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Preliminary calculations suggest that heterogeneous reactions are important in calculating the impact on ozone from emissions of trace gases from aircraft fleets. In this study, three heterogeneous chemical processes that occur on background sulfuric acid aerosols are included and their effects on O3, NO(x), Cl(x), HCl, N2O5, ClONO2 are calculated.
Atmospheric perturbations caused by the emission of nitrogen oxides from a projected fleet of stratospheric aircraft are studied with a two dimensional chemistry, transport model. Photochemistry of the lower stratosphere, the region where these aircraft may fly, is now known to be influenced by heterogeneous reactions involving sulfuric acid aerosols. This study examines the sensitivity of the atmospheric effects of aircraft to heterogeneous reactions. Information of background aerosols based on the SAGE 2 measurements have been used in the parameterization of the heterogeneous conversion rates. It is found that heterogeneous reactions make the lower stratospheric ozone less sensitive to perturbations in the odd nitrogen level. The calculated reduction in global ozone due to NO(x) injection from a fleet of Mach 2.4 aircraft is 1.28 percent if gas phase reactions only are considered in the model, and 0.06 percent if heterogeneous reactions are included.
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.
In this study, we sought to characterize variations in the abundance and distribution of subcloud H2SO4(g) in the Venus atmosphere by using a number of 13cm radio occultation measurements conducted with the Pioneer Venus Orbiter near the inferior conjunction of 1991. A total of ten data sets were examined and analyzed, producing vertical profiles of temperature and pressure in the neutral atmosphere, and sulfuric acid vapor abundance below the main cloud layer. Two of the vertical profiles of the abundance of H2SO4(g) were correlated with NIR images of the night side of Venus made during the same period of time by Boris Ragent (under a separate PVO Guest Investigator Grant). Initially, we had hoped that the combination of these two different types of data would make it possible to constrain or identify the composition of the large particles causing the features observed in the NIR images. However, the sparseness of the radio occultation data set, combined with the sparseness of the NIR data set (one image per day over an 8 day period) made it impossible to draw strong conclusions. Considered on their own, however, the parameters retrieved from the radio occultation experiments are valuable science products.
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.
Analysis of aerosol extinction profiles obtained by the spaceborne SAGE II sensor reveals that there was an anomalous increase of aerosol extinction below 18.5 km at latitudes poleward of 50 deg N from July 28 to September 9, 1990. This widespread increase of aerosol extinction in the lower stratosphere was apparently due to a remote high-latitude volcanic eruption that has not been reported to date. The increase in stratospheric optical depth in the northern polar region was about 50% in August and had diminished by October 1990. This eruption caused an increase in stratospheric aerosol mass of about 0.33 x 10(exp 5) tons, assuming the aerosol was composed of sulfuric acid and water.
An extensive flight series was carried out during May-June 1990 in the remote North and South Pacific free tropospheric aboard the NASA DC-8. Condensation nuclei counters and optical particle counters provided information on aerosol particles with diameters between 0.003 and 7.0 micrometers. Vertical profiles revealed aerosol layers to be a common feature of the free troposphere. Regions with highest aerosol mass tended to have the highest concentrations of surface-derived nuclei but the lowest concentrations of total nuclei. Regions with lowest aerosol mass tended to have the highest concentrations of the smaller 'ultrafine' condensation nuclei with diameters below 0.02 mircometers. Horizontal transects totaling over 35,000 km at about 9 to 10-km altitude exhibited variability of approximately 3 orders of magnitude in both aerosol mass and number concentrations over spatial scales ranging from 1 to 1000 km. At these altitudes an approximate inverse relationship between ultrafine concentrations and the surface area of the larger aerosol was evident. Regions having lowest aerosol mass were characterized by aerosol thermal volatility, indicative of a predominately sulfuric acid composition, and by very high concentrations of ultrafine nuclei, indicative of recent homogeneous nucleation. These conditions were frequently observed but were conspicuously evident above cloud over the intertropical convergence zone. The clean, free troposphere appears to be a significant source region for new tropospheric nuclei. A simplified model of the lifetime, coagulation, and cycling of these nuclei suggests that they constitute a source of cloud condensation nuclei in the lower troposphere.
Balloon profiles of chlorine monoxide (ClO), nitric oxide (NO), and ozone (O3) were measured on March 11, 1992 from 100 to 10 mb over Greenland (67.0 deg N, 50.6 deg W). Measurements from SAGE II indicate that the aerosol surface area in the region was enhanced by sulfur from the eruption of Mt. Pinatubo, reaching 50 times background near 20 km. Concentrations of ClO were enhanced and concentrations of NO were suppressed relative to low aerosol conditions consistent with the effects of hydrolysis of N2O5 on the surface of sulfuric acid aerosols. The data are consistent with a value of 2 x 10(exp -4) for the reaction probability of the heterogeneous hydrolysis of ClONO2, indicating a minor role for this reaction at as temperature of 220 K. At these temperatures, we find no evidence for the catastrophic loss of ozone predicted to occur under conditions of enhanced aerosol surface area.
Quantitative measurements of the wavelength dependence of aerosol extinction in the 750-3400/cm spectral region have been derived from 0.01/cm resolution stratospheric solar occultation spectra recorded by the ATMOS (Atmospheric Trace Molecule Spectroscopy) Fourier transform spectrometer about 9 1/2 months after the Mt Pinatubo volcanic eruption. Strong, broad aerosol features have been identified near 900, 1060, 1190, 1720, and 2900/cm below a tangent height of approximately 30 km. Aerosol extinction measurements derived from approximately 0.05/cm wide microwindows nearly free of telluric line absorption in the ATMOS spectra are compared with transmission calculations derived from aerosol size distribution profiles retrieved from correlative SAGE (Stratospheric Aerosol and Gas Experiment) II visible and near i.r. extinction measurements, seasonal and zonally averaged H2SO4 aerosol weight percentage profiles, and published sulfuric acid optical constants derived from room temperature laboratory measurements. The calculated shapes and positions of the aerosol features are generally consistent with the observations, thereby confirming that the aerosols are predominantly concentrated H2SO4-H2O droplets, but there are significant differences between the measured and calculated wavelength dependences of the aerosol extinction. We attribute these differences as primarily the result of errors in the calculated low temperature H2SO4-H2O optical constants. Errors in both the published room temperature optical constants and the limitations of the Lorentz-Lorenz relation are likely to be important.
An enhanced sulfate aerosol layer has been observed near 25 km accompanying springtime ozone depletion in the Antarctic stratosphere. We use a one-dimensional aerosol model that includes photochemistry, particle nucleation, condensational growth, coagulation, and sedimentation to study the origin of the layer. Annual cycles of sunlight, temperature, and ozone are incorporated into the model. Our results indicate that binary homogeneous nucleation leads to the formation of very small droplets of sulfuric acid and water under conditions of low temperature and production of H2SO4 following polar sunrise. Photodissociation of carbonyl sulfide (OCS) alone, however, cannot provide sufficient SO2 to create the observed condensation nuclei (CN) layer. When subsidence of SO2 from very high altitudes in the polar night vortex is incorporated into the model, the CN layer is reasonably reproduced. The model predictions, based on the subsidence in polar vortex, agree with in situ measurements of particle concentration, vertical distribution, and persistence during polar spring.
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.
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.
A survey is given of the accomplishments of airborne astronomy in solar-system science. They include identification of sulfuric acid in the clouds of Venus, establishment of Jupiter's internal heat source, discovery of water vapor and almost a dozen other molecules in Jupiter's atmosphere, important measurements of occultations of stars by Mars, Pluto, and Chiron, discovery of the rings of Uranus, and diagnosis of mineral composition on planetary surfaces.
The meteorite impact that formed the Chicxulub crater 65 million years ago caused a mass extinction of life. Analyses indicate that the projectile was either a 9.4-16.8 km diameter asteroid or a 14.2-24.0 km diameter comet. We estimate that 200 gigatons each of S02 and H2O were deposited globally in the stratosphere by the impact into water saturated sulfate-rich sediments. Conversion of these gases into sulfuric acid aerosols blocked an average of 68 percent of the sun's radiation for a period of 12 years. Global average temperatures probably dropped to near freezing in 5 years and remained near or below freezing for 7 years. Greenhouse warming due to impact-generated C02 was negligible, hence global cooling from sulfates was the major cause of climate change and contributed greatly to the mass extinction.
Based on the trajectory analysis presented in this paper, a new mechanism is described for the freezing of the stratospheric sulfate aerosols. Temperature histories based on 10-day back trajectories for six ER-2 flights during AASE-I (1989) and AAOE (1987) are presented. The mechanism requires, as an initial step, the cooling of a H2SO4/H2O aerosol to low temperatures. If a cooling cycle is then followed up by a warming to approximately 196-198 K, the aerosols may freeze due to the growth of the crystallizing embryos formed at the colder temperature. The HNO3 absorbed at colder temperatures may increase the nucleation rate of the crystalling embryos and therefore influence the crystallization of the supercooled aerosols upon warming. Of all the ER-2 flights described, only the polar stratospheric clouds (PSC), observed on the flights of January 24, and 25, 1989 are consistent with the thermodynamics of liquid ternary solutions of H2SO4/HNO3/H2O (type Ib PSCs). For those two days, back trajectories indicate that the air mass was exposed to sulfuric acid tetrahydrate (SAT) melting temperatures about 24 hours prior to being sampled by the ER-2. Temperature histories, recent laboratory measurements, and the properties of glassy solids suggest that stratospheric H2SO4 aerosols may undergo a phase transition to SAT upon warming at approximately 198 K after going through a cooling cycle to about 194 K or lower.
The nucleation and growth of different phases of simulated polar stratospheric cloud (PSC) particles were investigated in the laboratory. Solutions and mixtures of solutions at concentrations 1 to 5 m (molality) of ammonium sulfate, ammonium bisulfate, sodium chloride, sulfuric acid, and nitric acid were supercooled to prescribed temperatures below their equilibrium melting point. These solutions were contained in small diameter glass tubing of volumes ranging from 2.6 to 0.04 ml. Samples were nucleated by insertion of an ice crystal, or in some cases by a liquid nitrogen cooled wire. Crystallization velocities were determined by timing the crystal growth front passages along the glass tubing. Solution mixtures containing aircraft exhaust (soot) were also examined. Crystallization rates increased as deltaT2, where deltaT is the supercooling for weak solutions (2 m or less). The higher concentrated solutions (greater than 3 m) showed rates significantly less than deltaT2. This reduced rate suggested an onset of a glass phase. Results were applied to the nucleation of highly concentrated solutions at various stages of polar stratospheric cloud development within the polar stratosphere.
Understanding the physical processes of impact cratering on planetary surfaces and atmospheres as well as collisions of finite-size self-gravitating objects is vitally important to planetary science. The observation has often been made that craters are the most ubiquitous landform on the solid planets and the satellites. The density of craters is used to date surfaces on planets and satellites. For large ringed basin craters (e.g. Chicxulub), the issue of identification of exactly what 'diameter' transient crater is associated with this structure is exemplified by the arguments of Sharpton et al. (1993) versus those of Hildebrand et al. (1995). The size of a transient crater, such as the K/T extinction crater at Yucatan, Mexico, which is thought to be the source of SO,-induced sulfuric acid aerosol that globally acidified surface waters as the result of massive vaporization of CASO, in the target rock, is addressed by our present project. The impact process excavates samples of planetary interiors. The degree to which this occurs (e.g. how deeply does excavation occur for a given crater diameter) has been of interest, both with regard to exposing mantle rocks in crater floors, as well as launching samples into space which become part of the terrestrial meteorite collection (e.g. lunar meteorites, SNC's from Mars). Only in the case of the Earth can we test calculations in the laboratory and field. Previous calculations predict, independent of diameter, that the depth of excavation, normalized by crater diameter, is d(sub ex)/D = 0.085 (O'Keefe and Ahrens, 1993). For Comet Shoemaker-Levy 9 (SL9) fragments impacting Jupiter, predicted excavation depths of different gas-rich layers in the atmosphere, were much larger. The trajectory and fate of highly shocked material from a large impact on the Earth, such as the K/T bolide is of interest. Melosh et al. (1990) proposed that the condensed material from the impact upon reentering the Earth's atmosphere induced. radiative heating, and producing global firestorms. The observed reentry splash of the SL-9 impact-induced plumes that reimpact Jupiter (Boslough et al., 1994) supported Melosh's K/T model. The fate of early primitive planetary atmospheres during the latter stages of planetary accretion, resulting from impactors in the 100 to 103 km diameter require modeling, e.g. Newman et al. (1997). Ahrens (1990; 1993) and Chen and Ahrens (1997) found that upon delivery of most of the impact energy to the solid planet, very large ground motions arise, which couple sufficient kinetic energy to the atmosphere to cause substantial atmospheric escape. The trade-off of this model with that of Cameron (1997) who suggests that atmospheric blow-off occurs as a result of the massive impact-induced heating of the atmosphere and Pepin (1997) who uses this heating event to model differential hydrodynamic loss of lighter atmospheric gases, requires further research.
Balloon profiles of chlorine monoxide (ClO), nitric oxide (NO), and ozone (O3) were measured on March 11, 1992 from 100 to 10 mb over Greenland (67.0 deg N, 50.6 deg W). Measurements from SAGE II indicate that the aerosol surface area in the region was enhanced by sulfur from the eruption of Mt. Pinatubo, reaching 50 times background near 20 km. Concentrations of ClO were enhanced and concentrations of NO were suppressed relative to low aerosol conditions consistent with the effects of hydrolysis of N2O5 on the surface of sulfuric acid aerosols. The data are consistent with a value of 2 x 10(exp -4) for the reaction probability of the heterogeneous hydrolysis of ClONO2, indicating a minor role for this reaction at a temperature of 220 K. At these temperatures, we find no evidence for the catastrophic loss of ozone predicted to occur under conditions of enhanced aerosol surface area.