ALBERT

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 region: 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: We have determined the solar spectral absorption optical depth of atmospheric aerosols for specific case studies during several field programs (three cases have been reported previously; two are new results). We combined airborne measurements of the solar net radiant flux density and the aerosol optical depth with a detailed radiative transfer model for all but one of the cases. The field programs (SAFARI 2000, ACE Asia, PRIDE, TARFOX, INTEX-A) contained aerosols representing the major absorbing aerosol types: pollution, biomass burning, desert dust and mixtures. In all cases the spectral absorption optical depth decreases with wavelength and can be approximated with a power-law wavelength dependence (Absorption Angstrom Exponent or AAE). We compare our results with other recent spectral absorption measurements and discuss the limitations in using the AAE for calculating the solar absorption. We also discuss the resulting spectral single scattering albedo for these cases.

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 (expressed as Absorption Angstrom Exponent, or AAE). Taken together, these results hold promise of improving information on aerosol composition from remote measurements. The purpose of this paper is to show that AAE values for Aerosol Robotic Network (AERONET) retrievals from Sun-sky measurements describing the full aerosol vertical column 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. 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 promises 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. 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: Airborne sunphotometer measurements are used to evaluate retrievals of extinction aerosol optical depth (AOD) from spatially coincident and temporally near-coincident measurements by the Ozone Monitoring Instrument (OMI) aboard the Aura satellite during the March 2006 Megacity Initiative-Local And Global Research Observations/Phase B of the Intercontinental Chemical Transport Experiment (MILAGRO/INTEX-B). The 14-channel NASA Ames Airborne Tracking Sunphotometer (AATS) flew on nine missions over the Gulf of Mexico and four in or near the Mexico City area. Retrievals of AOD from near-coincident AATS and OMI measurements are compared for three flights over the Gulf of Mexico for flight segments when the aircraft flew at altitudes 60–70 m a.s.l., and for one flight over Mexico City when the aircraft flew ~420–590 m a.g.l. OMI-measured top of atmosphere (TOA) reflectances are routinely inverted to yield aerosol products such as AOD and aerosol absorption optical depth (AAOD) using two different retrieval algorithms: a near-UV (OMAERUV) and a multiwavelength (OMAERO) technique. This study uses the archived Collection 3 data products from both algorithms. In particular, AATS and OMI AOD comparisons are presented for AATS data acquired in 20 OMAERUV retrieval pixels (15 over water) and 19 OMAERO pixels (also 15 over water). At least four pixels for one of the over-water coincidences and all pixels for the over-land case were cloud-free. Coincident AOD retrievals from 17 pixels of the Moderate Resolution Imaging Spectroradiometer (MODIS) aboard Aqua are available for two of the over-water flights and are shown to agree with AATS AODs to within root mean square (RMS) differences of 0.00–0.06, depending on wavelength. Near-coincident ground-based AOD measurements from ground-based sun/sky radiometers operated as part of the Aerosol Robotic Network (AERONET) at three sites in and near Mexico City are also shown and are generally consistent with the AATS AODs (which exclude any AOD below the aircraft) both in magnitude and spectral dependence. The OMAERUV algorithm retrieves AODs corresponding to a non-absorbing aerosol model for all three over-water comparisons, whereas the OMAERO algorithm retrieves best-fit AODs corresponding to an absorbing biomass-burning aerosol model for two of the three over-water cases. For the four cloud-free pixels in one over-water coincidence (10 March), the OMAERUV retrievals underestimate the AATS AODs by ~0.20, which exceeds the expected retrieval uncertainty, but retrieved AODs agree with AATS values within uncertainties for the other two over-water events. When OMAERO retrieves AODs corresponding to a biomass-burning aerosol over water, the values significantly overestimate the AATS AODs (by up to 0.55). For the Mexico City coincidence, comparisons are presented for a non-urban region ~50–70 km northeast of the city and for a site near the center of the city. OMAERUV retrievals are consistent with AERONET AOD magnitudes for the non-urban site, but are nearly double the AATS and AERONET AODs (with differences of up to 0.29) in the center of the city. Corresponding OMAERO retrievals exceed the AATS and/or AERONET AODs by factors of 3 to 10.

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 have determined the solar spectral absorption optical depth of atmospheric aerosols for specific case studies during several field programs (three cases have been reported previously; two are new results). We combined airborne measurements of the solar net radiant flux density and the aerosol optical depth with a detailed radiative transfer model for all but one of the cases. The field programs (SAFARI 2000, ACE Asia, PRIDE, TARFOX, INTEX-A) contained aerosols representing the major absorbing aerosol types: pollution, biomass burning, desert dust and mixtures. In all cases the spectral absorption optical depth decreases with wavelength and can be approximated with a power-law wavelength dependence (Absorption Angstrom Exponent or AAE). We compare our results with other recent spectral absorption measurements and attempt to briefly summarize the state of knowledge of aerosol absorption spectra in the atmosphere. We discuss the limitations in using the AAE for calculating the solar absorption. We also discuss the resulting spectral single scattering albedo for these cases.

Description: Airborne sunphotometer measurements are used to evaluate retrievals of extinction aerosol optical depth (AOD) from spatially coincident and temporally near-coincident measurements by the Ozone Monitoring Instrument (OMI) aboard the Aura satellite during the March 2006 Megacity Initiative-Local And Global Research Observations/Phase B of the Intercontinental Chemical Transport Experiment (MILAGRO/INTEX-B). The 14-channel NASA Ames Airborne Tracking Sunphotometer (AATS) flew on nine missions over the Gulf of Mexico and four in or near the Mexico City area. Retrievals of AOD from near-coincident AATS and OMI measurements are compared for three flights over the Gulf of Mexico for flight segments when the aircraft flew at altitudes 60–70 m above sea level, and for one flight over the Mexico City area where the aircraft was restricted to altitudes ~320–800 m above ground level over the rural area and ~550–750 m over the city. OMI-measured top of atmosphere (TOA) reflectances are routinely inverted to yield aerosol products such as AOD and aerosol absorption optical depth (AAOD) using two different retrieval algorithms: a near-UV (OMAERUV) and a multiwavelength (OMAERO) technique. This study uses the archived Collection 3 data products from both algorithms. In particular, AATS and OMI AOD comparisons are presented for AATS data acquired in 20 OMAERUV retrieval pixels (15 over water) and 19 OMAERO pixels (also 15 over water). At least four pixels for one of the over-water coincidences and all pixels for the over-land case were cloud-free. Coincident AOD retrievals from 17 pixels of the Moderate Resolution Imaging Spectroradiometer (MODIS) aboard Aqua are available for two of the over-water flights and are shown to agree with AATS AODs to within root mean square (RMS) differences of 0.00–0.06, depending on wavelength. Near-coincident ground-based AOD measurements from ground-based sun/sky radiometers operated as part of the Aerosol Robotic Network (AERONET) at three sites in and near Mexico City are also shown and are generally consistent with the AATS AODs (which exclude any AOD below the aircraft) both in magnitude and spectral dependence. The OMAERUV algorithm retrieves AODs corresponding to a non-absorbing aerosol model for all three over-water comparisons whereas the OMAERO algorithm retrieves best-fit AODs corresponding to an absorbing biomass-burning aerosol model for two of the three over-water cases. For the four cloud-free pixels in one over-water coincidence (10 March), the OMAERUV retrievals underestimate the AATS AODs by ~0.20, which exceeds the expected retrieval uncertainty, but retrieved AODs agree with AATS values within uncertainties for the other two over-water events. When OMAERO retrieves AODs corresponding to a biomass-burning aerosol over water, the values significantly overestimate the AATS AODs (by up to 0.55). For the Mexico City coincidence, comparisons are presented for a non-urban region ~50–70 km northeast of the city and for a site near the center of the city. OMAERUV retrievals are consistent with AERONET AOD magnitudes for the non-urban site, but are nearly double the AATS and AERONET AODs (with differences of up to 0.29) in the center of the city. Corresponding OMAERO retrievals exceed the AATS and/or AERONET AODs by factors of 3 to 10.

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.