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NASA NTRS1986

Airborne lidar observations of Arctic polar stratospheric clouds

Polar stratospheric clouds (PSC's) have been detected repeatedly during Arctic and Antarctic winters since 1978/1979 by the SAM II (Stratospheric Aerosol Measurement II) instrument aboard the NIMBUS-7 satellite. PSC's are believed to form when supercooled sulfuric acid droplets freeze, and subsequently grow by deposition of ambient water vapor as the local stratospheric temperature falls below the frost point. In order to study the characteristics of PSC's at higher spatial and temporal resolution than that possible from the satellite observations, aircraft missions were conducted within the Arctic polar night vortex in Jan. 1984 and Jan. 1986 using the NASA Langley Research Center airborne dual polarization ruby lidar system. A synopsis of the 1984 and 1986 PSC observations is presented illustrating short range spatial changes in cloud structure, the variation of backscatter ratio with temperature, and the depolarization characterics of cloud layers. Implications are noted with regard to PSC particle characteristics and the physical process by which the clouds are thougth to form.

Poole, L. R.↗

NASA NTRS1990

Airborne lidar observations in the wintertime Arctic stratosphere - Polar stratospheric clouds

Polar stratospheric cloud (PSC) distributions in the wintertime Arctic stratosphere and their optical characteristics were measured with a multiwavelength airborne lidar system as part of the 1989 Airborne Arctic Stratospheric Expedition. PSCs were observed on 10 flights between January 6 and February 2, 1989, into the polar vortex. The PSCs were found in the 14-27 km altitude range in regions where the temperatures were less than 195 K. Two types of aerosols with different optical characteristics (Types 1a and 1b) were observed in PSCs thought to be composed of nitric acid trihydrate. Water ice PSCs (Type 2) were observed to have high scattering ratios (greater than 10) and high aerosol depolarizations (greater than 10 percent) at temperatures less than 190 K.

Browell, E. V.↗

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 NTRSDate not supplied

A Synopsis of the 8+ Year CALIOP Polar Stratospheric Cloud Data Record

Polar stratospheric clouds (PSCs) play a crucial role in the springtime chemical depletion of ozone at high latitudes. PSC particles (primarily supercooled ternary solution, or STS droplets) provide sites for heterogeneous chemical reactions that transform stable chlorine and bromine reservoir species into highly reactive ozone-destructive forms. Furthermore, large nitric acid trihydrate (NAT) PSC particles can irreversibly redistribute odd nitrogen through gravitational sedimentation (a process commonly known as denitrification), which prolongs the ozone depletion process by slowing the reformation of the stable chlorine reservoirs. Spaceborne observations from the CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) lidar on the CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations) satellite are providing a rich new dataset for studying PSCs. CALIPSO is an excellent platform for studying polar processes with CALIOP acquiring, on average, over 300,000 backscatter profiles daily at latitudes between 55o and 82o in both hemispheres. PSCs are detected in the CALIOP backscatter profiles using a successive horizontal averaging scheme that enables detection of strongly scattering PSCs (e.g., ice) at the finest possible spatial resolution (5 km), while enhancing the detection of very tenuous PSCs (e.g., low number density NAT) at larger spatial scales (up to 135 km). CALIOP PSCs are separated into composition classes (STS; liquid/NAT mixtures; and ice) based on the ensemble 532-nm scattering ratio (the ratio of total-to-molecular backscatter) and 532-nm particulate depolarization ratio (which is sensitive to the presence of non-spherical, i.e. NAT and ice particles). In this paper, we will provide an overview of the CALIOP PSC detection and composition classification algorithm and then examine the vertical and spatial distribution of PSCs in the Arctic and Antarctic on vortex-wide scales for entire PSC seasons over the more than eight-year data record.

Michael C Pitts↗

NASA NTRS1988

The ozone hole - The role of polar stratospheric cloud particles

The role of polar stratospheric clouds in the formation of the Antarctic ozone hole is considered. Several researchers have suggested that the decrease in ozone over Antarctica is related to the polar stratospheric clouds (PSCs) which had been observed in the antarctic winter stratosphere. Some of the pertinent characteristics of polar stratospheric clouds are discussed, and it is shown how these clouds may participate in the ozone destruction process. The satellite data for PSCs is analyzed, and statistical information regarding the number and maximum extinctions of these clouds is presented. Evidence that the polar stratospheric clouds are composed of frozen nitric acid is considered. It is suggested that the evaporation of the clouds, in late August and September, will release HOCl and HNO3 to the environment. This could be followed by the photodissociation of HOCl to OH and Cl, which would very effectively destroy ozone. However, the ozone destruction mechanism could be halted when enough of the evaporated nitric acid is photolized.

Hamill, Patrick↗

NASA NTRS1989

Persistence of polar stratospheric clouds in the southern polar region

Observations of Antarctic polar stratospheric clouds (PSCs) were examined using the 1-micron aerosol extinction ratio data from the SAM II satellite experiment for the years 1979-1982 and 1984-1987. PSCs were sighted between 10 and 25 km and were usually first observed by mid-June. Clouds disappeared earlier at higher altitudes (late August near 24 km, in most cases) and later at lower altitudes (late September or October near 16 km). It was found that PSCs persisted longer in 1985 and 1987 at 18 km and were more frequently observed in September and October 1987 than the other years. Inference of likely PSC formation regions from National Meteorological Center temperature data indicated that clouds would begin forming in late May and usually disappear in September. This analysis confirmed the persistence of colder conditions during the spring of 1987.

Mccormick, M. P.↗

NASA NTRS2009

Continuous Lidar Monitoring of Polar Stratospheric Clouds at the South Pole

Polar stratospheric clouds (PSC) play a primary role in the formation of annual ozone holes over Antarctica during the austral sunrise. Meridional temperature gradients in the lower stratosphere and upper troposphere, caused by strong radiative cooling, induce a broad dynamic vortex centered near the South Pole that decouples and insulates the winter polar airmass. PSC nucleate and grow as vortex temperatures gradually fall below equilibrium saturation and frost points for ambient sulfate, nitrate, and water vapor concentrations (generally below 197 K). Cloud surfaces promote heterogeneous reactions that convert stable chlorine and bromine-based molecules into photochemically active ones. As spring nears, and the sun reappears and rises, photolysis decomposes these partitioned compounds into individual halogen atoms that react with and catalytically destroy thousands of ozone molecules before they are stochastically neutralized. Despite a generic understanding of the ozone hole paradigm, many key components of the system, such as cloud occurrence, phase, and composition; particle growth mechanisms; and denitrification of the lower stratosphere have yet to be fully resolved. Satellite-based observations have dramatically improved the ability to detect PSC and quantify seasonal polar chemical partitioning. However, coverage directly over the Antarctic plateau is limited by polar-orbiting tracks that rarely exceed 80 degrees S. In December 1999, a NASA Micropulse Lidar Network instrument (MPLNET) was first deployed to the NOAA Earth Systems Research Laboratory (ESRL) Atmospheric Research Observatory at the Amundsen-Scott South Pole Station for continuous cloud and aerosol profiling. MPLNET instruments are eye-safe, capable of full-time autonomous operation, and suitably rugged and compact to withstand long-term remote deployment. With only brief interruptions during the winters of 2001 and 2002, a nearly continuous data archive exists to the present.

OZONE DESTRUCTION↗

NASA NTRS1988

Persistence of Antarctic polar stratospheric clouds

The persistence of Polar Stratospheric Clouds (PSCs) observed by the Stratospheric Aerosol Measurement (SAM) 2 satellite sensor over a 9-year period is compared and contrasted. Histograms of the SAM 2 1.0 micron extinction ratio data (aerosol extinction normalized by the molecular extinction) at an altitude of 18 km in the Antarctic have been generated for three 10-day periods in the month of September. Statistics for eight different years (1979 to 1982 and 1984 to 1987) are shown in separate panels for each figure. Since the SAM 2 system is a solar occultation experiment, observations are limited to the edge of the polar night and no measurements are made deep within the vortex where temperatures could be colder. For this reason, use is made of the NMC global gridded fields and the known temperature-extinction relationship to infer additional information on the occurrence and areal coverage of PSCs. Calculations of the daily areal coverage of the 195 K isotherm will be presented for this same period of data. This contour level lies in the range of the predicted temperature for onset of the Type 1 particle enhancement mode at 50 mb (Poole and McCormick, 1988b) and should indicate approximately when formation of the binary HNO3-H2O particles begins.

Mccormick, M. Patrick↗

NASA NTRS1995

Spectroscopic Evidence Against Nitric Acid Trihydrate in Polar Stratospheric Clouds

Heterogeneous reactions on polar stratospheric clouds (PSC's) play a key role in the photochemical mechanism thought to be responsible for ozone depletion in the Antarctic and Arctic. Reactions of PSC particles activate chlorine to forms that are capable of photochemical ozone destruction, and sequester nitrogen oxides (NOx) that would otherwise deactivate the chlorine. Although the heterogeneous chemistry is now well established, the composition of the clouds themselves is uncertain. It is commonly thought that they are composed of nitric acid trihydrate, although observations have left this question unresolved. Here we reanalyse infrared spectra of type 1 PSCs obtained in Antarctica in September 1987, using recently measured optical constants of the various compounds that might be present in PSCs. We find these PSCs were not composed of nitric acid trihydrate but instead had a more complex compositon, perhaps that of a ternary solution. Because cloud formation is sensitive to their composition, this finding will alter our understanding of the locations and conditions in which PSCs form. In addition, the extent of ozone loss depends on the ability of the PSCs to remove NOx permanently through sedimentation, The sedimentation rates depend on PSC particle size which in turn is controlled by the composition and formation mechanism.

Toon, Owen B.↗

NASA NTRS1995

Spectroscopic Evidence Against Nitric Acid Trihydrate in Polar Stratospheric Clouds

Heterogeneous reactions on polar stratospheric clouds (PSC's) play a key role in the photochemical mechanisms thought to be responsible for ozone depletion in the Antarctic and the Arctic. Reactions on PSC particles activate chlorine to forms that are capable of photochemical ozone destruction, and sequester nitrogen oxides (NOx) that would otherwise deactivate the chlorine. Although the heterogeneous chemistry is now well established, the composition of the clouds themselves is uncertain. It is commonly thought that they are composed of nitric acid trihydrate, although observations have left this question unresolved. Here we reanalyse infrared spectra of type I PCS's obtained in Antarctica in September 1987, using recently measured optical constraints of the various compounds that might be present in PSC's. We find that these PSC's were not composed of nitric acid trihydrate but instead had a more complex composition perhaps that of a ternary solution. Because cloud formation is sensitive to their composition, this finding will alter our understanding of the locations and conditions in which PSCs form. In addition, the extent of ozone loss depends on the ability of the PSC's to remove NOx permanently through sedimentation. The sedimentation rates depend on PSC particle size which in turn is controlled by the composition and formation mechanism.

Toon, Owen B.↗

NASA NTRS1985

The impact of polar stratospheric clouds on the heating rates of the winter polar stratosphere

The perturbation affecting IR radiative heating rates of the lower stratosphere that are prompted by the occurrence of polar stratospheric clouds (PSCs) during the Arctic and Antarctic winter are presently calculated by means of a multispectral radiative transfer code that allows for scattering, absorption, and thermal emission by particles and gases. Attention is given to perturbations arising from both the particulate opacity of the PSCs and the decrease of H2O vapor accompanying their formation. For plausible values of model parameters, the former, direct effect is always one of increased radiative cooling, while the indirect effect is always one of decreased cooling.

Pollack, J. B.↗

NASA NTRS2015

CALIPSO Polar Stratospheric Cloud Observations from 2006-2015

Pitts, Michael C.↗

NASA NTRS1995

Composition of Polar Stratospheric Clouds from Infrared Spectroscopy

Heterogeneous reactions on polar stratospheric clouds (PSCs) have recently been implicated in Arctic and Antarctic ozone destruction. Although the chemistry is well documented, the composition of the clouds remains uncertain. The most common PSCs (type I) are thought to be composed of HNO3/H2O mixtures. Although the exact process is not clear, type I PSCs are believed to nucleate on preexisting stratospheric sulfate aerosols (SSAs) composed of sulfuric acid and water. We are using infrared spectroscopy to study the composition and formation mechanism of type I PSCs. In the laboratory, we have used FTIR spectroscopy to probe the composition and phase of H2SO4/HNO3/H2O aerosols under winter polar stratospheric conditions. We have also used recently measured infrared optical constants for HNO3/H2O mixtures to analyze solar infrared extinction measurements of type I PSCs obtained in September 1987 over Antarctica. The results of these studies will be discussed in the context of current theories for polar stratospheric clouds formation.

Tolbert, M. A.↗

NASA NTRS1990

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.↗

NASA NTRS1984

Proceedings of a Workshop on Polar Stratospheric Clouds: Their Role in Atmospheric Processes

The potential role of polar stratospheric clouds in atmospheric processes was assessed. The observations of polar stratospheric clouds with the Nimbus 7 SAM II satellite experiment were reviewed and a preliminary analysis of their formation, impact on other remote sensing experiments, and potential impact on climate were presented. The potential effect of polar stratospheric clouds on climate, radiation balance, atmospheric dynamics, stratospheric chemistry and water vapor budget, and cloud microphysics was assessed. Conclusions and recommendations, a synopsis of materials and complementary material to support those conclusions and recommendations are presented.

Hamill, P.↗

NASA NTRS1992

Aerosols and polar stratospheric clouds measurements during the EASOE campaign

Preliminary results of observations performed using two different lidar systems during the EASOE (European Arctic Stratospheric Ozone Experiment), which has taken place in the winter of 1991-1992 in the northern hemisphere lattitude regions, are presented. The first system is a ground based multiwavelength lidar intended to perform measurements of the ozone vertical distribution in the 5 km to 40 km altitude range. It was located in Sodankyla (67 degrees N, 27 degrees E) as part of the ELSA experiment. The objectives of the ELSA cooperative project is to study the relation between polar stratospheric cloud events and ozone depletion with high vertical resolution and temporal continuity, and the evolution of the ozone distribution in relation to the position of the polar vortex. The second system is an airborne backscatter lidar (Leandre) which allows for the study of the 3-D structure and the optical properties of polar stratospheric clouds. The Leandre instrument is a dual-polarization lidar system, emitting at 532 nm, which allows for the determination of the type of clouds observed, according to the usual classification of polar stratospheric clouds. More than 60 hours of flight were performed in Dec. 1991, and Jan. and Feb. 1992 in Kiruna, Sweden. The operation of the Leandre instrument has led to the observation of the short scale variability of the Pinatubo volcanic cloud in the high latitude regions and to several episodes of polar stratospheric clouds. Preliminary analysis of the data is presented.

Haner, D.↗

NASA NTRS2005

Observations of Antarctic Polar Stratospheric Clouds by Geoscience Laser Altimeter System (GLAS)

Polar Stratospheric Clouds (PSCs) frequently occur in the polar regions during winter and are important because they play a role in the destruction of stratospheric ozone. During late September and early October 2003, GLAS frequently observed PSCs over western Antarctica. At the peak of this activity on September 29 and 30 we investigate the vertical structure and extent, horizontal coverage and backscatter characteristics of the PSCs using the GLAS data. The PSCs were found to cover an area approximately 10 to 15 % of the size of Antarctica in a region where enhanced PSC frequency has been noted by previous PSC climatology studies. The area of PSC formation was found to coincide with the coldest temperatures in the lower stratosphere. In addition, extensive cloudiness was seen within the troposphere below the PSCs indicating that tropospheric disturbances might have played a role in their formation.

Palm, Stephen P.↗

NASA NTRS1990

Radiative effects of polar stratospheric clouds

Radiative transfer calculations are performed for polar stratospheric clouds (PSCs) using newly acquired PSC properties and polar atmospheric data. PSC radiative effects depend strongly on upwelling thermal radiation and vary from infrared heating over warm polar surfaces, such as oceans, to cooling over cold surfaces, such as the Antarctic plateau. Heating and cooling rates of nitric acid PSCs are smaller than + or - 0.1 K/day. Rates for optically thicker ice PSCs vary from 1.0 to -0.2 K/day, those for orographically forced ice PSCs even from 3.0 to -0.5 K/day. Frequently observed optically thick cirrus decks near the tropopause provide a very cold radiative surface. These clouds not only act to prevent heating and enhance cooling in ice PSCs to -0.5 K/day and orographic ice PSCs to 2 K/day, but such cirrus cloud decks also cool the entire stratosphere by up to -0.5 K/day over warm surfaces, even in the absence of PSCs.

Kinne, S.↗