ALBERT

Description: We present a comparison of tropospheric NO2 from OMI measurements to the median of an ensemble of Regional Air Quality (RAQ) models, and an intercomparison of the contributing RAQ models and two global models for the period July 2008–June 2009 over Europe. The model forecasts were produced routinely on a daily basis in the context of the European GEMS ("Global and regional Earth-system (atmosphere) Monitoring using Satellite and in-situ data") project. The tropospheric vertical column of the RAQ ensemble median shows a spatial distribution which agrees well with the OMI NO2 observations, with a correlation r=0.8. This is higher than the correlations from any one of the individual RAQ models, which supports the use of a model ensemble approach for regional air pollution forecasting. The global models show high correlations compared to OMI, but with significantly less spatial detail, due to their coarser resolution. Deviations in the tropospheric NO2 columns of individual RAQ models from the mean were in the range of 20–34% in winter and 40–62% in summer, suggesting that the RAQ ensemble prediction is relatively more uncertain in the summer months. The ensemble median shows a stronger seasonal cycle of NO2 columns than OMI, and the ensemble is on average 50% below the OMI observations in summer, whereas in winter the bias is small. On the other hand the ensemble median shows a somewhat weaker seasonal cycle than NO2 surface observations from the Dutch Air Quality Network, and on average a negative bias of 14%. Full profile information was available for two RAQ models and for the global models. For these models the retrieval averaging kernel was applied. Minor differences are found for area-averaged model columns with and without applying the kernel, which shows that the impact of replacing the a priori profiles by the RAQ model profiles is on average small. However, the contrast between major hotspots and rural areas is stronger for the direct modeled vertical columns than the columns where the averaging kernels are applied, related to a larger relative contribution of the free troposphere and the coarse horizontal resolution in the a priori profiles compared to the RAQ models. In line with validation results reported in the literature, summertime concentrations in the lowermost boundary layer in the a priori profiles from the DOMINO product are significantly larger than the RAQ model concentrations and surface observations over the Netherlands. This affects the profile shape, and contributes to a high bias in OMI tropospheric columns over polluted regions. The global models indicate that the upper troposphere may contribute significantly to the total column and it is important to account for this in comparisons with RAQ models. A combination of upper troposphere model biases, the a priori profile effects and DOMINO product retrieval issues could explain the discrepancy observed between the OMI observations and the ensemble median in summer.

Description: We introduce a method for deriving aerosol spectral radiative forcing along with single scattering albedo, asymmetry parameter, and surface albedo from airborne vertical profile measurements of shortwave spectral irradiance and spectral aerosol optical thickness. The new method complements the traditional, direct measurement of aerosol radiative forcing efficiency from horizontal flight legs below gradients of aerosol optical thickness, and is particularly useful over heterogeneous land surfaces and for homogeneous aerosol layers where the horizontal gradient method is impractical. Using data collected by the Solar Spectral Flux Radiometer (SSFR) and the Ames Airborne Tracking Sunphotometer (AATS-14) during the MILAGRO (Megacity Initiative: Local and Global Research Observations) experiment, we validate an over-ocean spectral aerosol forcing efficiency from the new method by comparing with the traditional method. Retrieved over-land aerosol optical properties are compared with in-situ measurements and AERONET retrievals. The spectral forcing efficiencies over ocean and land are remarkably similar and agree with results from other field experiments.

Description: We have quantified the relationship between Aerosol Index (AI) measurements and plume height for young biomass burning plumes using coincident Ozone Monitoring Instrument (OMI) and Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) measurements. This linear relationship allows the determination of high-altitude plumes wherever AI data are available, and it provides a data set for validating global fire plume heights in chemistry transport models. We find that all plumes detected from June 2006 to February 2009 with an AI value ≥9 are located at altitudes higher than 5 km. Older high-altitude plumes have lower AI values than young plumes at similar altitudes. We have examined available AI data from the OMI and TOMS instruments (1978–2009) and find that large AI plumes occur more frequently over North America than over Australia or Russia/Northeast Asia. According to the derived relationship, during this time interval, 181 plumes, in various stages of their evolution, reached altitudes above 8 km.

Description: This paper presents estimates of the spectral solar absorption due to atmospheric aerosols during the 2006 MILAGRO/INTEX-B (Megacity Initiative-Local And Global Research Observations/Phase B of the Intercontinental Chemical Transport Experiment) field campaign. The aerosol absorption was derived from measurements of the spectral solar radiation and the spectral aerosol optical depth made on the J31 aircraft flying over the Gulf of Mexico and over Mexico City. We present the spectral single scattering albedo (SSA) and aerosol absorption optical depth (AAOD) for two flights over the Gulf of Mexico and three flights over Mexico City for wavelengths from 350 to approximately 1650 nm. The spectral aerosol optical properties of each case are different and illustrate the variability of the aerosol optical properties in the Mexico City area. The results can be described in terms of three different wavelength regions: The 350–500 nm region where the aerosol absorption often falls off sharply presumably due to organic carbonaceous particles and windblown dust; the 500–1000 nm region where the decrease with wavelength is slower presumably due to black carbon; and the near infrared spectral region (1000 nm to 1650 nm) where it is difficult to obtain reliable results since the aerosol absorption is relatively small and the gas absorption dominates. However, there is an indication of a small and somewhat wavelength independent absorption in the region beyond 1000 nm. For one of the flights over the Gulf of Mexico near the coastline it appears that a cloud/fog formation and evaporation led to an increase of absorption possibly due to a water shell remaining on the particles after the cloud/fog had dissipated. For two of the Mexico City cases, the single scattering albedo is roughly constant between 350–500 nm consistent with other Mexico City results. In three of the cases a single absorption Angstrom exponent (AAE) fits the aerosol absorption optical depth over the entire wavelength range of 350 to 1650 nm relatively well (r2〉 0.86).

Description: Recent results from diverse air, ground, and laboratory studies using both radiometric and in situ techniques show that the fractions of black carbon, organic matter, and mineral dust in atmospheric aerosols determine the wavelength dependence of absorption (often expressed as Absorption Angstrom Exponent, or AAE). Taken together, these results hold promise of improving information on aerosol composition from remote measurements. The main purpose of this paper is to show that AAE values for an Aerosol Robotic Network (AERONET) set of retrievals from Sun-sky measurements describing full aerosol vertical columns are also strongly correlated with aerosol composition or type. In particular, we find AAE values near 1 (the theoretical value for black carbon) for AERONET-measured aerosol columns dominated by urban-industrial aerosol, larger AAE values for biomass burning aerosols, and the largest AAE values for Sahara dust aerosols. These AERONET results are consistent with results from other, very different, techniques, including solar flux-aerosol optical depth (AOD) analyses and airborne in situ analyses examined in this paper, as well as many other previous results. Ambiguities in aerosol composition or mixtures thereof, resulting from intermediate AAE values, can be reduced via cluster analyses that supplement AAE with other variables, for example Extinction Angstrom Exponent (EAE), which is an indicator of particle size. Together with previous results, these results strengthen prospects for determining aerosol composition from space, for example using the Glory Aerosol Polarimetry Sensor (APS), which seeks to provide retrievals of multiwavelength single-scattering albedo (SSA) and aerosol optical depth (and therefore aerosol absorption optical depth (AAOD) and AAE), as well as shape and other aerosol properties. Multidimensional cluster analyses promise additional information content, for example by using the Ozone Monitoring Instrument (OMI) to add AAOD in the near ultraviolet and CALIPSO aerosol layer heights to reduce height-absorption ambiguity.

Description: 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).

Description: We have quantified the relationship between Aerosol Index (AI) measurements and plume height for young biomass burning plumes using coincident OMI and CALIPSO measurements. This linear relationship allows the determination of high-altitude plumes wherever AI data are available, and it provides a data set for validating global fire plume injection heights in chemistry transport models. We find that all plumes detected from June 2006 to February 2009 with an AI value ≥9 are located at altitudes higher than 5 km. Older high-altitude plumes have lower AI values than young plumes at similar altitudes. We have examined available AI data from the OMI and TOMS instruments (1978–2009) and find that large AI plumes occur more frequently over North America than over Australia or Russia/Northeast Asia. According to the derived relationship, during this time interval, 181 plumes reached altitudes above 8 km. One hundred and thirty-two had injection heights ≥8 km but below 12 km, and 49 were lofted to 12 km or higher, including 14 plumes injected above 16 km.

Description: We introduce a method for deriving aerosol spectral radiative forcing, along with single scattering albedo, asymmetry parameter and surface albedo from airborne vertical profile measurements of shortwave spectral irradiance and spectral aerosol optical thickness. The new method complements the traditional, direct measurement of aerosol radiative forcing efficiency from horizontal flight legs below gradients of aerosol optical thickness, and is particularly useful over heterogeneous land surfaces or for homogeneous aerosol layers where the horizontal gradient method is impractical. Using data collected by the Solar Spectral Flux Radiometer (SSFR) and the Ames Airborne Tracking Sunphotometer (AATS-14) during the MILAGRO (Megacity Initiative: Local and Global Research Observations) experiment, we validate an over-ocean spectral aerosol forcing efficiency from the new method by comparing with the traditional method. Retrieved over-land aerosol optical properties are compared with in-situ measurements and AERONET retrievals. The spectral forcing efficiencies over ocean and land are remarkably similar, and agree with results from other field experiments.

Description: 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. The Aerosol Polarimetry Sensor (APS), on the upcoming NASA Glory mission, has the potential to retrieve both cloud and aerosol properties because of its polarimetric, multiple view angle, and multi spectral observations. The APS airborne prototype is the Research Scanning Polarimeter (RSP), which has similar characteristics and can be used to demonstrate APS capabilities. 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 March 13th, 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 and the cloud droplet size distribution 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 case study in the context of the potential for future systematic APS observations of this kind, 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.