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NASA NTRS1997

A Laboratory Study on the Phase Transition for Polar Stratospheric Cloud Particles

The nucleation and growth of different phases of simulated polar stratospheric cloud (PSC) particles were investigated in the laboratory. Solutions and mixtures of solutions at concentrations 1 to 5 m (molality) of ammonium sulfate, ammonium bisulfate, sodium chloride, sulfuric acid, and nitric acid were supercooled to prescribed temperatures below their equilibrium melting point. These solutions were contained in small diameter glass tubing of volumes ranging from 2.6 to 0.04 ml. Samples were nucleated by insertion of an ice crystal, or in some cases by a liquid nitrogen cooled wire. Crystallization velocities were determined by timing the crystal growth front passages along the glass tubing. Solution mixtures containing aircraft exhaust (soot) were also examined. Crystallization rates increased as deltaT2, where deltaT is the supercooling for weak solutions (2 m or less). The higher concentrated solutions (greater than 3 m) showed rates significantly less than deltaT2. This reduced rate suggested an onset of a glass phase. Results were applied to the nucleation of highly concentrated solutions at various stages of polar stratospheric cloud development within the polar stratosphere.

Teets, Edward H., Jr.↗
NASA NTRS1990

Microphysics of polar stratospheric clouds

Theoretical research on the microphysics of polar stratospheric clouds (PSCs) is reviewed. Problems discussed include microphysical features of PSCs, the Antarctic ozone depletion, and a comparison of PSC microphysical characteristics with those of low-level polar stratus clouds over the Antarctic coast.

Saxena, V. K.↗
NASA NTRS1988

Evolution of polar stratospheric clouds during the Antarctic winter

The occurrence of Polar Stratospheric Clouds (PSCs), initially inferred from satellite measurements of solar extinction, have now also been noted by the recent scientific expeditions in the Antarctic. The presence of such clouds in the Antarctic has been postulated to play a significant role in the depletion of ozone during the transition from winter to spring. The mechanisms suggested involve both dynamical and chemical processes which, explicity or implicitly, are associated with the ice particles constituting the PSCs. It is, thus, both timely and necessary to investigate the evolution of these clouds and ascertain the nature and magnitude of their influences on the state of the Antarctic stratosphere. To achieve these objectives, a detailed microphysical model of the processes governing the growth and sublimation of ice particles in the polar stratosphere was developed, based on the investigations of Ramaswamy and Detwiler. The present studies focus on the physical processes that occur at temperatures below those required for the onset of ice deposition from the vapor phase. Once these low temperatures are attained, the deposition of water vapor onto nucleation particles becomes extremely significant. First, the factors governing the magnitude of growth and the growth rate of ice particles at various altitudes are examined. Second, the ice phase mechanisms are examined in the context of a column model with altitudes ranging from 100 to 5 mb pressure levels. The column microphysical model was used to perform simulations of the cloud evolution, using the observed daily temperatures. The effect due to the growth of the particles on the radiation fields are also investigated using a one dimensional radiative transfer model. Specifically, the perturbations in the longwave cooling and that in the shortwave heating for the late winter/early spring time period are analyzed.

Ramaswamy, V.↗
NASA NTRS1995

Estimation of polar stratospheric cloud infrared extinction climatology using visible satellite observations

Polar stratospheric clouds (PSC's) provide surfaces for heterogeneous processes which can dramatically alter the normal partitioning of odd nitrogen and chlorine families in the winter polar stratospheres, setting up conditions for significant ozone depletion as manifested in the springtime Antarctic ozone hole. The spatial and temporal distribution of PSC's is important for parameterizing PSC occurrence in multidimensional photochemical models whose use is essential for fully understanding observed Antarctic ozone losses as well as for accessing the possibility of a similar phemonenon occurring in the future in the Arctic. The Stratospheric Aerosol Measurement (SAM) 2 sensor, a single-channel (1mu m) photometer launched into a Sun-synchronous orbit aboard the Nimbus 7 satellite in October 1978, provided a unique database to establish the climatology of PSC's. Poole and Pitts (1994) used the record of high-latitude aerosol extinction obtained by SAM II from 1979-1989 to establish the climatology of PSC occurrences in the Arctic and Antarctic. Unfortunately, little information about PSC composition or type was detectable from the single-wavelength SAM II data.

Pitts, Michael C.↗
NASA NTRS1991

Polar stratospheric clouds and the ozone hole

An account is given of physical processes governing the formation of stratospheric particles, in order to dramatize the interactions between polar stratospheric clouds and the Antarctic ozone-destruction mechanism. Attention is given to the successive stages of particle nucleation, condensation/evaporation and sedimentation/coagulation phenomena, and the ways in which polar stratospheric clouds are observed. Considerable evidence exists that polar stratospheric cloud particles are composed of nitric acid. The relatively small Arctic ozone hole depletion is due to the much smaller duration of Arctic stratospheric clouds.

Hamill, Patrick↗
NASA NTRS1990

Optical backscatter characteristics of Arctic polar stratospheric clouds

Airborne lidar measurements have been made of polar stratospheric clouds (PSCs) during the Airborne Arctic Stratospheric Expedition in January-February 1989. These show the existence of a systematic relationship between the backscatter depolarization ratio and the (aerosol + molecular)/molecular backscatter ratio. The data are consistent with a two population PSC particle model.

Kent, G. S.↗
NASA NTRS1992

Radiative effects of polar stratospheric clouds during the Airborne Antarctic Ozone Experiment and the Airborne Arctic Stratospheric Expedition

Results are presented of a study of the radiative effects of polar stratospheric clouds during the Airborne Antarctic Ozone Experiment (AAOE) and the Airborne Arctic Stratospheric Expedition (AASE) in which daily 3D Type I nitric acid trihydrate (NAT) and Type II water ice polar stratospheric clouds (PSCs) were generated in the polar regions during AAOE and the AASE aircraft missions. Mission data on particular composition and size, together with NMC-analyzed temperatures, are used. For AAOE, both Type I and Type II clouds were formed for the time period August 23 to September 17, after which only Type I clouds formed. During AASE, while Type I clouds were formed for each day between January 3 and February 10, Type II clouds formed on only two days, January 24 and 31. Mie theory and a radiative transfer model are used to compute the radiative heating rates during the mission periods, for clear and cloudy lower sky cases. Only the Type II water ice clouds have a significant radiative effect, with the Type I NATO PSCs generating a net heating or cooling of 0.1 K/d or less.

Rosenfield, Joan E.↗
NASA NTRS2007

Characterization of Polar Stratospheric Clouds With Spaceborne Lidar: CALIPSO and the 2006 Antarctic Season

The role of polar stratospheric clouds in polar ozone loss has been well documented. The CALIPSO satellite mission offers a new opportunity to characterize PSCs on spatial and temporal scales previously unavailable. A PSC detection algorithm based on a single wavelength threshold approach has been developed for CALIPSO. The method appears to accurately detect PSCs of all opacities, including tenuous clouds, with a very low rate of false positives and few missed clouds. We applied the algorithm to CALIPSO data acquired during the 2006 Antarctic winter season from 13 June through 31 October. The spatial and temporal distribution of CALIPSO PSC observations is illustrated with weekly maps of PSC occurrence. The evolution of the 2006 PSC season is depicted by time series of daily PSC frequency as a function of altitude. Comparisons with virtual solar occultation data indicate that CALIPSO provides a different view of the PSC season than attained with previous solar occultation satellites. Measurement-based time series of PSC areal coverage and vertically-integrated PSC volume are computed from the CALIPSO data. The observed area covered with PSCs is significantly smaller than would be inferred from a temperature-based proxy such as TNAT but is similar in magnitude to that inferred from TSTS. The potential of CALIPSO measurements for investigating PSC microphysics is illustrated using combinations of lidar backscatter coefficient and volume depolarization to infer composition for two CALIPSO PSC scenes.

Pitts, Michael C.↗
NASA NTRS1992

Lidar Observations of Polar Stratospheric Clouds and Stratospheric Temperatures at the South Pole

Polar stratospheric clouds (PSC's) play a crucial role in the ozone chemistry of the polar regions. Current chemical models rely on the presence of these clouds to explain the rapid destruction of ozone observed each spring in Antarctica. We present lidar observations of PCS's and stratospheric temperatures at the South Pole throughout the Antarctic winter and spring of 1990.

Collins, Richard L.↗
NASA NTRS1996

Simultaneous Observations fo Polar Stratospheric Clouds and HNO3 over Scandinavia in January, 1992

Simultaneous observations of Polar Stratospheric Cloud aerosol extinction and HNO3 mixing ratios over Scandinavia are examined for January 9-10, 1992. Data measured by the Microwave Limb Sounder (MLS), Cryogenic Limb Array Etalon, Spectrometer (CLAES), and Improved Stratospheric and Mesospheric Sounder (ISAMA) experiments on the Upper Atmosphere Research Satellite (UARS) are examined at locations adjacent to parcel trajectory positions.

PSC polar stratospheric clouds uars upper atmosphe↗
NASA NTRS2006

The Sensitivity of Arctic Ozone Loss to Polar Stratospheric Cloud Volume and Chlorine and Bromine Loading in a Chemistry and Transport Model

The sensitivity of Arctic ozone loss to polar stratospheric cloud volume (V(sub PSC)) and chlorine and bromine loading is explored using chemistry and transport models (CTMs). A simulation using multi-decadal output from a general circulation model (GCM) in the Goddard Space Flight Center (GSFC) CTM complements one recycling a single year s GCM output in the Global Modeling Initiative (GMI) CTM. Winter polar ozone loss in the GSFC CTM depends on equivalent effective stratospheric chlorine (EESC) and polar vortex characteristics (temperatures, descent, isolation, polar stratospheric cloud amount). Polar ozone loss in the GMI CTM depends only on changes in EESC as the dynamics repeat annually. The GSFC CTM simulation reproduces a linear relationship between ozone loss and Vpsc derived from observations for 1992 - 2003 which holds for EESC within approx.85% of its maximum (approx.1990 - 2020). The GMI simulation shows that ozone loss varies linearly with EESC for constant, high V(sub PSC).

Douglass, A. R.↗
NASA NTRS1989

Studies of radiative effects for polar stratospheric clouds

Data from the Antarctic Ozone Experiment of 1987 are used to model the radiative effects of polar stratospheric clouds. Heating and cooling rates are examined, showing that the heating and/or cooling rates within a polar stratospheric cloud depend on particle size, composition, optical depth of the cloud, solar angle, and temperature profile. The rates for an optically thin Type I cloud are too small to drive vertical motions in the stratosphere, while optically thin Type II clouds cause a stratospheric cooling.

Kinne, S.↗
NASA NTRS2024

Antarctic polar stratospheric cloud composition as observed by ACE, CALIPSO and MIPAS

The composition of polar stratospheric clouds (PSCs) in the Antarctic is measured by infrared absorption spectroscopy by the Atmospheric Chemistry Experiment (ACE) satellite and compared to lidar (CALIPSO) and emission spectroscopy (MIPAS) results. ACE observations are compared first to CALIPSO for the period 2006–2020, then to MIPAS for the period 2005–2011, and then a set of triple coincidences is studied. In both CALIPSO-ACE and MIPAS-ACE comparisons, nitric acid trihydrate (NAT) detections are in excellent agreement (∼80 % of coincident compositions is found). Supercooled ternary solution (STS) detections are in good agreement for CALIPSO-ACE (∼60 %) but in poor agreement for MIPAS-ACE (39 %). This contrasts with ice detections, in poor agreement for CALIPSO-ACE (∼30 %) and in better agreement for MIPAS-ACE (45 %). Triple coincidences show that ACE STS detections are more reliable than MIPAS STS detections. The comparison between ACE observations and homogeneous CALIPSO PSCs shows that for 11 events, CALIPSO reports STS rather than supercooled nitric acid (SNA) clouds.

Atmospheric Chemistry Experiment↗
NASA NTRS2023

Comparison between ACE and CALIPSO observations of Antarctic polar stratospheric clouds

The depletion of stratospheric ozone is catalyzed by polar stratospheric clouds (PSCs) that form in the cold polar winter. The space-based lidar onboard CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations) has been the reference instrument for measuring PSCs. Recently, the infrared transmission spectra recorded by the Fourier transform instrument on the ACE (Atmospheric Chemistry Experiment) satellite has provided measurements of PSC composition. We report on coincident observations made by the CALIPSO and the ACE satellites for three late winter periods (2016, 2018 and 2019) and evaluate CALIPSO's determination of PSC composition relative to ACE’s findings. We found that CALIPSO and ACE generally agree well for the detection of nitric acid trihydrate (NAT) clouds. However, CALIPSO detects some NAT clouds where ACE detects supercooled ternary solutions of nitric and sulfuric acid (STS). Similarly, CALIPSO only partially detects ice in ACE's ice clouds. Overall, these results seem to show that CALIPSO’s NAT classification might be too inclusive. We also found that supercooled nitric acid (SNA) clouds, a new classification, are labelled as STS by CALIPSO

Léo Lavy↗
NASA NTRS1992

An experimental study of growth and phase change of polar stratospheric cloud particles

This report describes the progress made on understanding phase changes related to solutions which may comprise Polar Stratospheric Clouds. In particular, it is concerned with techniques for investigating specific classes of metastability and phase change which may be important not only in Polar Stratospheric Clouds but in all atmospheric aerosols in general. While the lower level atmospheric aerosol consists of mixtures of (NH4)(SO4)2, NH4HSO4, NaCl among others, there is evidence that aerosol at PSC levels is composed of acid aerosol, either injected from volcanic events (such as Pinatubo) or having diffused upward from the lower atmosphere. In particular, sulfuric acid and nitric acid are known to occur at PSC levels, and are suspected of catalyzing ozone destruction reactions by adsorption on surfaces of crystallized particles. The present study has centered on two approaches: (1) the extent of supercooling (with respect to ice) and supersaturation (with respect to hydrate) and the nature of crystal growth in acid solutions of specific molality; and (2) the nature of growth from the vapor of HNO3 - H2O crystals both on a substrate and on a pre-existing aerosol.

Hallett, John↗
NASA NTRS1989

Measurements of size and composition of particles in polar stratospheric clouds from infrared solar absorption spectra

Results are presented on polar stratospheric cloud (PSC) observations, based on IR measurements of solar extinction, made by the airborne JPL Mark IV interferometer during the Airborne Antarctic Ozone Expedition in 1987, together with the instrumentation and the theoretical aspects of data analysis. Thirty-three PSC cases were analyzed and categorized into two types, I and II, which were found to occur at different altitudes during September. Type I clouds, seen at altitudes above 15 km, contained particles with radii of about 0.5 micarons and nitric acid concentrations greater than 40 percent, while type II clouds, found usually below 15 km, contained particles with radii of 6 microns and larger, composed of water ice. In addition, particles of larger than the 15-micron-size detection limit were encounterd.

Kinne, S.↗
NASA NTRS1990

SAGE II observations of polar stratospheric clouds near 50 deg N January 31 - February 2, 1989

Polar stratospheric clouds (PSCs) form at very cold temperatures which typically occur only at high latitudes during local winter. However, meteorological circumstances in the Arctic during late January 1989 led to PSC formation unusually far to the south, at latitudes (near 50 deg N) being sampled during the period by the orbiting SAGE II instrument. These unusual PSC sightings and the evolution of meteorological conditions which produced the episode are described. Profiles of SAGE II extinction measurements at 0.525 and 1.02 microns show clear signatures of PSCs and indicate that the cloud particles were considerably larger than the background aerosol. It is most important to note that the clouds were sighted at a latitude where there was extensive sunlight, thus increasing the likelihood of ozone loss both locally and downstream due to enhancements in reactive chlorine expected from heterogeneous chemical processing within the PSCs.

Pitts, M. C.↗
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.↗