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With its height-resolved measurements and near global coverage, the CALIOP lidar onboard the CALIPSO satellite offers a new capability for aerosol retrievals in cloudy skies. Validation of these retrievals is difficult, however, as independent, collocated and co-temporal data sets are generally not available. In this paper, we evaluate CALIOP aerosol products above opaque water clouds by applying multiple retrieval techniques to CALIOP Level 1 profile data and comparing the results. This approach allows us to both characterize the accuracy of the CALIOP above-cloud aerosol optical depth (AOD) and develop an error budget that quantifies the relative contributions of different error sources. We focus on two spatial domains: the African dust transport pathway over the tropical North Atlantic and the African smoke transport pathway over the southeastern Atlantic. Six years of CALIOP observations (2007-2012) from the northern hemisphere summer and early fall are analyzed. The analysis is limited to cases where aerosol layers are located above opaque water clouds so that a constrained retrieval technique can be used to directly retrieve 532 nm aerosol optical depth and lidar ratio. For the moderately dense Sahara dust layers detected in the CALIOP data used in this study, the mean/median values of the lidar ratios derived from a constrained opaque water cloud (OWC) technique are 45.1/44.4 +/- 8.8 sr, which are somewhat larger than the value of 40 +/- 20 sr used in the CALIOP Level 2 (L2) data products. Comparisons of CALIOP L2 AOD with the OWC-retrieved AOD reveal that for nighttime conditions the L2 AOD in the dust region is underestimated on average by approx. 26% (0.183 vs. 0.247). Examination of the error sources indicates that errors in the L2 dust AOD are primarily due to using a lidar ratio that is somewhat too small. The mean/median lidar ratio retrieved for smoke is 70.8/70.4 +/- 16.2 sr, which is consistent with the modeled value of 70 +/- 28 sr used in the CALIOP L2 retrieval. Smoke AOD is found to be underestimated, on average, by approx. 39% (0.191 vs. 0.311). The primary cause of AOD differences in the smoke transport region is the tendency of the CALIOP layer detection scheme to prematurely assign layer base altitudes and thus underestimate the geometric thickness of smoke layers.

Aerosol variations and trends over different land and ocean regions during 1980-2009 are analyzed with the Goddard Chemistry Aerosol Radiation and Transport (GOCART) model and observations from multiple satellite sensors and ground-based networks. Excluding time periods with large volcanic influences, the tendency of aerosol optical depth (AOD) and surface concentration over polluted land regions is consistent with the anthropogenic emission changes.The largest reduction occurs over Europe, and regions in North America and Russia also exhibit reductions. On the other hand, East Asia and South Asia show AOD increases, although relatively large amount of natural aerosols in Asia makes the total changes less directly connected to the pollutant emission trends. Over major dust source regions, model analysis indicates that the dust emissions over the Sahara and Sahel respond mainly to the near-surface wind speed, but over Central Asia they are largely influenced by ground wetness. The decreasing dust trend in the tropical North Atlantic is most closely associated with the decrease of Sahel dust emission and increase of precipitation over the tropical North Atlantic, likely driven by the sea surface temperature increase. Despite significant regional trends, the model-calculated global annual average AOD shows little changes over land and ocean in the past three decades, because opposite trends in different regions cancel each other in the global average. This highlights the need for regional-scale aerosol assessment, as the global average value conceals regional changes, and thus is not sufficient for assessing changes in aerosol loading.

Black carbon, light-absorbing organic carbon (often called brown carbon) and mineral dust are the major light-absorbing aerosols. Currently the sources and formation of brown carbon aerosol in particular are not well understood. In this study we estimated globally the amount of light absorbing organic carbon and black carbon from AERONET measurements. We find that the columnar absorbing organic carbon (brown carbon) levels in biomass burning regions of South-America and Africa are relatively high (about 15-20 magnesium per square meters during biomass burning season), while the concentrations are significantly lower in urban areas in US and Europe. However, we estimated significant absorbing organic carbon amounts from the data of megacities of newly industrialized countries, particularly in India and China, showing also clear seasonality with peak values up to 30-35 magnesium per square meters during the coldest season, likely caused by the coal and biofuel burning used for heating. We also compared our retrievals with the modeled organic carbon by global Oslo CTM for several sites. Model values are higher in biomass burning regions than AERONET-based retrievals, while opposite is true in urban areas in India and China.