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A model for studying the composition and chemical effects of stratospheric aerosols

We developed polynomial expressions for the temperature dependence of the mean binary and water activity coefficients for H2SO4 and HNO3 solutions. These activities were used in an equilibrium model to predict the composition of stratospheric aerosols under a wide range of environmental conditions. For typical concentrations of H2O, H2SO4, HNO3, HCl, HBr, HF, and HOCl in the lower stratosphere, the aerosol composition is estimated as a function of the local temperature and the ambient relative humidity. For temperatures below 200 K, our results indicate that (1) HNO3 contributes a significant mass fraction to stratospheric aerosols, and (2) HCl solubility is considerably affected by HNO3 dissolution into sulfate aerosols. We also show that, in volcanically disturbed periods, changes in stratospheric aerosol composition can significantly alter the microphysics that leads to the formation of polar stratospheric clouds. The effects caused by HNO3 dissolution on the physical and chemical properties of stratospheric aerosols are discussed.

Tabazadeh, Azadeh↗

Satellite remote sensing of H2SO4 aerosol using the 8- to 12-microns window region: Application to Mount Pinatubo

Monitoring stratospheric aerosols containing H2SO4 using the brightness temperature (BT) difference between 11 and 8.3 microns (BT(sub 8)-BT(sub 11)) spectral channels is demonstrated using theoretical calculations and satellite observations. Assuming an aqueous solution of 50% and 75% sulfuric acid, radiative transfer calculations indicate that over oceans an increase in the optical depth of the stratospheric aerosol results in an increase in BT(sub 8)-BT(sub 11). Theoretical simulations suggest that the technique is sensitive to visible optical depths greater than approximately 0.15. The simulations also demonstrate a lack of sensitivity to the particle size distribution. Changes in pre- and post-Pinatubo observations by the High-resolution Infrared Radiation Sounder 2 (HIRS2) on board the NOAA 10 are consistent with observed optical depth measurements and confirm the sensitivity of these channels to the presence of the aerosol. The technique is also applied to cold tropical convective clouds and desert regions where the signal, though evident, is less conclusive. Time series analysis is applied to the NOAA 10 and NOAA 12 combined BT(sub 8-BT(sub 11) observations to detect the periodicity of the spread of the volcanic aerosol. Over a region of the southern Pacific a 18- to 26-day period is present. Model simulations were conducted to demonstrate a trispectral with observations near 8, 11, and 12 microns. The trispectral approach has high potential in that the spectral signature of cirrus, water vapor, and H2SO4 aerosols are different. Observations from NOAA 10 and NOAA 11 are combined to demonstrate the capabilities of these infrared wavelengths of detecting the aerosol. The signal is clearly evident when a region of the South Atlantic is compared for pre- and post-Pinatubo conditions.

Ackerman, Steven A.↗

Investigation of biomass burning and aerosol loading and transport in South America utilizing geostationary satellites

This study attempts to assess the extent of burning and associated aerosol transport regimes in South America and the South Atlantic using geostationary satellite observations, in order to explore the possible roles of biomass burning in climate change and more directly in atmospheric chemistry and radiative transfer processes. Modeling and analysis efforts have suggested that the direct and indirect radiative effects of aerosols from biomass burning may play a major role in the radiative balance of the earth and are an important factor in climate change calculations. One of the most active regions of biomass burning is located in South America, associated with deforestation in the selva (forest), grassland management, and other agricultural practices. As part of the NASA Aerosol Interdisciplinary Program, we are utilizing GOES-7 (1988) and GOES-8 (1995) visible and multispectral infrared data (4, 11, and 12 microns) to document daily biomass burning activity in South America and to distinguish smoke/aerosols from other multi-level clouds and low-level moisture. This study catalogues the areal extent and transport of smoke/aerosols throughout the region and over the Atlantic Ocean for the 1988 (July-September) and 1995 (June-October) biomass burning seasons. The smoke/haze cover estimates are compared to the locations of fires to determine the source and verify the haze is actually associated with biomass burning activities. The temporal resolution of the GOES data (half-hourly in South America) makes it possible to determine the prevailing circulation and transport of aerosols by considering a series of visible and infrared images and tracking the motion of smoke, haze and adjacent clouds. The study area extends from 40 to 70 deg W and 0 to 40 deg S with aerosol coverage extending over the Atlantic Ocean when necessary. Fire activity is estimated with the GOES Automated Biomass Burning Algorithm (ABBA). To date, our efforts have focused on GOES-7 and GOES-8 ABBA development, algorithm development for aerosol monitoring, data acquisition and archiving, and participation in the SCAR-C and SCAR-B field programs which have provided valuable information for algorithm testing and validation. Implementation of the initial version of the GEOS-8 ABBA on case studies in North, Central, and South America has demonstrated the improved capability for monitoring diurnal fire activity and smoke/aerosol transport with the GOES-8 throughout the Western Hemisphere.

Menzel, Paul↗

Multiwavelength Comparison of Modeled and Measured Remote Tropospheric Aerosol Backscatter Over Pacific Ocean

Aerosol concentrations and size distributions in the middle and upper troposphere over the remote Pacific Ocean were measured with a forward scattering spectrometer probe (FSSP) on the NASA DC-8 aircraft during NASA's Global Backscatter Experiment (GLOBE) in May-June 1990. The FSSP size channels were recalibrated based on refractive index estimates from flight-level aerosol volatility measurements with a collocated laser optical particle counter (LOPC). The recalibrated FSSP size distributions were averaged over 100-s intervals, fitted with lo-normal distributions and used to calculate aerosol backscatter coefficients at selected wavelengths. The FSSP-derived backscatter estimates were averaged over 300-s intervals to reduce large random fluctuations. The smoothed FSSP aerosol backscatter coefficients were then compared with LOPC-derived backscatter values and with backscatter measured at or near flight level from four lidar systems operating at 0.53, 1.06, 9.11, 9.25, and 10.59 micrometers. Agreement between FSSP-derived and lidar-measured backscatter was generally best at flight level in homogeneous aerosol fields and at high backscatter values. FSSP data often underestimated low backscatter values especially at the longer wavelengths due to poor counting statistics for larger particles (greater than 0.8 micrometers diameter) that usually dominate aerosol backscatter at these wavelengths. FSSP data also underestimated backscatter at shorter wavelengths when particles smaller than the FSSP lower cutoff diameter (0.35 micrometers) made significant contributions to the total backscatter.

Cutten, D. R.↗

Comparative Optical Measurements of Airspeed and Aerosols on a DC-8 Aircraft

NASA Dryden supported a cooperative flight test program on the NASA DC-8 aircraft in November 1993. This program evaluated optical airspeed and aerosol measurement techniques. Three brassboard optical systems were tested. Two were laser Doppler systems designed to measure free-stream-referenced airspeed. The third system was designed to characterize the natural aerosol statistics and airspeed. These systems relied on optical backscatter from natural aerosols for operation. The DC-8 aircraft carried instrumentation that provided real-time flight situation information and reference data on the aerosol environment. This test is believed to be the first to include multiple optical airspeed systems on the same carrier aircraft, so performance could be directly compared. During 23 hr of flight, a broad range of atmospheric conditions was encountered, including aerosol-rich layers, visible clouds, and unusually clean (aerosol-poor) regions. Substantial amounts of data were obtained. Important insights regarding the use of laser-based systems of this type in an aircraft environment were gained. This paper describes the sensors used and flight operations conducted to support the experiments. The paper also briefly describes the general results of the experiments.

Bogue, Rodney↗

Relationships between Optical Extinction, Backscatter and Aerosol Surface and Volume in the Stratosphere following the Eruption of Mt. Pinatubo

The eruption of the Mt. Pinatubo volcano in the Philippines in June 1991 has resulted in increases in the surface and mass concentrations of aerosol particles in the lower stratosphere. Airborne measurements made at midlatitudes between 15 and 21 km from August 1991 to March 1992 show that, prior to December 1991, the Pinatubo aerosol cloud varied widely in microphysical properties such as size distribution, number, surface and volume concentrations and was also spatially variable. Aerosol surface area concentration was found to be highly correlated to extinction at visible and near-infrared wavelengths throughout the measurement period. Similarly, backscatter at common lidar wavelengths was a good predictor of aerosol volume concentrations. These results support the use of satellite extinction measurements to estimate aerosol surface and of lidar measurements to estimate aerosol volume or mass if temporal changes in the relationships between the variables are considered.

Brock, Charles A.↗

Pulmonary Deposition of Aerosols in Microgravity

The intrapulmonary deposition of airborne particles (aerosol) in the size range of 0.5 to 5 microns is primarily due to gravitational sedimentation. In the microgravity (muG) environment, sedimentation is no longer active, and thus there should be marked changes in the amount and site of the deposition of these aerosol. We propose to study the total intrapulmonary deposition of aerosol spanning the range 0.5 to 5 microns in the KC-135 at both muG and at 1.8-G. This will be followed by using boli of 1.0 micron aerosol, inhaled at different points in a breath to study aerosol dispersion and deposition as a function of inspired depth. The results of these studies will have application in better understanding of pulmonary diseases related to inhaled particles (pneumoconioses), in studying drugs delivered by inhalation, and in understanding the consequence of long-term exposure to respirable aerosols in long-duration space flight.

Prisk, G. Kim↗

First results from the aerosol lidar and backscatter sonde intercomparison campaign STRAIT'1997 at table mountain facility during February-March 1997

First results of an intercomparison measurement campaign between three aerosol lidar instruments and in-situ backscatter sondes performed at Table Mountain Facility (34.4 deg N, 117.7 deg E, 2280 m asl) in February-March 1997 are presented. During the campaign a total of 414 hours of lidar data were acquired by the Aerosol-Temperature-Lidar (ATL, Goddard Space Flight Center) the Mobile-aerosol-Raman-Lidar (MARL, Alfred Wegener Institute), and the TMF-Aerosol-Lidar (TAL, Jet Propulsion Laboratory), and four backscatter sondes were launched. From the data set altitude profiles of backscatter ratio and volume depolarization of stratospheric background aerosols at altitudes between 15 and 25 km and optically thin high-altitude cirrus clouds at altitudes below 13 km are derived. On the basis of a sulfuric acid aerosol model color ratio profiles obtained from two wavelength lidar data are compared to the corresponding profiles derived from the sonde observations. We find an excellent agreement between the in-situ and ATL lidar data with respect to backscatter and color ratio. Cirrus clouds were present on 16 of 26 nights during the campaign. Lidar observations with 17 minute temporal and 120-300 m spatial resolution indicate high spatial and temporal variability of the cirrus layers. Qualitative agreement is found between concurrent lidar measurements of backscatter ratio and volume depolarization.

Beyerle, G.↗

Role of the Quasi-Biennial Oscillation in the Transport of Aerosols from the Tropical Stratospheric Reservoir to Midlatitudes

The temporal evolution of the stratospheric aerosol distribution in the tropical stratospheric reservoir after the eruption of Mount Pinatubo was observed from 1992 to 1995 by the HALOE instrument on the UARS satellite. Since the spatial gradient of aerosol loading is large at the boundaries of the tropical stratospheric reservoir due to the volcanic aerosols, the effect of the meridional circulation on the distribution is seen clearly. The mechanism for dispersal of aerosol in the lower stratosphere from the tropics into midlatitudes strongly depends on the phase of the equatorial zonal wind. The time-latitude cross sections of the normalized distribution of aerosol on isentropic surfaces are used to observe the equatorial variation as well as change in meridional dispersal during the quasi-biennial period. Observed tropical stratospheric winds are used with a simple analytical dynamical model to examine transport processes of tracers from the tropics during several phases of the quasi-biennial oscillation (QBO) from 1992 to 1995. The Lagrangian meridional circulation in the tropics is consistent with the vertical and meridional velocities correlated with the QBO in the zonal wind. We find that vertical motion plays a crucial role in vertical and subsequent meridional transport. The pattern of meridional divergence derived from the vertical velocity is closely related to the observed HALOE aerosol distributions and their temporal development in the equatorial region. The westerly (easterly) shear phase of the QBO is associated with sinking (rising) motions at the equator and subsequent poleward (equatorward) transport in the lower stratosphere.

Choi, Wookap↗

Intercomparison of Pulsed Lidar Data with Flight Level CW Lidar Data and Modeled Backscatter from Measured Aerosol Microphysics Near Japan and Hawaii

Aerosol backscatter coefficient data were examined from two nights near Japan and Hawaii undertaken during NASA's Global Backscatter Experiment (GLOBE) in May-June 1990. During each of these two nights the aircraft traversed different altitudes within a region of the atmosphere defined by the same set of latitude and longitude coordinates. This provided an ideal opportunity to allow flight level focused continuous wave (CW) lidar backscatter measured at 9.11-micron wavelength and modeled aerosol backscatter from two aerosol optical counters to be compared with pulsed lidar aerosol backscatter data at 1.06- and 9.25-micron wavelengths. The best agreement between all sensors was found in the altitude region below 7 km, where backscatter values were moderately high at all three wavelengths. Above this altitude the pulsed lidar backscatter data at 1.06- and 9.25-micron wavelengths were higher than the flight level data obtained from the CW lidar or derived from the optical counters, suggesting sample volume effects were responsible for this. Aerosol microphysics analysis of data near Japan revealed a strong sea-salt aerosol plume extending upward from the marine boundary layer. On the basis of sample volume differences, it was found that large particles were of different composition compared with the small particles for low backscatter conditions.

Cutten, D. R.↗

Combustion of Aerosolized Metal Particles in Microgravity

The combustion behavior and interaction effects of multiple metal particles are addressed in this project. The microgravity environment presents a unique opportunity to create an "aerosol" consisting of relatively large, 50-300 micron diameter particles, so that both cloud flame structure and individual particle combustion behavior can be characterized simultaneously. The microgravity experiments are conducted using the 2.2 s NASA Lewis Research Center drop tower. Each test includes aerosolizing metal particles under microgravity, a delay required to produce a steady aerosol, and igniting such an "aerosol" at constant pressure using a hot wire igniter. The flame structure and details of individual particle combustion are visualized using both high speed movie and regular speed video cameras. Combustion products are collected and analyzed after the experiment. A detailed description of the experimental apparatus is given elsewhere. Microgravity experiments with magnesium particle aerosols have been conducted and experiments with zirconium particles are currently in progress. A numerical, time dependent model of the flame propagation in magnesium aerosol is being developed.

Dreizin, E. L.↗

Intercomparison of Remote and Flight Level Measured Aerosol Backscatter Coefficient During GLOBE 2 Pacific Survey Mission

Aerosol backscatter coefficient data are examined from two local flights undertaken during NASA's GLObal Backscatter Experiment (GLOBE) in May - June, 1990. During each of these two flights the aircraft traversed different altitudes within a region of the atmosphere defined by the same set of latitude and longitude coordinates. This provides an ideal opportunity to allow flight level measured or modeled aerosol backscafter to be compared with pulsed lidar aerosol backscafter data that were obtained at these same altitudes either earlier or later than the flight level measurements. Aerosol backscafter comparisons were made at 1.06-, 9.11- and 9.25-mm wavelengths, using data from three lidar systems and two aerosol optical counters. The best agreement between all sensor's was found in the altitude region below 7 km where backscafter values were moderately high at all three wavelengths. Above this altitude the pulsed lidar backscafter data at 1.06- and 9.25-mm wavelengths were higher than the flight level data obtained from the CW lidar or derived from the optical counters. Possible reasons are offered to explain this discrepancy. During the Japan local flight, microphysics analysis revealed: (1) evidence of a strong advected seasalt aerosol plume from the marine boundary layer, and (2) where backscatter was low, the large lidar sampling volume included many large particles which were of different chemical composition to the small particle category sampled by the particle counters.

Cutten, D. R.↗

Aerosol Transport Over Equatorial Africa

Long-range and inter-hemispheric transport of atmospheric aerosols over equatorial Africa has received little attention so far. Most aerosol studies in the region have focussed on emissions from rain forest and savanna (both natural and biomass burning) and were carried out in the framework of programs such as DECAFE (Dynamique et Chimie Atmospherique en Foret Equatoriale) and FOS (Fires of Savanna). Considering the importance of this topic, aerosols samples were measured in different seasons at 4420 meters on Mt Kenya and on the equator. The study is based on continuous aerosol sampling on a two stage (fine and coarse) streaker sampler and elemental analysis by Particle Induced X-ray Emission. Continuous samples were collected for two seasons coinciding with late austral winter and early austral spring of 1997 and austral summer of 1998. Source area identification is by trajectory analysis and sources types by statistical techniques. Major meridional transports of material are observed with fine-fraction silicon (31 to 68 %) in aeolian dust and anthropogenic sulfur (9 to 18 %) being the major constituents of the total aerosol loading for the two seasons. Marine aerosol chlorine (4 to 6 %), potassium (3 to 5 %) and iron (1 to 2 %) make up the important components of the total material transport over Kenya. Minimum sulfur fluxes are associated with recirculation of sulfur-free air over equatorial Africa, while maximum sulfur concentrations are observed following passage over the industrial heartland of South Africa or transport over the Zambian/Congo Copperbelt. Chlorine is advected from the ocean and is accompanied by aeolian dust recirculating back to land from mid-oceanic regions. Biomass burning products are transported from the horn of Africa. Mineral dust from the Sahara is transported towards the Far East and then transported back within equatorial easterlies to Mt Kenya. This was observed during austral summer and coincided with the dying phase of 1997/98 El Nino.

Gatebe, C. K.↗

Satellite Remote Sensing of Aerosol Forcing

The role of aerosol forcing remains one of the largest uncertainties in estimating man's impact on the global climate system. One school of thought suggests that remote sensing by satellite sensors will provide the data necessary to narrow these uncertainties. While satellite measurements of direct aerosol forcing appear to be straightforward, satellite measurements of aerosol indirect forcing will be more complicated. Pioneering studies identified indirect aerosol forcing using AVHRR data in the biomass burning regions of Brazil. We have expanded this analysis with AVHRR to include an additional year of data and assimilated water vapor fields. The results show similar latitudinal dependence as reported by Kaufman and Fraser, but by using water vapor observations we conclude that latitude is not a proxy for water vapor and the strength of the indirect effect is not correlated to water vapor amounts. In addition to the AVHRR study we have identified indirect aerosol forcing in Brazil at much smaller spatial scales using the MODIS Airborne Simulator. The strength of the indirect effect appears to be related to cloud type and cloud dynamics. There is a suggestion that some of the cloud dynamics may be influenced by smoke destabilization of the atmospheric column. Finally, this study attempts to quantify remote sensing limitations due to the accuracy limits of the retrieval algorithms. We use a combination of numerical aerosol transport models, ground-based AERONET data and ISCCP cloud climatology to determine how much of the forcing occurs in regions too clean to determine from satellite retrievals.

Remer, Lorraine↗

Comparison of Aerosol Optical Properties and Water Vapor Among Ground and Airborne Lidars and Sun Photometers During TARFOX

We compare aerosol optical thickness (AOT) and precipitable water vapor (PWV) measurements derived from ground and airborne lidars and Sun photometers during TARFOX (Tropospheric Aerosol Radiative Forcing Observational Experiment). Such comparisons are important to verify the consistency between various remote sensing measurements before employing them in any assessment of the impact of aerosols on the global radiation balance. Total scattering ratio and extinction profiles measured by the ground-based NASA/GSFC Scanning Raman Lidar (SRL) system, which operated from Wallops Island, Virginia (37.86 deg N, 75.51 deg W), are compared with those measured by the Lidar Atmospheric Sensing Experiment (LASE) airborne lidar system aboard the NASA ER-2 aircraft. Bias and rms differences indicate that these measurements generally agreed within about 10%. Aerosol extinction profiles and estimates of AOT are derived from both lidar measurements using a value for the aerosol extinction/backscattering ratio S(sub a)=60 sr for the aerosol extinction/backscattering ratio, which was determined from the Raman lidar measurements.

Ferrare, R.↗

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 or 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'N, 16 deg 30'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 in 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 per sr. Comparisons of the MPL data with data from other co-located instruments showed good agreement during the dust episode.

Welton, Ellsworth J.↗

Estimation of Aerosol Direct Radiative Effects Over the Mid-Latitude North Atlantic from Satellite and In Situ Measurements

We estimate solar radiative flux changes due to aerosols over the mid-latitude North Atlantic by combining optical depths from AVHRR measurements with aerosol properties from the recent TARFOX program. Results show that, over the ocean the aerosol decreases the net radiative flux at the tropopause and therefore has a cooling effect. Cloud-free, 24-hour average flux changes range from -9 W/sq m near the eastern US coast in summer to -1 W/sq m in the mid-Atlantic during winter. Cloud-free North Atlantic regional averages range from -5.1 W/sq m in summer to -1.7 W/sq m in winter, with an annual average of -3.5 W/sq m. Cloud effects estimated from ISCCP data, reduce the regional annual average to -0.8 W/sq m. All values are for the moderately absorbing TARFOX aerosol (omega(0.55 microns) = 0.9); values for a nonabsorbing aerosol are approx. 30% more negative. We compare our results to a variety of other calculations of aerosol radiative effects.

Bergstrom, Robert W.↗

Modeling the Radiative Characteristics of Airborne Mineral Aerosols at Infrared Wavelengths

We explore the importance of the composition of airborne mineral aerosols for assessments of their direct radiative forcing at infrared wavelengths. Our calculations employing theory and data on spectral refractive indices show that the existing variations in refractive places can cause large changes in the major aerosol optical characteristics. Calculations of IR radiative forcings at the top of the atmosphere and IR downward and upward fluxes, based on an one-dimensional radiation transfer code, give a wide range of results for varying optical models of the mineral aerosols. We estimate that for a "low dust loading" scenario the changes in IR downward flux at the surface relative to dust free conditions are in the range from 7 to 14 W/sq m depending upon the mineral aerosol selected. Under "dry tropics" atmospheric conditions the IR forcing at the top of the atmosphere is in the range from 2 to 7 W/sq m. In turn, for a "high dust loading" scenario the calculated changes, relative to dust free conditions, in IR downward flux at the surface vary from 50 to 80 W/sq m , and the IR forcing at the top of the atmosphere varies from 125 W/sq m. Therefore, we conclude that incorporation of regionally and temporally varying dust mineralogical composition into general circulation models could be beneficial for decreasing the currently large uncertainties in the assessment of radiative forcing by the natural and anthropogenic components of the airborne mineral aerosols. Also the use of appropriate mineralogical data is required for remote sensing of the atmospheric aerosols using satellite infrared observations.

Sokolik, Irina N.↗