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Results are presented on measurements of NO and the sum of reactive nitrogen species, NO(y), which include NO, NO2, NO3, N2O5, HNO3, and ClONO2 (in addition to ClO, O3, H2O, and N2O measurements), obtained aboard the NASA ER-2 aircraft flying over the Antarctica between the latitudes of 53 and 72 deg S during the Airborne Antarctic Ozone Experiment. The boundary of the chemically perturbed region (CPR), as indicated by a sharp increase in the level of ClO, occurred near 66 deg S; outside or equatorward of the CPR, the NO(y) mixing ratios ranged between 6 and 12 ppbv, with values decreasing poleward and reaching total NO(y) levels of 4 ppbv or less within 5-deg poleward of the boundary. Data presented in this paper clearly associate the Antarctic ozone decrease with perturbed conditions of ClO, NO(y), and H2O, which are in turn associated with processes defined as nonstandard heterogeneous chemistry, denitrification, and dehydration, respectively.

Particle Measuring Systems laser particle spectrometer (ASAS-X and FSSP) probes were used to measure aerosol particle concentrations and size distributions during 11 ER-2 flights between Punta Arenas (53 deg S) and Antarctica (up to 72 deg S) from August 17 to September 22, 1987. The time resolution was 10 s, corresponding to a spatial resolution of 2 km. The data were divided into two size classes (0.05-0.25 and 0.53-5.5 micron radius) to separate the small particle from the coarse particle populations. Results show that the small-particle concentrations are typical for a background aerosol during volcanic quiescence. This concentration is generally constant along a flight track; in only one instance a depletion of small particles during a polar stratospheric cloud (PSC) encounter was measured, suggesting a nucleation of type I PSC particles on background aerosols. Temporary increases of the coarse particle concentrations indicated the presence of tenuous polar stratospheric clouds that were encountered most frequently at the southernmost portion of a flight track and when the aircraft descended to lower altitudes. During 'particle events', particle modes were found at 0.6-micron radius, corresponding to type I PSCs, and occasionally, at 2.0-micron radius corresponding to type II PSCs.

Filter samples obtained as part of the AAOE to determine the total nitrate, sulfate, acidic chloride, and acidic fluoride content along the flight path of the NASA ER-2 are studied. These compounds were obtained in the aerosol and vapor phase. The ratio of particulate sulfate observed outside the chemically perturbed region (CPR) of the vortex to that inside the CPR was 2.6. The ratio of total acidic chloride to total acidic flouride within the CPR is near 1, indicating the removal of chloride from the air mass or the partitioning of chloride into an unmeasured species.

The 1987 Airborne Antarctic Ozone Experiment, in which the NO3, Cl, and SO4 contents of stratospheric aerosols were estimated, is discussed. The aerosol size and chemical composition measurements were carried out on samples collected during August 17 to September 4, 1987. The data indicate that condensed nitrate is found below a threshold temperature of 193.6 + or - 3.0 K, which is generally found at latitudes exceeding 64 deg S. A negative correlation exists between condensed nitrate and ozone correlation.

The formulation and evolution of polar stratospheric ice clouds are simulated using a one-dimensional model of cloud microphysics. It is found that the optical thickness and particle size of ice clouds depend on the cooling rate of the air in which the cloud formed. It is necessary that there be an energy barrier to ice nucleation upon the preexisting aerosols in order to account for the cooling rate dependence of the cloud properties.

Measurements of total reactive nitrogen, NOy, total water vapor, and aerosols were made as part of the Airborne Antarctic Ozone Experiment. The measurements were made using instruments located onboard the NASA ER-2 aircrafts which conducted twelve flights over the Antarctic continent reaching altitudes of 18 km at 72 S latitude. Each instrument utilized an ambient air sample and provided a measurement up to 1 Hz or every 200 m of flight path. The data presented focus on the flights of Aug. 17th and 18th during which Polar Stratospheric Clouds (PSCs) were encountered containing concentrations of 0.5 to 1.0 micron diameter aerosols greater than 1 cm/cu. The temperature pressure during these events ranged as low as 184 K near 75 mb pressure, with water values near 3.5 ppm by volume (ppmv). With the exception of two short periods, the PSC activity was observed at temperatures above the frost point of water over ice. The data gathered during these flights are analyzed and presented.

Measurements of NO and total reactive N, NOy, were made as part of the Airborne Antarctic Ozone Experiment conducted in Punta Arenas, Chile during Aug. and Sept. 1987. The total reactive N reservoir includes the species NO, NO2, NO3, N2 O5, HNO3, and ClONO2. The instrument was located on board the NASA ER2 aircraft which conducted 12 flights over the Antarctic continent reaching altitudes of 18 km at 72 deg S latitude. The NOy technique utilized the conversion of component NOy species to NO on a gold catalyst and the subsequent detection of NO by the chemiluminescence reaction of NO with ozone. Since the inlet sample line is heated and the catalyst operates at 300 C, NOy incorporated in aerosols evaporates and is converted to NO. NO was measured on two separate flights by removing the catalyst from the sample inlet line.

Models indicate that stratospheric aerosols play a major role in the destruction of ozone during the Austral winter. Although many in situ measurements of stratospheric aerosols were made during the Airborne Antarctic Ozone Experiment, changes of aerosol concentration and size distributions across the polar vortex are important to understanding changes of chemical species taking place during this time. Therefore comparing the in situ measurements with measurements made by satellites scanning wider areas will give a clearer picture of the possible role played by aerosols during this period. The wire impactor size distributions are compared to those from the aerosol spectrometers and a best fit size distribution determined. Aerosol extinctions are calculated from the in situ measurements and compared to the extinctions measured by the satellites. Five comparisons are made with SAGE 2 and four with SAM 2. Extinctions agree as close as a factor of two.

Nitric and hydrochloric acids have been postulated to condense in the winter polar stratosphere to become an important component of polar stratospheric clouds. One implication is that the removal of NO(y) from the gas phase by this mechanism allows high Cl(x) concentrations to react with O3, because the formation of ClNO3 is inhibited. Contributions of NO3 and Cl to the stratospheric aerosol were determined during the 1987 Airborne Antarctic Ozone Experiment by testing for the presence of nitrates and chlorides in the condensed phase. Aerosol particles were collected on four 500 micron diameter gold wires, each pretreated differently to give results that were specific to certain physical and chemical aerosol properties. One wire was carbon-coated for concentration and size analyses by scanning electron microscopy; X-ray energy dispersive analyses permitted the detection of S and Cl in individual particles. Three more wires were coated with Nitron, barium chloride and silver nitrate, respectively, to detect nitrate, sulfate and chloride in aerosol particles. All three ions, viz., sulfates, nitrates and chlorides were detected in the Antarctic stratospheric aerosol. In terms of number concentrations, the aerosol was dominated by sulfates, followed by chlorides and nitrates. An inverse linear regression can be established between nitrate concentrations and ozone mixing ratio, and between temperature and nitrates.

The condensation nucleus counter (CNC) flown of the NASA ER-2 in the Airborne Antarctic Ozone Experiment provides a measurement of the number mixing ratio of particles which can be grown by exposure to supersaturated n-butyl alcohol vapor to diameters of a few microns. Such particles are referred to as condensation nuclei (CN). The ER-2 CNC was calibrated with aerosols of known size and concentration and was found to provide an accurate measure of the number concentration of particles larger than about 0.02 micron. Since the number distribution of stratospheric aerosols is usually dominated by particles less than a few tenths of micron in diameter, the upper cutoff of the ER-2 CNC has not been determined experimentally. However, theory suggests that the sampling and counting efficiency should remain near one for particles as large as 1 micron in diameter. Thus, the CN mixing ratio is usually a good measure of the mixing ratio of submicron particles.

The history of minimum temperatures at 50 and 70 mb is examined from NMC, UK Met 0 and ECMWF analyses. MSU channel 24 data are similarly inspected. South Pole sonde data are used to calculate saturation humidity mixing ratio as a function of altitude and time throughout 1987. Saturation with respect to ice could be maintained for water mixing ratios of 3.5 ppmv for a period of about 80 days from mid-June to mid-September. Dehydration to mixing ratios of 1 ppmv or less was possible sporadically. Data from the ER-2 flights between 53 S and 72 S are used in conjunction with particle size measurements and air parcel trajectories to demonstrate the dehydration occurring over Antarctica. Water mixing ratios at the latitude of Punta Arenas (53 S), in conjunction with tracer measurements and trajectory analysis, show that at potential temperatures from about 325 to 400 K, the dryness (less than 3 ppmv) had its origin over Antarctica rather than in the tropics. Water mixing ratios within the Antarctic vortex varied from 1.5 to 3.8 ppmv, with a strong isentropic gradient being evident in the region of high potential vorticity gradients.

Measurements of total reactive nitrogen, NOy, total water vapor, and aerosols were made as part of the Airborne Antarctic Ozone Experiment. The measurements were made using instruments located onboard the NASA ER-2 aircrafts which conducted twelve flights over the Antarctic continent reaching altitudes of 18 km at 72 S latitude. Each instrument utilized an ambient air sample and provided a measurement up to 1 Hz or every 200 m of flight path. The data presented focus on the flights of Aug. 17th and 18th during which Polar Stratospheric Clouds (PSCs) were encountered containing concentrations of 0.5 to 1.0 micron diameter aerosols greater than 1 cm/cu. The temperature pressure during these events ranged as low as 184 K near 75 mb pressure, with water values near 3.5 ppm by volume (ppmv). With the exception of two short periods, the PSC activity was observed at temperatures above the frost point of water over ice. The data gathered during these flights are analyzed and presented.

The temperature dependence is examined of optical properties measured in the Antarctic during 1987 at the 70 mb level (near 18 km), a level chosen to correlate the results with in situ measurements made from the NASA-Ames ER-2 aircraft during the 1987 Airborne Antarctic Ozone Experiment (AAOE). The data set consists of extinction measurements by Sam 2 inside the Antarctic polar vortex from May to October 1987; and backscatter measurements by the UV-DIAL (Ultraviolet Differential Absorption Lidar) system aboard the Ames DC-8 aircraft during selected AAOE flights. Observed trends are compared with results from a revised version of Pole and McCormick's model to classify the PSC observations by Type (1 or 2) and infer the temporal behavior of the ambient aerosol and ambient vapor mixing ratios. The sample figures show monthly ensembles of the 70-mb Sam 2 extinction ratio (the ratio of aerosol or PSC extinction to molecule extinction) as a function of NMC temperature at the beginning (June) and (October) of the 1987 Antarctic winter. Both ensembles show two rather distinct clusters of points: one oriented in the near vertical direction which depicts the change with temperature of the ambient aerosol extinction ratio; and a second cluster oriented in the near horizontal direction whose position on the vertical scale marks a change in particle phase (i.e., PSC formation) and whose length (the extinction enhancement related to that of the ambient aerosol) is an indicator of PSC type.

Stratospheric aerosols collected over the western U.S. from late 1982 to early 1984 show the strong effects of El Chichon's eruption. Although mineral particles disappeared during this period, large acid droplets were still common. Because these have never been seen in prevolcanic, background-level collections, they apparently result from increased droplet growth made possible by the unusual abundance of sulfate. Aerosol size distributions show a wide variety of multimodal curves due to mixing of air masses containing aerosols of various ages or histories. Toward the end of the study time there are fewer large aerosols because of gravitational settling and poleward transport. The result is a steady reduction in sulfate, as most aerosol mass is concentrated in a small number of large droplets. Even the later sulfate levels are, however, five times typical prevolcanic background contents. Thus the influence of El Chichon on high-altitude was still considerable 22 months after eruption.

Comparisons are made between aerosol size distributions measured by instrumented aircraft and the SAGE II sensor on the ERB satellite performing limb scans of the same atmospheric region. Particle radii ranging from 0.0001-200 microns were detected, with good agreement being obtained between the size distributions detected by impactors and probes at radii over 0.15 micron. The distributions were used to calculate aerosol extinction values which were compared with values from SAGE II scans.

Dominant effects of the El Chichon eruption on stratospheric aerosols at 19.8 to 20.7 km are: (1) vapor depositional growth of the small-aerosol (background) mode; (2) development of a large-particle mode by sedimentation from the highest altitudes in the cloud; (3) a change in the large-particle mode from sulfate-coated silicates to sulfate aerosols, some with silicate cores; (4) a 100-fold increase in sulfate mass in the large particle mode. Terminal velocities of large silicate particles, maximum r = 2.3 micron, sampled 1 month after eruption, and calibrated with the aid of lidar data, indicate initial injection to 26 to 27 km. Smaller velocities of sulfate aerosols, median r = 0.5 micron, are compatible with major growth in 2 to 3 months at 27 to 28 km. Aerosol settling accounts for the descent of the main lidar return to 26.5 km in August and to 20 to 21 km in December.

Samples of stratospheric aerosols collected with U-2 aircraft for several months following the first three major eruptions of Mount St. Helens were analyzed for ash and liquid acid content. Ash grain sizes and compositions vary depending on collection altitude, location within the drifting cloud, and days following their injection. s computers Size distributions of ash particles vary with altitude. Generally small particles are depleted more rapidly at low altitudes (12 km) than at higher altitudes (17-18 km). Although samples collected 1 day after the first eruption of May 18, 1980, were dry, flow marks on the aircraft indicated parts of the cloud contained heavy acid concentrations. Indeed, all other samples obtained within 1 to 4 days after later eruptions (May 25 and June 12, 1980) were covered with copious amounts of liquid acid. Proportions of liquid to ash varied considerably depending on sampling location and cloud age. Because the acid-coated ash globules were large, they rapidly fell from the stratosphere until, by late June 1980, only a residue of acid droplets remained. Size distributions and concentrations of these droplets varied considerably.

Stratospheric aerosol samples were collected using a wire impactor during the year following the eruption of Mt. St. Helens. Analysis of samples shows that aerosol volume increased for 6 months due to gas-to-particle conversion and then decreased to background levels in the following 6 months.

To investigate the possibility that significant amounts of tropical tropospheric air may be convectively introduced into the stratosphere, aerosol samplings over Panama were made at various altitudes using a wire impactor collector. The percentage of particle sizes less than the mean mode decreases with height above the tropopause, suggesting depletion of small particles, possibly due to coagulation. Larger aerosols (greater than 0.3 micron in diam.) are more abundant farther above the tropopause, indicating growth, mainly by condensation. The total particle concentration decreases with increasing height above the tropopause, and also with increasing temperature. Aerosols containing smaller-size particles are thus found closer to the tropopause, and larger-size, more-evolved aerosols occur at higher altitudes. These data indicate that convective activity at the Intertropical Convergence Zone may be a source mechanism for stratospheric aerosols.

Samples from the stratosphere obtained by U-2 aircraft after the first three major eruptions of Mount St. Helens contained large globules of liquid acid and ash. Because of their large size, these globules had disappeared from the lower stratosphere by late June 1980, leaving behind only smaller acid droplets. Particle size distributions and mineralogy of the stratospheric ash grains demonstrate inhomogeneity in the eruption clouds.

A sampling and analysis technique that uses the binomial distribution to characterize stratospheric aerosol populations at the 95% level of confidence is described. Particle samples obtained over Alaska during July 15-19, 1979, are used; the results show the presence of more small particles at lower altitude than at high altitudes. Calculations of the surface area and volume distributions for all aerosol samples collected are given. Evidence from these data suggests either that Aitken nuclei are injected or diffused across the tropopause and rise into the stratosphere, where they mature into larger particles, or nuclei form in the lower stratosphere and become mature aerosols at high altitude. Samples obtained at another site give the same results, supporting the view that the process of injection or nucleation and maturing of aerosols with altitude may be global and need not occur only in locations exhibiting unique meteorologic features.

Stratospheric aerosols were collected at Poker Flat, Alaska, in July, 1979, to determine particle properties, confirm coincident satellite SAGE measurements, and compare similar results obtained with different airborne samplers. Because of the steep slopes in size-distribution curves for larger particles, it is found that properties such as concentrations, aerosol mass, and optical extinction are very sensitive to small errors in radii. It is calculated that the concentration measurements agree with photoelectric particle counter results when a 16% radius change is introduced. An 8% radius change matches our calculated sulfate mass with filter mass measurements. And a 13% radius change results in agreement between the calculated optical extinction and coincident SAGE satellite results. Recognizing that different instruments can produce 10-20% differences in measured sizes, it is believed the results of these comparative measurements of SAGE and in situ instruments are essentially in agreement.

Trace ammonia in laboratory air reacts easily with sulfuric acid aerosol samples to form crystalline ammonium sulfate. Argon atmospheres, however, protect sampling surfaces from ammonia contamination. It is found that atmospheric aerosols treated in this way contain only sulfuric acid. After an hour exposed to laboratory air, these same samples convert to ammonium sulfate. Aerosol particles have been collected, using argon control, to determine if the absence of crystalline sulfate is common. But so far there is no evidence that aerosols are neutralized by ammonia in the stratosphere.

Stratospheric aerosols were collected at the 20 km altitude zone by direct impaction on 0.2mm palladium wires in view of the previously observed minimum in particle size frequency distribution between 0.1 and 0.2 microns. Since no minimum in size distribution around 0.2 microns was found, it is concluded that previous equipment was inefficient in collection in this range. Concentration results suggest that low particle concentrations result from small particles agglomerating to form larger ones. Since no indentations were found on the wires used in this experiment, and since there were no differences in the number of particles found on oil-coated surfaces vs uncoated surfaces, the particles in the stratosphere must be liquid, liquid coated, or a slurry.

To investigate whether injection sources of the stratospheric aerosol layer could be detected in the tropical stratosphere, an examination of the aerosol vertical and horizontal size distribution around the Intertropical Convergence Zone (ITCZ) at the Panama Canal Zone was performed during the summer of 1977. By comparing these data with similar measurements in temperate and polar regions, it was hoped to discover variations in particle size that would indicate whether a young aerosol is forming and entering the stratosphere at the ITCZ; where the aerosol matures; and finally, where it reenters the troposphere. The methods used in the investigations and the results obtained from the analyses are described.

We have obtained stratospheric aerosols from tropical to northern latitudes using special collectors on U-2 aircraft during 1976 and 1977. Aerosols characterized by large numbers of small particles are found in the tropical zone suggesting this is a region of particle growth; whereas aerosols containing mostly larger particles are distributed throughout the Northern Hemisphere indicating a well-mixed, mature population. We find the aerosol layer extends from higher altitudes near the equator to lower ones toward the pole. Although this gradient suggests mature aerosols may leave the stratosphere at high latitudes, the data are, as yet, inconclusive. Comparisons of our data with those of other investigators using different instruments are generally encouraging, suggesting that if similar populations were sampled, the results would be similar. When our calculated sulfate mass mixing ratios are compared with those measured directly by others, we find better agreement is achieved if we assume more dilute sulfate and water mixtures than previously proposed.

Extraterrestrial particles collected during U-2 flights in the stratosphere were divided into four groups: chondritic, iron-sulfur--nickel, mafic silicates, and others. The chondritic aggregates are typically composed of Fe, Mg, Si, C, S, Ca, and Ni. Detectable levels of He-4 implanted from the solar wind occur in some. Olivine, spinel, and possibly pyrrhotite and a hydrated layered-lattice silicate were identified. The chondritic ablation particles contain no sulfur and appear to have been melted. Magnetite, olivine, and pyroxene were identified. The iron-sulfur-nickel type particles resemble meteoritic iron sulfide with a small amount of nickel, and contain magnetite and troilite. The mafic silicate type particles are iron magnesium silicate grains with clumps of chondritic aggregate particles adhering to their surfaces. Olivine and possibly pyrrhotite and pyroxene were identified. Most of the iron-nickel type particles are spherules and include taenite and wustite. The other type particles include nickel-iron mounds on spheroidal glassy-like grains having chondritic-like elemental abundances.

Study of the nature of cosmic dust particles collected by two recoverable rockets launched at Fort Churchill, Canada, in the spring of 1970, before the noctilucent cloud season in order to avoid the interference of uplifted atmospheric aerosols during the determination of the concentration of background cosmic dust. The study was designed to verify the results of a previous study for which dust particles were collected in the summer of 1968 by a rocket launched through a noctilucent cloud at the same location. The findings support the hypothesis that occasional high concentrations of dust in the mesosphere are due to uplifted aerosols which could be of a terrestrial or cosmic origin.

Investigation of dust concentrations in the upper atmosphere at the polar regions by sounding rocket flights. The results indicate no normal existence of high concentration of dust and show no variation in the concentration of particles in the upper atmosphere as a function of the time of day.

Methods for analyzing atmospheric aerosols and particulate contaminants from natural and industrial sources are briefly described. Their development was spurred by interest in cosmic dust investigations. These methods make it possible to analyze individual particles ranging in size from 0.01 to 1000 microns for elemental and mineralogical content. The described methods include transmission electron microscopy, scanning electron microscopy, electron probe microanalysis, X-ray diffraction, optical mineralogy, and density measurement.

Economic impact of modifications to DC-8 aircraft nacelles to reduce fan-compressor noise - Part 5

Photographic observation of noctilucent cloud occurrence over geographical location during sounding rocket flight

Noctilucent cloud particle size composition and origin from sounding rocket flight and control collecting surfaces

Microparticle collection experiments during 1966 Orionid and Leonid meteor showers accomplished by Luster and ALARR /air launched-air recovered rocket/ instruments

Particle concentrations and size distribution on Luster sounding rocket surfaces exposed to Leonid meteroid shower, comparing contamination and extraterrestrial origins

Micrometeoroid penetration of metal thin film on Gemini 9 and 12, finding no evidence of impact