiation interactions. The first field deployment of the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) campaign was conducted in September of 2016 out of Walvis Bay, Namibia. Data collected during ORACLES-2016 are used to derive aerosol properties from an unprecedented number of simultaneous measurement techniques over this region. Here, we present results from six of the eight independent instruments or instrument combinations, all applied to measure or retrieve aerosol absorption and single-scattering albedo. Most but not all of the biomass burning aerosol was located in the free troposphere, in relative humidities typically ranging up to 60 %. We present the single-scattering albedo (SSA), absorbing and total aerosol optical depth (AAOD and AOD), and absorption, scattering, and extinction Ångström exponents (AAE, SAE, and EAE, respectively) for specific case studies looking at near-coincident and near-colocated measurements from multiple instruments, and SSAs for the broader campaign average over the month-long deployment. For the case studies, we find that SSA agrees within the measurement uncertainties between multiple instruments, though, over all cases, there is no strong correlation between values reported by one instrument and another. We also find that agreement between the instruments is more robust at higher aerosol loading (AOD400>0.4). The campaign-wide average and range shows differences in the values measured by each instrument. We find the ORACLES-2016 campaign-average SSA at 500 nm (SSA500) to be between 0.85 and 0.88, depending on the instrument considered (4STAR, AirMSPI, or in situ measurements), with the interquartile ranges for all instruments between 0.83 and 0.89. This is consistent with previous September values reported over the region (between 0.84 and 0.90 for SSA at 550nm). The results suggest that the differences observed in the campaign-average values may be dominated by instrument-specific spatial sampling differences and the natural physical variability in aerosol conditions over the SEA, rather than fundamental methodological differences.

Formaldehyde (HCHO) column data from satellites are widely used as a proxy for emissions of volatile organic compounds (VOCs), but validation of the data has been extremely limited. Here we use highly accurate HCHO aircraft observations from the NASA SEAC4RS (Studies of Emissions, Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys) campaign over the southeast US in August–September 2013 to validate and intercompare six retrievals of HCHO columns from four different satellite instruments (OMI, GOME2A, GOME2B and OMPS; for clarification of these and other abbreviations used in the paper, please refer to Appendix A) and three different research groups. The GEOS-Chem chemical transport model is used as a common intercomparison platform. All retrievals feature a HCHO maximum over Arkansas and Louisiana, consistent with the aircraft observations and reflecting high emissions of biogenic isoprene. The retrievals are also interconsistent in their spatial variability over the southeast US (r = 0.4–0.8 on a 0.5° × 0.5° grid) and in their day-to-day variability (r = 0.5–0.8). However, all retrievals are biased low in the mean by 20–51 %, which would lead to corresponding bias in estimates of isoprene emissions from the satellite data. The smallest bias is for OMI-BIRA, which has high corrected slant columns relative to the other retrievals and low scattering weights in its air mass factor (AMF) calculation. OMI-BIRA has systematic error in its assumed vertical HCHO shape profiles for the AMF calculation, and correcting this would eliminate its bias relative to the SEAC4RS data. Our results support the use of satellite HCHO data as a quantitative proxy for isoprene emission after correction of the low mean bias. There is no evident pattern in the bias, suggesting that a uniform correction factor may be applied to the data until better understanding is achieved.

Aerosol extinction coefficients (σa) and lidar ratios (LRs) are retrieved over the ocean from CALIPSO's Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) attenuated backscatter profiles by solving the lidar equation constrained with aerosol optical depths (AODs) derived by applying the Synergized Optical Depth of Aerosols (SODA) algorithm to ocean surface returns measured by CALIOP and CloudSat's Cloud Profiling Radar. σa and LR are retrieved for two independent scenarios that require somewhat different assumptions: (a) a single homogeneous atmospheric layer (1L) for which the LR is constant with height and (b) a vertically homogeneous layer with a constant LR overlying a marine boundary layer with a homogenous LR fixed at 25 sr (two-layer method, 2L). These new retrievals differ from the standard CALIPSO version 4.1 (V4) product, as the CALIOP–SODA method does not rely on an aerosol classification scheme to select LR. CALIOP–SODA σa and LR are evaluated using airborne high-spectral-resolution lidar (HSRL) observations over the northwest Atlantic. CALIOP–SODA LR (1L and 2L) positively correlates with its HSRL counterpart (linear correlation coefficient r>0.67), with a negative bias smaller than 17.4 % and a good agreement for σa (r≥0.78) with a small negative bias (≤|-9.2%|). Furthermore, a global comparison of optical depths derived by CALIOP–SODA and CALIPSO V4 reveals substantial discrepancies over regions dominated by dust and smoke (0.24), whereas Aqua's Moderate resolution Imaging Spectroradiometer (MODIS) and SODA AOD regional differences are within 0.06. Global maps of CALIOP–SODA LR feature high values over littoral zones, consistent with expectations of continental aerosol transport offshore. In addition, seasonal transitions associated with biomass burning from June to October over the southeast Atlantic are well reproduced by CALIOP–SODA LR.