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Administrative Report on Training Awards

During the tenure of this award, the recipient (David Harker) conducted areas of research which resulted in the award of a doctorate degree (August 1999) from the University of Wyoming. The primary science activity was investigation of silicate dust mineralogy in comets, particularly comet C/1995 O1 (Hale-Bopp). Determination of the dust mineralogy permits us to address an important astrophysical question of relevance to the origins and evolution of solar systems, "Do comets contain relic interstellar dust grains? Since, comets represent the frozen reservoirs of primitive proto-solar dust and ice, we can gain insight into the problem of understanding the formation of protoplanetesimals in the. early solar nebula. Mid-infrared spectrophotometry (7 - 14 micron, R approx. = 180 - 360) of Hale-Bopp was obtained with the NASA/Ames HIFOGS at four distinct epochs pre- and post- perihelion ion from 1996 October through 1997 June. These observations were conducted at the Wyoming Infrared Observatory and the NASA Infrared Telescope Facility, and were supported by funds from this training grant. The emission at mid-IR wavelengths in cometary comae arises from carbon grains, and small silicate grains which produce resonance features. Hale-Bopp had the strongest silicate feature observed from any comet to date. Theoretical calculations utilizing Mie Scattering Theory were employed to construct Synthetic cometary spectra to fit with the observed HIFOGS 10 microns spectral feature of Hale-Bopp. Our analysis suggests that the observed spectra can be modeled with the Hanner grain size distribution peaked at alpha((sub p) = 0.2 microns of fractal porous grains with porosity parameter D = 2.5. This model spectrum also fits photometry points in the 3 - 5 microns region. Comparison with the ISO SWS spectrum of Hale-Bopp obtained 1996 October reveals that the crystalline olivine grains must be at it temperature hotter than computed from Mie theory.

Woodward, Charles E.↗

"Electrostructural Phase Changes" In Charged Particulate Clouds: Planetary and Astrophysical Implications

There is empirical evidence that freely-suspended triboelectrostatically charged particulate clouds of dielectric materials undergo rapid conversion from (nominally) monodispersed "aerosols" to a system of well-defined grain aggregates after grain motion or fluid turbulence ceases within the cloud. In United States Microgravity Laboratory Space Shuttle experiments USML-1 and USML-2, it was found that ballistically-energized grain dispersions would rapidly convert into populations of filamentary aggregates after natural fluid (air) damping of grain motion. Unless continuously disrupted mechanically, it was impossible to maintain a non-aggregated state for the grain clouds of sand-size materials. Similarly, ground- based experiments with very fine dust-size material produced the same results: rapid, impulsive "collapse" of the dispersed grains into well-defined filamentary structures. In both ground-based and microgravity experiments, the chains or filaments were created by long-range dipole electrostatic forces and dipole-induced dielectric interactions, not by monopole interactions. Maintenance of the structures was assisted by short-range static boundary adhesion forces and van der Waals interactions. When the aggregate containers in the USML experiments were disturbed after aggregate formation, the quiescently disposed filaments would rearrange themselves into fractal bundles and tighter clusters as a result of enforced encounters with one another. The long-range dipole interactions that bring the grains together into aggregates are a product of randomly-distributed monopole charges on the grain surfaces. In computer simulations, it has been shown that when the force vectors of all the random charges (of both sign) on a grain are resolved mathematically by assuming Coulombic interaction between them, the net result is a dipole moment on individual grains, even though the grains are electrically neutral insofar as there is no predominance, on their surface, of one charge sign over another. The random charges of both sign derive from natural grain-to-grain interactions that produce triboelectrification via charge exchange every time grain surfaces make contact with one another. The conversion from a random distribution of grains (upon which there are randomly distributed charges) into an organization of electrostatically-ordered aggregates, can be regarded (within the framework of granular-material science) as an "electrical or Coulombic phase change" of the particulate cloud. It is not totally dissimilar from the more normal phase-change concept in which, for example, a gas with long free-path-molecules suddenly becomes a solid as a result of structural ordering of the molecules (notably, also the result of electronic forces, albeit at a different scale). In both the gas-to-solid case, and the aerosol-to-aggregate case, the same materials and charges are present before and after the phase change, but their arrangement now has a higher degree of order and a lower-energy configuration. An input of energy into the system is required to reverse the situation. The aggregates in the USML experiments were observed to undergo at least two phase changes as noted above. The point about phase changes, and by implication, the "electrostructural" reorganizations in particulate clouds, is the following: (a) they can occur very rapidly, almost spontaneously, above a critical cloud density, (b) in going from a higher energy state to a lower energy state, they convert to a denser system, (c) energy must be required to reverse the situation, implying that energy is released during the high-to-low energy phase change. In applying this information to natural particulate clouds, some inferences can be made (it is stressed that reference is still to dielectric materials attracted by dipole forces). There are several natural settings to which the USML observations apply, and to which the phase-change implications likewise apply. Dense clouds of triboelectrically-charged, kinetically-energized grains are to be found in volcanic eruptions (particularly on earth), aeolian dust storms (particularly on Mars), meteorite impact ejecta curtains (on all planets), in "immature" debris rings around planets (e.g., that from which our own Moon may have condensed), and in gravitationally collapsing protoplanetary dust/planetesimal debris disks where dielectric granules are being increasingly brought into collisional relationships with one another (increasing both charge exchange and physical proximity). It is noted that in many of these cases, the degree of electrical charging on the grains is likely to be much higher than that in the USML experiments where charging was not enhanced above the "normal", naturally encountered level for the particular materials (quartz, glass, and various silicate minerals). Application of the phase-change concept suggests that volcanic, aeolian, and impact debris clouds may, under certain circumstances, undergo rapid, impulsive, or even catastrophic collapse into a denser state that will lead to rapid precipitation or fall-out of suspended particulates. Although this idea has been suggested previously by the author , the phase change concept possibly permits some new insights into cloud-system behavior. For example, in a protoplanetary debris disk, the work of gravity may suddenly be enhanced by electrostatically driven collapse of the system when materials reach a critical intergranular spacing or grain number density. This might reduce the rate of planet formation by orders of magnitude (considering the ratio of g-forces to electrostatic ones for very small grains in close proximity), and indeed, it might drive the collapse into a system configuration that would perhaps not be created by gravity alone. Additional information is contained in the original.

Marshall, J. R.↗

Nonprotective Alumina Growth in Sulfur-Doped NiAl(Zr)

The 1200 C oxidation behavior of NiAl was examined at various levels of sulfur and zirconium dopants to test the possibility of a critical S/Zr ratio required for adhesion. Cyclic furnace testing for 200 1 -hr cycles and interrupted testing for 500 hr were used as screening tests. Pure NiAl and NiAl(Zr) with 0. 14 at.% Zr were chosen as model base compositions; they exhibited normal, slow-growing scales (3 Mg/sq cm) with excellent adhesion for the Zr-doped alloys. NiAl with about 120 ppma S exhibited a substantial weight loss (-20 Mg/sq cm) in cyclic tests and a very large weight gain (+60 Mg/sq cm) in interrupted tests. The major surface phase remained as alpha -Al2O3. Sulfur doping the NiAl(Zr) alloy caused massive weight gains of 80 - 100 Mg/sq cm, swelling, cracking, and nearly complete conversion into NiAl2O4, and alpha- Al2O3. The initial objective of determining critical S/Zr ratios for adhesion was therefore unattainable. Initiation of the catastrophic attack was examined after a 10 hr exposure, revealing a few sites of broad, raised, and cracked ridges. In cross-section, the ridges appeared as modular intrusions, with a complex, fractal, oxide-metal interface. They were primarily alumina (with occasional entrapped islands of NiAl2O4 or pure Ni metal). They possessed a unique microstructure consisting of 0.3 microns lamellae, separated by 0.1 microns open channels. This allowed for rapid growth controlled by gaseous diffusion. The microstructure is discussed in terms of SO2 evolution and a sulfur-driven de-passivation process.

Smialek, James L.↗

MOLA-derived Roughness Data Used to Predict Surface Scattering for Mars Subsurface Radar Sounding

The Mars Express orbiter, to be launched by the European Space Agency in 2003, will carry a low-frequency radar sounding instrument, MARSIS (Mars Advanced Radar for Subsurface and Ionospheric Sounding). The primary goal of MARSIS is to map the distribution of water, both solid and (if present) liquid, in the upper several km of the martian crust. Detecting discontinuities in the crust, such as an ice-water transition, presents many challenges for a Mars orbital radar sounder. One challenge that must be overcome is the presence of radar scattering (echoes) from the surface of Mars, expected to be detected by the sounder antennas at the same time as any echoes aris-ing from subsurface interfaces. As the transmitted spherical wavefront spreads within the crust of Mars,. it also interacts with surface topography at off-nadir positions, creating a "clutter" signal that can mask the subsurface echoes. The MARSIS instrument will utilize Doppler filtering to limit the off-nadir clutter in the along-track direction, and a nadir-null secondary antenna to identify strong off-nadir clutter from the cross-track direction. To evaluate the effects of off-nadir surface clutter and the capability of these schemes to reduce the clutter, it is necessary to predict the range of scattering behavior that may be expected from martian surface topography. In this paper, we utilize Mars Orbital Laser Altimeter (MOLA) data from the current Mars Global Surveyor mission to characterize the topographic roughness of a variety of martian terrain types, at scales relevant to the MARSIS clutter problem. Segments of MOLA altimetry profiles are reduced to the topographic parameters rms slope and fractal dimension, which then are used as inputs to a near-nadir radar scattering model to predict the strength of the clutter signal. Additional information is contained in the original extended abstract.

Plaut, J. J.↗

On the Implementation of a Land Cover Classification System for SAR Images Using Khoros

The Synthetic Aperture Radar (SAR) sensor is widely used to record data about the ground under all atmospheric conditions. The SAR acquired images have very good resolution which necessitates the development of a classification system that process the SAR images to extract useful information for different applications. In this work, a complete system for the land cover classification was designed and programmed using the Khoros, a data flow visual language environment, taking full advantages of the polymorphic data services that it provides. Image analysis was applied to SAR images to improve and automate the processes of recognition and classification of the different regions like mountains and lakes. Both unsupervised and supervised classification utilities were used. The unsupervised classification routines included the use of several Classification/Clustering algorithms like the K-means, ISO2, Weighted Minimum Distance, and the Localized Receptive Field (LRF) training/classifier. Different texture analysis approaches such as Invariant Moments, Fractal Dimension and Second Order statistics were implemented for supervised classification of the images. The results and conclusions for SAR image classification using the various unsupervised and supervised procedures are presented based on their accuracy and performance.

Medina Revera, Edwin J.↗

Effective Forces Between Colloidal Particles

Colloidal suspensions have proven to be excellent model systems for the study of condensed matter and its phase behavior. Many of the properties of colloidal suspensions can be investigated with a systematic variation of the characteristics of the systems and, in addition, the energy, length and time scales associated with them allow for experimental probing of otherwise inaccessible regimes. The latter property also makes colloidal systems vulnerable to external influences such as gravity. Experiments performed in micro-ravity by Chaikin and Russell have been invaluable in extracting the true behavior of the systems without an external field. Weitz and Pusey intend to use mixtures of colloidal particles with additives such as polymers to induce aggregation and form weak, tenuous, highly disordered fractal structures that would be stable in the absence of gravitational forces. When dispersed in a polarizable medium, colloidal particles can ionize, emitting counterions into the solution. The standard interaction potential in these charged colloidal suspensions was first obtained by Derjaguin, Landau, Verwey and Overbeek. The DLVO potential is obtained in the mean-field linearized Poisson-Boltzmann approximation and thus has limited applicability. For more precise calculations, we have used ab initio density functional theory. In our model, colloidal particles are charged hard spheres, the counterions are described by a continuum density field and the solvent is treated as a homogeneous medium with a specified dielectric constant. We calculate the effective forces between charged colloidal particles by integrating over the solvent and counterion degrees of freedom, taking into account the direct interactions between the particles as well as particle-counterion, counterion-counterion Coulomb, counterion entropic and correlation contributions. We obtain the effective interaction potential between charged colloidal particles in different configurations. We evaluate two- and three-body forces in the bulk as well as study the influence of soft walls. We qualitatively explain the effects of the walls on the forces and demonstrate that many-body effects are negligible in our system. With adjustments in the parameters, the DLVO pair-potential can describe the results quantitatively. Besides electrostatic interactions, entropic depletion effects that arise from (hard-core) exclusion play an important role in determining the behavior of multi-component colloidal suspensions. A standard theory for depletion forces is due to Asakura and Oosawa and is based on the ideal gas approximation. To go beyond this approximation, we have studied entropic forces in molecular dynamics simulations of systems of hard spheres (the effects of the solvent have been ignored). The effective depletion forces for these systems can be found either from equilibrium distribution functions or from direct momentum transfer calculations. Our results obtained by either method show qualitative differences from the Asakura-Oosawa forces, indicating a longer range, higher value at contact and most importantly a more complicated structure, comprising of several maxima and minima. Our calculations include the determination of effective forces between two spheres, a hard sphere and a wall, and the behavior of a hard sphere near a step-edge and a corner. We also demonstrate that such entropic forces do not necessarily satisfy pairwise additivity.

Tehver, Riina↗

Satellite Remote Sensing of Tropical Precipitation and Ice Clouds for GCM Verification

This project, supported by the NASA New Investigator Program, has primarily been funding a graduate student, Darren McKague. Since August 1999 Darren has been working part time at Raytheon, while continuing his PhD research. Darren is planning to finish his thesis work in May 2001, thus some of the work described here is ongoing. The proposed research was to use GOES visible and infrared imager data and SSM/I microwave data to obtain joint distributions of cirrus cloud ice mass and precipitation for a study region in the Eastern Tropical Pacific. These joint distributions of cirrus cloud and rainfall were to be compared to those from the CSU general circulation model to evaluate the cloud microphysical amd cumulus parameterizations in the GCM. Existing algorithms were to be used for the retrieval of cloud ice water path from GOES (Minnis) and rainfall from SSM/I (Wilheit). A theoretical study using radiative transfer models and realistic variations in cloud and precipitation profiles was to be used to estimate the retrieval errors. Due to the unavailability of the GOES satellite cloud retrieval algorithm from Dr. Minnis (a co-PI), there was a change in the approach and emphasis of the project. The new approach was to develop a completely new type of remote sensing algorithm - one to directly retrieve joint probability density functions (pdf's) of cloud properties from multi-dimensional histograms of satellite radiances. The usual approach is to retrieve individual pixels of variables (i.e. cloud optical depth), and then aggregate the information. Only statistical information is actually needed, however, and so a more direct method is desirable. We developed forward radiative transfer models for the SSM/I and GOES channels, originally for testing the retrieval algorithms. The visible and near infrared ice scattering information is obtained from geometric ray tracing of fractal ice crystals (Andreas Macke), while the mid-infrared and microwave scattering is computed with Mie scattering. The radiative transfer is performed with the Spherical Harmonic Discrete Ordinate Method (developed by the PI), and infrared molecular absorption is included with the correlated k-distribution method. The SHDOM radiances have been validated by comparison to version 2 of DISORT (the community "standard" discrete-ordinates radiative transfer model), however we use SHDOM since it is computationally more efficient.

Evans, K. Franklin↗

Near-Nadir Radar Scattering from Venus

Analysis of Magellan altimeter data using a fractal-surface scattering model. Additional information is contained in the original extended abstract.

Campbell, Bruce A.↗

Cloud Spatial Structure and 3D Radiative Transfer

Cloud radiative properties are sensitive to drop size and other parameters of cloud micro-structure, but also to cloud shape, spacing, and other parameters of cloud macro-structure, including internal fractal structure. New information on cloud structure is being derived from a variety of cloud radars and lidars. Ongoing field programs such as DoE/ARM are improving the measurement and modelling of physical and radiative properties of clouds. A parallel effort is underway to improve cloud remote sensing, especially from the new suite of EOS (Earth Observing System) instruments which are beginning to provide higher spectral, spatial resolution, and/or angular resolution. Key parameters for improving pixel-scale retrievals are cloud thickness and photon mean-free-path, which together determine the scale of "radiative smoothing" of cloud fluxes and radiances. This scale has been observed as a change in the spatial spectrum of Landsat cloud radiances, and was also recently found with the Goddard micropulse lidar, by searching for returns from directions nonparallel to the incident beam. "Offbeam" Lidar returns are now being used to estimate the cloud "radiative Green's function", (G). G depends on cloud thickness and may be used to retrieve that important quantity. G is also being applied to improving simple estimates of cloud radiative properties that are based on the "Independent Pixel Approximation" or IPA. This and other measurements of 3D transfer in clouds, coupled with Monte Carlo and other 3D transfer methods, are beginning to provide a better understanding of the dependence of radiation on cloud inhomogeneity, and to suggest new retrieval and parameterization algorithms which take account of cloud inhomogeneity. An international "Intercomparison of 3D Radiation Codes" or I3RC, program is underway to coordinate and evaluate the variety of 3D radiative transfer methods now available, and to make them more widely available. Information is on the Web at: http://climate.gsfc.nasa.gov/I3RC. Input consists of selected cloud fields derived from data sources such as radar, microwave and satellite, and from models involved in the GEWEX Cloud Systems Studies. Output is selected radiative quantities that characterize the large-scale properties of the fields of radiative fluxes and heating. Several example cloud fields will be used to illustrate the effects of cloud inhomogeneity and 3D radiation.

Cahalan, Robert F.↗

Cloud Spatial Structure and 3D Radiative Transfer

Cloud radiative properties are sensitive to drop size and other parameters of cloud micro-structure, but also to cloud shape, spacing, and other parameters of cloud macro-structure, including internal fractal structure. New information on cloud structure is being derived from a variety of cloud radars and lidars. Ongoing field programs such as DoE/ARM (atmospheric radiation measurement) are improving the measurement and modelling of physical and radiative properties of clouds. A parallel effort is underway to improve cloud remote sensing, especially from the new suite of EOS (Earth observing system) instruments which are beginning to provide higher spectral, spatial resolution, and/or angular resolution. Key parameters for improving pixel-scale retrievals are cloud thickness and photon mean-free-path, which together determine the scale of 'radiative smoothing' of cloud fluxes and radiances. This scale has been observed as a change in the spatial spectrum of Landsat cloud radiances, and was also recently found with the Goddard micropulse lidar, by searching for returns from directions nonparallel to the incident beam. 'Offbeam' Lidar returns are now being used to estimate the cloud 'radiative Green's function' (G). G depends on cloud thickness and may be used to retrieve that important quantity. G is also being applied to improving simple estimates of cloud radiative properties that are based on the 'Independent Pixel Approximation' or IPA. This and other measurements of 3D (three dimensional) transfer in clouds, coupled with Monte Carlo and other 3D transfer methods, are beginning to provide a better understanding of the dependence of radiation on cloud inhomogeneity, and to suggest new retrieval and parameterization algorithms which take account of cloud inhomogeneity. An international 'Intercomparison of 3D Radiation Codes' (I3RC) program is underway to coordinate and evaluate the variety of 3D radiative transfer methods now available, and to make them more widely available. Information is on the Web at: http://climate.gsfc.nasa.gov/I3RC. Input consists of selected cloud fields derived from data sources such as radar, microwave and satellite, and from models involved in the GEWEX Cloud Systems Studies. Output is selected radiative quantities that characterize the large-scale properties of the fields of radiative fluxes and heating. Several example cloud fields will be used to illustrate the effects of cloud inhomogeneity and 3D radiation.

Cahalan, Robert F.↗

Grain Properties of Comet C/1995 O1 (Hale-Bopp) Deduced Through Computational Techniques

We present the computational analysis of the 7.6 - 13.2 micrometer infrared (IR) spectrophotometry (R approximately equal to 120) of comet C/1995 O1 (Hale-Bopp) in conjunction with concurrent observations which extend the spectral energy distribution from the near-infrared to far-infrared wavelengths. The observations include temporal epochs pre-perihelion, (1996 October UT and 1997 February UT), near perihelion (1997 April UT), and postperihelion (1997 June UT). Through the computational modeling of small amorphous carbon, and crystalline and amorphous silicate grains in Hale-Bopp's coma, we find that as the comet approached perihelion, the grain size distribution (the Hanner modified power law) steepened (N = 3.4 pre-perihelion, to N = 3.7 near and post-perihelion) along with an increase in the fractal porosity of larger (greater than 1 micrometer) grains. The peak of the grain size distribution remained constant (ap = 0.2 micrometer) at each epoch. We attribute the emergence of the 9.3 micrometer peak near perihelion to crystalline orthopyroxeno grains released from inside the nucleus. Crystalline silicates (olivine and orthopyroxene) make up about 30% (by mass) of the submicron sized (less than 1 micrometer) dust grains in Hale-Bopp's coma during each epoch.

Harker, David E.↗

NATO Advanced Study Institute on Spectroscopy

This booklet presents an account of the course 'Spectroscopy of Systems with Spatially Confined Structures' held in Erice-Sicily, Italy, from June 15 to June 30, 2001. This meeting was organized by the International School of Atomic and Molecular Spectroscopy of the 'Ettore Majorana' Centre for Scientific Culture. The purpose of this course was to present and discuss nanometer-scale physics, a rapidly progressing field. The top-down approach of semiconductor technology will soon meet the scales of the bottom-up approaches of supramolecular chemistry and of spatially localized excitations in ionic crystals. This course dealt with the fabrication, measurement and understanding of the relevant structures and brought together the scientific communities responsible for these development. The advances in this area of physics have already let to applications in optoelectronics and will likely lead to many more. The subjects of the course included spatially resolved structures such as quantum wells, quantum wires and quantum dots, single atoms and molecules, clusters, fractal systems, and the development of related techniques like near-field spectroscopy and confocal microscopy to study such systems.

DiBartolo, Baldassare↗

Physics of Colloids in Space-2 (PCS-2)

The Physics of Colloids-2 (PCS-2) experiment is aimed at investigating the basic physical properties of several types of colloidal suspensions. The three broad classes of colloidal systems of interest are binary colloids, colloid-polymer mixtures, and fractal gels. The objective is to understand their phase behavior as well as the kinetics of the phase transitions in the absence of gravity. The nucleation, growth, and morphology characteristics of the crystals and gels that form would be studied using confocal microscopy. These will be observed directly with excellent time resolution, and therefore extensive information about the different phases and their growth mechanisms will be gained. With the laser tweezers, it will be possible to measure the strength of these structures and to modify them in a controlled way, and the spectrophotometer will provide the possibility to probe their optical properties. We believe that this experiment will provide the basis for future 'colloid engineering' in which complicated structures with novel properties (e.g., photonic crystals) will be grown by controlled self-assembly.

Sankaran, Subramanian↗

Statistical Models of Landscape Pattern and the Effects of Coarse Resolution of Satellite Imagery on Estimation of Area

Analysis of classified satellite imagery was conducted to characterize errors in estimates of area based on coarse resolution satellite imagery which are due to distortions in sizes of small fragments, and to explore the feasibility of correcting for these errors using a statistical modeling approach. Sizes of bodies of open water on ERS-1 SAR and fire scars on Landsat MSS imagery were measured. Statistical analysis of the smaller scars and ponds as observed with this imagery of relatively fine resolution demonstrated that the distribution of the sizes could be modeled by either of two types of statistical distributions - a power distribution related to fractal processes or a simple exponential distribution. Comparison of the distribution of small bum scars as observed with Landsat to the distribution observed with AVHRR showed distortions due to the coarse spatial resolution of AVHRR caused a net overestimation of bum area. This bias was primarily caused by detection in 2 or 3 AVHRR pixels of bums whose true size was on the order of an AVHRR pixel.

Hlavka, Christine A.↗

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.↗

Stratospheric Sulfuric Acid and Black Carbon Aerosol Measured During POLARIS and its Role in Ozone Chemistry

Stratospheric aerosol can affect the environment in three ways. Sulfuric acid aerosol have been shown to act as sites for the reduction of reactive nitrogen and chlorine and as condensation sites to form Polar Stratospheric Clouds, under very cold conditions, which facilitate ozone depletion. Recently, modeling studies have suggested a link between BCA (Black Carbon Aerosol) and ozone chemistry. These studies suggest that HNO3, NO2, and O3 may be reduced heterogeneously on BCA particles. The ozone reaction converts ozone to oxygen molecules, while HNO3 and NO2 react to form NOx. Finally, a buildup of BCA could reduce the single-scatter albedo of aerosol below a value of 0.98, a critical value that has been postulated to change the effect of stratospheric aerosol from cooling to warming. Correlations between measured BCA amounts and aircraft usage have been reported. Attempts to link BCA to ozone chemistry and other stratospheric processes have been hindered by questions concerning the amount of BCA that exists in the stratosphere, the magnitude of reaction probabilities, and the scarcity of BCA measurements. The Ames Wire Impactors (AWI) participated in POLARIS as part of the complement of experiments on the NASA ER-2. One of our main objectives was to determine the amount of aerosol surface area, particularly BCA, available for reaction with stratospheric constituents and assess if possible, the importance of these reactions. The AWI collects aerosol and BCA particles on thin Palladium wires that are exposed to the ambient air in a controlled manner. The samples are returned to the laboratory for subsequent analysis. The product of the AWI analysis is the size, surface area, and volume distributions, morphology and elemental composition of aerosol and BCA. This paper presents results from our experiments during POLARIS and puts these measurements in the context of POLARIS and other missions in which we have participated. It describes modifications to the AWI data analysis procedures in which the collection of BCA is modeled as a fractal aggregate. The new analysis results in an increase in BCA surface area of approximately 24 and an increase in mass of 7-10 from the previous method. For the current study, BCA surface area is used in computer models that attempt to predict measured NOx/NOy ratios and O3 depletion rates. Inclusion of the HNO3 reaction with BCA in one model tends to improve the agreement of calculated to measured NOx/NOy ratio. However, it was found that these trends are viable only if the reactions are catalytic.

Strawa, Anthony W.↗

Stratospheric Aerosol Measurements

Stratospheric aerosols affect the atmospheric energy balance by scattering and absorbing solar and terrestrial radiation. They also can alter stratospheric chemical cycles by catalyzing heterogeneous reactions which markedly perturb odd nitrogen, chlorine and ozone levels. Aerosol measurements by satellites began in NASA in 1975 with the Stratospheric Aerosol Measurement (SAM) program, to be followed by the Stratospheric Aerosol and Gas Experiment (SAGE) starting in 1979. Both programs employ the solar occultation, or Earth limb extinction, techniques. Major results of these activities include the discovery of polar stratospheric clouds (PSCs) in both hemispheres in winter, illustrations of the impacts of major (El Chichon 1982 and Pinatubo 1991) eruptions, and detection of a negative global trend in lower stratospheric/upper tropospheric aerosol extinction. This latter result can be considered a triumph of successful worldwide sulfur emission controls. The SAGE record will be continued and improved by SAGE III, currently scheduled for multiple launches beginning in 2000 as part of the Earth Observing System (EOS). The satellite program has been supplemented by in situ measurements aboard the ER-2 (20 km ceiling) since 1974, and from the DC-8 (13 km ceiling) aircraft beginning in 1989. Collection by wire impactors and subsequent electron microscopic and X-ray energy-dispersive analyses, and optical particle spectrometry have been the principle techniques. Major findings are: (1) The stratospheric background aerosol consists of dilute sulfuric acid droplets of around 0.1 micrometer modal diameter at concentration of tens to hundreds of monograms per cubic meter; (2) Soot from aircraft amounts to a fraction of one percent of the background total aerosol; (3) Volcanic eruptions perturb the sulfuric acid, but not the soot, aerosol abundance by several orders of magnitude; (4) PSCs contain nitric acid at temperatures below 195K, supporting chemical hypotheses implicating manmade fluorocarbons as cause of the --'ozone hole'; (5) The current soot loading is too small to be of environmental (radiative and chemical) consequence. However, the fractal nature of soot distinguishes it aerodynamically and radiatively from sulfuric acid droplets such that its stratospheric residence time is longer, mainly because of vertical transport against gravity due to gravito-photophoretic forces. Thus it may accumulate and become of environmental concern in the future.

Pueschel, Rudolf, F.↗

Scale Dependence of Statistics of Spatially Averaged Rain Rate Seen in TOGA COARE Comparison with Predictions from a Stochastic Model

A characteristic feature of rainfall statistics is that they in general depend on the space and time scales over which rain data are averaged. As a part of an earlier effort to determine the sampling error of satellite rain averages, a space-time model of rainfall statistics was developed to describe the statistics of gridded rain observed in GATE. The model allows one to compute the second moment statistics of space- and time-averaged rain rate which can be fitted to satellite or rain gauge data to determine the four model parameters appearing in the precipitation spectrum - an overall strength parameter, a characteristic length separating the long and short wavelength regimes and a characteristic relaxation time for decay of the autocorrelation of the instantaneous local rain rate and a certain 'fractal' power law exponent. For area-averaged instantaneous rain rate, this exponent governs the power law dependence of these statistics on the averaging length scale $L$ predicted by the model in the limit of small $L$. In particular, the variance of rain rate averaged over an $L \times L$ area exhibits a power law singularity as $L \rightarrow 0$. In the present work the model is used to investigate how the statistics of area-averaged rain rate over the tropical Western Pacific measured with ship borne radar during TOGA COARE (Tropical Ocean Global Atmosphere Coupled Ocean Atmospheric Response Experiment) and gridded on a 2 km grid depends on the size of the spatial averaging scale. Good agreement is found between the data and predictions from the model over a wide range of averaging length scales.

Kundu, Prasun K.↗