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NASA NTRS1993

The atmospheric effects of stratospheric aircraft. Report of the 1992 Models and Measurements Workshop. Volume 1: Workshop objectives and summary

This Workshop on Stratospheric Models and Measurements (M&M) marks a significant expansion in the history of model intercomparisons. It provides a foundation for establishing the credibility of stratospheric models used in environmental assessments of chlorofluorocarbons, aircraft emissions, and climate-chemistry interactions. The core of the M&M comparisons involves the selection of observations of the current stratosphere (i.e., within the last 15 years): these data are believed to be accurate and representative of certain aspects of stratospheric chemistry and dynamics that the models should be able to simulate.

Prather, Michael J.↗
NASA NTRS1993

The atmospheric effects of stratospheric aircraft. Report of the 1992 Models and Measurements Workshop. Volume 2: Comparisons with global atmospheric measurements

This Workshop on Stratospheric Models and Measurements (M&M) marks a significant expansion in the history of model intercomparisons. It provides a foundation for establishing the credibility of stratospheric models used in environmental assessments of chlorofluorocarbons, aircraft emissions, and climate-chemistry interactions. The core of the M&M comparisons involves the selection of observations of the current stratosphere (i.e., within the last 15 years): these data are believed to be accurate and representative of certain aspects of stratospheric chemistry and dynamics that the models should be able to simulate.

Prather, Michael J.↗
NASA NTRS1993

The atmospheric effects of stratospheric aircraft. Report of the 1992 Models and Measurements Workshop. Volume 3: Special diagnostic studies

This Workshop on Stratospheric Models and Measurements (M&M) marks a significant expansion in the history of model intercomparisons. It provides a foundation for establishing the credibility of stratospheric models used in environmental assessments of chlorofluorocarbons, aircraft emissions, and climate-chemistry interactions. The core of the M&M comparisons involves the selection of observations of the current stratosphere (i.e., within the last 15 years): these data are believed to be accurate and representative of certain aspects of stratospheric chemistry and dynamics that the models should be able to simulate.

Prather, Michael J.↗
NASA NTRS1992

Propagation of planetary waves between the troposphere and stratosphere

The propagation of planetary waves between the troposphere and stratosphere is investigated using a linear, time-dependent, primitive equation model. It is found that the tropopause acts like a valve for the propagation of planetary waves. The key parameters controlling the valve are the vertical gradient of buoyancy frequency and the vertical shear of the zonal winds at the tropopause. For a given wind profile smaller gradient of buoyancy frequency enhances the propagation of planetary waves. For a given profile of buoyancy frequency the larger the shear, the more the wave activity is trapped in the troposphere, and therefore, there is less left to propagate into the stratosphere. The transmission across the tropopause is, however, not sensitive to zonal winds in the upper stratosphere. The propagation of planetary waves is very sensitive to transience. More transient waves propagate more vertically within the troposphere, and for more transient waves, more wave activity is transferred into the stratosphere from the troposphere.

Chen, Ping↗
NASA NTRS1993

Uptake of formaldehyde by sulfuric acid solutions - Impact on stratospheric ozone

The study investigates the uptake of CH2O by low temperature sulfuric acid solutions representative of global stratospheric particulate. It is argued that if similar uptake occurs under stratospheric pressures of CH2O, i.e., 1000 times lower than used in the present study, then the removal of CH2O from the gas phase can take away a significant source of odd hydrogen in the mid- and high-latitude lower stratosphere. It is shown that with the inclusion of this reaction, concentrations of OH and H2O are reduced by as much as 4 percent under background levels of aerosols and more than 15 percent under elevated (volcanic) conditions. The accumulation of CH2O in stratospheric aerosols over a season, reaching about 1 M solutions, will alter the composition and may even change the reactivity of these sulfuric acid-water mixtures.

Tolbert, Margaret A.↗
NASA NTRS1993

The bromine content of micrometeorites - Arguments for stratospheric contamination

Bromine-salt nanocrystals are associated with a porous chondritic micrometeorite (W7029E5) that was collected in the lower stratosphere. These salt nanocrystals occur together with volcanic Na and K salt nanocrystals embedded in sulfuric acid droplets that were originally adhered to the particle. These materials were concentrated during hexane rinsing as part of routine curation procedures at the NASA Johnson Space Center Cosmic Dust Curatorial Facility. This observation is fortuitous to the extent that the concentration of nanocrystals and sulfuric acid is an experimental artifact of curation. If bromine is a stratospheric contaminant due to surface adsorption, there should be a positive linear relationship between the mass-normalized residence time and bromine content of individual micrometeorites. I show that the predicted correlation exists using a new model to calculate the stratospheric residence time of individual nonspherical micrometeorites in the slow-settling Wilson-Huang regime of the stratosphere.

Rietmeijer, Frans J. M.↗
NASA NTRS1993

CLAES observations of ClONO2 and HNO3 in the Antarctic stratosphere, between June 15 and September 17, 1992

The Cryogenic Array Etalon Spectrometer (CLAES) on the NASA Upper Atmosphere Research Satellite (UARS) began viewing the stratosphere in October 1991. This paper presents preliminary retrievals of ClONO2 and HNO3 from the CLAES measurements for selected days in June, July, August, and September of 1992 for the Southern Hemisphere. The data shows that by July 10, lower stratospheric ClONO2 and HNO3 have developed high 'collar' regions surrounding the polar vortex, and low values inside the vortex. This general structure is sustained through September 17, although the ClONO2 values inside the vortex increase significantly by this date. The data suggests that substantial sequestration of gaseous HNO3 in polar stratospheric clouds occurs in the early winter Antarctic stratosphere, accompanied by the conversion of ClONO2 to reactive chlorine through heterogeneous processes on the PSCs.

Roche, A. E.↗
NASA NTRS1993

Physical chemistry of the H2SO4/HNO3/H2O system - Implications for polar stratospheric clouds

Polar stratospheric clouds (PSCs) play a key role in stratospheric ozone depletion. Surface-catalyzed reactions on PSC particles generate chlorine compounds that photolyze readily to yield chlorine radicals, which in turn destroy ozone very efficiently. The most prevalent PSCs form at temperatures several degrees above the ice frost point and are believed to consist of HNO3 hydrates; however, their formation mechanism is unclear. Results of laboratory experiments are presented which indicate that the background stratospheric H2SO4/H2O aerosols provide an essential link in this mechanism: These liquid aerosols absorb significant amounts of HNO3 vapor, leading most likely to the crystallization of nitric acid trihydrate (NAT). The frozen particles then grow to form PSCs by condensation of additional amounts of HNO3 and H2O vapor. Furthermore, reaction probability measurements reveal that the chlorine radical precursors are formed readily at polar stratospheric temperatures not just on NAT and ice crystals, but also on liquid H2SO4 solutions and on solid H2SO4 hydrates. These results imply that the chlorine activation efficiency of the aerosol particles increases rapidly as the temperature approaches the ice frost point regardless of the phase or composition of the particles.

Molina, M. J.↗
NASA NTRS1993

The atmospheric effects of stratospheric aircraft: A third program report

A third report from the Atmospheric Effects of Stratospheric Aircraft (AESA) component of NASA's High-Speed Research Program (HSRP) is presented. Market and technology considerations continue to provide an impetus for high-speed civil transport research. A recent United Nations Environment Program scientific assessment showed that considerable uncertainty still exists about the possible impact of aircraft on the atmosphere. The AESA was designed to develop the body of scientific knowledge necessary for the evaluation of the impact of stratospheric aircraft on the atmosphere. The first Program report presented the basic objectives and plans for AESA. This third report marks the midpoint of the program and presents the status of the ongoing research on the impact of stratospheric aircraft on the atmosphere as reported at the third annual AESA Program meeting in June 1993. The focus of the program is on predicted atmospheric changes resulting from projected HSCT emissions. Topics reported on cover how high-speed civil transports (HSCT) might affect stratospheric ozone, emissions scenarios and databases to assess potential atmospheric effects from HSCT's, calculated results from 2-D zonal mean models using emissions data, engine trace constituent measurements, and exhaust plume/aircraft wake vortex interactions.

Stolarski, Richard S.↗
NASA NTRS1992

Comparison of the impact of volcanic eruptions and aircraft emissions on the aerosol mass loading and sulfur budget in the stratosphere

Data obtained by the Stratospheric Aerosol and Gas Experiment (SAGE) 1 and 2 were used to study the temporal variation of aerosol optical properties and to assess the mass loading of stratospheric aerosols from the eruption of volcanos Ruiz and Kelut. It was found that the yearly global average of optical depth at 1.0 micron for stratospheric background aerosols in 1979 was 1.16 x 10(exp -3) and in 1989 was 1.66 x 10(exp -3). The eruptions of volcanos Ruiz and Kelut ejected at least 5.6 x 10(exp 5) and 1.8 x 10(exp 5) tons of materials into the stratosphere, respectively. The amount of sulfur emitted per year from the projected subsonic and supersonic fleet is comparable to that contained in the background aerosol particles in midlatitudes from 35 deg N to 55 deg N.

Yue, Glenn K.↗
NASA NTRS1994

Effects of stratospheric aerosol surface processes on the LLNL two-dimensional zonally averaged model

We have investigated the effects of incorporating representations of heterogeneous chemical processes associated with stratospheric sulfuric acid aerosol into the LLNL two-dimensional, zonally averaged, model of the troposphere and stratosphere. Using distributions of aerosol surface area and volume density derived from SAGE II satellite observations, we were primarily interested in changes in partitioning within the Cl- and N- families in the lower stratosphere, compared to a model including only gas phase photochemical reactions. We have considered the heterogeneous hydrolysis reactions N2O5 + H2O(aerosol) yields 2 HNO3 and ClONO2 + H2O(aerosol) yields HOCl + HNO3 alone and in combination with the proposed formation of nitrosyl sulfuric acid (NSA) in the aerosol and its reaction with HCl. Inclusion of these processes produces significant changes in partitioning in the NO(y) and ClO(y) families in the middle stratosphere.

Connell, Peter S.↗
NASA NTRS1994

An investigation of the processes controlling ozone in the upper stratosphere

Photolysis of vibrationally excited oxygen produced by ultraviolet photolysis of ozone in the upper stratosphere is incorporated into the Lawrence Livermore National Laboratory 2-D zonally averaged chemical-radiative-transport model of the troposphere and stratosphere. The importance of this potential contributor of odd oxygen to the concentration of ozone is evaluated based upon recent information on vibrational distributions of excited oxygen and upon preliminary studies of energy transfer from the excited oxygen. When the energy transfer rate constants of previous work are assumed, increases in model ozone concentrations of up to 40 percent in the upper stratosphere are found, and the ozone concentrations of the model agree with measurements, including data from the Upper Atmosphere Research Satellite. However, the increase is about 0.4 percent when the larger energy transfer rate constants suggested by more recent experimental work are applied in the model. This indicates the importance of obtaining detailed information on vibrationally excited oxygen properties to evaluation of this process for stratospheric modelling.

Patten, Kenneth O., Jr.↗
NASA NTRS1994

A general circulation model study of the climatic effect of observed stratospheric ozone depletion between 1980 and 1990

The total ozone mapping spectrometer (TOMS) and stratospheric aerosol and gas experiment (SAGE) measurements show a significant reduction in the stratospheric ozone over the middle and high latitudes of both hemispheres between the years 1979 and 1991 (WMO, 1992). This change in ozone will effect both the solar and longwave radiation with climate implications. However, recent studies (Ramaswamy et al., 1992; WMO, 1992) indicate that the net effect depends not only on latitudes and seasons, but also on the response of the lower stratospheric temperature. In this study we use a general circulation model (GCM) to calculate the climatic effect due to stratospheric ozone depletion and compare the effect with that due to observed increases of trace gases CO2, CH4, N2O, and CFC's for the period 1980-1990. In the simulations, we use the observed changes in ozone derived from the TOMS data. The GCM used is a version of the NCAR community climate model referenced in Wang et al. (1991). For the present study we run the model in perpetual January and perpetual July modes in which the incoming solar radiation and climatological sea surface temperatures are held constant.

Dudek, Michael P.↗
NASA NTRS1994

Laboratory simulations of NAT formation approaching stratospheric conditions

Previous laboratory studies have established the stability conditions of nitric acid trihydrate (NAT), of which type 1 polar stratospheric cloud (PSC 1) particles are thought to be composed. However, NAT samples in lab studies were almost always formed under conditions very different from those of the stratosphere. In order to better understand the in situ growth of PSC 1 particle populations, samples of water and nitric acid were deposited under conditions of temperature and pressure which more closely approximate the polar stratosphere. The compositions of the solids, measured shortly after deposition, depended on the H2O:HNO3 ratio in the vapor from which the solids were condensed. Solids formed from vapor mixtures that approached stratospheric contained significantly less HNO3 than the 25 mol percent expected of NAT.

Marti, James↗
NASA NTRS1994

Age as a diagnostic of stratospheric transport

Estimates of stratospheric age from observations of long-lived trace gases with increasing tropospheric concentrations invoke the implicit assumption that an air parcel has been transported intact from the tropopical tropopause. However, because of rapid and irreversible mixing in the stratosphere, a particular air parcel cannot be identified with one that left the troposphere at some prior time. The parcel contains a mix of air with a range of transit times, and the mean value over this range is the most appropriate definition of age. The measured tracer concentration is also a mean over the parcel, but its value depends both on the transit time distribution and the past history of the tracer in the troposphere. In principle, only if the tropospheric concentration is increasing linearly can the age be directly inferred. We illustrate these points by employing both a one-dimensional diffusive analog of stratospheric transport, and the general circulation model (GCM) of the Goddard Institute for Space Studies (GISS). Within the limits of the GCM, we estimate the time over which tropospheric tracer concentrations must be approximately linear in order to determine stratospheric age unambiguously; the concentration of an exponentially increasing tracer is a function only of age if the growth time constant is greater than about 7 years, which is true for all the chlorofluorocarbons. More rapid source variations (for example, the annual cycle in CO2) have no such direct relationship with age.

Hall, Timothy M.↗
NASA NTRS1994

Intrusions into the lower stratospheric Arctic vortex during the winter of 1991-1992

Investigations of the kinematics of the lower stratospheric Arctic vortex during the winter of 1991-1992 using the contour advection with surgery technique reveal three distinct events in which there was substantial intrusion of midlatitude air into the vortex, in apparent contradiction of the view that the polar vortex constitutes an isolated air mass. Two of these events, in late January and mid-February, were well documented. They were predicted in high-resolution forecasts by the European Centre for Medium-Range Weather Forecasts, most clearly in experimental forecasts with reduced diffusion. Direct confirmation of the presence of the intrusions and of their calculated locations was provided by aerosol observations from the airborne differential absorption laser lidar aboard the NASA DC-8, taken as part of the second Airborne Arctic Stratospheric Expedition campaign; aerosol-rich air of midlatitude origin was seen in the expected position of the intrusions. The reality of the February event was also confirmed by in situ measurements from the NASA ER-2. Such events may be significant for the chemical processes taking place within the winter vortex. The intrusions were evidently related to the meteorology of the northern stratosphere during this winter and in particular to persistent tropospheric blocking over the northeastern Atlantic Ocean and western Europe and concomitant ridging into the lower stratospheric vortex in this region. Nevertheless, preliminary investigations have indicated that such events are not uncommon in other northern hemisphere winters, although no such events were found in the southern hemisphere during the Antarctic winter of 1987.

Plumb, R. A.↗
NASA NTRS1994

Effect of vibrationally excited oxygen on ozone production in the stratosphere

Photolysis of vibrationally excited oxygen produced by ultraviolet photolysis of ozone in the upper stratosphere is incorporated into the Lawrence Livermore National Laboratory two-dimensional zonally averaged chemical-radiative-transport model of the troposphere and stratosphere. The importance of this potential contributor of odd oxygen to the concentration of ozone is evaluated based on recent information on vibrational distributions of excited oxygen and on preliminary studies of energy transfer from the excited oxygen. When energy transfer rate constants similar to those of Toumi et al. (1991) are assumed, increases in model ozone concentrations of up to 4.0% in the upper stratosphere are found, and the model ozone concentrations are found to agree slightly better with measurements, including recent data from the Upper Atmosphere Research Satellite. However, the ozone increase is only 0.3% when the larger energy transfer rate constants indicated by recent experimental work are applied to the model. An ozone increase of 1% at 50 km requires energy transfer rate constants one-twentieth those of the preliminary observations. As a result, vibrationally excited oxygen processes probably do not contribute enough ozone to be significant in models of the upper stratosphere.

Patten, K. O., Jr.↗
NASA NTRS1994

Aerosol effect on Umkehr ozone profiles using Stratospheric Aerosol and Gas Experiment II measurements

This study examines 1211 cases of coincident ozone profiles derived from 1164 Umkehrs and 928 Stratospheric Aerosol and Gas Experiment II (SAGE II) profiles within 1000 km and 12 hours between October 1984 and April 1989 to study the stratospheric-aerosol effect on Umkehr ozone profiles. Because of the close correspondence of stratospheric aerosol optical depth at the SAGE II-measured 0.525-micrometer wavelength and the extrapolated 0.32 Umkehr wavelength determined in this study we use the 0.525-micrometer data to determine the aerosol effect on Umkehr profiles. At the 95% confidence level, we find the following errors to the Umkehr ozone amounts: in Umkehr layer 9 (-2.9 +/- 2.1), layer 8 (-2.3 +/- 1.1), layer 7 (0.1 +/- 1.1), layer 6 (2.2 +/- 1.0), layer 5 (-1.5 +/- 0.8), and layer 4 (-2.4 +/- 1.7) in percent ozone amount per 0.01 stratospheric aerosol optical depth. These results agree with previous theoretical and empirical studies within their respective error bounds in layers 9, 8, and 7. The results in layers 6, 5, and 4 differ significantly from those in previous works. Using only those eight stations with more than 47 coincidences results in mean aerosol effects that are not significantly different from the 14-station results. Because SAGE II and Umkehr produce different ozone retrievals in layer 9 and because the intralayer correlation of SAGE II ozone and aerosol in layer 9 is nonzero, one must exercise some caution in attributing the entire SAGE II-Umkehr difference in this layer to an aerosol effect.

Newchurch, M. J.↗