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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.↗

An analysis of lidar observations of polar stratospheric clouds

Lidar observations by Browell et al. (1990) are interpreted using single scattering calculations for nonspherical particles and aerosol microphysical calculations. Many of the lidar observations are consistent with particles containing 10 ppbv of condensed nitric acid vapor and an equivalent mass of water. The lidar observations of these Type 1 clouds identify two subtypes, whose properties are deduced. Type 1b particles are spherical, or nearly spherical, and typically have radii near 0.5 micron; Type 1a particles are not spherical, and have a spherical volume equivalent radius exceeding 1.0 micron. Several factors may cause variations in the size of the particles. The most significant factors are the cooling rate and the degree to which the air parcels cool below the condensation point. Specific examples in which cooling rate and cooling point may have led to variations in particle size are found in the Browell et al. (1990) data set. Condensation of 1 ppmm of water or less is quantitatively sufficient to account for the magnitude of the lidar backscatter observed from water ice clouds. The ice particles are not spherical in shape. The sizes of particles in water ice clouds cannot be determined because they are much larger than the wavelength of the lidar.

Toon, Owen B.↗

Denitrification of the polar winter stratosphere - Implications of SAM II cloud formation temperatures

The SAM II extinction profiles and the associated temperature profiles are used to determine the amount of denitrification of the winter polar stratospheres. Clear evidence of the denitrification process in the Antarctic data is seen. There are indications in the Arctic data that denitrification mechanisms may be at work there also. At the latitudes observed by the SAM II satellite system, denitrification begins before the formation of extensive ice clouds and may be due to sedimentation of nitric acid particles. However, the possibility of dinitrification by type II PSCs at latitudes not observed by SAM II cannot be excluded.

Hamill, Patrick↗

Condensation of HNO3 on falling ice particles - Mechanism for denitrification of the polar stratosphere

Ice particles created in polar stratospheric cooling events are predicted to descend into Type I PSCs and accrete a coating of nitric acid trihydrate (NAT) that inhibits evaporation. Coated particles efficiently strip HNO3 from the atmosphere, providing a mechanism for denitrification without significant dehydration. Coatings that disintegrate may release large particles of NAT that influence subsequent particle growth.

Wofsy, S. C.↗

The polar stratospheric cloud event of January 24, 1989. I - Microphysics

Rapid adiabatic cooling induced by synoptic forcing led to polar stratospheric cloud (PSC) formation on January 24, 1989, at altitudes sampled by the ER-2 aircraft. Particle characteristics measured by the Forward Scattering Spectrometer Probe (FSSP) on the ER-2 were compared to those calculated using a theoretical PSC microphysics model. Although calculations were sensitive to local changes in cooling rate, generally favorable agreement was found, that in particle surface area being especially important since this parameter dictates heterogeneous chemical rates. The overall model performance suggests that the current approach for simulating Type 1 (nitric acid trihydrate) PSC formation under rapid cooling conditions is well founded and can be used to study the effects of heterogeneous chemistry on stratospheric composition.

Poole, L. R.↗

Observations of denitrification and dehydration in the winter polar stratospheres

It is argued that denitrification of the Arctic stratosphere can be explained by the selective growth and sedimentation of aerosol particles rich in nitric acid. Because reactive nitrogen species moderate the destruction of ozone by chlorine-catalyzed reactions by sequestering chlorine in reservoir species such as ClONO2, the possibility of the removal of reactive nitrogen without dehydration should be allowed for in attempts to model ozone depletion in the Arctic. Indeed, denitrification along with elevated concentrations of reactive chlorine observed in 1989 indicate that the Arctic was chemically primed for ozone destruction without an extended period of temperatures below the frost point, as is characteristic of the Antarctic.

Fahey, D. W.↗

Sub-visual Cirrus detection and characterization

Analysis of archived cold optics (COR) radiometer data is yielding useful information on the diurnal, geographic, seasonal and altitude variability of atmospheric background radiance levels in the 11 micron window region. This database is a compilation of Kuiper Infrared Technology Experiment (KITE) and Atmospheric Radiance Study (ARS) observations under a wide variety of conditions. Correlating the measurements from these two studies with the LOWTRAN model code has revealed several important results. First, the 11 micron window appears to be filled-in, i.e., the troughs on either side of the nitric acid peak are shallower than expected. Second, the amplitude of the background radiances measured exceeds the model predictions by a factor of 2 to 3 or more. This is thought to be due to the existence of thin, high altitude cirrus clouds (sub-visual cirrus) above the sensor platform. These high background levels are observed under quiescent conditions in the South Pacific (Marshall Islands), as well as over the continental United States (the West Coast). In the tropics, there appears to be little diurnal variability, a plausible seasonal variation and a linear dependence between 7.2 and 11.4 micron band data, indicating possible multi-spectral approaches to detection of sub-visual cirrus clouds. Theoretical analysis of the magnitude of the effects of a sub-visual cirrus cloud on atmospheric background radiances measured by a near-horizontal sensor is in progress.

Schmidt, E.↗

Annular denuder systems: Precision and applicability to stratospheric sampling

Annular denuder systems (ADS) are designed to sample both gases and particles from ambient air without cross interference. The ADS's were used to detect chemical gradients over rural forest canopies. Accurate and precise methods for the sampling and analysis of low concentrations of gaseous and particulate species over short sampling periods were developed. Typical analytical precision data for nitrate and sulfate are shown. Both sampling and analytical precision data for a 2 hour test using four collocated ADS's are presented. On this particular day, the overall precision for HNO3 was unusually poor. The overall precision for the major constituents of interest is generally about 3 to 5 percent for typical ambient concentrations. The ADS's could potentially be used to determine the concentrations of HNO3 and fine-particle nitrate in the stratosphere, and to simultaneously characterize the chemical composition of stratospheric aerosols. Assuming 50 mb pressure, a 2 hour sampling time, a 50 Lpm sampling rate, and a low blank value, an overal precision of about 15 percent should be possible for 1 ppbv of HNO3 or nitrate, which would include nitric-acid trihydrate (NAT); and pump-driven systems could accommodate more complex systems involving denuders and filter packs in sequence. Alternate coatings could possibly be developed to selectively sample species such as Cl2 and ClNO3. The ADS's might also be useful in laboratory studies of heterogeneous chemical reactions involving NAT aerosols.

Randtke, Stephen J.↗

Laboratory and field studies of stratospheric aerosols: Phase changes under high supersaturation

It is well known that water in the form of isolated small droplets supercool as much as 40 C below their equilibrium melting point. Solutions similarly supercool (with respect to water) and supersaturate (with respect of the solute). Experiments are described in which bulk solutions typical of atmospheric aerosols (nitric acid, sulfuric acid, and hydrates; ammonium sulfate; ammonium bisulfate; sodium chloride) are supercooled and/or supersaturated and nucleated to initiate crystal growth. Supersaturation of 300 percent is readily attainable, with linear growth of crystals increasing roughly as (supercooling/supersaturation)sup 2. The implication of the experiments is that the situation of metastability in polar stratosphere clouds is very likely, with nucleation only occuring under a high degree of supercooling or supersaturation.

Hallet, John↗

Measurements in polar stratospheric clouds over Antarctica in September 1989

The results of six balloon flights at McMurdo Station, Antarctica, under varying temperature conditions, are used in a study of polar stratospheric clouds during Sept. 1989. A particle counter, with size resolution in the 0.5 micron radius region, indicates that cloud size distributions are always bimodal. Mode radii ranging from 0.05 to 0.10 microns were observed for the small particle mode, representing the sulfate layer or condensational growth enhancements of it. The data are not inconsistent with the expected increase in size with decreasing temperature of the small particle mode in the sulfate layer owing to deliquescence although this phenomenon is often masked by nitric acid trihydrate (NAT) condensation when temperatures are sufficiently low. Mode radii generally ranged from 1.5 to 3.5 micron for the large particle mode at concentrations 3 to 4 orders of magnitude lower than the small particle mode. The large particle mode, which normally comprises most of the mass, is presumably caused by NAT condensation on larger particles of the sulfate layer and indicates HNO3 mixing ratios of 1 to 5 ppbv for most of the cloud layers observed, suggesting substantial denitrification. On several occasions, distributions were observed with mode radii as high as 7 microns, and correspondingly large inferred mass, indicating water ice clouds in the 12 to 15 km region. On other occasions, absence of such clouds at very low temperatures indicated water vapor mixing ratios of less than 3 ppmv suggesting dehydration. Generally, the inferred HNO3 mixing ratios were higher in the lower stratosphere, suggesting redistribution through particle sedimentation.

Deshler, Terry↗

Nucleation and growth of HNO3-3H2O particles in the polar stratosphere

Growth of nitric acid trihydrate (NAT) particles on background stratospheric aerosols is examined for an isolated air parcel cooled at a uniform rate. During the process of nucleation, the saturation ratio of HNO3 vapor reaches a maximum value between 2 and 15, corresponding to supercooling by 1-4 K. If cooling rates exceed 0.5-1 K/day, small particles of NAT are produced. A major fraction of the available condensation nuclei is activated and removal of HNO3 by gravitational settling is slow. If cooling rates are less than 0.5-1 K/day, the number of aerosols that nucleate is reduced, leading to differential growth of large NAT particles. Observations of 5 micron radius particles in clouds at temperatures above the water frost point may reflect condensation of NAT on ice particles that fall through a column of air as it is cooled. Rapid condensation of HNO3 on ice particles is promoted by the high supersaturation attained during nucleation and maintained during subsequent cooling. This process provides a mechanism for irreversible removal of HNO3.

Wofsy, Steven C.↗

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.↗

The consequences of global biomass burning

Global biomass burning encompasses forest burning for land clearing, the annual burning of grasslands, the annual burning of agricultural stubble and waste after harvests, and the burning of wood as fuel. These activities generate CO2, CH4 and other hydrocarbons, CO, H2, NO, NH3, and CH3Cl; of these, CO, CH4 and the hydrocarbons, and NO, are involved in the photochemical production of tropospheric O3, while NO is transformed to NO2 and then to nitric acid, which falls as acid rain. Biomass burning is also a major source of atmospheric particulates and aerosols which affect the transmission of incoming solar radiation and outgoing IR radiation through the atmosphere, with significant climatic effects.

Levine, Joel S.↗

Depletion of Arctic ozone in the winter 1990

Ozone mixing ratios were measured by ozonesondes on board balloons launched from Esrange, near Kiruna, Sweden (68 deg N, 20 deg E) from January 11 to February 9, 1990. The data obtained prior to a sudden warming on February 7, 1990 show that at potential temperatures between 460 and 640 K, the ozone mixing ratio just inside the polar vortex was systematically smaller than that outside, the largest difference being 29 percent at around 525 K. The ozone mixing ratio at 525 K inside the vortex decreased at a rate of about 1.5 percent per day between January 26 and February 4. The temperatures simultaneously observed were quite often low enough to allow for formation of nitric acid trihydrate particles around this altitude. Depletion of ozone due to highly perturbed chemical conditions in late January and early February is strongly suggested.

Koike, M.↗

Polar stratospheric clouds and ozone depletion

A review is presented of investigations into the correlation between the depletion of ozone and the formation of polar stratospheric clouds (PSCs). Satellite measurements from Nimbus 7 showed that over the years the depletion from austral spring to austral spring has generally worsened. Approximately 70 percent of the ozone above Antarctica, which equals about 3 percent of the earth's ozone, is lost during September and October. Various hypotheses for ozone depletion are discussed including the theory suggesting that chlorine compounds might be responsible for the ozone hole, whereby chlorine enters the atmosphere as a component of chlorofluorocarbons produced by humans. The three types of PSCs, nitric acid trihydrate, slowly cooling water-ice, and rapidly cooling water-ice clouds act as important components of the Antarctic ozone depletion. It is indicated that destruction of the ozone will be more severe each year for the next few decades, leading to a doubling in area of the Antarctic ozone hole.

Toon, Owen B.↗

Ground-based infrared measurements of HNO3 total column abundances - Long-term trend and variability

The long-term trend and variability of the total column amount of atmospheric nitric acid (HNO3) have been investigated. The study was based on time series of infrared solar absorption spectra recorded at two sites, the International Scientific Station of the Jungfraujoch (ISSJ) in the Swiss Alps (altitude 3.6 km, latitude 46.5 N, longitude 8.0 E) and the National Solar Observatory McMath solar telescope facility on Kitt Peak (altitude 2.1 km, latitude 31.9 N, longitude 111.6 W), Arizona. Measurements of HNO3 absorption features recorded at Kitt Peak between 1980 and 1990 and measurements of the same features in ISSJ solar spectra obtained in June 1951 and June 1986 to June 1990 provide quantitative estimates of the long-term trend in the HNO3 total vertical column. It is found that the trend deduced for each site is equal to zero within the measurement uncertainty. The modern ISSJ measurements show that the fitted trend is (-0.16 + or - 0.50) percent/yr, 2 sigma, which indicates that there has been no detectable change in HNO3 total column over three decades. The Kitt Peak measurements show marked variability in the HNO3 total column, but no obvious seasonal cycle is observed.

Rinsland, C. P.↗

Studies of stratospheric particulates

A sophisticated computer model of polar stratospheric clouds was developed and used to study the properties of ice clouds. The model has recently been extended to investigate nitric acid clouds and ice clouds as well as their interactions with stratospheric gases. The model is now being applied to interpret data collected during recent expeditions to the Antarctic and the Arctic. Some work has also been done to understand the properties of noctilucent clouds and their implications for the chemistry and dynamics of the upper stratosphere.

Toon, Owen B.↗

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↗