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At least 505 records · Page 28

Stratospheric ion and aerosol chemistry and possible links with cirrus cloud microphysics - A critical assessment

Aspects of stratospheric ion chemistry and physics are assessed as they relate to aerosol formation and the transport of aerosols to upper tropospheric regions to create conditions favorable for cirrus cloud formation. It is found that ion-induced nucleation and other known phase transitions involving ions and sulfuric acid vapor are probably not efficient processes for stratospheric aerosol formation, and cannot compete with condensation of sulfuric acid on preexisting particles of volcanic or meteoritic origin which are larger than about 0.15 micron in radius. Thus, galactic cosmic rays cannot have a significant impact on stratospheric aerosol population. Changes in the stratospheric aerosol burden due to volcanos are up to two orders of magnitude larger than changes in ion densities. Thus, volcanic activity may modulate the radiative properties of cirrus clouds.

Mohnen, Volker A.↗

Stratospheric profiles of heavy water vapor isotopes and CH3D from analysis of the ATMOS Spacelab 3 infrared solar spectra

The isotopic composition of stratospheric water vapor and methane was investigated. Stratospheric profiles of HDO, (H-18)2O, (H-17)2O, and CH3D were derived from solar occultation spectra recorded on April 30 - May 1, 1985 by the Atmospheric Trace Molecule Spectroscopy Fourier transform spectrometer aboard Spacelab 3. The profiles of the three water-vapor isotopes showed an increase in the volume mixing ratio with altitude. The measured profiles of D/H in water vapor showed a large depletion in the lower stratosphere (about 63 percent relative to standard mean ocean water, SMOW, at 20 km) and a small increase in D/H with altitude at higher altitudes, up to 34 km. The D/H ratio in stratospheric methane was close to the corresponding isotopic ratio in SMOW.

Rinsland, C. P.↗

Recent trends in stratospheric ozone - Implications of ozone and temperature correlation

The relation between ozone and temperature in the upper stratosphere is used to estimate the drift in the SBUV spectrometer on Nimbus-7 and the linear trend in ozone from 1979 to 1986. The ozone and temperature variabilities are coupled through chemical and dynamical processes. In the upper stratosphere they are anticorrelated through temperature-dependent loss rates, while in the lower stratosphere their variabilities are positively correlated through dynamical coupling. These relations are used to determine the ozone sensitivity to temperature and ozone trends in terms of temperature trends. It is shown that in the upper stratosphere (approximately 2 mbar), the eight-year trend in ozone is a manifestation of dynamical perturbations. It varies from about +4 percent at the equator to about -1 to -2 percent at high latitudes in both hemispheres.

Chandra, S.↗

Troposphere-stratosphere interactions in a one-dimensional model of Jovian photochemistry

The case of a chemically unreactive species flowing downward through the stratosphere and troposphere with a constant flux is presently treated by a one-dimensional Jovian atmosphere model which encompasses the coupling between a rapidly mixed troposphere and a stagnant stratosphere, so that the contrast between the peak stratosphere and tropopause concentrations is reflective of the variation between the lower stratosphere and upper troposphere eddy diffusion coefficients. Numerical simulations of unreactive CO and C2H6 species indicate that upper troposphere abundances may possess a substantial photochemical contribution. The implications of these modeling results for higher spectral resolution observations are noted.

Landry, Bridget↗

The behavior of wave 2 in the Southern Hemisphere stratosphere during late winter and early spring

The behavior of wave 2 in the Southern Hemisphere (SH) winter and early spring stratosphere has been examined in detail using 10 years of NMC data. Wave 2 is characterized by a broad meridional structure peaking between 55 and 65 S, and regular eastward propagation, with periods ranging from 5 to 40 days. The range of maximum geopotential height amplitudes is from 600 to 1000 m for a year. Consideration is also given to the relationship of wave 2 to other features of stratospheric circulation, Eliassen-Palm fluxes, and synoptic maps. The results obtained show that the zonal mean state of the SH stratosphere frequently satisfies conditions for instability. It is concluded that both instability of zonally symmetric and asymmetric states, and nonlinear interactions between wave 1 and wave 2 are of importance for determining the behavior of wave 2 in the SH winter and spring stratosphere.

Manney, G. L.↗

Air mass origins and troposphere-to-stratosphere exchange associated with mid-latitude cyclogenesis and tropopause folding inferred from Be-7 measurements

The 1984 extratropical mission of NASA's Stratosphere-Troposphere Exchange Project (STEP) studied cross-jet transport in regions of cyclogenesis and tropopause folding. Correlations of Be-7, ozone, water vapor, and potential vorticity measured on a NASA U-2 research aircraft flying in high shear regions above the jet core are indicative of mixing between the cyclonic and the anticyclonic sides of the jet and are consistent with the hypothesis that small-scale entrainments of upper tropospheric air into the lower stratosphere during cyclogenesis are important in maintaining the vertical gradients of Be-7, ozone, water vapor and other trace constituents in the lower few kilometers of the midlatitude stratosphere. Correlations between Be-7, and ozone suggest a lower tropical stratospheric origin for the ozone-poor lamina observed above the jet core.

Kritz, Mark A.↗

Condensational growth and trace species scavenging in stratospheric sulfuric acid/water aerosol droplets

Stratospheric aerosols play a significant role in the environment. The composition of aerosols is believed to be a liquid solution of sulfuric acid and water with numerous trace species. Of these trace species, ozone in particular was recognized as being very important in its role of shielding the environment from harmful ultraviolet radiation. Also among the trace species are HCl and ClONO2, the so called chlorine reservoir species and various oxides of nitrogen. The quantity of stratospheric aerosol and its particle size distribution determines, to a large degree, the chemistry present in the stratosphere. Aerosols experience 3 types of growth: nucleation, condensation, and coagulation. The application of condensation investigations to the specific problem of stratospheric aerosols is discussed.

Tompson, Robert V., Jr.↗

Stratospheric Backscatter, Extinction, and Lidar Ratio Profiling After the Mt. Pinatubo Eruptions

Since August 1991 the stratospheric aerosol layer is continuously monitored with a combination Raman elastic-backscatter lidar, groundbased systems. XeCl excimer laser is used as the radiation source. Signals elastically backscattered from air molecules and particles and inelastically Raman backscattered from nitrogen molecules are detected. The measurements of these two signal profiles up to 35 km height allows the separate and independent determination of aerosol extinction and backscatter properties in the perturbed lower stratosphere. The extinction coefficient is derived from the nitrogen Raman signal profile, while the backscatter coefficient is obtained from the elastic-to-inelastic backscatter signal ratio. In this way, also the extinction-to-backscatter, or lidar, ratio profile is determined. For the first time, lidar ratios are determined in the perturbed stratospheric layer by the use of remote sensing only. The lidar ratio contains information about the size range of the stratospheric particles which are assumed to be sulfuric acid droplets, and it is needed in the calculation of aerosol optical properties from data taken with a typical backscatter lidar.

Ansmann, Albert↗

Lidar Measurements of Aerosol and Ozone Distributions During the 1992 Airborne Arctic Stratospheric Expedition

The LaRC airborne lidar system was operated from the ARC DC-8 aircraft during the 1992 Airborne Arctic Stratospheric Expedition (ASEE-2) to investigate the distribution of stratospheric aerosols and O3 across the Arctic vortex from Jan. to Mar. 1992. Monthly flights were made across the Arctic vortex from Anchorage, Alaska, to Stavanger, Norway, and then back to Bangor, Maine, and additional round-trip flights north into the vortex were made each month from either Stavanger or Bangor depending on the location of the vortex that month. The airborne lidar system uses the differential absorption lidar (DIAL) technique at laser wavelengths of 301.5 and 310.8 nm to measure O3 profiles above the DC-8 over the 12-25 km altitude range. Lidar measurements of aerosol backscatter and depolarization profiles over the 12-30 km altitude range are made simultaneously with the O3 measurements using infrared (IR) and visible (VIS) laser wavelengths of 603 and 1064 nm, respectively. The measurements of Pinatubo aerosols, polar stratospheric clouds, and O3 made with the airborne DIAL system during the AASE-2 expedition and to chemical and dynamical process that contribute to O3 depletion in the wintertime Arctic stratosphere.

Browell, E. V.↗

Kelvin wave variability in the upper stratosphere observed in SBUV ozone data

The Solar Backscatter UV ozone data collected for the eight years between 1979 and 1986 are used to analyze the signatures of equatorially trapped Kelvin waves in the upper stratosphere. The data reveal a strong semiannual modulation of Kelvin wave activity, confirming the results of previous rocketsonde observations. A comparison of the eight-year-average ensemble spectra to the semiannual oscillation in the stratospheric zonal winds revealed a seasonal asymmetry in the strength of Kelvin waves, which mimics the asymmetry observed in the zonal winds. No consistent relationship was observed with the quasi-biennial oscillation in the lower stratosphere, while correlations with the upper stratospheric winds are weak or nonexistent.

Randel, William J.↗

Dynamics of the 4-day wave in the Southern Hemisphere polar stratosphere

Horizontal wind and temperature data are employed to investigate the dynamics of the 4-day wave in the Southern Hemisphere polar stratosphere. They were derived from synoptic maps of satellite-measured brightness temperatures, which were generated using the fast Fourier synoptic mapping technique of Salby (1982). Circulation statistics from these data are compared to those from the NMC operational stratospheric analyses, demonstrating improvements afforded by detailed treatment of asynoptic sampling effects. The 40-day wave is isolated using temporally filtered data. Several events of wave growth and decay are observed in the upper stratosphere during August 1980. Derived zonal-mean and eddy statistics suggest that the 4-day wave results from an instability of the zonal-mean flow near 55-60S, at and above 1 mb. It is inferred from climatological data that the source of the instability is the 'double-jet' structure in the upper stratosphere and mesosphere.

Randel, William J.↗

Planetary-scale waves in the Southern Hemisphere winter and early spring stratosphere - Stability analysis

A barotropic stability model linearized about a zonally symmetric flow is used to examine the stability characteristics of horizontal zonal-mean flow profiles representative of the Southern Hemisphere middle stratosphere during winter and early spring, with emphasis on periods when planetary wave growth appears confined to the stratosphere. Unstable modes of eastward-travelling waves 2 and 3 are found to have period sand spatial structures, similar to observations. Wave-2 and wave-3 momentum fluxes are similar in observations and model results and are consistent with the transfer of kinetic energy from the zonal-mean flow to the wave. When a barotropic model with a zonally symmetric basic flow is used, wave 3 is usually most unstable. Including a stationary wave 1 in the basic flow destabilizes both wave 2 and wave 3, but has little effect on their periods or spatial structures. The similarity between observed fields and model results in a number of cases when wave 2 appears to grow within the stratosphere suggests that in situ instabilities play a role in the evolution of the eastward-traveling wave-2 characteristic of the Southern Hemisphere winter and early spring stratosphere.

Manney, G. L.↗

Future aircraft and potential effects on stratospheric ozone and climate

Initial studies with LLNL models of global atmospheric chemical, radiative, and transport processes have indicated that substantial decreases in stratospheric ozone concentrations could result from emissions of NO(x) from aircraft flying in the stratosphere, depending on fleet size and magnitude of the engine emissions. These studies used homogeneous chemical reaction rates (e.g., gas-phase chemistry). Recent evidence indicates that reactions on particles in the stratosphere may be important. Heterogeneous chemical reactions convert NO(x) (NO and NO2) molecules to HNO3. This decreases the odd oxygen loss from the NO(x) catalytic cycle and increases the odd oxygen loss from the Cl(x) catalytic cycle. By including these heterogeneous reactions in the LLNL model, the relative partitioning of odd oxygen loss between these two families changes, with the result that emissions of NO(x) from proposed aircraft fleets flying in the stratosphere now increase ozone. Having these heterogeneous processes present also increases ozone concentration in the troposphere relative to gas-phase only chemistry calculations for emissions of NO(x) from subsonic aircraft.

Kinnison, Douglas E.↗

Stratospheric HNO3 measurements from 0.002/cm resolution solar occultation spectra and improved spectroscopic line parameters in the 5.8-micron region

Very-high-resolution FWHM solar-occultation spectra are investigated with a balloon-borne interferometer using revised spectroscopic line parameters for HNO3, O3, and H2O. The O3 and H2O data are evaluated to determine their capacity for interference in the HNO3 line which is studied in the nu sub 2 band at 5.8 microns. The line parameters developed with the stratospheric data are compared to data based on a HITRAN compilation as well as laboratory spectra with a 0.002/cm resolution. The line list is calculated and shown to include J and Ka transitions which improve the line parameters for HNO3 by accounting for the weaker absorption features in the stratospheric spectra. The stratospheric HNO3 profile developed analytically is compared to those based on reported measurements, and the one developed with the stratospheric solar spectra is found to be consistent with the measurements and confirm inherent measurement biases.

Goldman, A.↗

Natural and anthropogenic perturbations of the stratospheric ozone layer

The paper reviews potential causes for reduction in the ozone abundance. The response of stratospheric ozone to solar activity is discussed. Ozone changes are simulated in relation with the potential development of a fleet of high-speed stratospheric aircraft and the release in the atmosphere of chlorofluorocarbons. The calculations are performed by a two-dimensional chemical-radiative-dynamical model. The importance of heterogeneous chemistry in polar stratospheric clouds and in the Junge layer (sulfate aerosol) is emphasized. The recently reported ozone trend over the last decade is shown to have been largely caused by the simultaneous effects of increasing concentrations of chlorofluorocarbons and heterogeneous chemistry. The possibility for a reduction in stratospheric ozone following a large volcanic eruption such as that of Mount Pinatubo in 1991 is discussed.

Brasseur, Guy P.↗

Long-term tropospheric and lower stratospheric ozone variations from ozonesonde observations

An analysis is presented of the long-term mean pressure-latitude seasonal distribution of tropospheric and lower stratospheric ozone for the four seasons covering, in part, over 20 years of ozonesonde data. The observed patterns show minimum ozone mixing ratios in the equatorial and tropical troposphere except in regions where net photochemical production is dominant. In the middle and upper troposphere, and low stratosphere to 50 mb, ozone increases from the tropics to subpolar latitudes of both hemispheres. In mid stratosphere, the ozone mixing ratio is a maximum over the tropics. The observed vertical ozone gradient is small in the troposphere but increases rapidly above the tropopause. The amplitude of the annual variation increases from a minimum in the tropics to a maximum in polar regions. Also, the amplitude increases with height at all latitudes up to about 30 mb where the phase of the annual variation changes abruptly. The phase of the annual variation is during spring in the boundary layer, summer in mid troposphere, and spring in the upper troposhere and lower stratosphere.

London, J.↗

On the age of stratospheric air and ozone depletion potentials in polar regions

Observations of the nearly inert, man-made chlorofluorocarbon CFC-115 obtained during January 1989 are used to infer the age of air in the lower stratosphere. These observations together with estimated release rates suggest an average age of high-latitude air at pressure altitudes near 17-21 km of about 3 to 5 yr. This information is used together with direct measurements of HCFC-22, HCFC-142b, CH3Br, H-1301, H-1211, and H-2402 to examine the fractional dissociation of these species within the Arctic polar lower stratosphere compared to that of CFC-11 and hence to estimate their local ozone depletion potentials in this region. It is shown that these HCFCs are much less efficiently dissociated within the stratosphere than CFC-11, lowering their ozone depletion potentials to only about 30-40 percent of their chlorine loading potentials. In contrast, the observations of CH3Br and the Halons considered confirm that they are rapidly dissociated within the stratosphere, with important implications for their ozone depletion potentials.

Pollock, W. H.↗

Predicted aircraft effects on stratospheric ozone

The possibility that the current fleet of subsonic aircraft may already have caused detectable changes in both the troposphere and stratosphere has raised concerns about the impact of such operations on stratospheric ozone and climate. Recent interest in the operation of supersonic aircraft in the lower stratosphere has heightened such concerns. Previous assessments of impacts from proposed supersonic aircraft were based mostly on one-dimensional model results although a limited number of multidimensional models were used. In the past 15 years, our understanding of the processes that control the atmospheric concentrations of trace gases has changed dramatically. This better understanding was achieved through accumulation of kinetic data and field observations as well as development of new models. It would be beneficial to start examining the impact of subsonic aircraft to identify opportunities to study and validate the mechanisms that were proposed to explain the ozone responses. The two major concerns are the potential for a decrease in the column abundance of ozone leading to an increase in ultraviolet radiation at the ground, and redistribution of ozone in the lower stratosphere and upper troposphere leading to changes in the Earth's climate. Two-dimensional models were used extensively for ozone assessment studies, with a focus on responses to chlorine perturbations. There are problems specific to the aircraft issues that are not adequately addressed by the current models. This chapter reviews the current status of the research on aircraft impact on ozone with emphasis on immediate model improvements necessary for extending our understanding. The discussion will be limited to current and projected commercial aircraft that are equipped with air-breathing engines using conventional jet fuel. The impacts are discussed in terms of the anticipated fuel use at cruise altitude.

Ko, Malcolm K. W.↗