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At least 343 records · Page 19

Cryogenic Limb Array Etalon Spectrometer (CLAES) - Experiment overview

The Cryogenic Limb Array Etalon Spectrometer (CLAES) is one of a complement of instruments on the NASA Upper Atmosphere Research Satellite which is expected to study atmospheric photochemistry, energy input, and dynamics following a 1991 launch. CLAES measures stratospheric altitude profiles of temperature, pressure, O3, H2O, CH4, N2O, NO, NO2, N2O5, HNO3, ClONO2, HCl, CFC-11, and CFC-12. These data are obtained typically between 10 and 60 km, with 2.5-km vertical resolution and 500-km horizontal grid size. Coverage is obtained between latitudes 80 deg north and south, thereby providing substantial coverage of the Antarctic spring polar ozone-hole region. CLAES derives the listed geophysical parameters from measurement of earth-limb spectral emissions between 3.5 and 13 microns. Brief discussions of the measurement concept, instrument design, and performance are presented, followed by a more detailed discussion of scientific capabilities and measurement modes.

Roche, Aidan E.↗

New spectral features of stratospheric trace gases identified from high-resolution infrared balloon-borne and laboratory spectra

A new Michelson-type interferometer system operating in the infrared at very high resolution has been used to record numerous balloon-borne solar absorption spectra of the stratosphere, ground-based solar absorption spectra, and laboratory spectra of molecules of atmospheric interest. In the present work results obtained for several important stratospheric trace gases, HNO3, CIONO2, HO2NO2, NO2, and COF2, in the 8- to 12-micron spectral region are reported. Many new features of these gases have been identified in the stratospheric spectra. Comparison of the new spectra with line-by-line simulations shows that previous spectral line parameters are often inadequate and that new analysis of high-resolution laboratory and atmospheric spectra and improved theoretical calculations will be required for many bands. Preliminary versions of several sets of improved line parameters under development are discussed.

Goldman, A.↗

Measurements of nitric oxide and total reactive nitrogen in the Antarctic stratosphere - Observations and chemical implications

Results are presented on measurements of NO and the sum of reactive nitrogen species, NO(y), which include NO, NO2, NO3, N2O5, HNO3, and ClONO2 (in addition to ClO, O3, H2O, and N2O measurements), obtained aboard the NASA ER-2 aircraft flying over the Antarctica between the latitudes of 53 and 72 deg S during the Airborne Antarctic Ozone Experiment. The boundary of the chemically perturbed region (CPR), as indicated by a sharp increase in the level of ClO, occurred near 66 deg S; outside or equatorward of the CPR, the NO(y) mixing ratios ranged between 6 and 12 ppbv, with values decreasing poleward and reaching total NO(y) levels of 4 ppbv or less within 5-deg poleward of the boundary. Data presented in this paper clearly associate the Antarctic ozone decrease with perturbed conditions of ClO, NO(y), and H2O, which are in turn associated with processes defined as nonstandard heterogeneous chemistry, denitrification, and dehydration, respectively.

Fahey, D. W.↗

Computer processing of tunable diode laser spectra

A computer-controlled tunable diode laser spectrometer and spectral analysis software are described. The three-channel system records simultaneously the transmission of a subject gas, a temperature-stabilized etalon, and a calibration gas. The software routines are applied to diode laser spectra of HNO3 and NO2 to illustrate the procedures adopted for conversion of raw spectral data to useful transmission and harmonic spectra. Extraction of line positions, absorption intensities, collisional broadening coefficients, and gas concentrations from recorded spectra is also described.

May, Randy D.↗

Dual-polarization airborne lidar observations of polar stratospheric cloud evolution

Dual-polarization 0.532 micron lidar data show systematic polar stratospheric cloud (PSC) evolution along a portion of the Airborne Arctic Stratospheric Expedition DC-8 flight of January 31, 1989. This flight leg was roughly aligned with air parcel motion on isentropic surfaces from 400-500 K, where the local adiabatic cooling rate was about 20 K/day. Type 1 PSCs show low depolarization ratios and scattering ratios which approach intermediate limiting values as ambient temperature decreases. These data suggest that Type 1 particles formed by rapid cooling may be nearly spherical and are restricted in size by partitioning of a limited HNO3 vapor supply among many competing growth sites. Type 2 PSCs appear at temperatures below estimated local frost points with increases in depolarization and scattering typical of larger ice crystals.

Poole, L. R.↗

Incorporation of stratospheric acids into water ice

Hydrochloric and hydrofluoric acids are absorbed within the water ice lattice at mole fractions maximizing below 0.00001 and 0.0001 in a variety of solid impurity studies. The absorption mechanism may be substitutional or interstitial, leading in either case to a weak permeation of stratospheric ices by the acids at equilibrium. Impurities could also inhabit grain boundaries, and the acid content of atmospheric ice crystals will then depend on details of their surface and internal microstructures. Limited evidence indicates similar properties for the absorption of HNO3. Water ice lattices saturated with acid cannot be a significant local reservoir for HCl in the polar stratosphere.

Elliott, Scott↗

Redistribution of reactive odd nitrogen in the lower arctic stratosphere

In-situ measurements of total reactive odd nitrogen NO(y), were made from the NASA DC-8 aircraft in the lower arctic stratosphere during the 1989 Airborne Arctic Stratospheric Expedition. Throughout January and February, NO(y) mixing ratios were typically between 0.5 and 3 parts per billion by volume (ppbv) at altitudes between 10 and 12.5 km. During several flights late in the mission, events of unusually light NO(y) occurred with mixing ratios up to 12 ppbv at these altitudes. Simultaneous measurements of N2O, O3, and H2O during these events suggest that large changes in NO(y) are not expected. The elevated NO(y) values are interpreted as a vertical redistribution of NO(y) in the lower stratosphere resulting from gravitational sedimentation of aerosol particles containing HNO3. No evidence of the redistribution of H2O is noted, consistent with observations of denitrification without dehydration higher in the stratosphere.

Huebler, G.↗

The Balloon Intercomparison Campaigns - An introduction and overview

The Balloon Intercomparison Campaigns of 1982 and 1983 involved a comparison of measurements by 21 instruments from seven countries, assembled on four gondolas, assigned to collect data on the vertical profiles of HCl, HNO3, NO2, NO, O3, and many other stratospheric constituents. Most of these sensors supplied data on more than two constituents. This paper describes the instruments and the constituents measured by each of the sensor and the parameters of each balloon flight, together with some results.

Watson, R. T.↗

Remote sensing of the troposphere by infrared emission spectroscopy

This paper describes the concept of a cryogenic IR imaging Fourier transform spectrometer, called the Tropospheric Emission Spectrometer (TES), designed for observations of the troposphere and lower stratosphere from a near-earth orbit, using natural thermal emission and reflected sunlight. The principal molecular species to be measured by TES are O3, CO, CO2, N2O, H2O, H2O2, NO, NO2, HNO3, NH3, CH4, C2H6, C2H2, SO2, COS, CFCl3, and CF2Cl2. The TES is scheduled for a launch on the second polar platform of the Earth Observing System in 1998.

Beer, Reinhard↗

Peroxyacetyl nitrate measurements during CITE 2 - Atmospheric distribution and precursor relationships

Results are reported from airborne PAN measurements obtained at altitudes 0-6 km over the continental U.S. and the eastern Pacific during the NASA Global Tropospheric Experiment Chemical Instrumentation Test and Evaluation 2 (CITE 2) in summer 1986. The CITE 2 flights and instrumentation are described, and the results are presented in extensive graphs and characterized in detail. It is shown that PAN is an important reactive N-containing species in the troposphere. Although the PAN mixing ratios were highly variable, in general high mixing ratios of 100-300 parts per trillion by volume (pptv) were found at 4-6 km, and very low ratios (5-20 pptv) were detected in the marine boundary layer. Good correlation was seen between the CITE 2 PAN values and those for O3, NO(y), NO(x), HNO3, C2H6, CO, and CFCl3.

Singh, H. B.↗

A model of stratospheric chemistry and transport on an isentropic surface

This paper presents a new photochemical transport model designed to simulate the behavior of stratospheric trace species in the middle stratosphere. The model has an Eulerian grid with the latitude and longitude coordinates on a single isentropic surface (hemispheric or global), in which both the dynamical and the photochemical processes can be accurately represented. The model is intgegrated for 12 days with winds and temperatures supplied by three-dimensional integration of an idealized wavenumber-one disturbance. The results for the long-lived tracers such as N2O showed excellent correlation with the potential vorticity distribution, validating the transport scheme. Calculations with zonally averaged wind and temperature fields showed that discrepancies in the calculation of the zonal mean were less than 10 percent for O3 and HNO3, compared with the zonal mean of the previous results.

Austin, John↗

Measurements of reactive nitrogen oxides (NO/y/) within and above a tropical forest canopy in the wet season

Measurements of ambient concentrations of reactive nitrogen oxides were made in the Amazon rain forest, near Manaus, Brazil, continuously at 39 m (above the canopy), and on several days and nights at 19 m (within the canopy). Concentrations were very low, typically 100-700 pptv, except for brief periods when up to 5000 pptv of NO(y) was observed, indicating polluted air from the urban area of Manaus. The forest was a net sink for NO(y) with the NO(y) flux = -7.6 + or - 5.0) x 10 to the 9th molecules/sq cm per sec in unpolluted periods, even though soils emitted NO at a significant rate (8.9 + or - 1.5 x 10 to the 9th molecules/sq cm per sec). The deposition rate for NO(y) appeared to be much larger during the daytime than at night, suggesting that uptake was controlled either by plant processes (stomatal opening) or by supply of reactive components of NO(y) (e.g., HNO3) during the daytime. Implications for regional and global atmospheric chemistry are discussed.

Bakwin, Peter S.↗

New insights in the photochemistry of grain mantles: The identification of the 4.62 and 6.87 micron bands

The mid-IR spectral region of molecular clouds is known to show the fingerprints of molecules frozen in the icy mantles of the interstellar grains. To study the complex chemical and physical interactions on the ice mantles accreted on grains in molecular clouds numerous UV irradiation and diffusion experiments were performed. The irradiation of binary ices was studied. Using isotopic labelling on NH3/CO and NH3/O2 ices numerous compounds were identified, of which OCN(-), NO2(-), NO3(-), and NH4(+) ions reveal a new type of chemical reactions. It appeared that these compounds were formed by proton transfer reactions induced by the interaction between an acid (HNCO, HNO2, HNO3) and a base (NH3) through a hydrogen bond. This mechanism was confirmed by a study of photolyzed diluted argon mixtures. The main astrophysically relevant data from the overall study are presented. The 4.62 micron band in W33A can be reproduced with NH3/CO containing irradiated ices and was identified with OCN(-). The 6.87 micron band in W33A and other photostellar objects is reproduced with NH3/O2 containing ices and is identified with NH4(+).

Grim, Ruud↗

Kelvin wave-induced trace constituent oscillations in the equatorial stratosphere

Kelvin wave induced oscillations in ozone (O3), water vapor (H2O), nitric acid (HNO3) and nitrogen dioxide (NO2) in the equatorial stratosphere are analyzed using Limb Infrared Monitor of the Stratosphere (LIMS) data. Power and cross-spectrum analyses reveal coherent eastward propagating zonal wave 1 and 2 constituent fluctuations, due to the influence of Kelvin waves previously documented in the LIMS data. Comparison is made between a preliminary and the archival versions of the LIMS data; significant differences are found, demonstrating the sensitivity of constituent retrievals to derived temperature profiles. Because Kelvin waves have vanishing meridional velocity, analysis of tracer transport in the meridional plane is substantially simplified. Kelvin wave vertical advection is demonstrated by coherent, in-phase temperature-tracer oscillations, co-located near regions of strong background vertical gradients.

Randel, William J.↗

Stratospheric photochemical studies with Atmospheric Trace Molecule Spectroscopy (ATMOS) measurements

The photochemical partitioning of stratospheric odd chlorine and odd nitrogen is examined utilizing diurnal model calculations and data from the ATMOS experiment. This experiment, conducted during April-May 1985, employed a solar occultation method to obtain vertical profiles of temperature and various other trace constituents at 30 deg N and 48 deg S latitudes. The ATMOS data set confirms the presence of N2O5 in the stratosphere; however, the observed mixing ratios at sunset are more than a factor of 2 less than the calculated values. It is shown that the conversion of N2O5 into HNO3 could take place in the presence of aerosol surfaces quickly enough to affect the N2O5 mixing ratio below 30 km. Inclusion of the heterogeneous reaction brings the calculated N2O5 profile below 30 km into closer agreement with the ATMOS data.

Natarajan, Murali↗

The potential for ozone depletion in the Arctic polar stratosphere

The nature of the Arctic polar stratosphere is observed to be similar in many respects to that of the Antarctic polar stratosphere, where an ozone hole has been identified. Most of the available chlorine (CHl and ClONO2) was converted by reactions on polar stratospheric clouds to reactive ClO and Cl2O2 thoroughout the Arctic polar vortex before midwinter. Reactive nitrogen was converted to HNO3, and some, with spatial inhomogeneity, fell out of the stratosphere. These chemical changes ensured characteristic ozone losses of 10 to 15 percent at altitudes inside the polar vortex where polar stratospheric clouds had occurred. These local losses can translate into 5 to 8 percent losses in the vertical column abundance of ozone. As the amount of stratospheric chlorine inevitably increases by 50 percent over the next two decades, ozone losses recognizable as an ozone hole may well appear.

Brune, W. H.↗

Role of heterogeneous conversion of N2O5 on sulphate aerosols in global ozone losses

The reaction rate of N2O5 on sulphate aerosols is included in a model to predict global ozone loss and the column abundances of atmospheric gases. Because the reaction of N2O5 and the aerosols can take place in the stratospheric sulphate aerosol layer, it is included in the 2D model so that the results can be compared to abundances derived from satellite data and ground-based measurements. The N2O5/sulphate reaction is the only heterogeneous reaction in the model, in which aerosol loading is assumed to be constant and only diurnal values are examined. The decadal ozone trends resulting from calculations based on the model are found to be closer to the observed values. An important conclusion is that measurements of OH, ClO, HNO3, NO, and NO2 in the region of about 14-25 km are needed to examine significant changes in their abundances resulting from the inclusion of the N2O5/sulphate aerosol reaction.

Rodriguez, Jose M.↗

Nighttime reactive nitrogen measurements from stratospheric infrared thermal emission observations

IR thermal emission spectra of the earth's atmosphere in the 700-2000/cm region were obtained with a cryogenically cooled high-resolution interferometer spectrometer on a balloon flight from Palestine, Texas, on September 15-16, 1986. The observations exhibit spectral features of a number of stratospheric constituents, including important species of the reactive nitrogen family. An analysis of the observed data for simultaneously measured vertical distributions of O3, H2O, N2O, NO2, N2O5, HNO3, and ClONO2 is presented. These measurements permit the first direct determination of the nighttime total reactive nitrogen concentrations, and the partitioning of the important elements of the NO(x) family. Comparisons of the total reactive nitrogen budget are made with the measurements by the ATMOS experiment and with the predictions of one-dimensional and two-dimensional photochemical models.

Abbas, Mian M.↗