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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.

The southeast 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 activity that occurs 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 (AOD) 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° and 15°W–15°E (excluding land) among the ESMs. 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 and their similarities in the mean AODs are the result of cancellation of high and low AOD biases. GEOS-FP, MERRA-2, and ALADIN produce 24 %–36 % less AOD and tend to misplace more aerosols in the PBL compared to aircraft-based observations. 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.

Author(s): Pistone, K; Eisenman, I; Ramanathan, V | Abstract: During recent decades, there has been dramatic Arctic sea ice retreat. This has reduced the top-of-atmosphere albedo, adding more solar energy to the climate system. There is substantial uncertainty regarding how much ice retreat and associated solar heating will occur in the future. This is relevant to future climate projections, including the timescale for reaching global warming stabilization targets. Here we use satellite observations to estimate the amount of solar energy that would be added in the worst-case scenario of a complete disappearance of Arctic sea ice throughout the sunlit part of the year. Assuming constant cloudiness, we calculate a global radiative heating of 0.71nW/m2 relative to the 1979 baseline state. This is equivalent to the effect of one trillion tons of CO2 emissions. These results suggest that the additional heating due to complete Arctic sea ice loss would hasten global warming by an estimated 25nyears.

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 southeast 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 collocated and readily available. In this study, we derive heating rate profiles and curtains from aircraft measurements during the NASA ObseRvations of CLouds above Aerosols 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). The 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.

Biomass burning smoke is advected over the southeast 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. The NASA EVS-2 (Earth Venture Suborbital-2) ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) project deployed for field campaigns off the west coast of Africa in three consecutive years (Sept., 2016; Aug., 2017; and Oct., 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 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, 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 under-estimates in modeled plume concentrations, leading in general to under-estimates 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 (2018) and September (2017). Uncertainties in the measured absorption Ångstrom exponent were large but propagate into a negligible (

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 ECMWF and MERRA-2 reanalyses and specialized WRF-Chem simulations, we trace the plume-vapor relationship to an initial humid, smoky continental source region, where it is subjected to conditions of strong westward advection, namely the South African Easterly Jet (AEJ-S). Our analysis indicates that airmasses 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) which produced fairly consistent vertical gradients in CO and water vapor, decreasing with altitude and varying in time, but 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. HYSPLIT back trajectories support this interpretation. Better understanding of the conditions and processes which cause the water vapor to covary with plume strength is important to accurately quantify direct, semi-direct, and indirect aerosol effects in this region.

This work establishes an observationally-driven link from mid-visible aerosol optical depth (AOD) and other scene parameters to broadband shortwave irradiance (and by extension, the direct aerosol radiative effect, DARE), based on observations from the 2016 and 2017 field campaigns of ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS). Specifically, this is done by two parameterizations, one spanned by the mid-visible AOD and scene albedo below the aerosol layer, and another one with a third input, the mid-visible aerosol single scattering albedo (SSA). These parameterizations build on the earlier concept of radiative forcing efficiency, which describes the dependence of DARE on the AOD, and extend it to make the dependence on the other two scene parameters explicit. The parameterizations are founded on 9 cases from the campaigns, for which we retrieve the spectral aerosol properties of SSA and asymmetry parameter (g) directly from the radiative fluxes, based on the method presented in Cochrane et al. (2019). These properties are used as the basis of the parameterizations, capturing the natural variability of the study region as sampled. The majority of the case-to-case variability within the ORACLES DARE dataset is attributable to the dependence on AOD and scene albedo. This is captured by the first parameterization, which is advantageous when satellite retrievals provide only limited information such as AOD and scene albedo. However, the second parameterization explains even more of the case-to-case variability by introducing the mid-visible SSA as third parameter. For both parameterizations, we provide the necessary coefficients, uncertainties, and code required for the user to reconstruct the parameterization for their use.

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 southeast 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 0.80–0.85, 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 (the critical albedo) occurs just above 0.2 in the mid-visible. 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.

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

Aerosol overlying clouds increase uncertainty of standard remotely sensed properties. We present results of a hyperspectral-based retrieval technique to obtain cloud properties, and its calculated radiative effect, from cloud-transmitted light.

To realize the potential of spectrometers for airborne sunphotometry, a hybrid instrument incorporating radiometers and miniature spectrometers is being built. This brings with it several challenges in amplifier design, thermal management and stray-light control.

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.

In a recent paper (1), we assessed the magnitude of the increase in net solar radiation in the Arctic region during recent decades as a result of the change in albedo associated with sea ice retreat. Legates et al. (2) have commented on this. We appreciate their interest in our work.