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NASA NTRS1993

Shock-induced devolatization of calcium sulfate and implications for K-T extinctions

Calcium sulfate devolatization during the impact at Chicxulub, Mexico and dispersal in the stratosphere of the resultant sulfuric acid aerosol have been suggested as a possible mechanism for the Cretaceous-Tertiary extinctions. In this paper, we investigated two shock-induced devolatization reactions of calcium sulfate up to 42 GPa in the laboratory: CaSO4 + SiO2 yields CaSiO3 + SO3(degassed) and CaSO4 yields CaO + SO2(degassed) + 1/2 O2(degassed). We found both to proceed to a much less extent than calculated by equilibrium thermodynamic calculations. Reaction products are found to be 10(exp -2) times those calculated for equilibrium. Consequently our estimate of the amount of sulfur oxides degassed into the atmosphere from shock devolatization of CaS04 in the Chicxulub lithographic section (6x10(exp 15)-2x10(exp 16)g in sulfur mass) is lower by a factor of 70 to 400 than previous estimates; the related environmental stress arising from the resultant global cooling of approximately 4 K and fallout of acid rain does not appear to suffice to explain the widespread K-T extinctions.

Chen, Guangqing↗
NASA NTRS1994

Surface ices in the outer solar system

Planetary volatile inventories are products of several factors: (1) condensation-accretion of pre-planetary material which determines the bulk volatile inventory; (2) energy history of a planet, including timing, causes, and mechanisms of degassing; (3) the volatile sinks, including temporary, long term, and permanent; and (4) external processes operating on the volatile inventory. Information regarding the current surface compositions provide insight into both internal and surface-atmosphere evolutionary history. Our discussion focuses upon the surface composition of outer solar system planets and satellites as determined by spacecraft and telescopic spectral observations. We provide a review and an update of the recent work by Cruikshank and Brown that includes more recent observations and interpretations. In the context of formation and evolution of solar system bodies, the interesting ices typically considered are simple molecules formed from elements having high cosmic abundances. These mainly include ices of H2O, NH3, SO2, H2S, CH4, CO, CO2, and N2. In the solid state, these ices have vibrational spectral features, analogous to their gaseous counterparts but rotational transitions are quenched, that lie in the near- and mid-infrared. The overtone and combination modes, occurring in the visible and near-IR region, are of particular importance as standard observational techniques used to identify these ices rely upon reflected solar energy. Table I summarizes the ices found on various bodies in the outer solar system. H2O is most abundant surface material in the inner and middle regions while more volatile species appear to dominate surfaces in the outermost edge of the outer solar system.

Roush, Ted L.↗
NASA NTRS1993

Remote sensing of smoke, clouds, and fire using AVIRIS data

Clouds remain the greatest element of uncertainty in predicting global climate change. During deforestation and biomass burning processes, a variety of atmospheric gases, including CO2 and SO2, and smoke particles are released into the atmosphere. The smoke particles can have important effects on the formation of clouds because of the increased concentration of cloud condensation nuclei. They can also affect cloud albedo through changes in cloud microphysical properties. Recently, great interest has arisen in understanding the interaction between smoke particles and clouds. We describe our studies of smoke, clouds, and fire using the high spatial and spectral resolution data acquired with the NASA/JPL Airborne Visible/Infrared Imaging Spectrometer (AVIRIS).

Gao, Bo-Cai↗
NASA NTRS1995

MODTRAN3: An update and recent validations against airborne high resolution interferometer measurements

MODTRAN, the Moderate Resolution Atmospheric Radiance and Transmittance Model, encompasses all the capabilities of LOWTRAN 7, the widely used 20 cm(exp -1) resolution radiance code, but incorporates a much more sensitive molecular band model with 2 cm(exp -1) resolution. MODTRAN contains many important elements that other band model based radiative transfer codes do not incorporate. It shares with FASCODE: spherical geometry, single and multiple scattering default atmospheric profile descriptors (gases, aerosols, clouds, fogs, and rain), and molecular continua (H2O, CO2, O3, O2, N2). In addition, it can calculate the solar/lunar direct and scattered radiation. MODTRAN3 was released to the general public in November 1994. It has several important features that the previous version, MODTRAN2, does not have. Chloro-fluorocarbon (CFC) and related heavy molecules (whose spectroscopic properties first appear on the HITRAN92 data base as temperature-dependent cross sections) have been incorporated into pseudo-band models, with provision for using both default and user supplied profiles. The addition of SO2 and O2 in the UV, along with upgraded ozone Chappuis bands in the visible is also part of MODTRAN3. An improved multiple scattering algorithm, the DIScrete Ordinate Radiative Transfer (DISORT) has also been incorporated into MODTRAN3. MODTRAN is very fast: simple timing runs of MODTRAN3 vs. FASCOD3 show an improvement of more than a factor of 100 for a typical 500 cm(exp -1) spectral interval and comparable vertical layering. Speed is an important consideration in heating/cooling rates calculations, where a large number of radiative transfer calculations are needed. The MODTRAN3 used in this study is based on HITRAN92, but as mentioned, above, it will be upgraded to HITRAN94 upon its release at the end of 1994. MODTRAN has been adopted by: some researchers in the AVIRIS program as one radiative transfer code to derive surface reflectance from AVIRIS measurements. The accuracy of the code is very important because any errors in the radiative transfer calculation will directly translate into errors in the derived surface reflectance. In this paper, the new solar irradiance calculated by Kurucz, which is adopted in MODTRAN3, will be presented. Recent validations of MODTRAN3 with airborne high resolution interferometer measurements over ocean will be discussed. Good agreeement between model calculations and measurements was achieved.

Anderson, Gail P.↗
NASA NTRS1995

Analyses of TIMS and AVIRIS data, integrated with field and laboratory spectra, for lithological and mineralogical interpretation of Vulcano Island, Italy

Vulcano Island is part of the Eolian archipelago, located about 25 km from the northeast coast of Sicily. The archipelago comprises seven major volcanic islands, two of which are active volcanoes (Vulcano and Stromboli). Vulcano covers an area of about 50 square km, and is about 10 km long. Explosive volcanic activity has predominated in the geological evolution of Vulcano Island, and there is no evidence that this pattern has ceased. Rather, the current situation is one of unrest, so a strict regimen of continuous geophysical and geochemical monitoring has been undertaken over the last decade. Though the year-round population of Vulcano is small (under 1000), during the summer the island becomes a very popular resort, and has thousands of additional tourists at any time throughout the high season, thus substantially increasing the number of people potentially at risk from an explosive eruption or other hazards such as noxious gas emissions (e.g., CO2, H2S, SO2). During the past ten years, remote sensing data have been repetitively acquired with optical and microwave airborne sensors. The present work shows the preliminary results of a study based on the integration of various remote sensing data sets with field spectroscopy, and other laboratory analyses, for the geological and geomorphological mapping of the island. It is hoped that such work will also usefully contribute to the evaluation of the volcanic hazard potential of the islands as well as to the evaluation of the status of its current activity.

Buongiorno, M. Fabrizia↗
NASA NTRS1993

Condensation and vaporization studies of CH3OH and NH3 ices: Major implications for astrochemistry

In an extension of previously reported work on ices containing H2O, CO, CO2, SO2, H2S, and H2, we present measurements of the physical and infrared spectral properties of ices containing CH3OH and NH3. The condensation and sublimation behavior of these ice systems is discussed and surface binding energies are presented for all of these molecules. The surface binding energies can be used to calculate the residence times of the molecules on grain surfaces as a function of temperature. It is demonstrated that many of the molecules used to generate radio maps of and probe conditions in dense clouds, for example CO and NH3, will be significantly depleted from the gas phase by condensation onto dust grains. Attempts to derive total column densities solely from radio maps that do not take condensation effects into account may vastly underestimate the true column densities of any given species. Simple CO condensation onto and vaporization off of grains appears to be capable of explaining the observed depletion of gas phase CO in cold, dense molecular cores. This is not the case for NH3, however, where thermal considerations alone predict that all of the NH3 should be condensed onto grains. The fact that some gas phase NH3 is observed indicates that additional desorption processes must be involved. The surface binding energies of CH3OH, in conjunction with this molecule's observed behavior during warm up in H2O-rich ices, is shown to provide an explanation of the large excess of CH3OH seen in many warm, dense molecular cores. The near-infrared spectrum and associated integrated band strengths of CH3OH-containing ice are given, as are middle infrared absorption band strengths for both CH3OH and NH3.

Sandford, Scott A.↗
NASA NTRS1994

Ozone within the El Chichon aerosol cloud inferred from solar backscatter ultraviolet continuous-scan measurements

Large amounts of SO2 injected into the stratosphere by the El Chichon volcanic eruption greatly enhanced the sulfuric acid aerosol loading. According to laboratory studies, the increase in aerosol surface area would lead to a loss of ozone. Radiation measurements from the solar backscatter ultraviolet spectroradiometer are used to probe the absorbing and scattering properties of the stratosphere after the eruption. The backscattered radiation is enhanced for wavelengths greater than 290 nm, with a peak at about 302 nm. The enhancements associated with aerosol backscattering and ozone change can be separated. A decrease in column ozone of 8 to 30 Dobson units was deduced within the aerosol layer at an altitude between 20 and 30 km following the month of the eruption.

Wen, Guoyong↗
NASA NTRS1994

The impact of high altitude aircraft on the ozone layer in the stratosphere

The paper discusses the potential effects on the ozone layer of gases released by the engines of proposed high altitude supersonic aircraft. The major problem arises from the emissions of nitrogen oxides which have the potential to destroy significant quantities of ozone in the stratosphere. The magnitude of the perturbation is highly dependent on the cruise altitude of the aircraft. Furthermore, the depletion of ozone is substantially reduced when heterogeneous conversion of nitrogen oxides into nitric acid on sulfate aerosol particles is taken into account in the calculation. The sensitivity of the aerosol load on stratospheric ozone is investigated. First, the model indicates that the aerosol load induced by the SO2 released by aircraft is increased by about 10-20% above the background aerosols at mid-high latitude of the Northern Hemisphere at 15 km for the NASA emission scenario A (the NASA emission scenarios are explained in Tables I to III). This increase in aerosol has small effects on stratospheric ozone. Second, when the aerosol load is increased following a volcanic eruption similar to the eruption of El Chichon (Mexico, April 1982), the ozone column in spring increases by as much as 9% in response to the injection of NOx from the aircraft with the NASA emission scenario A. Finally, the modeled suggests that significant ozone depletion could result from the formation of additional polar stratospheric clouds produced by the injection of H2O and HNO3 by the aircraft engines.

Tie, Xue XI↗
NASA NTRS1994

Shock-induced devolatilization of calcium sulfate and implications for K-T extinctions

The devolatilization of calcium sulfate, which is present in the target rock of the Chicxulub, Mexico impact structure, and dispersal in the stratosphere of the resultant sulfuric acid aerosol have been suggested as a possible mechanism for the Cretaceous-Tertiary extinctions. We measured the amount of SO2 produced from two shock-induced devolatilization reactions of calcium sulfate up to 42 GPa in the laboratory. We found both to proceed to a much lower extent than calculated by equilibrium thermodynamic calculations. Reaction products are found to be approx. 10(exp -2) times those calculated for equilibrium. Upon modeling the quantity of sulfur oxides degassed into the atmosphere from shock devolatilization of CaSO4 in the Chicxulub lithographic section, the resulting 9 x 10(exp 16) to 6 x 10(exp 17) g (in sulfur mass) is lower by a factor of 10-100 than previous upper limit estimates, the related environmental stress arising from the resultant global cooling and fallout of acid rain is insufficient to explain the widespread K-T extinctions.

Chen, Guangqing↗
NASA NTRS1994

Observation of hydration of single, modified carbon aerosols

We have compared the hydration behavior of single carbon particles that have been treated by exposure to gaseous H2SO4 with that of untreated particles. Untreated carbon particles did not hydrate as the relative humidity varied from 0 to 80% at 23 C. In contrast, treated particles hydrated under subsaturation conditions; mass increases of up to 30% were observed. The mass increase is consistent with sulfuric acid equilibration with the ambient relative humidity in the presence of inert carbon. For the samples studied, the average amount of absorbed acid was 14% +/- 6% by weight, which corresponds to a surface coverage of approximately 0.1 monolayer. The mass fraction of surface-absorbed acid is comparable to the soluble mass fraction observed by Whitefield et al. (1993) in jet aircraft engine aerosols. Estimates indicate this mass fraction corresponds to 0.1% of the available SO2 exiting an aircraft engine ending up as H2SO4 on the carbon aerosol. If this heterogeneous process occurs early enough in the exhaust plume, it may compete with homogeneous nucleation as a mechanism for producing sulfuric acid rich aerosols.

Wyslouzil, B. E.↗
NASA NTRS1993

Operational overview of the NASA GTE/CITE 3 airborne instrument intercomparisons for sulfur dioxide, hydrogen sulfide, carbonyl sulfide, dimethyl sulfide, and carbon disulfide

This paper reports the overall experimental design and gives a brief overview of results from the third airborne Chemical Instrumentation Test and Evaluation (CITE 3) mission conducted as part of the National Aeronautics and Space Administration's Global Tropospheric Experiment. The primary objective of CITE 3 was to evaluate the capability of instrumentation for airborne measurements of ambient concentrations of SO2, H2S, CS, dimethyl sulfide, and carbonyl sulfide. Ancillary measurements augmented the intercomparison data in order to address the secondary objective of CITE 3 which was to address specific issues related to the budget and photochemistry of tropospheric sulfur species. The CITE 3 mission was conducted on NASA's Wallops Flight Center Electra aircraft and included a ground-based intercomparison of sulfur standards and intercomparison/sulfur science flights conducted from the NASA Wallops Flight Facility, Wallops Island, Virginia, followed by flights from Natal, Brazil. Including the transit flights, CITE 3 included 16 flights encompassing approximately 96 flight hours.

Hoell, James M., Jr.↗
NASA NTRS1994

Physical and chemical structure of the IC 63 nebula. 1: Millimeter and far-infrared observations

We present results of a (sub)millimeter and far-infrared study of the reflection/emission nebula IC 63, located close to the BO.5p star gamma Cas. The source has been mapped in the (12)CO 2 - 1 and 3 - 2, (13)CO 2 - 1, and CS 2 - 1 lines and shows a small molecular cloud less than 1'x 2' in extent, which coincides with the brightest optical nebulosity and IRAS 100 micrometer emission. IC 63 is therefore an excellent example of a nearby (d approximately = 230 pc), edge-on photon-dominated region (PDR). Various other molecules have been observed at the peak position through their rotational transitions, in order to probe the physical parameters and to derive abundances. The measured CO, HCO(+) HCN, CS and H2CO line ratios suggest that the cloud is warm, T approximately = 50 K, and dense, n (H2) approximately = 5 x 10(exp 4)/cu cm. Excitation of molecules by electrons may play a significant role in this PDR. On the basis of these physical conditions, column densities have been determined from the observed line strengths. Several different methods are discussed to constrain the H2 column density, including the use of measured submillimeter continuum fluxes. The resulting abundances of species such as CN and CS are similar to those found in cold, dark clouds like TMC-1 and L134N. However, the abundances of other simple molecules such as HNC, HCO(+) and possibly C2H are lower by factors of at least three, probably because of the enhanced photodissociation rates at a distance of 1.3 pc from a B star. Surprisingly, only the abundance of the H2S molecule appears enhanced. More complex, volatile molecules such as CH3OH CH3CN and HNCO, and the sulfur-oxides SO and SO2 have not been found in this cloud. Limited observations of molecules in the reflection nebulea NGC 2023 are presented as well, and the resulting molecular abundances are compared with those found for IC 63.

Jansen, David J.↗
NASA NTRS1994

Formation of Na-containing molecular ions at Io

Fast sodium atoms, which appear to be associated with the motion of the magnetic 'field lines' downstream from Io (Schneider et al. 1991), are thought to be produced by dissociation of NaX(+) in Io's plasma torus. It was suggested that these molecular ions are formed near Io's exobase by electron-impact ionization and picked up be the corotating filed lines (Wilson and Schneider 1994). Because electron cooling processes dominate electron-impact ionization in Io's corona, two reactions are suggested here as sources of NaX(+) and, hence, as the ultimate sources of the observed fast Na. First, the charge-exchange cross sections for forming NaX(+) are shown to be large for plasma torus ions (O(+), S(+), O(2+), S(3+)) colliding with NaX molecules in Io's corona. Sputtering from the surface (Chrisey et al. 1988) and rapid transport to the exobase is a potential source of NaX, where X is O,S, Na, or a molecular species such as NaS or O2. Second ions of the more abundant molecules (e.g., SO(+), SO2(+), O2(+), and S2(+)) can react efficiently with atomic Na in Io's corona to form NaX(+). Here cross sections are estimated for these two processes, as well as for charge exchange in O(+) and S(+) on Na collisions.

Johnson, R. E.↗
NASA NTRS1995

The effect of plasma heating on sublimation-driven flow in Io's atmosphere

The atmospheric flow on Io is numerically computed in a flat 2-D axisymmetric geometry for a sublimation atmosphere on the trailing hemisphere subjected to plasma bombardment, UV heating, and IR cooling. Calculations are performed for subsolar vapor pressures of approximately 6.5 x 10(exp -3) Pa (approximately 3 x 10(exp 18) SO2/sq cm) and 6.8 x 10(exp -4) Pa (approximately 4 x 10(exp 17) SO2/sq cm); the latter approximates the vapor pressure of F. P. Fanale et al. (1982). The amount of plasma energy deposited in the atmosphere is 20% of the plasma flow energy due to corotation (J. A. Linker et al., 1988). It is found that plasma heating significantly inflates the upper atmosphere, increasing both the exobase altitude and the amount of surface covered by more than an exospheric column of gas. This in turn controls the supply of the Io plasma torus (M. A. McGrath and R. E. Johnson, 1987). The horizontal flow of mass and energy is also important in determining the exobase altitude; and it is shown that IR cooling can be important, although our use of the equilibrium, cool-to-space approximation for a pure SO2 gas (E. Lellouch et al., 1992) may overestimate this effect. The calculated exobase altitudes are somewhat lower than those suggested by McGrath and Johnson (1987) for supplying the torus, indicating the details of the plasma energy deposition and sputter ejection rate near the exobase, as well as the IR emission from this region need to be examined. In addition, the molecules sublimed (or sputtered) from the surface are transported to the exobase in times short compared to the molecular photodissociation time. Therefore, the exobase is dominated by molecular species and the exobase is supplied by a small region of the surface.

Wong, Mau C.↗
NASA NTRS1995

Global tropospheric experiment at the Hong Kong Atmosphere Chemistry Measurement Station

The major activities of the Global Tropospheric Experiment at the Hong Kong Atmospheric Chemistry Measurement Station are presented for the period 1 January - 31 December 1995. Activities included data analysis, reduction, and archiving of atmospheric measurements and sampling. Sampling included O3, CO, SO2, NO, TSP, RSP, and ozone column density. A data archive was created for the surface meteorological data. Exploratory data analysis was performed, including examination of time series, frequency distributions, diurnal variations and correlation. The major results have been or will be published in scientific journals as well as presented at conferences/workshops. Abstracts are attached.

Carroll, Mary Ann↗
NASA NTRS1995

Charged Particle Alterations of Surfaces in the Solar System

The surfaces of 'airless' bodies in the solar system are exposed to the ambient plasma, micrometeorites, and the solar UV. The effects of these space weathering agents on surfaces in the solar system has been studied in this project. In the last three years work was carried out on volatile depletion at Mars, on sputtering of the lunar surface, on absorption by implanted S in vapor-deposited H2O and its relevance to observations of Europa's surface in the UV, and on the spectral changes produced on irradiating SO2 and its possible relevance to Io. In addition, the role of plasma-induced charging of E-ring grains was evaluated because of its relevance to E-ring particle source and the lifetime of the E-ring. Finally, the detection of sputtered material from Dione by the CAPS instrument on CASSINI was evaluated as a tool for analysis of satellite surface composition, and the role of sputtering on the ambient OH in the vicinity of the ice satellites and the E-ring was evaluated.

Johnson, R. E.↗
NASA NTRS1996

An Experimental Study of Atmospheric Homogeneous Nucleation: Cluster Growth and Gas-Particle Reactions of H2SO4

The work proposed on this project included both field and laboratory studies. The laboratory studies were to consist of measurements of H2SO4 uptake and evaporation from aerosols of varying chemical composition, while the field component would include measurements of H2SO4 and other compounds which would be conducted as part of a large field campaign. By chance, the opportunity to conduct such an H2SO4/aerosol/ultrafine particle study in conjunction with an OH intercomparison/photochemistry study became available very early in this project (September 1993). This study was conducted at Caribou, Colorado in conjunction with several other groups from NCAR, NOAA and a number of universities. Our group measured OH, H2SO4, SO2, and H20, while Dr. McMurfy's group measured ultrafine particles, and total particle number and size distribution. In addition measurements of HO2/RO2, O3, NO, NO2, NO(y) CO, hydrocarbons, CH2O, and other chemical compounds and meteorological parameters were performed by the other participants and a new laser oblation/mass spectrometry technique was also employed by the NOAA Aeronomy Laboratory to study aerosol composition. The study of aerosol production and growth in conjunction with photochemical measurements is highly advantageous because particle growth precursors such as H2SO4.or MSA are formed by OH initiated sulfur oxidation. The large number of hydrocarbon measurements included in this study were also important in understanding particle growth.

Eisele, F. L.↗
NASA NTRS1996

Workshop on Evolution of Martian Volatiles

This volume contains papers that were presented on February 12-14, 1996 at the Evolution for Martian Volatiles Workshop. Topics in this volume include: returned Martian samples; acidic volatiles and the Mars soil; solar EUV Radiation; the ancient Mars Thermosphere; primitive methane atmospheres on Earth and Mars; the evolution of Martian water; the role of SO2 for the climate history of Mars; impact crater morphology; the formation of the Martian drainage system; atmospheric dust-water ice Interactions; volatiles and volcanos; accretion of interplanetary dust particles; Mars' ionosphere; simulations with the NASA Ames Mars General Circulation Model; modeling the Martian water cycle; the evolution of Martian atmosphere; isotopic composition; solar occultation; magnetic fields; photochemical weathering; NASA's Mars Surveyor Program; iron formations; measurements of Martian atmospheric water vapor; and the thermal evolution Models of Mars.

Jakosky, B.↗