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NASA NTRS1994

Spectral signatures of polar stratospheric clouds and sulfate aerosol

Multiwavelength observations of Antarctic and midlatitude aerosol by the Cryogenic Limb Array Etalon Spectrometer (CLAES) experiment on the Upper Atmosphere Research Satellite (UARS) are used to demonstrate a technique that identifies the location of polar stratospheric clouds. The technique discussed uses the normalized area of the triangle formed by the aerosol extinctions at 925, 1257, and 1605/cm (10.8, 8.0, and 6.2 micrometers) to derive a spectral aerosol measure M of the aerosol spectrum. Mie calculations for spherical particles and T-matrix calculations for spheriodal particles are used to generate theoretical spectral extinction curves for sulfate and polar stratospheric cloud particles. The values of the spectral aerosol measure M for the sulfate and polar stratospheric cloud particles are shown to be different. Aerosol extinction data, corresponding to temperatures between 180 and 220 K at a pressure of 46 hPa (near 21-km altitude) for 18 August 1992, are used to demonstrate the technique. Thermodynamic calculations, based upon frost-point calculations and laboratory phase-equilibrium studies of nitric acid trihydrate, are used to predict the location of nitric acid trihydrate cloud particles.

Massie, S. T.↗
NASA NTRS1986

Characteristics of Arctic polar stratospheric clouds and as measured by airborne lidar

Airborne lidar measurements of backscattering from polar stratospheric clouds (PSCs) obtained in January 1984 are examined. The flights, principal characteristics of the lidar system, and the meteorological conditions during the flights are described. The characteristics and conditions for the formation of PSCs and the optical characteristics of the clouds are discussed. The properties of the North Polar vortex and El Chichon stratospheric aerosol are studied. Variations in the aerosol optical properties with temperature and water vapor concentrations are analyzed and modeled using a model based on volcanic aerosols and water vapor concentration. The modeled and experimental backscattering-temperature relationship are compared and good correlation is observed at pressure levels of 100 and 70 mb.

Kent, G. S.↗
NASA NTRS1988

Influence of polar stratospheric clouds on the depletion of Antarctic ozone

Precipitation of nitrate in polar stratospheric clouds (PSCs) can provide a significant sink for Antarctic stratospheric odd nitrogen. It is argued that the depth of the Ozone Hole is sensitive to the occurrence of temperatures below about 196 K. An increase in the prevalence of temperatures below 196 K would enhance ozone loss by increasing the spatial extent and persistence of PSCs, and by decreasing the level of HNO3 that remains following PSC evaporation. Concentrations of halogen gases in the 1960s and earlier were insufficient to support major ozone loss, even if thermal conditions were favorable.

Salawitch, Ross J.↗
NASA NTRS1989

The interannual variability of polar stratospheric clouds and related parameters in Antarctica during September and October

Antarctic polar stratospheric cloud (PSC) sightings by the orbiting SAM II sensor during September and October show a pronounced quasi-biennial oscillation (QBO) signal, and October sightings have increased markedly over the past 10 years in years of westerly QBO phase. The QBO in PSC frequency is likely to affect the rate of Antarctic heterogeneous chemical processes and, hence, ozone depletion. Studies of the observed long-term temperature trend suggest that the decadal PSC trend probably results from the ozone decline, through its effect on stratospheric heating rates. A more detailed analysis of data from 1986 to 1987 shows that there were more PSCs in 1987, and that they persisted much later into the spring season as compared to 1986. Qualitatively similar behavior was found for the OClO column abundances and 18-km ozone depletion observed at McMurdo Station during these 2 years. These observations suggest that both the intensity and duration of heterogeneous chemical processes are likely greater during colder OBQ-westerly phase years.

Poole, Lamont R.↗
NASA NTRS1993

Vapor pressures of solid hydrates of nitric acid - Implications for polar stratospheric clouds

Thermodynamic data are presented for hydrates of nitric acid: HNO3.H2O, HNO3.2H2O, HNO3.3H2O, and a higher hydrate. Laboratory data indicate that nucleation and persistence of metastable HNO3.2H2O may be favored in polar stratospheric clouds over the slightly more stable HNO3.3H2O. Atmospheric observations indicate that some polar stratospheric clouds may be composed of HNO3.2H2O and HNO3.3H2O. Vapor transfer from HNO3.2H2O to HNO3.3H2O could be a key step in the sedimentation of HNO3, which plays an important role in the depletion of polar ozone.

Worsnop, Douglas R.↗
NASA NTRS1988

Airborne lidar observations of Arctic polar stratospheric clouds - Indications of two distinct growth stages

Airborne lidar observations of Arctic polar stratospheric clouds (PSCs) during January 1984 and January 1986 show contrast suggestive of two distinct PSC growth stages delineated by the frost-point temperature. Results obtained at temperatures 2-6 K above the frost point indicate a stage of significant, but limited, particle growth such as proposed in recent models of PSC formation by co-deposition of HNO3 and H2O vapors. Results obtained at a temperature near the frost point indicate the formation of somewhat larger crystalline particles.

Poole, Lamont R↗
NASA NTRS1994

Real refractive indices of infrared-characterized nitric-acid/ice films: Implications for optical measurements of polar stratospheric clouds

The infrared spectra of nitric-acid/ice films representative of polar stratospheric clouds (PSCs) were collected with simultaneous optical interference measurements to determine the real refractive indices at lambda = 632 nm. Ice and amphorous nitric-acid/ice films were prepared by condensation of water and nitric acid vapors onto a wedged Al2O3 substrate. The real refractive indices of these films were determined from the optical interference of a reflected helium-neon laser during film growth. The indices of the amphorous films varied smoothly from n = 1.30 for ice to n = 1.49 for nitric acid, similar to observations in previous work. We were unable to obtain the refractive index of crystlline films during adsorption because of optical scattering caused by surface roughness. Therefore crystlline nitric acid hydrate films were prepared by annealing amphorous nitric-acid/ice films. Further heating caused desorption of the crystalline hydrate films. During desorption, the refractive indices for ice, NAM (nitric acid monohydrate), alpha- and beta-NAT (nitric acid trihydrate) films were measured using the optical interference technique. In agreement with earlier data, the real refractive indices for ice and NAM determined in desorption were n = 1.30 +/- 0.01 and n = 1.53 +/- 0.03, respectively. The real refractive indices for alpha- and beta-NAT were found to be n = 1.51 +/- 0.01 and n greater than or equal to 1.46, respectively. Our measurements also suggest that the shape of crystalline nitric acid particles may depend on whether they nucleate from the liquid or by vapor deposition. If confirmed by future studies, this observation may provide a means of distinguishing the nucleation mechanism of crystalline PSCs.

Middlebrook, Ann M.↗
NASA NTRS1990

Nitric acid in polar stratospheric clouds - Similar temperature of nitric acid condensation and cloud formation

As shown independently by two different techniques, nitric acid aerosols and polar stratospheric clouds (PSCs) both form below similar threshold temperatures. This supports the idea that the PSC particles involved in chlorine activation and ozone depletion in the winter polar stratosphere are composed of nitric acid. One technique used to show this is the inertial impaction of nitric acid aerosols using an Er-2 aircraft; the other method is remote sensing of PSCs by the Stratospheric Aerosol Measurement (SAM II) satellite borne optical sensor. Both procedures were in operation during the Arctic Airborne Stratospheric Expedition in 1989, and the Airborne Antarctic Ozone Experiment in 1987. Analysis of Arctic particles gathered in situ indicates the presence of nitric acid below a 'first appearance' temperature Tfa = 202 K. This is the same highest temperature at which PSCs are seen by the SAM II satellite. In comparison, a 'first appearance' temperature Tfa = 198 K as found for the Antarctic samples.

Pueschel, Rudolf F.↗
NASA NTRS1986

Characteristics of polar stratospheric clouds during the formation of the Antarctic ozone hole

Measured properties of Antarctic polar stratospheric clouds are described, and the possible relationship between the clouds and the formation of the ozone hole is considered. It is shown that the ozone hole develops and the clouds dissipate in the same place and at the same time. There may be a causal relationship between cloud particle evaporation and ozone depletion. A heterogeneous mechanism involving chemical reactions in the cloud droplets is suggested.

Hamill, Patrick↗
NASA NTRS1994

A study of Type I polar stratospheric cloud formation

Mechanisms for the formation of Type I (nitric acid-based) polar stratospheric clouds (PSCs) are discussed. If the pre-existing sulfate aerosols are liquid prior to PSC formation, then nitric acid particles (Type Ib) form by HNO3 dissolution in aqueous H2SO4 solution droplets. This process does not require a nucleation step for the formation of HNO3 aerosols, so most pre-existing aerosols grow to become relatively small HNO3-containing particles. At significantly lower temperatures, the resulting supercooled solutions (Type Ib) may freeze to form HNO3 ice particles (Type Ia). If the pre-existing sulfate aerosols are initially solid before PSC formation, then HNO3 vapor can be deposited directly on the frozen sulfate particles. However, because an energy barrier to the condensation exists a nucleation mechanism is involved. Here, we suggest a unique nucleation mechanism that involves formation of HNO3/H20 solutions on the sulfate ice particles. These nucleation processes may be highly selective, resulting in the formation of relatively small number of large particles.

Tabazadeh, A.↗
NASA NTRS2006

Detection of Ice Polar Stratospheric Clouds from Assimilation of Atmospheric Infrared Sounder Data

A novel technique is presented for detection of ice polar stratospheric clouds (PSCs) that form at extremely low temperatures in the lower polar stratosphere during winter. Temperature is a major factor in determining abundance of PSCs, which in turn provide surfaces for heterogeneous chemical reactions leading to ozone loss and radiative cooling. The technique infers the presence of ice PSCs using radiances from the Atmospheric Infrared Sounder (AIRS) in the Goddard Earth Observing System version 5 (GEOS-5) data assimilation system. Brightness temperatures are computed from short-term GEOS-5 forecasts for several hundred AIRS channels, using a radiation transfer module. The differences between collocated AIRS observations and these computed values are the observed-minus-forecast (O-F) residuals in the assimilation system. Because the radiation model assumes clear-sky conditions, we hypothesize that these O-F residuals contain quantitative information about PSCs. This is confirmed using sparse data from the Polar Ozone and Aerosol Measurement (POAM) III occultation instrument. The analysis focuses on 0-F residuals for the 6.79pm AIRS moisture channel. At coincident locations, when POAM III detects ice clouds, the AIRS O-F residuals for this channel are lower than -2K. When no ice PSCs are evident in POAM III data, the AIRS 0-F residuals are larger. Given this relationship, the high spatial density of AIRS data is used to construct maps of regions where 0-F residuals are lower than -2K, as a proxy for ice PSCs. The spatial scales and spatio-temporal variations of these PSCs in the Antarctic and Arctic are discussed on the basis of these maps.

Stajner, Ivanka↗
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 NTRS1992

More rapid polar ozone depletion through the reaction of HOCl with HCl on polar stratospheric clouds

The direct reaction of HOCl with HCl is shown here to play a critical part in polar ozone loss. Observations of high levels of OClO and ClO in the springtime Antarctic stratosphere confirm that most of the available chlorine is in the form of ClO(x). But current photochemical models have difficulty converting HCl to ClO(x) rapidly enough in early spring to account fully for the observations. Here, a chemical model is used to show that the direct reaction of HOCl with HCl provides the missing mechanism. As alternative sources of nitrogen-containing oxidants have been converted in the late autumn to inactive HNO3 by known reactions on the sulfate layer aerosols, the reaction of HOCl with HCl on polar stratospheric clouds becomes the most important pathway for releasing that stratospheric chlorine which goes into polar night as HCl.

Prather, Michael J.↗
NASA NTRS1996

Comparisons Between the Formation of Polar Stratospheric Clouds and Cirrus Clouds

Analyses of lidar data taken during the 1989 AASE I program show that polar stratospheric clouds most often contain frozen particles, but sometimes contain spherical, presumably liquid, particles. In this paper the mechanisms that lead to the freezing of particles, and to the formation of liquid particles will be discussed based largely upon analyses of existing data. For example, trajectory studies help shed light on the conditions that lead to particle freezing. During April of 1996 an experiment using the NASA DC-8 and ER-2 aircraft will be conducted over the central U.S. Some of the goals of the project are to better understand the mechanisms of cirrus cloud formation, and to investigate the properties of freezing nuclei in the upper troposphere. Results from this field program will be presented as they apply to the topic of ice crystal nucleation. Comparisons will be drawn between the mechanisms that lead to new particle formation in the polar stratosphere, and the mechanisms that lead to new particles formation in the upper troposphere.

Toon, Owen B.↗
NASA NTRS1990

Heterogeneous conversion of COF2 to HF in polar stratospheric clouds

It is argued that the reaction COF2 + H2O - 2HF + CO2 should proceed on surfaces of polar stratospheric clouds, based on laboratory evidence for this reaction in condensed phase and on analysis of column observations of HF during the Airborne Arctic Stratospheric Expedition. If the hypothesis is confirmed, observations of COF2 and HF could provide unambiguous indication of heterogeneous processing of polar air, and could help elucidate the influence of heterogeneous chemistry on concentrations of HCl, ClNO3, and chlorine oxide radicals.

Wofsy, Steven C.↗
NASA NTRS1994

Freezing temperatures of H2SO4/HNO3/H2O mixtures: Implications for polar stratospheric clouds

The freezing temperatures of H2SO4/HNO3/H2O mixtures were systematically documented. Nitric acid was found to affect freezing significantly. Measurements show that nitric acid can cause substantial supercooling over a broad composition range. However, some ternary compositions, like to those in polar stratospheric clouds (PSCs), have high freezing temperatures. The freezing of PSC particles could be controlled by the temperature and vapor pressure of both nitric acid and water in a non-linear way. Formation of polar stratospheric clouds may be forecasted on the basic of conditions of temperature and vapor contents of water and nitric acid.

Song, Naihui↗
NASA NTRS1988

Polar stratospheric clouds and the Antarctic ozone hole

A theoretical model for the formation and growth of polar stratospheric clouds (PSCs) has been developed. Results for the calculated temperature dependence of optical backscattering are found to agree well with values obtained during two Arctic airborne-lidar experiments. Results for PSC formation in Antarctica show that at the 70-mbar level, about 80 percent of the HNO3 and about 30 percent of the H2O vapor available may be sequestered in relatively large PSC particles at a temperature near 189 K.

Poole, Lamont R.↗
NASA NTRS1994

Arctic polar stratospheric cloud measurements by means of a four wavelength depolarization lidar

A four wavelength depolarization backscattering lidar has been operated during the European Arctic Stratospheric Ozone Experiment (EASOE) in Sodankyl, in the Finnish Arctic. The lidar performed measurements during the months of December 1991, January, February and March 1992. The Finnish Meteorological Institute during the same period launched regularly three Radiosondes per day, and three Ozone sondes per week. Both Mt. Pinatubo aerosols and Polar Stratospheric Clouds were measured. The use of four wavelengths, respectively at 355 nm, 532 nm , 750 nm, and 850 nm permits an inversion of the lidar data to determine aerosol particle size. The depolarization technique permits the identification of Polar Stratospheric Clouds. Frequent correlation between Ozone minima and peaks in the Mt. Pinatubo aerosol maxima were detected. Measurements were carried out both within and outside the Polar Vortex.

Stefanutti, L.↗