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NASA NTRS1992

Ionization and excitation in cool giant stars. I - Hydrogen and helium

The influence that non-LTE radiative transfer has on the electron density, ionization equilibrium, and excitation equilibrium in model atmospheres representative of both oxygen-rich and carbon-rich red giant stars is demonstrated. The radiative transfer and statistical equilibrium equations are solved self-consistently for H, H(-), H2, He I, C I, C II, Na I, Mg I, Mg II, Ca I, and Ca II in a plane-parallel static medium. Calculations are made for both radiative-equilibrium model photospheres alone and model photospheres with attached chromospheric models as determined semiempirically with IUE spectra of g Her (M6 III) and TX Psc (C6, 2). The excitation and ionization results for hydrogen and helium are reported.

Luttermoser, Donald G.↗
NASA NTRS1992

Particle size distributions in Arctic polar stratospheric clouds, growth and freezing of sulfuric acid droplets, and implications for cloud formation

The paper uses particle size and volume measurements obtained with the forward scattering spectrometer probe model 300 during January and February 1989 in the Airborne Arctic Stratospheric Experiment to investigate processes important in the formation and growth of polar stratospheric cloud (PSC) particles. It is suggested on the basis of comparisons of the observations with expected sulfuric acid droplet deliquescence that in the Arctic a major fraction of the sulfuric acid droplets remain liquid until temperatures at least as low as 193 K. It is proposed that homogeneous freezing of the sulfuric acid droplets might occur near 190 K and might play a role in the formation of PSCs.

Dye, James E.↗
NASA NTRS1993

Background stratospheric aerosol and polar stratospheric cloud reference models

A global aerosol climatology is evolving from the NASA satellite experiments SAM II, SAGE I, and SAGE II. In addition, polar stratospheric cloud (PSC) data have been obtained from these experiments over the last decade. An undated reference model of the optical characteristics of the background aerosol is described and a new aerosol reference model derived from the latest available data is proposed. The aerosol models are referenced to the height above the tropopause. The impact of a number of volcanic eruptions is described. In addition, a model describing the seasonal, longitudinal, and interannual variations in PSCs is presented.

Mccormick, M. P.↗
NASA NTRS1992

Optical effects of polar stratospheric clouds on the retrieval of TOMS total ozone

Small areas of sharply reduced ozone density appear frequently in the maps produced from polar region total ozone mapping spectrometer (TOMS) data. These mini-holes are of the order of 1000 km in extent with a lifetime of a few days. On the basis of measurements from ground-based instruments, balloon-borne ozonesondes, and simultaneous measurements of aerosol and ozone concentrations during aircraft flights in the Arctic and Antarctic regions, the appearance of polar stratospheric clouds (PSCs) are frequently associated with false reductions in ozone derived from the TOMS albedo data. By combining radiative transfer calculations with the observed PSC and ozone data, it is shown that PSCs located near or above the ozone density maximum (with optical thickness greater than 0.1) can explain most of the differences between TOMS ozone data and ground or in situ ozone measurements. Several examples of real and false TOMS mini-hole phenomenon are investigated using data from the 1989 Airborne Arctic Stratospheric Expedition (AASE) and from balloon flights over Norway and Sweden.

Torres, O.↗
NASA NTRS1992

Reactive nitrogen, ozone, and nitrate aerosols observed in the Arctic stratosphere in January 1990

Ozone mixing ratios in the vicinity of the 525-K potential temperature surface in January and early February of 1990 were observed to decrease sharply across the edge of the vortex boundary, where the vortex position was estimated from Ertel's potential vorticity. The changes in NO(y) mixing ratio with respect to altitude measured on January 18 and 31 were quite well correlated with those of ozone between 15 and 24 km, indicating that NO(y) also had a large gradient across the edge of the vortex. This is interpreted as being mainly due to the significant denitrification that occurred inside the vortex. The total amount of gas and particulate phase HNO3 was close to the NO(y) amount at the altitude of the 22- to 23-km region, suggesting that the conversion of non-HNO3 reactive nitrogen to HNO3 had occurred with a PSC.

Kondo, Y.↗
NASA NTRS1992

An atlas of selected calibrated stellar spectra

Five hundred and fifty six stars in the IRAS PSC-2 that are suitable for stellar radiometric standards and are brighter than 1 Jy at 25 microns were identified. In addition, 123 stars that meet all of our criteria for calibration standards, but which lack a luminosity class were identified. An approach to absolute stellar calibration of broadband infrared filters based upon new models of Vega and Sirius due to Kurucz (1992) is presented. A general technique used to assemble continuous wide-band calibrated infrared spectra is described and an absolutely calibrated 1-35 micron spectrum of alpha(Tau) is constructed and the method using new and carefully designed observations is independently validated. The absolute calibration of the IRAS Low Resolution Spectrometer (LRS) database is investigated by comparing the observed spectrum of alpha(Tau) with that assumed in the original LRS calibration scheme. Neglect of the SiO fundamental band in alpha(Tau) has led to the presence of a specious 'emission' feature in all LRS spectra near 8.5 microns, and to an incorrect spectral slope between 8 and 12 microns. Finally, some of the properties of asteroids that effect their utility as calibration objects for the middle and far infrared region are examined. A technique to determine, from IRAS multiwaveband observations, the basic physical parameters needed by various asteroid thermal models that minimize the number of assumptions required is developed.

Walker, Russell G.↗
NASA NTRS1991

Aircraft laser infrared absorption spectrometer (ALIAS) for polar ozone studies

The ALIAS instrument is a very high resolution (0.0003/cm) scanning, tunable diode laser spectrometer designed to make direct, simultaneous measurements of NO2, HNO3, HCl, CH4, and either O3 or N2O (including vertical profiles of CH4 and N2O) in the polar stratosphere at sub-part-per-billion level sensitivities over integration times from 3 to 30 s. Unique features include a sample inlet/throttle system designed to achieve near-isokinetic sampling, in PSC events, an in-flight wavelength reference cell rack, mechanical fringe-spoilers, a four-laser/four-detector dewar with 24-hr hold-time operating at a fixed temperature without electrical regulation, and in-flight fast correlation routines for spectral drift compensation prior to spectral addition. Instrument design and test flight results are discussed in the light of ALIAS's role in the Winter 1991 Arctic aircraft stratospheric ozone campaigns out of Fairbanks, Alaska, and Bangor, Maine.

Webster, C. R.↗
NASA NTRS1993

Heterogeneous chemistry on Antarctic polar stratospheric clouds - A microphysical estimate of the extent of chemical processing

A detailed model of polar stratospheric clouds (PSCs), which includes nucleation, condensational growth. and sedimentation processes, has been applied to the study of heterogeneous chemical reactions. For the first time, the extent of chemical processing during a polar winter has been estimated for an idealized air parcel in the Antarctic vortex by calculating in detail the rates of heterogeneous reactions on PSC particles. The resulting active chlorine and NO(x) concentrations at first sunrise are analyzed with respect to their influence upon the Antarctic ozone hole using a photochemical model. It is found that the species present at sunrise are primarily influenced by the relative values of the heterogeneous reaction rate constants and the initial gas concentrations. However, the extent of chlorine activation is also influenced by whether N2O5 is removed by reaction with HCl or H2O. The reaction of N2O5 with HCl, which occurs rapidly on type 1 PSCs, activates the chlorine contained in the reservoir species HCl. Hence the presence and surface area of type 1 PSCs early in the winter are crucial in determining ozone depletion.

Drdla, K.↗
NASA NTRS1993

Fourier transform infrared studies of the interaction of HCl with model polar stratospheric cloud films

Heterogeneous reactions involving hydrochloric acid adsorbed on the surfaces of polar stratospheric clouds (PSCs) are postulated to contribute to polar ozone loss. Using FTIR spectroscopy to probe the condensed phase, we have examined the interaction of HCl with ice and nitric acid trihydrate (NAT) films representative of types II and I PSCs, respectively. For HCl pressures in the range of 10 exp -7 to 10 exp -5 Torr, our FTIR studies show that a small amount of crystalline HCl-6H2O formed on or in ice at 155 K. However, for higher HCl pressures, we observed that the entire film of ice rapidly converted into an amorphous 4:1 H2O:HCl mixture. From HCl-uptake experiments with P(HCl) = 8 x 10 exp -7 Torr, we estimate roughly that the diffusion coefficient of HCl in ice is around 2 x 10 exp -12 sq cm/s at 158 K. For higher temperatures more closely approximating those found in the stratosphere, we were unable to detect bulk HCl uptake by ice. Indirect evidence suggests that HCl adsorption onto the surface of model PSC films inhibited the evaporation of both ice and NAT by 3-5 K.

Koehler, Birgit G.↗
NASA NTRS1993

Spectroscopic studies of model polar stratospheric cloud films

Fourier transform infrared (FTIR) spectroscopy has been used to study nitric-acid/ice films representative of type I polar stratospheric clouds (PSCs). These studies reveal that in addition to amorphous nitric acid/ice mixtures, there are three stable stoichiometric hydrates of nitric acid: nitric-acid monohydrate (NAM), dihydrate (NAD), and trihydrate (NAT). We also observe two distinct crystalline forms of the trihydrate, which we denote alpha- and beta-NAT. These two forms appear to differ in their concentration of crystalline defects, but not in their chemical composition. In addition to probing the composition of type I PSCs, we have also used FTIR spectroscopy to study the interaction of HCl with model PSC films. In this work we find that for HCl pressures in the range 10 exp -5 to 10 exp -7 Torr, HCl is taken up by ice at 155 K to form a thin layer of HCl.6H2O. At 193 K, the uptake of HCl by ice was consistent with less than or equal to monolayer coverage. Uptake of HCl by alpha and beta-NAT at 175 K was also consistent with less than or equal to monolayer coverage.

Tolbert, Margaret A.↗
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

Studies of dynamical processes affecting the distribution of stratospheric ozone

The purpose of the research was to understand large-scale tracer transport processes in the stratosphere. Two approaches were taken. The first is analysis of tracer observations, especially satellite observations of ozone concentration and total column ozone. The second is numerical simulation of tracer transport processes. Topics researched include: quasi-biennial oscillation (QBO) and stratospheric ozone; mixing in the polar vortices; polar stratospheric clouds (PSC) properties from Antarctic lidar data; and statistical methods for numerical experiments.

Bowman, Kenneth P.↗
NASA NTRS1993

Stratospheric aircraft exhaust plume and wake chemistry

Progress to date in an ongoing study to analyze and model emissions leaving a proposed High Speed Civil Transport (HSCT) from when the exhaust gases leave the engine until they are deposited at atmospheric scales in the stratosphere is documented. A kinetic condensation model was implemented to predict heterogeneous condensation in the plume regime behind an HSCT flying in the lower stratosphere. Simulations were performed to illustrate the parametric dependence of contrail droplet growth on the exhaust condensation nuclei number density and size distribution. Model results indicate that the condensation of water vapor is strongly dependent on the number density of activated CN. Incorporation of estimates for dilution factors into a Lagrangian box model of the far-wake regime with scale-dependent diffusion indicates negligible decrease in ozone and enhancement of water concentrations of 6-13 times background, which decrease rapidly over 1-3 days. Radiative calculations indicate a net differential cooling rate of the plume about 3K/day at the beginning of the wake regime, with a total subsidence ranging between 0.4 and 1 km. Results from the Lagrangian plume model were used to estimate the effect of repeated superposition of aircraft plumes on the concentrations of water and NO(y) along a flight corridor. Results of laboratory studies of heterogeneous chemistry are also described. Kinetics of HCl, N2O5 and ClONO2 uptake on liquid sulfuric acid were measured as a function of composition and temperature. Refined measurements of the thermodynamics of nitric acid hydrates indicate that metastable dihydrate may play a role in the nucleation of more stable trihydrates PSC's.

Miake-Lye, R. C.↗
NASA NTRS1994

Stratospheric minor species vertical distributions during polar winter by balloon borne UV-Vis spectrometry

A light, relatively cheap and easy to operate balloonborne UV-visible spectrometer was designed for investigating ozone photochemistry in the Arctic winter. The instrument was flown 11 times during the European Arctic Stratospheric Ozone Experiment (EASOE) in winter 1991-92 in Northern Scandinavia. The first simultaneous measurements of vertical distributions of aerosols, PSC's, O3, NO2 and OClO inside the vortex during flight no. 6 on 16 January, in cold conditions are reported, which show that nitrogen oxides were almost absent (lower than 100 ppt) in the stratosphere below 22 km, while a layer of relatively large OClO concentration (15 ppt) was present at the altitude of the minimum temperature.

Pommereau, J. P.↗
NASA NTRS1994

Measurements of the vertical profile, diurnal variation, and secular change of ClO in the stratosphere over Thule, Greenland, February-March, 1992

We report observations of stratospheric chlorine monoxide over the altitude range approx. 16 to 50 km at Thule, Greenland from Feb. 8 to Mar. 24, 1992. A new, more sensitive ground-based mm-wave spectrometer was employed for these measurements, similar in principle to that used earlier for the discovery of low altitude ClO in the Antarctic springtime. In this report, we discuss different aspects of vertical distribution, secular trends, and diurnal variation of ClO in the Arctic stratosphere, based on a preliminary analysis of our Thule data. We see no evidence for large (approx. 1.2-1.5 ppb) amounts of ClO in the lower stratosphere at any time during February or March, in agreement with UARS-MLS findings for this period, and in marked contrast to findings reported for the Arctic in January. We have some evidence for small enhancements (approx. 0.2-0.5 ppb) in the 18-30 km range in late February-early March, which might be associated with volcanic aerosol, rather than PSC, processing.

Dezafra, Robert L.↗
NASA NTRS1994

Ozone, aerosols and polar stratospheric clouds measurements during the EASOE Campaign

Preliminary results are presented of observations obtained during the EASOE campaign, with an airborne backscatter lidar and a ground-based DIAL ozone lidar system. Although the main signature observed on the lidar signals was due to the Pinatubo cloud which erupted in June 1991, distinct PSC events were detected on several occasions by the airborne lidar often in relation with orographic wave activity over the norvegian mountains. The ozone profiles obtained in Sodankyla with the ground based lidar are locally perturbed by the presence of the volcanic cloud. After a first correction of the aerosols effect, they present however a reasonably good agreement with the ozone sondes profiles performed on the same site.

Godin, S.↗
NASA NTRS1994

Observation of ozone and aerosols in the Antarctic ozone hole of 1991 under the Polar Patrol Balloon (PPB) Project. Preliminary result

We present preliminary results for the PPB (Polar Patrol Balloon) experiment. The balloon was launched at 07:55 UT on 23 September and dropped at 21 UT on 28 September 1991. During the period, ozone and aerosol concentrations were measured correspondingly along the track. During the Lagrangian type observation, drastic change of ozone concentration in 'same air mass' and positive correlation between ozone concentration and sulfate aerosol amount were obtained at the level within 80-78 hPa. During the descent motion at 80 deg S active PSC's (type-1 and -2) were observed from 200 hPa to 80 hPa.

Hayashi, Masahiko↗
NASA NTRS1995

Nucleation and growth of crystals under cirrus and polar stratospheric cloud conditions

Laboratory studies examine phase changes of hygroscopic substances which occur as aerosol in stratosphere and troposphere (sodium chloride, ammonium sulfate, ammonium bisulfate, nitric acid, sulfuric acid), under controlled conditions, in samples volume 1 to 10(exp -4) ml. Crystallization of salts from supersaturated solutions is examined by slowly evaporating a solution drop on a substrate, under controlled relative humidity, until self nucleation occurs; controlled nucleation of ice in a mm capillary U-tube gives a measured ice crystallization velocity at known supercooling. Two states of crystallization occur for regions where hydrates exist. It is inferred that all of the materials readily exist as supersaturated/supercooled solutions; the degree of metastability appears to be slightly enhanced by inclusion of aircraft produced soot. The crystallization velocity is taken as a measure of viscosity. Results suggest an approach to a glass transition at high molality, supersaturation and/or supercooling within the range of atmospheric interest. It is hypothesized that surface reactions occur more readily on solidified particles - either crystalline or glass, whereas volume reactions are more important on droplets with sufficiently low viscosity and volume diffusivity. Implications are examined for optical properties of such particles in the atmosphere. In a separate experiment, crystal growth was examined in a modified thermal vapor diffusion chamber over the range of cirrus temperature (-30 to -70 C) and under controlled supersaturation and air pressure. The crystals grew at a velocity of 1-2 microns/s, thickness 60-70 micron, in the form of thin column crystals. Design criteria are given for a system to investigate particle growth down to -100 C, (PSC temperatures) where nitric acid particles can be grown under similar control and in the form of hydrate crystals.

Hallett, John↗