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CMIP6 climate models have difficulties representing the strong absorption properties of biomass‐burning aerosols (BBA) over the Southeast Atlantic and the associated direct forcing. This study takes advantage of unique in situ and remote sensing observations to evaluate the vertical profile and chemical composition of BBA, which are key properties for modeling radiative interactions. Over land, CMIP6 models show a sharper vertical decrease in carbonaceous aerosol concentration than observed, indicating insufficient vertical mixing. Over the ocean, most models transport BBA lower, between 1 and 1.5 km, than observed. This could be due to both excessive subsidence and lack of self‐lofting of BBA. In addition, the ratio between black carbon and organic aerosol mass concentrations is underestimated by about 0.1 compared to observations. These biases limit the ability of models to capture the absorption above clouds in this region, which could have implications for the regional radiative and climatic impact of African BBA.

We examine the relationship between the number concentration of boundary-layer cloud condensation nuclei (CCN) and light extinction to investigate underlying aerosol processes and satellite-based CCN estimates. For a variety of airborne and ground-based observations not dominated by dust, regression identifies the CCN (cm−3) at 0.4 ± 0.1% supersaturation with 100.3α +1.3σ0.75 where σ (Mm−1) is the 500 nm extinction coefficient by dried particles and α is the Angstrom exponent. The deviation of 1 km horizontal average data from this approximation is typically within a factor of 2.0. ∂logCCN / ∂logσ is less than unity because, among other explanations, growth processes generally make aerosols scatter more light without increasing their number. This, barring special meteorology–aerosol connections, associates a doubling of aerosol optical depth with less than a doubling of CCN, contrary to previous studies based on heavily averaged measurements or a satellite algorithm.

We present statistics on the horizontal variability of aerosol optical depth (AOD) directly measured from the NASA P-3 aircraft. Our measurements during two contrasting phases (in Alaska and Canada) of the ARCTAS mission arguably constrain the variability in most aerosol environments common over the globe. In the Canada phase, which features local emissions, 499 nm AOD has a median relative standard deviation (stdrel, med) of 19 % and 9 % and an autocorrelation (r) of 0.37 and 0.71 over 20 km and 6 km horizontal segments, respectively. In the Alaska phase, which features long-range transport, the variability is considerably lower (stdrel, med = 3 %, r = 0.92 even over 35.2 km). Compared to the magnitude of AOD, its wavelength dependence varies less in the Canada phase, more in the Alaska phase. We translate these findings from straight-line flight tracks into grid boxes and points, to help interpretation and design of satellite remote sensing, suborbital observations and transport modeling.

We assess the consistency between instantaneously collocated level-2 aerosol optical depth (AOD) retrievals from MODIS-Aqua (C5) and CALIOP (Version 2 & 3), comparing the standard MODIS AOD (MYD04_L2) data to the AOD calculated from CALIOP aerosol extinction profiles for both the previous release (V2) and the latest release (V3) of CALIOP data. Based on data collected in January 2007, we investigate the most useful criteria for screening the MODIS and CALIOP retrievals to achieve the best agreement between the two data sets. Applying these criteria to eight months of data (Jan, Apr, Jul, Oct 2007 and 2009), we find an order of magnitude increase for the CALIOP V3 data density (by comparison to V2), that is generally accompanied by equal or better agreement with MODIS AOD. Differences in global, monthly mean, over-ocean AOD (532 nm) between CALIOP and MODIS range between 0.03 and 0.04 for CALIOP V3, with CALIOP generally biased low, when all available data from both sensors are considered. Root-mean-squares (RMS) differences in instantaneously collocated AOD retrievals by the two instruments are reduced from values ranging between 0.14 and 0.19 using the unscreened V3 data to values ranging from 0.09 to 0.1 for the screened data. A restriction to scenes with cloud fractions less than 1% (as defined in the MODIS aerosol retrievals) generally results in improved correlation (R2>0.5), except for the month of July when correlations remain relatively lower. Regional assessments show hot spots in disagreement between the two sensors in Asian outflow during April and off the coast of South Africa in July.

Estimation of Direct Climate Forcing (DCF) due to aerosols in cloudy areas has historically been a difficult task, mainly because of a lack of appropriate measurements. Recently, passive remote sensing instruments have been developed that have the potential to retrieve both cloud and aerosol properties using polarimetric, multiple view angle, and multi spectral observations, and therefore determine DCF from aerosols above clouds. One such instrument is the Research Scanning Polarimeter (RSP), an airborne prototype of a sensor on the NASA Glory satellite, which unfortunately failed to reach orbit during its launch in March of 2011. In the spring of 2006, the RSP was deployed on an aircraft based in Veracruz, Mexico, as part of the Megacity Initiative: Local and Global Research Observations (MILAGRO) field campaign. On 13 March, the RSP over flew an aerosol layer lofted above a low altitude marine stratocumulus cloud close to shore in the Gulf of Mexico. We investigate the feasibility of retrieving aerosol properties over clouds using these data. Our approach is to first determine cloud droplet size distribution using the angular location of the cloud bow and other features in the polarized reflectance. The selected cloud was then used in a multiple scattering radiative transfer model optimization to determine the aerosol optical properties and fine tune the cloud size distribution. In this scene, we were able to retrieve aerosol optical depth, the fine mode aerosol size distribution parameters and the cloud droplet size distribution parameters to a degree of accuracy required for climate modeling. This required assumptions about the aerosol vertical distribution and the optical properties of the coarse aerosol size mode. A sensitivity study was also performed to place this study in the context of future systematic scanning polarimeter observations, which found that the aerosol complex refractive index can also be observed accurately if the aerosol optical depth is larger than roughly 0.8 at a wavelength of (0.555 μm).

The Cloud Aerosol LIdar with Orthogonal Polarization (CALIOP), on board the CALIPSO platform, has measured profiles of total attenuated backscatter coefficient (level 1 products) since June 2006. CALIOP's level 2 products, such as the aerosol backscatter and extinction coefficient profiles, are retrieved using a complex succession of automated algorithms. The goal of this study is to help identify potential shortcomings in the CALIOP version 2 level 2 aerosol extinction product and to illustrate some of the motivation for the changes that have been introduced in the next version of CALIOP data (version 3, released in June 2010). To help illustrate the potential factors contributing to the uncertainty of the CALIOP aerosol extinction retrieval, we focus on a one-day, multi-instrument, multiplatform comparison study during the CALIPSO and Twilight Zone (CATZ) validation campaign on 4 August 2007. On that day, we observe a consistency in the Aerosol Optical Depth (AOD) values recorded by four different instruments (i.e. space-borne MODerate Imaging Spectroradiometer, MODIS: 0.67 and POLarization and Directionality of Earth's Reflectances, POLDER: 0.58, airborne High Spectral Resolution Lidar, HSRL: 0.52 and ground-based AErosol RObotic NETwork, AERONET: 0.48 to 0.73) while CALIOP AOD is a factor of two lower (0.32 at 532 nm). This case study illustrates the following potential sources of uncertainty in the CALIOP AOD: (i) CALIOP's low signal-to-noise ratio (SNR) leading to the misclassification and/or lack of aerosol layer identification, especially close to the Earth's surface; (ii) the cloud contamination of CALIOP version 2 aerosol backscatter and extinction profiles; (iii) potentially erroneous assumptions of the aerosol extinction-to-backscatter ratio (Sa) used in CALIOP's extinction retrievals; and (iv) calibration coefficient biases in the CALIOP daytime attenuated backscatter coefficient profiles. The use of version 3 CALIOP extinction retrieval for our case study seems to partially fix factor (i) although the aerosol retrieved by CALIOP is still somewhat lower than the profile measured by HSRL; the cloud contamination (ii) appears to be corrected; no particular change is apparent in the observation-based CALIOP Sa value (iii). Our case study also showed very little difference in version 2 and version 3 CALIOP attenuated backscatter coefficient profiles, illustrating a minor change in the calibration scheme (iv).

Airborne sunphotometer measurements acquired by the NASA Ames Airborne Tracking Sunphotometer (AATS-14) aboard the NASA P-3 research aircraft are used to evaluate dark-target over-land retrievals of extinction aerosol optical depth (AOD) from spatially and temporally near-coincident measurements by the Moderate Resolution Imaging Spectroradiometer (MODIS) during the summer 2008 Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) field campaign. The new MODIS Collection 6 aerosol data set includes retrievals of AOD at both 10 km × 10 km and 3 km × 3 km (at nadir) resolution. In this paper we compare MODIS and AATS AOD at 553 nm in 58 10 km and 134 3 km retrieval grid cells. These AOD values were derived from data collected over Canada on four days during short time segments of five (four Aqua and one Terra) satellite overpasses of the P-3 during low-altitude P-3 flight tracks. Three of the five MODIS–AATS coincidence events were dominated by smoke: one included a P-3 transect of a well-defined smoke plume in clear sky, but two were confounded by the presence of scattered clouds above smoke. The clouds limited the number of MODIS retrievals available for comparison, and led to MODIS AOD retrievals that underestimated the corresponding AATS values. This happened because the MODIS aerosol cloud mask selectively removed 0.5 km pixels containing smoke and clouds before the aerosol retrieval. The other two coincidences (one Terra and one Aqua) occurred during one P-3 flight on the same day and in the same general area, in an atmosphere characterized by a relatively low AOD (< 0.3), spatially homogeneous regional haze from smoke outflow with no distinguishable plume. For the ensemble data set for MODIS AOD retrievals with the highest-quality flag, MODIS AOD agrees with AATS AOD within the expected MODIS over-land AOD uncertainty in 60% of the retrieval grid cells at 10 km resolution and 69% at 3 km resolution. These values improve to 65 % and 74%, respectively, when the cloud-affected case with the strongest plume is excluded. We find that the standard MODIS dark-target over-land retrieval algorithm fails to retrieve AOD for thick smoke, not only in cloud-contaminated regions but also in clear sky. We attribute this to deselection, by the cloud and/or bright surface masks, of 0.5 km resolution pixels that contain smoke.

The Chesapeake Lighthouse Aircraft Measurements for Satellites (CLAMS) experiment took place from 10 July to 2 August 2001 in a combined ocean–land region that included the Chesapeake Lighthouse [Clouds and the Earth’s Radiant Energy System (CERES) Ocean Validation Experiment (COVE)] and the Wallops Flight Facility (WFF), both along coastal Virginia. This experiment was designed mainly for validating instruments and algorithms aboard the Terra satellite platform, including the Moderate Resolution Imaging Spectroradiometer (MODIS). Over the ocean, MODIS retrieved aerosol optical depths (AODs) at seven wavelengths and an estimate of the aerosol size distribution. Over the land, MODIS retrieved AOD at three wavelengths plus qualitative estimates of the aerosol size. Temporally coincident measurements of aerosol properties were made with a variety of sun photometers from ground sites and airborne sites just above the surface. The set of sun photometers provided unprecedented spectral coverage from visible (VIS) to the solar near-infrared (NIR) and infrared (IR) wavelengths. In this study, AOD and aerosol size retrieved from MODIS is compared with similar measurements from the sun photometers. Over the nearby ocean, the MODIS AOD in the VIS and NIR correlated well with sun-photometer measurements, nearly fitting a one-to-one line on a scatterplot. As one moves from ocean to land, there is a pronounced discontinuity of the MODIS AOD, where MODIS compares poorly to the sun-photometer measurements. Especially in the blue wavelength, MODIS AOD is too high in clean aerosol conditions and too low under larger aerosol loadings. Using the Second Simulation of the Satellite Signal in the Solar Spectrum (6S) radiative code to perform atmospheric correction, the authors find inconsistency in the surface albedo assumptions used by the MODIS lookup tables. It is demonstrated how the high bias at low aerosol loadings can be corrected. By using updated urban/industrial aerosol climatology for the MODIS lookup table over land, it is shown that the low bias for larger aerosol loadings can also be corrected. Understanding and improving MODIS retrievals over the East Coast may point to strategies for correction in other locations, thus improving the global quality of MODIS. Improvements in regional aerosol detection could also lead to the use of MODIS for monitoring air pollution.

Absorbing aerosols play an important, but uncertain, role in the global climate. Much of this uncertainty is due to a lack of adequate aerosol measurements. While great strides have been made in observational capability in the previous years and decades, it has become increasingly apparent that this development must continue. Scanning polarimeters have been designed to help resolve this issue by making accurate, multi-spectral, multi-angle polarized observations. This work involves the use of the Research Scanning Polarimeter (RSP). The RSP was designed as the airborne prototype for the Aerosol Polarimetery Sensor (APS), which was due to be launched as part of the (ultimately failed) NASA Glory mission. Field observations with the RSP, however, have established that simultaneous retrievals of aerosol absorption and vertical distribution over bright land surfaces are quite uncertain. We test a merger of RSP and High Spectral Resolution Lidar (HSRL) data with observations of boreal forest fire smoke, collected during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS). During ARCTAS, the RSP and HSRL instruments were mounted on the same aircraft, and validation data were provided by instruments on an aircraft flying a coordinated flight pattern. We found that the lidar data did indeed improve aerosol retrievals using an optimal estimation method, although not primarily because of the contraints imposed on the aerosol vertical distribution. The more useful piece of information from the HSRL was the total column aerosol optical depth, which was used to select the initial value (optimization starting point) of the aerosol number concentration. When ground based sun photometer network climatologies of number concentration were used as an initial value, we found that roughly half of the retrievals had unrealistic sizes and imaginary indices, even though the retrieved spectral optical depths agreed within uncertainties to independent observations. The convergence to an unrealistic local minimum by the optimal estimator is related to the relatively low sensitivity to particles smaller than 0.1 (μm) at large optical thicknesses. Thus, optimization algorithms used for operational aerosol retrievals of the fine mode size distribution, when the total optical depth is large, will require initial values generated from table look-ups that exclude unrealistic size/complex index mixtures. External constraints from lidar on initial values used in the optimal estimation methods will also be valuable in reducing the likelihood of obtaining spurious retrievals.

Haywood et al. (2004) show that an aerosol layer above a cloud can cause a bias in the retrieved cloud optical thickness and effective radius. Monitoring for this potential bias is difficult because space‐based passive remote sensing cannot unambiguously detect or characterize aerosol above cloud. We show that cloud retrievals from aircraft measurements above cloud and below an overlying aerosol layer are a means to test this bias. The data were collected during the Intercontinental Chemical Transport Experiment (INTEX‐A) study based out of Portsmouth, New Hampshire, United States, above extensive, marine stratus cloud banks affected by industrial outflow. Solar Spectral Flux Radiometer (SSFR) irradiance measurements taken along a lower level flight leg above cloud and below aerosol were unaffected by the overlying aerosol. Along upper level flight legs, the irradiance reflected from cloud top was transmitted through an aerosol layer. We compare SSFR cloud retrievals from below‐aerosol legs to satellite retrievals from the Moderate Resolution Imaging Spectroradiometer (MODIS) in order to detect an aerosol‐induced bias. In regions of small variation in cloud properties, we find that SSFR and MODIS‐retrieved cloud optical thickness compares within the uncertainty range for each instrument while SSFR effective radius tend to be smaller than MODIS values (by 1–2 μm) and at the low end of MODIS uncertainty estimates. In regions of large variation in cloud properties, differences in SSFR and MODIS‐retrieved cloud optical thickness and effective radius can reach values of 10 and 10 μm, respectively. We include aerosols in forward modeling to test the sensitivity of SSFR cloud retrievals to overlying aerosol layers. We find an overlying absorbing aerosol layer biases SSFR cloud retrievals to smaller effective radii and optical thickness while nonabsorbing aerosols had no impact.