Search

The springtime atmosphere over the southeast Atlantic Ocean (SEA) is subjected to a consistent layer of biomass burning (BB) smoke from widespread fires on the African continent. An elevated humidity signal is coincident with this layer, consistently proportional to the amount of smoke present. The combined humidity and BB aerosol has potentially significant radiative and dynamic impacts. Here, we use aircraft-based observations from the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) deployments in conjunction with reanalyses to characterize covariations in humidity and BB smoke across the SEA. The observed plume–vapor relationship, and its agreement with the European Centre for Medium-Range Weather Forecasts (ECMWF) Reanalysis version 5 (ERA5) and Copernicus Atmosphere Monitoring Service (CAMS) reanalysis, persists across all observations, although the magnitude of the relationship varies as the season progresses. Water vapor is well represented by the reanalyses, while CAMS tends to underestimate carbon monoxide especially under high BB. While CAMS aerosol optical depth (AOD) is generally overestimated relative to ORACLES AOD, the observations show a consistent relationship between carbon monoxide (CO) and aerosol extinction, demonstrating the utility of the CO tracer to understanding vertical aerosol distribution. We next use k-means clustering of the reanalyses to examine multi-year seasonal patterns and distributions. We identify canonical profile types of humidity and of CO, allowing us to characterize changes in vapor and BB atmospheric structures, and their impacts as they covary. While the humidity profiles show a range in both total water vapor concentration and in vertical structure, the CO profiles primarily vary in terms of maximum concentration, with similar vertical structures in each. The distribution of profile types varies spatiotemporally across the SEA region and through the season, ranging from largely one type in the northeast and southwest to more evenly distributed between multiple types where air masses meet in the middle of the SEA. These distributions follow patterns of transport from the humid, smoky source region (greatest influence in the northeast of the SEA) and the seasonal changes in both humidity and smoke (increasing and decreasing through the season, respectively). With this work, we establish a framework for a more complete analysis of the broader radiative and dynamical effects of humid aerosols over the SEA.

Inadequate knowledge about the complex microphysical and optical processes of the aerosol–cloud system severely restricts our ability to quantify the resultant impact on climate. Contrary to the negative radiative forcing (cooling) exerted by aerosols in cloud-free skies over dark surfaces, the absorbing aerosols, when lofted over the clouds, can potentially lead to significant warming of the atmosphere. The sign and magnitude of the aerosol radiative forcing over clouds are determined mainly by the amount of aerosol loading, the absorption capacity of aerosols or single-scattering albedo (SSA), and the brightness of the underlying cloud cover. In satellite-based algorithms that use measurements from passive sensors, the assumption of aerosol SSA is known to be the largest source of uncertainty in quantifying above-cloud aerosol optical depth (ACAOD). In this paper, we introduce a novel synergy algorithm that combines direct airborne measurements of ACAOD and the top-of-atmosphere (TOA) spectral reflectance from Ozone Monitoring Instrument (OMI) and Moderate Resolution Imaging Spectroradiometer (MODIS) sensors of NASA's A-train satellites to retrieve (1) SSA of light-absorbing aerosols lofted over the clouds and (2) aerosol-corrected cloud optical depth (COD). Radiative transfer calculations show a marked sensitivity of the TOA measurements to ACAOD, SSA, and COD, further suggesting that the availability of accurate ACAOD allows retrieval of SSA for above-cloud aerosol scenes using the “color ratio” algorithm developed for satellite sensors carrying ultraviolet (UV) and visible-near-IR (VNIR) wavelength bands. The proposed algorithm takes advantage of airborne measurements of ACAOD acquired from the High Spectral Resolution Lidar-2 (HSRL-2) and Spectrometer for Sky-Scanning, Sun-Tracking Atmospheric Research (4STAR) sun photometer operated during the ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) field campaign (September 2016, August 2017, and October 2018) over the southeastern Atlantic Ocean and synergizes them with TOA reflectance from OMI and MODIS to derive spectral SSA in the near-UV (354–388 nm) and VNIR (470–860 nm), respectively. When compared against the ORACLES airborne remote sensing and in situ measurements and the inversion dataset of the ground-based Aerosol Robotic Network (AERONET) over land, the retrieved spectral SSAs from the satellites, on average, were found to be within agreement of ∼ 0.01 – the difference well within the uncertainties involved in all these inversion datasets. The retrieved SSA above the clouds at UV–Vis-NIR wavelengths shows a distinct increasing trend from August to October, which is consistent with the ORACLES in situ measurements, AERONET inversions, and previous findings. The sensitivity analysis quantifying theoretical uncertainties in the retrieved SSA shows that errors in the measured ACAOD, aerosol layer height, and the ratio of the imaginary part of the refractive index (spectral dependence) of aerosols by 20 %, 1 km, and 10 %, respectively, produce an error in the retrieved SSA at 388 nm (470 nm) by 0.017 (0.015), 0.008 (0.002), and 0.03 (0.005). The development of the proposed aerosol–cloud algorithm implies a possible synergy of Cloud–Aerosol Lidar with Orthogonal Polarization (CALIOP) and OMI–MODIS passive sensors to deduce a global product of ACAOD and SSA. Furthermore, the presented synergy algorithm assumes implications for future missions, such as the Atmosphere Observing System (AOS) and the Earth Cloud Aerosol and Radiation Explorer (EarthCARE). The availability of the intended global dataset can help constrain climate models with the much-needed observational estimates of the radiative effects of aerosols in cloudy regions and expand our ability to study aerosol effects on clouds.

The southeastern Atlantic is home to an expansive smoke aerosol plume overlying a large cloud deck for approximately a third of the year. The aerosol plume is mainly attributed to the extensive biomass burning activities that occur in southern Africa. Current Earth system models (ESMs) reveal significant differences in their estimates of regional aerosol radiative effects over this region. Such large differences partially stem from uncertainties in the vertical distribution of aerosols in the troposphere. These uncertainties translate into different aerosol optical depths (AODs) in the planetary boundary layer (PBL) and the free troposphere (FT). This study examines differences of AOD fraction in the FT and AOD differences among ESMs (WRF-CAM5, WRF-FINN, GEOS-Chem, EAM-E3SM, ALADIN, GEOS-FP, and MERRA-2) and aircraft-based measurements from the NASA ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) field campaign. Models frequently define the PBL as the well-mixed surface-based layer, but this definition misses the upper parts of decoupled PBLs, in which most low-level clouds occur. To account for the presence of decoupled boundary layers in the models, the height of maximum vertical gradient of specific humidity profiles from each model is used to define PBL heights. Results indicate that the monthly mean contribution of AOD in the FT to the total-column AOD ranges from 44 % to 74 % in September 2016 and from 54 % to 71 % in August 2017 within the region bounded by 25∘ S–0∘ N–S and 15∘ W–15∘ E (excluding land) among the ESMs. ALADIN and GEOS-Chem show similar aerosol plume patterns to a derived above-cloud aerosol product from the Moderate Resolution Imaging Spectroradiometer (MODIS) during September 2016, but none of the models show a similar above-cloud plume pattern to MODIS in August 2017. Using the second-generation High Spectral Resolution Lidar (HSRL-2) to derive an aircraft-based constraint on the AOD and the fractional AOD, we found that WRF-CAM5 produces 40 % less AOD than those from the HSRL-2 measurements, but it performs well at separating AOD fraction between the FT and the PBL. AOD fractions in the FT for GEOS-Chem and EAM-E3SM are, respectively, 10 % and 15 % lower than the AOD fractions from the HSRL-2. Their similar mean AODs reflect a cancellation of high and low AOD biases. Compared with aircraft-based observations, GEOS-FP, MERRA-2, and ALADIN produce 24 %–36 % less AOD and tend to misplace more aerosols in the PBL. The models generally underestimate AODs for measured AODs that are above 0.8, indicating their limitations at reproducing high AODs. The differences in the absolute AOD, FT AOD, and the vertical apportioning of AOD in different models highlight the need to continue improving the accuracy of modeled AOD distributions. These differences affect the sign and magnitude of the net aerosol radiative forcing, especially when aerosols are in contact with clouds.

Biomass burning smoke is advected over the southeastern Atlantic Ocean between July and October of each year. This smoke plume overlies and mixes into a region of persistent low marine clouds. Model calculations of climate forcing by this plume vary significantly in both magnitude and sign. NASA EVS-2 (Earth Venture Suborbital-2) ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) had deployments for field campaigns off the west coast of Africa in 3 consecutive years (September 2016, August 2017, and October 2018) with the goal of better characterizing this plume as a function of the monthly evolution by measuring the parameters necessary to calculate the direct aerosol radiative effect. Here, this dataset and satellite retrievals of cloud properties are used to test the representation of the smoke plume and the underlying cloud layer in two regional models (WRF-CAM5 and CNRM-ALADIN) and two global models (GEOS and UM-UKCA). The focus is on the comparisons of those aerosol and cloud properties that are the primary determinants of the direct aerosol radiative effect and on the vertical distribution of the plume and its properties. The representativeness of the observations to monthly averages are tested for each field campaign, with the sampled mean aerosol light extinction generally found to be within 20 % of the monthly mean at plume altitudes. When compared to the observations, in all models, the simulated plume is too vertically diffuse and has smaller vertical gradients, and in two of the models (GEOS and UM-UKCA), the plume core is displaced lower than in the observations. Plume carbon monoxide, black carbon, and organic aerosol masses indicate underestimates in modeled plume concentrations, leading, in general, to underestimates in mid-visible aerosol extinction and optical depth. Biases in mid-visible single scatter albedo are both positive and negative across the models. Observed vertical gradients in single scatter albedo are not captured by the models, but the models do capture the coarse temporal evolution, correctly simulating higher values in October (2018) than in August (2017) and September (2016). Uncertainties in the measured absorption Ångstrom exponent were large but propagate into a negligible (<4 %) uncertainty in integrated solar absorption by the aerosol and, therefore, in the aerosol direct radiative effect. Model biases in cloud fraction, and, therefore, the scene albedo below the plume, vary significantly across the four models. The optical thickness of clouds is, on average, well simulated in the WRF-CAM5 and ALADIN models in the stratocumulus region and is underestimated in the GEOS model; UM-UKCA simulates cloud optical thickness that is significantly too high. Overall, the study demonstrates the utility of repeated, semi-random sampling across multiple years that can give insights into model biases and how these biases affect modeled climate forcing. The combined impact of these aerosol and cloud biases on the direct aerosol radiative effect (DARE) is estimated using a first-order approximation for a subset of five comparison grid boxes. A significant finding is that the observed grid box average aerosol and cloud properties yield a positive (warming) aerosol direct radiative effect for all five grid boxes, whereas DARE using the grid-box-averaged modeled properties ranges from much larger positive values to small, negative values. It is shown quantitatively how model biases can offset each other, so that model improvements that reduce biases in only one property (e.g., single scatter albedo but not cloud fraction) would lead to even greater biases in DARE. Across the models, biases in aerosol extinction and in cloud fraction and optical depth contribute the largest biases in DARE, with aerosol single scatter albedo also making a significant contribution.

Aerosol heating due to shortwave absorption has implications for local atmospheric stability and regional dynamics. The derivation of heating rate profiles from space-based observations is challenging because it requires the vertical profile of relevant properties such as the aerosol extinction coefficient and single-scattering albedo (SSA). In the southeastern Atlantic, this challenge is amplified by the presence of stratocumulus clouds below the biomass burning plume advected from Africa, since the cloud properties affect the magnitude of the aerosol heating aloft, which may in turn lead to changes in the cloud properties and life cycle. The combination of spaceborne lidar data with passive imagers shows promise for future derivations of heating rate profiles and curtains, but new algorithms require careful testing with data from aircraft experiments where measurements of radiation, aerosol, and cloud parameters are better colocated and readily available. In this study, we derive heating rate profiles and vertical cross sections (curtains) from aircraft measurements during the NASA ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) project in the southeastern Atlantic. Spectrally resolved irradiance measurements and the derived column absorption allow for the separation of total heating rates into aerosol and gas (primarily water vapor) absorption. The nine cases we analyzed capture some of the co-variability of heating rate profiles and their primary drivers, leading to the development of a new concept: the heating rate efficiency (HRE; the heating rate per unit aerosol extinction). HRE, which accounts for the overall aerosol loading as well as vertical distribution of the aerosol layer, varies little with altitude as opposed to the standard heating rate. The large case-to-case variability for ORACLES is significantly reduced after converting from heating rate to HRE, allowing us to quantify its dependence on SSA, cloud albedo, and solar zenith angle.

In this work we report the airborne aerosol optical depth (AOD) from measurements within freshly emitted anthropogenic plumes arising from mining and processing operations in the Athabasca Oil Sands Region (AOSR) in the context of ground-based AERONET climatological daily averaged AODs at Fort McMurray (Alberta, Canada). During two flights on 9 and 18 June 2018, the NASA airborne 4STAR (Spectrometers for Sky-Scanning, Sun-Tracking Atmospheric Research) Sun photometer registered high fine-mode (FM, µm) in-plume AODs of up to 0.4 and 0.9, respectively, in the vicinity of the plume source ( km). Particle composition shows that the plumes were associated with elevated concentrations of sulfates and ammonium. These high AODs significantly exceed climatological averages for June and were not captured by the nearby AERONET instrument (mean daily AODs of 0.10±0.01 and 0.07±0.02, maximum AOD of 0.12) due possibly to horizontal inhomogeneity of the plumes, plume dilution and winds which in certain cases were carrying the plume away from the ground-based instrument. The average 4STAR out-of-plume (background) AODs deviated only marginally from AERONET daily averaged values. While 4STAR AOD peaks were generally well correlated in time with peaks in the in situ-measured particle concentrations, we show that differences in particle size are the dominant factor in determining the 4STAR-derived AOD. During the two flights of 24 June and 5 July 2018 when plumes likely travelled distances of 60 km or more, the average 4STAR FM AOD increased by 0.01–0.02 over ∼50 km of downwind particle evolution, which was supported by the increases in layer AODs calculated from the in situ extinction measurements. Based on these observations as well as the increases in organic mass, we attribute the observed AOD increase, at least in part, to secondary organic aerosol formation. The in-plume and out-of-plume AODs for this second pair of flights, in contrast to clear differences in in situ optical and other measurements, were practically indistinguishable and compared favourably to AERONET within 0.01–0.02 AOD. This means that AERONET was generally successful in capturing the background AODs, but missed some of the spatially constrained high-AOD plumes with sources as close as 30–50 km, which is important to note since the AERONET measurements are generally thought to be representative of the regional AOD loading. The fact that industrial plumes can be associated with significantly higher AODs in the vicinity of the emission sources than previously reported from AERONET can potentially have an effect on estimating the AOSR radiative impact.

In southern Africa, widespread agricultural fires produce substantial biomass burning (BB) emissions over the region. The seasonal smoke plumes associated with these emissions are then advected westward over the persistent stratocumulus cloud deck in the southeast Atlantic (SEA) Ocean, resulting in aerosol effects which vary with time and location. Much work has focused on the effects of these aerosol plumes, but previous studies have also described an elevated free tropospheric water vapor signal over the SEA. Water vapor influences climate in its own right, and it is especially important to consider atmospheric water vapor when quantifying aerosol–cloud interactions and aerosol radiative effects. Here we present airborne observations made during the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) campaign over the SEA Ocean. In observations collected from multiple independent instruments on the NASA P-3 aircraft (from near-surface to 6–7 km), we observe a strongly linear correlation between pollution indicators (carbon monoxide (CO) and aerosol loading) and atmospheric water vapor content, seen at all altitudes above the boundary layer. The focus of the current study is on the especially strong correlation observed during the ORACLES-2016 deployment (out of Walvis Bay, Namibia), but a similar relationship is also observed in the August 2017 and October 2018 ORACLES deployments. Using reanalyses from the European Centre for Medium-Range Weather Forecasts (ECMWF) and Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2), and specialized WRF-Chem simulations, we trace the plume–vapor relationship to an initial humid, smoky continental source region, where it mixes with clean, dry upper tropospheric air and then is subjected to conditions of strong westward advection, namely the southern African easterly jet (AEJ-S). Our analysis indicates that air masses likely left the continent with the same relationship between water vapor and carbon monoxide as was observed by aircraft. This linear relationship developed over the continent due to daytime convection within a deep continental boundary layer (up to ∼5–6 km) and mixing with higher-altitude air, which resulted in fairly consistent vertical gradients in CO and water vapor, decreasing with altitude and varying in time, but this water vapor does not originate as a product of the BB combustion itself. Due to a combination of conditions and mixing between the smoky, moist continental boundary layer and the dry and fairly clean upper-troposphere air above (∼6 km), the smoky, humid air is transported by strong zonal winds and then advected over the SEA (to the ORACLES flight region) following largely isentropic trajectories. Hybrid Single-Particle Lagrangian Integrated Trajectory model (HYSPLIT) back trajectories support this interpretation. This work thus gives insights into the conditions and processes which cause water vapor to covary with plume strength. Better understanding of this relationship, including how it varies spatially and temporally, is important to accurately quantify direct, semi-direct, and indirect aerosol effects over this region.

Marine stratocumulus cloud properties over the Southeast Atlantic Ocean are impacted by contact between above-cloud biomass burning aerosols and cloud tops. Different vertical separations (0 to 2000 m) between the aerosol layer and cloud tops were observed on six research flights in September 2016 during the NASA ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) field campaign. There were 30 contact profiles, where an aerosol layer with aerosol concentration (Na) > 500 cm−3 was within 100 m of cloud tops, and 41 separated profiles, where the aerosol layer with Na > 500 cm−3 was located more than 100 m above cloud tops. For contact profiles, the average cloud droplet concentration (Nc) in the cloud layer was up to 68 cm−3 higher, the effective radius (Re) up to 1.3 µm lower, and the liquid water content (LWC) within 0.01 g m−3 compared to separated profiles. Free-tropospheric humidity was higher in the presence of biomass burning aerosols, and contact profiles had a smaller decrease in humidity (and positive buoyancy) across cloud tops with higher median above-cloud Na (895 cm−3) compared to separated profiles (30 cm−3). Due to droplet evaporation from entrainment mixing of warm, dry free-tropospheric air into the clouds, the median Nc and LWC for contact profiles decreased with height by 21 and 9 % in the top 20 % of the cloud layer. The impact of droplet evaporation was stronger during separated profiles as a greater decrease in humidity (and negative buoyancy) across cloud tops led to greater decreases in median Nc (30 %) and LWC (16 %) near cloud tops. Below-cloud Na was sampled during 61 profiles, and most contact profiles (20 out of 28) were within high-Na (> 350 cm−3) boundary layers, while most separated profiles (22 out of 33) were within low-Na (< 350 cm−3) boundary layers. Although the differences in below-cloud Na were statistically insignificant, contact profiles within low-Na boundary layers had up to 34.9 cm−3 higher Nc compared to separated profiles. This is consistent with a weaker impact of droplet evaporation in the presence of biomass burning aerosols within 100 m above cloud tops. For contact profiles within high-Na boundary layers, the presence of biomass burning aerosols led to higher below-cloud Na (up to 70.5 cm−3) and additional droplet nucleation above the cloud base along with weaker droplet evaporation. Consequently, the contact profiles in high-Na boundary layers had up to 88.4 cm−3 higher Nc compared to separated profiles. These results motivate investigations of aerosol–cloud–precipitation interactions over the Southeast Atlantic since the changes in Nc and Re induced by the presence of above-cloud biomass burning aerosols are likely to impact precipitation rates, liquid water path, and cloud fraction, and modulate closed-to-open-cell transitions.

Southern Africa produces almost a third of the Earth's biomass burning (BB) aerosol particles, yet the fate of these particles and their influence on regional and global climate is poorly understood. ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) is a 5-year NASA EVS-2 (Earth Venture Suborbital-2) investigation with three intensive observation periods designed to study key atmospheric processes that determine the climate impacts of these aerosols. During the Southern Hemisphere winter and spring (June–October), aerosol particles reaching 3–5 km in altitude are transported westward over the southeast Atlantic, where they interact with one of the largest subtropical stratocumulus (Sc) cloud decks in the world. The representation of these interactions in climate models remains highly uncertain in part due to a scarcity of observational constraints on aerosol and cloud properties, as well as due to the parameterized treatment of physical processes. Three ORACLES deployments by the NASA P-3 aircraft in September 2016, August 2017, and October 2018 (totaling ∼350 science flight hours), augmented by the deployment of the NASA ER-2 aircraft for remote sensing in September 2016 (totaling ∼100 science flight hours), were intended to help fill this observational gap. ORACLES focuses on three fundamental science themes centered on the climate effects of African BB aerosols: (a) direct aerosol radiative effects, (b) effects of aerosol absorption on atmospheric circulation and clouds, and (c) aerosol–cloud microphysical interactions. This paper summarizes the ORACLES science objectives, describes the project implementation, provides an overview of the flights and measurements in each deployment, and highlights the integrative modeling efforts from cloud to global scales to address science objectives. Significant new findings on the vertical structure of BB aerosol physical and chemical properties, chemical aging, cloud condensation nuclei, rain and precipitation statistics, and aerosol indirect effects are emphasized, but their detailed descriptions are the subject of separate publications. The main purpose of this paper is to familiarize the broader scientific community with the ORACLES project and the dataset it produced.

In this paper, we use observations from the NASA ORACLES (ObseRvations of CLouds above Aerosols and their intEractionS) aircraft campaign to develop a framework by way of two parameterizations that establishes regionally representative relationships between aerosol-cloud properties and their radiative effects. These relationships rely on new spectral aerosol property retrievals of the single scattering albedo (SSA) and asymmetry parameter (ASY). The retrievals capture the natural variability of the study region as sampled, and both were found to be fairly narrowly constrained (SSA: 0.83 ± 0.03 in the mid-visible, 532 nm; ASY: 0.54 ± 0.06 at 532 nm). The spectral retrievals are well suited for calculating the direct aerosol radiative effect (DARE) since SSA and ASY are tied directly to the irradiance measured in the presence of aerosols – one of the inputs to the spectral DARE. The framework allows for entire campaigns to be generalized into a set of parameterizations. For a range of solar zenith angles, it links the broadband DARE to the mid-visible aerosol optical depth (AOD) and the albedo (α) of the underlying scene (either clouds or clear sky) by way of the first parameterization: P(AOD, α). For ORACLES, the majority of the case-to-case variability of the broadband DARE is attributable to the dependence on the two driving parameters of P(AOD, α). A second, extended, parameterization PX(AOD, α, SSA) explains even more of the case-to-case variability by introducing the mid-visible SSA as a third parameter. These parameterizations establish a direct link from two or three mid-visible (narrowband) parameters to the broadband DARE, implicitly accounting for the underlying spectral dependencies of its drivers. They circumvent some of the assumptions when calculating DARE from satellite products or in a modeling context. For example, the DARE dependence on aerosol microphysical properties is not explicit in P or PX because the asymmetry parameter varies too little from case to case to translate into appreciable DARE variability. While these particular DARE parameterizations only represent the ORACLES data, they raise the prospect of generalizing the framework to other regions.

To help satellite retrieval of aerosols and studies of their radiative effects, we demonstrate that daytime aerosol optical depth over low-level clouds is similar to that in neighboring clear skies at the same heights. Based on recent airborne lidar and sun photometer observations above the southeast Atlantic, the mean aerosol optical depth (AOD) difference at 532 nm is between 0 and −0.01, when comparing the cloudy and clear sides, each up to 20 km wide, of cloud edges. The difference is not statistically significant according to a paired t test. Systematic differences in the wavelength dependence of AOD and in situ single scattering albedo are also minuscule. These results hold regardless of the vertical distance between cloud top and aerosol layer bottom. AOD aggregated over ∼2∘ grid boxes for each of September 2016, August 2017 and October 2018 also shows little correlation with the presence of low-level clouds. We posit that a satellite retrieval artifact is entirely responsible for a previous finding of generally smaller AOD over clouds (Chung et al., 2016), at least for the region and time of our study. Our results also suggest that the same values can be assumed for the intensive properties of free-tropospheric biomass-burning aerosol regardless of whether clouds are present below.

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.

The southeast Atlantic (SEA) region is host to a climatologically significant biomass burning aerosol layer overlying marine stratocumulus. We present the first results of the directly measured above-cloud aerosol optical depth (ACAOD) from the recent ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) airborne field campaign during August and September 2016. In our analysis, we use data from the Spectrometers for Sky-Scanning Sun-Tracking Atmospheric Research (4STAR) instrument and found an average ACAOD of 0.32 at 501 nm (range of 0.02 to 1.04), with an average Ångström exponent (AE) above clouds of 1.71. The AE is much lower at 1.25 for the full column (including below-cloud-level aerosol, with an average of 0.36 at 501 nm and a range of 0.02 to 0.74), indicating the presence of large aerosol particles, likely marine aerosol, in the lower atmospheric column. The ACAOD is observed from 4STAR to be highest near the coast at about 12∘ S, whereas its variability is largest at the southern edge of the average aerosol plume, as indicated by 12 years of MODIS observations. In comparison to MODIS-derived ACAOD and long-term fine-mode plume-average AOD along a diagonal routine track extending out from the coast of Namibia, the directly measured ACAOD from 4STAR is slightly lower than the ACAOD product from MODIS. The peak ACAOD expected from MODIS AOD retrievals averaged over a long term along the routine diagonal flight track (peak of 0.5) was measured to be closer to coast in 2016 at about 1.5–4∘ E, with 4STAR ACAOD averages showing a peak of 0.42. When considering the full observation set over the SEA, by spatially binning each sampled AOD, we obtain a geographically representative mean ACAOD of 0.37. Vertical profiles of AOD showcase the variability in the altitude of the aerosol plume and its separation from the cloud top. We measured larger AOD at a high altitude near the coast than farther from the coast, while generally observing a larger vertical gap farther from the coast. Changes in AOD with altitude are correlated with carbon monoxide, a gas tracer of the biomass burning aerosol plume. Vertical extent of gaps between aerosol and cloud show a wide distribution, with a near-zero gap being most frequent. The gap distribution with longitude is observed to be largest at about 7∘ E, farther from coast than expected from previous studies.

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.

This study presents and evaluates an updated algorithm for quantification of absorbing aerosols above clouds (AACs) from passive satellite measurements. The focus is biomass burning in the south-eastern Atlantic Ocean during the 2016 and 2017 ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) field campaign deployments. The algorithm retrieves the above-cloud aerosol optical depth (AOD) and underlying liquid cloud optical depth and is applied to measurements from the Sea-viewing Wide Field-of-view Sensor (SeaWiFS), Moderate Resolution Imaging Spectroradiometer (MODIS), and Visible Infrared Imaging Radiometer Suite (VIIRS) from 1997 to 2017. Airborne NASA Ames Spectrometers for Sky-Scanning, Sun-Tracking Atmospheric Research (4STAR) and NASA Langley High Spectral Resolution Lidar 2 (HSRL2) data collected during ORACLES provide important validation for spectral AOD for MODIS and VIIRS; as the SeaWiFS mission ended in 2010, it cannot be evaluated directly. The 4STAR and HSRL2 comparisons are complementary and reveal performance generally in line with uncertainty estimates provided by the optimal estimation retrieval framework used. At present the two MODIS-based data records seem the most reliable, although there are differences between the deployments, which may indicate that the available data are not yet sufficient to provide a robust regional validation. Spatiotemporal patterns in the data sets are similar, and the time series are very strongly correlated with each other (correlation coefficients from 0.95 to 0.99). Offsets between the satellite data sets are thought to be chiefly due to differences in absolute calibration between the sensors. The available validation data for this type of algorithm are limited to a small number of field campaigns, and it is strongly recommended that such airborne measurements continue to be made, both over the southern Atlantic Ocean and elsewhere.

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.

There are many contributing factors which determine the micro- and macrophysical properties of clouds, including atmospheric vertical structure, dominant meteorological conditions, and aerosol concentration, all of which may be coupled to one another. In the quest to determine aerosol effects on clouds, these potential relationships must be understood. Here we describe several observed correlations between aerosol conditions and cloud and atmospheric properties in the Indian Ocean winter monsoon season.In the CARDEX (Cloud, Aerosol, Radiative forcing, Dynamics EXperiment) field campaign conducted in February and March 2012 in the northern Indian Ocean, continuous measurements were made of atmospheric precipitable water vapor (PWV) and the liquid water path (LWP) of trade cumulus clouds, concurrent with measurements of water vapor flux, cloud and aerosol vertical profiles, meteorological data, and surface and total-column aerosol from instrumentation at a ground observatory and on small unmanned aircraft. We present observations which indicate a positive correlation between aerosol and cloud LWP only when considering cases with low atmospheric water vapor (PWV −2), a criterion which acts to filter the data to control for the natural meteorological variability in the region.We then use the aircraft and ground-based measurements to explore possible mechanisms behind this observed aerosol–LWP correlation. The increase in cloud liquid water is found to coincide with a lowering of the cloud base, which is itself attributable to increased boundary layer humidity in polluted conditions. High pollution is found to correlate with both higher temperatures and higher humidity measured throughout the boundary layer. A large-scale analysis, using satellite observations and meteorological reanalysis, corroborates these covariations: high-pollution cases are shown to originate as a highly polluted boundary layer air mass approaching the observatory from a northwesterly direction. The source air mass exhibits both higher temperatures and higher humidity in the polluted cases. While the warmer temperatures may be attributable to aerosol absorption of solar radiation over the subcontinent, the factors responsible for the coincident high humidity are less evident: the high-aerosol conditions are observed to disperse with air mass evolution, along with a weakening of the high-temperature anomaly, while the high-humidity condition is observed to strengthen in magnitude as the polluted air mass moves over the ocean toward the site of the CARDEX observations. Potential causal mechanisms of the observed correlations, including meteorological or aerosol-induced factors, are explored, though future research will be needed for a more complete and quantitative understanding of the aerosol–humidity relationship.

The introduction of cloud condensation nuclei and radiative heating by sunlight-absorbing aerosols can modify the thickness and coverage of low clouds, yielding significant radiative forcing of climate. The magnitude and sign of changes in cloud coverage and depth in response to changing aerosols are impacted by turbulent dynamics of the cloudy atmosphere, but integrated measurements of aerosol solar absorption and turbulent fluxes have not been reported thus far. Here we report such integrated measurements made from unmanned aerial vehicles (UAVs) during the CARDEX (Cloud Aerosol Radiative Forcing and Dynamics Experiment) investigation conducted over the northern Indian Ocean. The UAV and surface data reveal a reduction in turbulent kinetic energy in the surface mixed layer at the base of the atmosphere concurrent with an increase in absorbing black carbon aerosols. Polluted conditions coincide with a warmer and shallower surface mixed layer because of aerosol radiative heating and reduced turbulence. The polluted surface mixed layer was also observed to be more humid with higher relative humidity. Greater humidity enhances cloud development, as evidenced by polluted clouds that penetrate higher above the top of the surface mixed layer. Reduced entrainment of dry air into the surface layer from above the inversion capping the surface mixed layer, due to weaker turbulence, may contribute to higher relative humidity in the surface layer during polluted conditions. Measurements of turbulence are important for studies of aerosol effects on clouds. Moreover, reduced turbulence can exacerbate both the human health impacts of high concentrations of fine particles and conditions favorable for low-visibility fog events., Competing Interests: The authors declare no conflict of interest.

The decline of Arctic sea ice has been documented in over 30 y of satellite passive microwave observations. The resulting darkening of the Arctic and its amplification of global warming was hypothesized almost 50 y ago but has yet to be verified with direct observations. This study uses satellite radiation budget measurements along with satellite microwave sea ice data to document the Arctic-wide decrease in planetary albedo and its amplifying effect on the warming. The analysis reveals a striking relationship between planetary albedo and sea ice cover, quantities inferred from two independent satellite instruments. We find that the Arctic planetary albedo has decreased from 0.52 to 0.48 between 1979 and 2011, corresponding to an additional 6.4 ± 0.9 W/m(2) of solar energy input into the Arctic Ocean region since 1979. Averaged over the globe, this albedo decrease corresponds to a forcing that is 25% as large as that due to the change in CO2 during this period, considerably larger than expectations from models and other less direct recent estimates. Changes in cloudiness appear to play a negligible role in observed Arctic darkening, thus reducing the possibility of Arctic cloud albedo feedbacks mitigating future Arctic warming.