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At least 91 records · Page 5

Effects of the Mount Pinatubo eruption on the radiative and chemical processes in the troposphere and stratosphere

The Lawrence Livermore National Laboratory two-dimensional zonally-averaged chemical-radiative-transport model of the global atmosphere was used to study the effects of the 15 June 1991 eruption of the Mt. Pinatubo volcano on stratospheric processes. SAGE 2 time-dependent aerosol surface area density and optical extinction data were used as input into the model. By 22 December 1991, a maximum equatorial change of -1.8 percent in column ozone was derived from heterogeneous chemical processes that convert NO(x) into HNO3 on sulfuric acid aerosols. Radiative feedbacks from increased aerosol optical thickness independently changes column ozone by approximately -3.5 percent for the same period. This occurs from increasing the net heating of the lower stratosphere, which indirectly increases chemical reaction rates via their temperature dependence and from changes in actinic fluxes, which directly modify photodissociation rates. Including both heterogeneous and radiative effects changes column ozone by -5.5 percent. The model-derived change overestimates the decrease in column ozone relative to the TOMS instrument on the Nimbus 7 satellite. Maximum local ozone decreases of 12 percent were derived in the equatorial region, at 25 km. Model-derived column NO2 peaked (-14 percent) at 30 deg S in October 1991. The timing of the NO2 peak is consistent with observation, but the model underestimates the magnitude of the decrease. Local concentrations of NO(x) (NO + NO2), ClO(x) (Cl + ClO), and HO(x) (OH + HO2), in the lower stratosphere between 30 deg S and 30 deg N, were calculated to have changed by -40 percent, +100 to +160 percent, and +120 to +140 percent respectively.

Kinnison, Douglas E.↗

Measurements of the composition of aerosol component of Venusian atmosphere with Vega 1 lander, preliminary data

Preliminary investigation of mass spectra of gaseous products of pyrolyzed Venusian cloud particles collected and analyzed by the complex device of mass-spectrometer and collector pyrolyzer on board Vega 1 lander revealed the presence of heavy particles in the upper cloud layer. Based on 64 amu peak (SO2+), an estimate of the lower limit of the sulfuric acid aerosol content at the 62 to 54 km heights of approximately 2.0 mg/cu m is obtained. A chlorine line (35 and 37 amu) is also present in the mass spectrum with a lower limit of the chlorine concentration of approximately 0.3 mg/ cu m.

Surkov, Y. A.↗

The atmospheric effects of El Chichon

The eruption of the Mexican volcano El Chichon in late March and early April of 1982 injected an unusually large amount of volcanic material into the stratosphere. This event demonstrates for the first time that a relatively small but sulfur-rich volcanic eruption can produce a dense, widespread stratospheric cloud. Sulfuric acid aerosol is formed by the photochemical reaction of sulfur gases released by a volcano with water vapor in the atmosphere. The aerosol causes a decrease in the mean global temperature because the droplets both absorb solar radiation and scatter it back into space. Attention is given to details concerning the volcanic eruption, the relation of El Chichon to the Mexican and Guatemalan volcanic belts, sources for the sulfur erupted by the volcano, and the mechanisms involved in the formation of sulfuric acid.

Rampino, M. R.↗

Southern Hemisphere Lidar Measurements of the Aerosol Clouds from Mt. Pinatubo and Mt. Hudson

On 19 Jul., 1991, during tests to determine the ability of the newly-modified CSIRO Ns:YAG lidar to measure signals from the stratosphere before the arrival of dust from the eruption of Mt. Pinatubo, a strongly scattering layer was detected at an altitude of 2 km. That evening, the spectacular sunset and twilight were typical of volcanically disturbed conditions. Lidar measurements at 532 nm were made between 1400 and 1500 EST (0400-0500 UT) on 19 Jul. through broken cloud. Approximately 3800 laser firings were averaged in 256 shot blocks. These and subsequent data have been analyzed to produce profiles of aerosol volume backscatter function and scattering ratio. Clouds again prevented a clear view of the twilights on the next two nights, although there was some evidence for an enhanced glow. The evidence suggested that the aerosol layer had disappeared. An explanation for this disappearance and the earlier than expected arrival of the layer over Melbourne was required. Nimbus 7 TOMS data for 23 Jun. showed that the SO2 from the eruption had extended at least 11000 km to the west and that the southern boundary of the cloud had reached 15 degrees S just 8 days after the climactic eruption. It can be assumed that this cloud also contained dust and sulphuric acid aerosol. It was proposed that a section had then been broken away from the main cloud and carried south by a large scale eddy between the low latitude easterlies and the strong mid-latitude westerlies which finally carried the aerosol cloud over southern Australia. Accompanying 30 mb wind data showed a counter clockwise circulation, responsible for the transport, located in the South Atlantic Ocean.

Young, Stuart A.↗

Effects on stratospheric ozone from high-speed civil transport: Sensitivity to stratospheric aerosol loading

The potential impact of high-speed civil transport (HSCT) aircraft emissions on stratospheric ozone and the sensitivity of these results to changes in aerosol loading are examined with a two-dimensional model. With aerosols fixed at background levels, calculated ozone changes due to HSCT aircraft emissions range from negligible up to 4-6% depletions in column zone at northern high latitudes. The magnitude of the ozone change depends mainly on the NO(x) increase due to aircraft emissions, which depends on fleet size, cruise altitude, and engine design. The partitioning of the odd nitrogen species in the lower stratosphere among NO, NO2, N2O5, is strongly dependent on the concentration of sulfuric acid aerosol particles, and thus the sensitivity of O3 to NO(x) emissions changes when the stratospheric aerosol loading changes. Aerosol concentrations 4 times greater than background levels have not been unusual in the last 2 decades. Our model results show that a factor of 4 increase in aerosol loading would significantly reduce the calculated ozone depletion due to HSCT emissions. Because of the neutral variabiltiy of stratospheric aerosols, the possible impact of HSCT emissions on ozone must be viewed as a range of possible results.

Weisenstein, Debra K.↗

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↗

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↗

Studies of exhaust products from solid propellant rocket motors fired in an environmental chamber

Experiments are described in which it was attempted to define the state of HCl when rocket motors using ammonium perchlorate and powdered aluminum filler in the fuel system are fired under various relative humidity conditions. A small, variable load rocket motor was developed so that controlled quantities of exhaust products could be produced in an environmental chamber. A technique is described for distinguishing the difference between HCl existing as a gas or existing as an acid aerosol.

Dawbarn, R.↗

An improved Venus cloud model

An inhomogeneous cloud model for Venus is presented in which a (transparent) sulfuric acid aerosol extends above the tropopause, but an (absorbing) sulfur aerosol consisting of much larger particles does not. It is shown that the temperature dependence of the absorption spectrum of sulfur, combined with the lapse rate in the planet's atmosphere, can explain the color of Venus. A simple 'black-white' radiative-transfer model is developed, the spectral reflectance of the cloud model is computed for the 60-km level in Marov's (1972) model atmosphere, and strong evidence is obtained that sulfur is the UV absorber on Venus. The wavelength variation of contrast in UV cloud features is analyzed, and absorption is found to increase with depth at every wavelength due to the inward increase in temperature. The black-white model is applied to CO2 absorption, variations in CO2 and UV absorption with phase angle are compared, and line profiles are calculated for pressure-broadened CO2 lines. The theoretical results are compared with Venera 9 and 10 data.

Young, A. T.↗

Adsorption and chemical reaction of gaseous mixtures of hydrogen chloride and water on aluminum oxide and application to solid-propellant rocket exhaust clouds

Hydrogen chloride (HCl) and aluminum oxide (Al2O3) are major exhaust products of solid rocket motors (SRM). Samples of calcination-produced alumina were exposed to continuously flowing mixtures of gaseous HCl/H2O in nitrogen. Transient sorption rates, as well as maximum sorptive capacities, were found to be largely controlled by specific surface area for samples of alpha, theta, and gamma alumina. Sorption rates for small samples were characterized linearly with an empirical relationship that accounted for specific area and logarithmic time. Chemisorption occurred on all aluminas studied and appeared to form from the sorption of about a 2/5 HCl-to-H2O mole ratio. The chemisorbed phase was predominantly water soluble, yielding chloride/aluminum III ion mole ratios of about 3.3/1 suggestive of dissolved surface chlorides and/or oxychlorides. Isopiestic experiments in hydrochloric acid indicated that dissolution of alumina led to an increase in water-vapor pressure. Dissolution in aqueous SRM acid aerosol droplets, therefore, might be expected to promote evaporation.

Cofer, W. R., III↗

Hydrogen chloride partitioning in a Titan III exhaust cloud diluted with ambient air

Measurements and analysis are presented of the partitioning of HCl between hydrochloric acid aerosol and gaseous HCl in a Titan III exhaust cloud, as the cloud is diluted with humid ambient air. Partitioning was determined by measuring the gaseous HCl concentration with a recently developed airborne Gas Filter Correlation detector and simultaneously with a chemiluminescence detector which measures total HCl. Although equilibrium predictions for HCl aerosol formation indicated that no HCl aerosol should exist in the exhaust cloud for the meteorological conditions of this launch, the measurements indicated significant HCl aerosol formation. These measurements will provide verification for advanced modeling programs now under development.

Sebacher, D. I.↗

COS in the stratosphere

Carbonyl sulfide (COS) has been detected in the stratosphere, and mixing ratio measurements are reported for altitudes of 15.2 to 31.2 km. A large volume, cryogenic sampling system mounted on board a U-2 aircraft has been used for lower stratosphere measurements and a balloon platform for measurement at 31.2 km. These observations and measurements strongly support the concept that stratospheric COS is an important precursor in the formation of sulfuric acid aerosols.

Inn, E. C. Y.↗

The ultraviolet markings on Venus - An analysis of the Venera 9 data

The results of Venera 9 measurements of the emergent intensity from the cloud tops of Venus are surveyed. It is reported that these radiance distributions at 3500 A contain information on the vertical and horizontal structure of the clouds and show the effects of the small and large scale ultra violet markings. Attention is given to model calculations with a Mie phase function for 1.05 micron sulfuric acid aerosols which indicate that the clouds have a layered structure. It is stressed that large-scale horizontal inhomogeneities (in excess of 1000 km) must be considered to supplement any analysis based on a horizontally homogeneous model. It is shown that the shape of the observed radiance distributions is affected by the ultraviolet 'Y' feature and the equatorial band.

Lestrade, J. P.↗

Analysis of the measured effects of the principal exhaust effluents from solid rocket motors

The feasibility of conducting environmental chamber tests using a small rocket motor to study the physical processes which occur when the exhaust products from solid motors mix with the ambient atmosphere was investigated. Of particular interest was the interaction between hydrogen chloride, aluminum oxide, and water vapor. Several types of instruments for measuring HCl concentrations were evaluated. Under some conditions it was noted that acid aerosols were formed in the ground cloud. These droplets condensed on Al2O3 nuclei and were associated with the rocket exhaust cooling during the period of plume rise to stabilization. Outdoor firings of the solid rocket motors of a 6.4 percent scaled model of the space shuttle were monitored to study the interaction of the exhaust effluents with vegetation downwind of the test site. Data concerning aluminum oxide particles produced by solid rocket motors were evaluated.

Dawbarn, R.↗

Ground cloud hydrogen chloride measurements from three Titan launches at the Kennedy Space Center during 1978 and 1979

Total hydrogen chloride and gaseous hydrogen chloride concentrations were measured in the exhaust cloud produced at three Titan 3 launches at the Kennedy Space Center in March 1978, December 1978, and November 1979 to determine the degree of hydrogen chloride partitioning in a solid rocket exhaust cloud between gaseous hydrogen chloride and hydrochloric acid aerosol as a function of ambient relative humidity. Moderately low relative humidity conditions were present during a daytime launch on Mar 25, 1978, and high relative humidity conditions were present during a nighttime launch on December 13, 1978. Gaseous hydrogen chloride concentrations and meteorological data, as a function of time after launch, are presented. Hydrogen chloride is present in both the gaseous and aerosol phase in the exhaust cloud. Total HCl concentrations ranged from 18 parts per million by volume (ppm) several minutes after launch down to 1 ppm after the cloud stabilization period, depending on the meteorological conditions. Gaseous HCl concentrations ranged from 2 to 3 ppm several minutes after launch to less than 1 ppm after cloud stabilization. These measured concentrations indicated significant HCl aerosol formation.

Seabacher, D. I.↗

Photochemistry of SO2 in Venus' upper cloud layers

The photochemical and transport processes that occur in the Venusian atmosphere in and above the upper cloud region are characterized with attention to the correlation with the Pioneer Venus spectrometer results for the cloud top SO2 distribution. The model uses upward-flowing SO2 and H2O to replace the sulfur and hydrogen lost through the lower boundary by the settling of sulfuric acid aerosols. Oxygen for the oxidation of SO2 to SO3 prior to hydration to H2SO4 is supplied by the photolysis of CO2. A model with SO2 as the major sulfur-bearing gas is consistent with the Pioneer data.

Winick, J. R.↗

The 1980 stratospheric-tropospheric exchange experiment

Data are presented from the Stratospheric-Tropospheric Water Vapor Exchange Experiment. Measurements were made during 11 flights of the NASA U-2 aircraft which provided data from horizontal traverser and samplings in and about the tops of extensive cirrus-anvil clouds produced by overshooting cumulus turrets. Aircraft measurements were made of water vapor, ozone, ambient and cloud top temperature, fluorocarbons, nitrous oxide, nitric acid, aerosols, and ice crystal populations. Balloonsondes were flown about twice daily providing data on ozone, wind fields, pressure and temperature to altitudes near 30 km. Satellite photography provided detailed cloud and cloud top temperature information. Descriptions of individual experiments and detailed compilations of all results are provided.

Margozzi, A. P.↗

Overview of the polar ozone issue

The causes of the Antarctic ozone depletion are discussed together with the role of the polar stratospheric clouds (PSCs, which are ice clouds that form towards spring over Antarctica in the altitude range of 10-20 km) in the process of ozone depletion. Evidence is presented suggesting that heterogeneous chemical reactions occurring on the surfaces of the PSCs could dramatically deplete the abundances of reactive nitrogen compounds and enhance those of reactive chlorine species which are responsible for ozone depletion. It was also shown that the surface reactions are not limited to ice clouds but can also take place on the liquid sulfuric acid aerosols present at lower latitudes, indicating that heterogeneous chemistry may take place to some extent on a global scale. Finaly, observations of low-abundance NO2 in north polar regions suggests that heterogeneous removal of reactive nitrogen may well be occurring in the Arctic, with possible attendant applications for Arctic ozone.

Solomon, Susan↗