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A Study of Stratospheric Aerosols and Their Effect on Inorganic Chlorine Partitioning Using Balloon, In Situ, and Satellite Observations

Heterogeneous reactions on the surface of aerosols lead to a decrease in the concentration of nitrogen radicals and an increase in the concentration of chlorine and hydrogen radical species. As a consequence, enhanced sulfate aerosol levels in the lower stratosphere resulting from volcanic eruptions lead to lower concentrations of ozone due to more rapid loss by chlorine and hydrogen radicals. This study focuses on continuing the effort to quantify the effect of sulfate aerosols on the partitioning of inorganic chlorine species at midlatitudes. The study begins with an examination of balloon-borne measurements of key chlorine species obtained by the JPL MkIV interferometer for different aerosol loading conditions. A detailed comparison of the response of HCl to variations in aerosol surface area observed by MkIV, ER-2 instruments, HALOE, and ATMOS is carried out by examining HCl vs CH4 correlation diagrams, since CH4 is the only tracer measured on each platform. Finally, the consistency between theory and observed changes in ClO and HCl due to variations in aerosol surface area is examined.

Osterman, G. B.↗

What we Hope to Learn about Global Mineral Dust Aerosols from EOS Multi-Angle Imaging SpectroRadiometer (MISR)

On global scales, just a few broad atmospheric aerosol compositional groups are commonly observed. Of these, "mineral dust" is the only group which both contains non-spherical particles, and typically has size distributions with enough large particles for particle shape to affect its visible-light-scattering properties. The MISR instrument is scheduled for launch into a 10:30 AM sun-synchronous, polar orbit aboard the EOS Terra satellite in 1999. MISR will measure the upwelling visible radiance from Earth in 4 spectral bands centered at 446, 558, 672, and 866 nm, at each of 9 emission angles spread out in the forward and aft directions along the flight path at +/-70.5 deg, +/-60.0 deg, +/-45.6 deg, +/-26.1deg, and nadir. Over a period of 7 minutes, as the spacecraft flies along, a 360 km wide swath of Earth will successively be viewed by each of the cameras, allowing MISR to sample a very large range of scattering angles; in mid latitudes, the instrument will observe scattering angles between about 60 deg and 160 deg. Global coverage will be acquired about once in 9 days at the equator; the nominal mission lifetime is 6 years. The distinction in single scattering phase function between natural distributions of spherical and randomly oriented, non-spherical particles, with a broad range of aspect ratios, shows up strongly for scattering angles ranging from about 90 deg to near 180 deg. For non-spherical particle distributions, single scattering phase functions tend to be much flatter in this region than for spherical particles. Since MISR samples the relevant range of scattering angles very well, we expect to be able to make critical distinctions between natural distributions of spherical and randomly oriented, non-spherical particles with MISR data. We anticipate that the new multiangle, multispectral data from MISR will also contain other information about particle properties, a major step beyond current spacecraft remote sensing retrievals, which obtain aerosol optical depth based on entirely assumed particle microphysical properties. According to simulations over cloud-free, calm ocean, for pure particles with natural ranges of optical depth, particle size, and indices of refraction, MISR should retrieve column optical depth for all but the darkest particles, to an uncertainty of at most 0.05 or 20%, whichever is larger, even if the particle properties are poorly known. For one common particle type, soot, constraints on the optical depth over dark ocean are very poor. The simulated measurements also should allow us to separate two to four compositional groups based on indices of refraction, and to identify three to four distinct size groups between 0.1 and 2.0 microns characteristic radius at most latitudes. The technique is most sensitive to particle microphysical properties in the "accumulation mode" sizes. where particle scattering undergoes the transition from Rayleigh to large-particle regimes for the MISR wavelengths. Based on these results, we expect to distinguish air masses containing different aerosol types, routinely and globally, with multiangle remote sensing data. Such data complements in situ and field data, which can provide details about aerosol size and composition locally that are needed to assess the radiative effects of aerosols quantitatively. Both field data and correlations in space and time with likely source and sink regions will also be helpful in developing a global picture of mineral dust aerosol budgets. Further work on the expected sensitivity of MISR to natural mixtures of pure particles, including climatologically likely mineral dust components, is currently underway.

Kahn, Ralph↗

A 3-D Model Study of Aerosol Composition and Radiative Forcing in the Asian-Pacific Region

The Georgia Tech/Goddard Global Ozone Chemistry Aerosol Radiation and Transport (GOCART) model will be used in analyzing the aerosol data in the ACE-Asia program. Our objectives are (1) to understand the physical, chemical, and optical properties of aerosol and the processes that control these properties over the Asian-Pacific region, (2) to determine the aerosol radiative forcing over the Asian-Pacific region, and (3) to investigate the interaction between aerosol and tropospheric chemistry. We will present the GOCART aerosol simulations of sulfate, dust, carbonaceous, and sea salt concentrations, their optical thicknesses, and their radiative effects. We will also show the comparisons of model results with data taken from previous field campaigns, ground-based sun photometer measurements, and satellite observations. Finally, we will present our plan for the ACE-Asia study.

Chin, Mian↗

Aerosol Modeling for the Global Model Initiative

The goal of this project is to develop an aerosol module to be used within the framework of the Global Modeling Initiative (GMI). The model development work will be preformed jointly by the University of Michigan and AER, using existing aerosol models at the two institutions as starting points. The GMI aerosol model will be tested, evaluated against observations, and then applied to assessment of the effects of aircraft sulfur emissions as needed by the NASA Subsonic Assessment in 2001. The work includes the following tasks: 1. Implementation of the sulfur cycle within GMI, including sources, sinks, and aqueous conversion of sulfur. Aerosol modules will be added as they are developed and the GMI schedule permits. 2. Addition of aerosol types other than sulfate particles, including dust, soot, organic carbon, and black carbon. 3. Development of new and more efficient parameterizations for treating sulfate aerosol nucleation, condensation, and coagulation among different particle sizes and types.

Weisenstein, Debra K.↗

Baseline Maritime Aerosol: Methodology to Derive the Optical Thickness and Scattering Properties

Satellite Measurements of the global distribution of aerosol and their effect on climate should be viewed in respect to a baseline aerosol. In this concept, concentration of fine mode aerosol particles is elevated above the baseline by man-made activities (smoke or urban pollution), while coarse mode by natural processes (e.g. dust or sea-spray). Using 1-3 years of measurements in 10 stations of the Aerosol Robotic network (ACRONET we develop a methodology and derive the optical thickness and properties of this baseline aerosol for the Pacific and Atlantic Oceans. Defined as the median for periods of stable optical thickness (standard deviation < 0.02) during 2-6 days, the median baseline aerosol optical thickness over the Pacific Ocean is 0.052 at 500 am with Angstrom exponent of 0.77, and 0.071 and 1.1 respectively, over the Atlantic Ocean.

Kaufman, Yoram J.↗

Validation of MODIS Aerosol Retrieval Over Ocean

The MODerate resolution Imaging Spectroradiometer (MODIS) algorithm for determining aerosol characteristics over ocean is performing with remarkable accuracy. A two-month data set of MODIS retrievals co-located with observations from the AErosol RObotic NETwork (AERONET) ground-based sunphotometer network provides the necessary validation. Spectral radiation measured by MODIS (in the range 550 - 2100 nm) is used to retrieve the aerosol optical thickness, effective particle radius and ratio between the submicron and micron size particles. MODIS-retrieved aerosol optical thickness at 660 nm and 870 nm fall within the expected uncertainty, with the ensemble average at 660 nm differing by only 2% from the AERONET observations and having virtually no offset. MODIS retrievals of aerosol effective radius agree with AERONET retrievals to within +/- 0.10 micrometers, while MODIS-derived ratios between large and small mode aerosol show definite correlation with ratios derived from AERONET data.

Remer, Lorraine A.↗

Dust Aerosols at the Source Region During ACE-ASIA: A Surface/Satellite Perspective

ACE (Aerosol Characterization Experiment)-Asia is designed to study the compelling variability in spatial and temporal scale of both pollution-derived and naturally occurring aerosols, which often exist in high concentrations over eastern Asia and along the rim of the western Pacific. The phase-I of ACE-Asia was conducted from March-May 2001 in the vicinity of the Gobi desert, East Coast of China, Yellow Sea, Korea, and Japan, along the pathway of Kosa (severe events that blanket East Asia with yellow desert dust, peaked in the Spring season). Asian dust typically originates in desert areas far from polluted urban regions. During transport, dust layers can interact with anthropogenic sulfate and soot aerosols from heavily polluted urban areas. Added to the complex effects of clouds and natural marine aerosols, dust particles reaching the marine environment can have drastically different properties than those from the source. Thus, understanding the unique temporal and spatial variations of Asian dust is of special importance in regional-to-global climate issues such as radiative forcing, the hydrological cycle, and primary biological productivity in the mid-Pacific Ocean. During ACE-Asia we have measured continuously aerosol physical/optical/radiative properties, column precipitable water amount, and surface reflectivity over homogeneous areas from surface. The inclusion of flux measurements permits the determination of dust aerosol radiative flux in addition to measurements of loading and optical thickness. At the time of the Terra/MODIS, SeaWiFS, TOMS and other satellite overpasses, these ground-based observations can provide valuable data to compare with satellite retrievals over land. Preliminary results will be presented and discussed their implications in regional climatic effects.

Tsay, Si-Chee↗

Columnar Aerosol Single-Scattering Albedo and Phase Function Retrieved from Sky Radiance Over the Ocean: Measurements of African Dust

The single-scattering albedo and phase function of African mineral dust are retrieved from ground-based measurements of sky radiance collected in the Florida Keys. The retrieval algorithm employs the radiative transfer equation to solve by iteration for these two properties which best reproduce the observed sky radiance using an assumed aerosol vertical structure and measured aerosol optical depth. Thus, no assumptions regarding particle size, shape, or composition are required. The single-scattering albedo, presented at fourteen wavelengths between 380 and 870 nm, displays a spectral shape expected of iron-bearing minerals but is much higher than current dust models allow. This indicates the absorption of light by mineral dust is significantly overestimated in climate studies. Uncertainty in the retrieved albedo is less than 0.02 due to the small uncertainty in the solar-reflectance-based calibration (12.2%) method employed. The phase function retrieved at 860 nm is very robust under simulations of expected experimental errors, indicating retrieved phase functions at this wavelength may be confidently used to describe aerosol scattering characteristics. The phase function retrieved at 443 nm is very sensitive to expected experimental errors and should not be used to describe aerosol scattering. Radiative forcing by aerosol is the greatest source of uncertainty in current climate models. These results will help reduce uncertainty in the absorption of light by mineral dust. Assessment of the radiative impact of aerosol species is a key component to NASA's Earth System Enterprise.

Cattrall, Christopher↗

Remote Sensing of Non-Aerosol (anomalous) Absorption in Cloud Free Atmosphere

The interaction of sunlight with atmospheric gases, aerosols and clouds is fundamental to the understanding of climate and its variation. Several studies questioned our understanding of atmospheric absorption of sunlight in cloudy or in cloud free atmospheres. Uncertainty in instruments' accuracy and in the analysis methods makes this problem difficult to resolve. Here we use several years of measurements of sky and sun spectral brightness by selected instruments of the Aerosol Robotic Network (AERONET), that have known and high measurement accuracy. The measurements taken in several locations around the world show that in the atmospheric windows 0.44, 0.06, 0.86 and 1.02 microns the only significant absorbers in cloud free atmosphere is aerosol and ozone. This conclusions is reached using a method developed to distinguish between absorption associated with the presence of aerosol and absorption that is not related to the presence of aerosol. Non-aerosol absorption, defined as spectrally independent or smoothly variable, was found to have an optical thickness smaller than 0.002 corresponding to absorption of sunlight less than 1W/sq m, or essentially zero.

Kaufman, Yoram J.↗

Soot Aerosol from Aircraft: Is there Enough to Cause Middle-Latitude Lower Stratospheric Ozone

Soot aerosol from aircraft has been implicated to cause long-term ozone depletion at mid-latitudes in the lower stratosphere at a rate of approx. equals 5%,per decade. During the 1996 SUCCESS field campaign, we sampling aerosols in the exhaust wake of a Boeing 757 aircraft and determined emission indices for sulfuric acid (EIH2SO4=4.8E-2 and 5.7E- 1. g/kgFUEL for 75 and 675 ppm fuel-sulfur, respectively) and soot (EIsoot=7.5E-4 g/kgFUEL). The corresponding fuel-sulfur to H2SO4 conversion efficiency was 25 % and 30%,respctively. Applying the H2SO4 emission index to the 1990 fuel by the world's commercial fleets of 1.3E11 kg, a conversion efficiency of 30% would have led to an annual contribution to the atmospheric sulfur budget by aircraft of 2.E7 kg H2SO4, if the fuels averaged 500 ppmm.The soot emission index given above yielded a 1990 injection of soot aerosol by aircraft of 1.E5 kg. Thus, soot amounts to only one half of one percent of the aerosol generated by aircraft. The fractal nature of soot may increase its actual surface area by about a factor of 10. The findings, however, of (1) stratospheric soot loadings commensurate with aircraft fuel consumption, based on the emission index given above and the assumption of stratospheric residence times of the order of one year; and (2) a trend in stratospheric soot loading of approx.6% per year since 1981, similar to the annual increase of aircraft operations since that time, implicate aircraft as stratospheric polluters. A trend similar to soot of H2SO4 aerosol loading could not be deciphered, neither from in situ measurements nor SAGE II extinction, against the "noise" due to volcanic eruptions, The current single scatter albedo of the stratospheric aerosol is omega = 0.993+/-0.004.

Pueschel, R. F.↗

Light Absorption of Stratospheric Aerosols: Long-Term Trend and Contribution by Aircraft

Measurements of aerosol light-absorption coefficients are useful for studies of radiative transfer and heating rates. Ogren appears to have published the first light- absorption coefficients in the stratosphere in 1981, followed by Clarke in 1983 and Pueschel in 1992. Because most stratospheric soot appears to be due to aircraft operations, application of an aircraft soot aerosol emission index to projected fuel consumption suggests a threefold increase of soot loading and light absorption by 2025. Together, those four data sets indicate an increase in mid-visible light extinction at a rate of 6 % per year. This trend is similar to the increase per year of sulfuric acid aerosol and of commercial fleet size. The proportionality between stepped-up aircraft operations above the tropopause and increases in stratospheric soot and sulfuric acid aerosol implicate aircraft as a source of stratospheric pollution. Because the strongly light-absorbing soot and the predominantly light-scattering sulfuric acid aerosol increase at similar rates, however, the mid-visible stratospheric aerosol single scatter albedo is expected to remain constant and not approach a critical value of 0.98 at which stratospheric cooling could change to warming.

Pueschel , R. F.↗

MODIS and AERONET Characterization of the Global Aerosol

Recently produced daily MODIS aerosol data for the whole year of 2001 are used to show the concentration and dynamics of aerosol over ocean and large parts of the continents. The data were validated against the Aerosol Robotic Network (AERONET) measurements over land and ocean. Monthly averages and a movie based on the daily data are produced and used to demonstrate the spatial and temporal evolution of aerosol. The MODIS wide spectral range is used to distinguish fine smoke and pollution aerosol from coarse dust and salt. The movie produced from the MODIS data provides a new dimension to aerosol observations by showing the dynamics of the system. For example in February smoke and dust emitted from the Sahel and West Africa is shown to travel to the North-East Atlantic. In April heavy dust and pollution from East Asia is shown to travel to North America. In May-June pollution and dust play a dynamical dance in the Arabian Sea and Bay of Bengal. In Aug-September smoke from South Africa and South America is shown to pulsate in tandem and to periodically to be transported to the otherwise pristine Southern part of the Southern Hemisphere.

Kaufman, Yoram↗

Remote Sensing of Aerosol and their Effect on Climate

Smoke aerosol, pollution or dust affects the distribution of sunlight reaching the Earth. It enhances reflection of sunlight back to space and absorption in the atmosphere. Aerosol particles also affect cloud formation, thickness and formation of precipitation. The concentration of aerosol and their properties vary rapidly, due to the heterogeneity of sources and a short lifetime of about a week. Satellite and ground based network of remote sensing instruments were developed for continues measurement of the global distribution of aerosol and variation of their concentration and properties. I shall present examples of such measurements from the Terra spacecraft and the Aerosol Robotic Network, and explore the pathways to integrate these measurements into models that calculate the aerosol radiative forcing of climate.

Kaufman, Yoram↗

Overview of ACE-Asia Spring 2001 Investigations On Aerosol-Radiation Interactions

ACE-Asia's extensive measurements from land, ocean, air and space quantified aerosol-radiation interactions. Results from each platform type, plus satellite-suborbital combinations, include: 1. Time series of multiwavelength aerosol optical depth (ADD), Angstrom exponent (alpha), single-scattering albedo (SSA), and size distribution from AERONET radiometry at 13 stations. In China and Korea AOD and alpha were strongly anticorrelated (reflecting transient dust events); dust volume-size modes peaked near 8 microns diameter; and SSA(dust) greater than SSA(pollution). 2. Calculations and measurements of photosynthetically active radiation and aerosols in China yield 24-h average downward surface radiative forcing per AOD(500 nm) of -27 W/sq m (400-700 nm). 3. The Hawaii-Japan cruise sampled a gradient with AOD(500 nm) extremes of 0.1 and 1.1. Shipboard measurements showed that adding dust to pollution increased SSA(550 nm, 55% RH), typically from -0.91 to approx. 0.97. Downwelling 8-12 micron radiances showed aerosol effects, especially in the major April dust event, with longwave forcing estimated at -5 to 15 W/sq m. 4. Extinction profiles from airborne sunphotometry and total-direct-diffuse radiometry show wavelength dependence often varying strongly with height, reflecting layering of dust-dominated over pollution-dominated aerosols. Comparing sunphotometric extinction profiles to those from in situ measurements (number and composition vs size, or scattering and absorption) shows layer heights agree, but extinction sometimes differs. 5. Airborne solar spectral flux radiometry yields absorption spectra for layers. Combining with AOD spectra yields best-fit aerosol single scattering albedo spectra. 6. Visible, NIR and total solar fluxes combined with AOD give radiative forcing efficiencies at surface and aloft.

Russell, P. B.↗

Wavelength Dependence of the Absorption of Black Carbon Particles: Predictions and Results from the TARFOX Experiment and Implications for the Aerosol Single Scattering Albedo

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 lamda(exp -1) variation between 0.40 and 1.0 micrometers. 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(exp -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 allied 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.

Bergstrom, Robert W.↗

Ground-Based Lidar Measurements of Aerosols During ACE-2: Instrument Description, Results, and Comparisons with Other Ground-Based and Airborne Measurements

A micro-pulse lidar system (MPL) was used to measure the vertical and horizontal distribution of aerosols during the Aerosol Characterization Experiment 2 (ACE-2) in June and July of 1997. The MPL measurements were made at the Izana observatory (IZO), a weather station located on a mountain ridge (28 deg 18 min N, 16 deg 30 min W, 2367 m asl) near the center of the island of Tenerife, Canary Islands. The MPL was used to acquire aerosol backscatter, extinction, and optical depth profiles for normal background periods and periods influenced by Saharan dust from North Africa. System tests and calibration procedures are discussed, and an analysis of aerosol optical profiles acquired during ACE-2 is presented. MPL data taken during normal IZO conditions (no dust) showed that upslope aerosols appeared during the day and dissipated at night and that the layers were mostly confined to altitudes a few hundred meters above IZO. MPL data taken during a Saharan dust episode on 17 July showed that peak aerosol extinction values were an order of magnitude greater than molecular scattering over IZO, and that the dust layers extended to 5 km asl. The value of the dust backscatter-extinction ratio was determined to be 0.027 +/- 0.007 sr(exp -1). Comparisons of the MPL data with data from other collocated instruments showed good agreement during the dust episode.

Welton, Ellsworth J.↗

Regional Aerosol Optical Depth Characteristics from Satellite Observations: ACE-1, TARFOX and ACE-2 Results

Analysis of the aerosol properties during 3 recent international field campaigns ACE-1, TARFOX and ACE-2 are described using satellite retrievals from NOAA AVHRR data. Validation of the satellite retrieval procedure is performed with airborne, shipboard, and land-based sunphotometry during ACE-2. The intercomparison between satellite and surface optical depths has a correlation coefficient of 0.93 for 630 nm wavelength and 0.92 for 860 nm wavelength, The standard error of estimate is 0.025 for 630 nm wavelength and 0.023 for 860 nm wavelength. Regional aerosol properties are examined in composite analysis of aerosol optical properties from the ACE-1, TARFOX and ACE-2 regions. ACE-1 and ACE-2 regions have strong modes in the distribution of optical depth around 0.1, but the ACE-2 tails toward higher values yielding an average of 0.16 consistent with pollution and dust aerosol intrusions. The TARFOX region has a noticeable mode of 0.2, but has significant spread of aerosol optical depth values consistent with the varied continental aerosol constituents off the eastern North American Coast.

Durkee, P. A.↗

Effects of Aircraft On Aerosol Abundance in the Upper Troposphere

A significant increase in sulfuric acid aerosol concentration was detected above 10 km pressure altitude during a cross-corridor flight out of Shannon on October 23, 1997. The source of this aerosol is ascribed to commercial aircraft operations in flight corridors above 10 km, because (1) a stable atmosphere prevented vertical air mass exchanges and thus eliminated surface sources, (2) air mass back trajectories documented the absence of remote continental sources, and (3) temperature profiler data showed the tropopause at least one kilometers above flight altitude throughout the flight. Particle volatility identified 70% H2SO4, 20% (NH4)2SO4 and 10% nonvolatile aerosol in the proximity of flight corridors, and (10-30)% H2SO4, up to 50% (NH4)2SO4, and (40-60)% nonvolatile aerosols in air that was not affected by aircraft operations below 10 km. Only a very small fraction of the nonvolatile particles (determined with a condensation nucleus counter) could be morphologically identified as soot aerosol (validated by scanning electron microscopy of wire impactor samples). The newly formed H2SO4 particles did not measurably affect surface area and volume of the background aerosol due to their small size, hence did not affect radiative transfer directly.

Ferry, G. V.↗