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).

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.

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 multi-wavelength 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.

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).

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.

Abstract. 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.

No abstract available.

We investigated the effects of fire-induced plume-rise on the simulation of carbon monoxide (CO) over Africa and its export during SAFARI 2000 using the NCAR Community Atmosphere Model (CAM) with a CO tracer and a plume-rise parameterization scheme. The plume-rise parameterization scheme simulates the consequences of strong buoyancy of hot gases emitted from biomass burning, including both dry and cloud-associated (pyro-cumulus) lofting. The current implementation of the plume-rise parameterization scheme into the global model provides an opportunity to examine the effect of plume-rise on long-range transport. The CAM simulation with the plume-rise parameterization scheme seems to show a substantial improvement of the agreements between the modeled and aircraft-measured vertical distribution of CO over Southern Africa biomass-burning area. The plume-rise mechanism plays a crucial role in lofting biomass-burning pollutants to the middle troposphere. In the presence of deep convection we found that the plume-rise mechanism results in a decrease of CO concentration in the upper troposphere. The plume-rise depletes the boundary layer, and thus leaves lower concentrations of CO to be lofted by the deep convection process. The effect of the plume-rise on free troposphere CO concentration is more important for the source area (short-distance transport) than for remote areas (long-distance transport). A budget analysis of CO burden over Southern Africa reveals the plume-rise process to have a similar impact as the chemical production of CO by OH and CH4. In addition, the plume-rise process has an minor impact on the regional export. These results further confirm and extend previous findings in a regional model study. Effective lofting of large concentration of CO by the plume-rise mechanism also has implications for local air quality forecasting in areas affected by other fire-related pollutants.

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.

We present a synthesis of single scattering albedo for biomass burning aerosol from the SAFARI 2000 field campaign. Values at 550 nm were derived from three methods: airborne in situ measurements of aerosol scattering and absorption; airborne flux radiometry; and ground-based sun-photometer/radiometer retrievals from AERONET. Collocated comparisons indicate that uncertainties are well understood for all three methods. The new ( Version 2) AERONET retrieval gives substantially lower single scattering albedo over bright surfaces, and the comparisons herein represent the first independent check of this retrieval. Combined in situ and AERONET data yield a regional value of 0.85 +/- 0.02 ( mean and total uncertainty), which we propose is representative of single scattering albedo for the Southern African region during the biomass burning season. This value agrees with the "highly absorbing smoke" model used in MODIS aerosol retrievals, but indicates that many of the AeroCom models overestimate single scattering albedo for this region and season.

The optical properties of the light-absorbing, carbonaceous substance often called “soot,” “black carbon,” or “carbon black" have been the subject of some debate. These properties are necessary to model how aerosols affect climate, and our review is targeted specifically for that application. We recommend the term light-absorbing carbon to avoid conflict with operationally based definitions. Absorptive properties depend on molecular form, particularly the size of sp 2-bonded clusters. Freshly-generated particles should be represented as aggregates, and their absorption is like that of particles small relative to the wavelength. Previous compendia have yielded a wide range of values for both refractive indices and absorption cross section. The absorptive properties of light-absorbing carbon are not as variable as is commonly believed. Our tabulation suggests a mass-normalized absorption cross section of 7.5 ± 1.2 m2/g at 550 nm for uncoated particles. We recommend a narrow range of refractive indices for strongly-absorbing carbon particles, of which the highest is 1.95–0.79i. Our refractive indices are consistent with most measurements reported in the literature, and values used in present-day climate modeling are in error. Realistic refractive indices underpredict measured absorption by about 30% when used with common theories for spherical particles or aggregates. Field programs since about 1970 have measured quantities relevant to light absorption, but have only recently made enough measurements to isolate the light-absorbing carbonaceous component and determine its absorptive properties.

Contact Information Odele Hofmann ph. 303.492.8653 odele.hofmann@lasp.colorado.edu OVERVIEW During the ICARTT campaign of 2004, we measured solar spectral irradiance with the SSFR (Solar Spectral Flux Radiometer) to retrieve cloud properties. We compare these cloud retrievals to in situ microphysical measurements by the FSSP (Forward Scattering Spectrometer Probe) and to other remote sensing observations from MIDAS (Miniturized Differential Absorption Spectrometer ). AATS-14 (Ames Airborne Tracking Sunphotometer) aerosol measurements were used to examine the effects of aerosols on cloud retrievals. For four cases, we compare the SSFR retrieved cloud optical depths and effective cloud droplet radii with MODIS (Moderate Resolution Imaging Spectroradiometer).

As part of the Asian Pacific Regional Aerosol Characterization Experiment (ACE‐Asia), the upward and downward spectral solar radiant fluxes were measured with the Spectral Solar Flux Radiometer (SSFR), and the aerosol optical depth was measured with the Ames Airborne Tracking Sunphotometer (AATS‐14) aboard the Center for Interdisciplinary Remotely‐Piloted Aircraft Studies (CIRPAS) Twin Otter aircraft. In this paper, we examine the data obtained for two cases: a moderately thick aerosol layer, 12 April, and a relatively thin aerosol case, 16 April 2001. On both days, the Twin Otter flew vertical profiles in the Korean Strait southeast of Gosan Island. For both days we determine the aerosol spectral absorption of the layer and estimate the spectral aerosol absorption optical depth and single‐scattering albedo. The results for 12 April show that the single‐scattering albedo increases with wavelength from 0.8 at 400 nm to 0.95 at 900 nm and remains essentially constant from 950 to 1700 nm. On 16 April the amount of aerosol absorption was very low; however, the aerosol single‐scattering albedo appears to decrease slightly with wavelength in the visible region. We interpret these results in light of the two absorbing aerosol species observed during the ACE‐Asia study: mineral dust and black carbon. The results for 12 April are indicative of a mineral dust‐black carbon mixture. The 16 April results are possibly caused by black carbon mixed with nonabsorbing pollution aerosols. For the 12 April case we attempt to estimate the relative contributions of the black carbon particles and the mineral dust particles. We compare our results with other estimates of the aerosol properties from a Sea‐Viewing Wide Field‐of View Sensor (SeaWiFS) satellite analysis and aerosol measurements made aboard the Twin Otter, aboard the National Oceanic and Atmospheric Administration Ronald H. Brown ship, and at ground sites in Gosan and Japan. The results indicate a relatively complicated aerosol mixture of both industrial pollution (including black carbon) and mineral dust. This underscores the need for careful measurements and analysis to separate out the absorption effects of mineral dust and black carbon in the east Asia region.

During the dry season component of the Southern African Regional Science Initiative (SAFARI) in late winter 2000, the net solar spectral irradiance was measured at flight levels throughout biomass burning haze layers. From these measurements, the flux divergence, fractional absorption, instantaneous heating rate, and absorption efficiency were derived. Two cases are examined: on 24 August 2000 off the coast of Mozambique in the vicinity of Inhaca Island and on 6 September 2000 in a very thick continental haze layer over Mongu, Zambia. The measured absolute absorption was substantially higher for the case over Mongu where the measured midvisible optical depth exceeded unity. Instantaneous heating from aerosol absorption was 4 K d−1 over Mongu, Zambia and 1.5 K d−1 near Inhaca Island, Mozambique. However, the spectral absorption efficiency was nearly identical for both cases. Although the observations over Inhaca Island preceded the “river of smoke” from the southern African continent by nearly 2 weeks, the evidence here suggests a continental influence in the lower tropospheric aerosol far from source regions of burning.

Using measurements of the spectral solar radiative flux and optical depth for 2 days (24 August and 6 September 2000) during the SAFARI 2000 intensive field experiment and a detailed radiative transfer model, we estimate the spectral single scattering albedo of the aerosol layer. The single scattering albedo is similar on the 2 days even though the optical depth for the aerosol layer was quite different. The aerosol single scattering albedo was between 0.85 and 0.90 at 350 nm, decreasing to 0.6 in the near infrared. The magnitude and decrease with wavelength of the single scattering albedo are consistent with the absorption properties of small black carbon particles. We estimate the uncertainty in the single scattering albedo due to the uncertainty in the measured fractional absorption and optical depths. The uncertainty in the single scattering albedo is significantly less on the high‐optical‐depth day (6 September) than on the low‐optical‐depth day (24 August). On the high‐optical‐depth day, the uncertainty in the single scattering albedo is 0.02 in the midvisible whereas on the low‐optical‐depth day the uncertainty is 0.08 in the midvisible. On both days, the uncertainty becomes larger in the near infrared. We compute the radiative effect of the aerosol by comparing calculations with and without the aerosol. The effect at the top of the atmosphere (TOA) is to cool the atmosphere by 13 W m−2 on 24 August and 17 W m−2 on 6 September. The effect on the downward flux at the surface is a reduction of 57 W m−2 on 24 August and 200 W m−2 on 6 September. The aerosol effect on the downward flux at the surface is in good agreement with the results reported from the Indian Ocean Experiment (INDOEX).

Measurements are presented of the wavelength dependence of the aerosol absorption coefficient taken during the Tropical Aerosol Radiative Forcing Observational Experiment (TARFOX) over the northern Atlantic. The data show an approximate lambda(-1) variation between 0.40 and 1.0 mum. The theoretical basis of the wavelength variation of the absorption of solar radiation by elemental carbon [or black carbon (BC)] is explored. For a wavelength independent refractive index the small particle absorption limit simplifies to a lambda(-1) variation in relatively good agreement with the data. This result implies that the refractive indices of BC were relatively constant in this wavelength region, in agreement with much of the data on refractive indices of BC. However, the result does not indicate the magnitude of the refractive indices.The implications of the wavelength dependence of BC absorption for the spectral behavior of the aerosol single scattering albedo are discussed. It is shown that the single scattering albedo for a mixture of BC and nonabsorbing material decreases with wavelength in the solar spectrum (i.e., the percentage amount of absorption increases). This decease in the single scattering albedo with wavelength for black carbon mixtures is different from the increase in single scattering albedo for most mineral aerosols (dusts). This indicates that, if generally true, the spectral variation of the single scattering albedo can be used to distinguish aerosol types. It also highlights the importance of measurements of the spectral variation of the aerosol absorption coefficient and single scattering albedo.