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The water balance of a hurricane is controlled by boundary layer inflow, near vertical motion in the eyewall causing coalescence precipitation at above and residual ice precipitation at below freezing temperatures, and cirrus outflow at below -40 C aloft. In this paper we address the question of efficiency of water removal by this cirrus outflow which is important for the release of latent heat at high altitudes and its role in the dynamic flow at that level. During NASA's 1998 Convection and Moisture Experiment campaign we acquired microphysical outflow data in order to (1) determine the release and redistribution of latent heat near the top of hurricanes, (2) aid in TRMM algorithm development for remote sensing of precipitation, and (3) determine the optical/radiative characteristics of hurricane outflow. The data were acquired with Particle Measuring Systems two dimensional imaging spectrometers. On 23 August and again during the hurricane's landfall on 26 August, 1998, the NASA DC-8 aircraft penetrated hurricane 'Bonnie' four times each near 200 hPa pressure altitude. The eye crossing times were determined by (1) zero counts of cloud particles, (2) approximately 5 C increases in static and potential temperatures, and (3) minima in speeds and changes of direction of horizontal winds. The vertical winds showed shear between -6 m per second and +4 m per second and tangential winds approached 30 m per second in the eyewall. The particle volumes in the eyewall (determined by the pixels the particles shadowed in the direction of flight [x-direction] and normally to it by the number of diodes that they shadowed [y-direction]) ranged between 0.5 and 5.0 cubic centimeters per cubic meter. With a particle density near 0.2 g per cubic centimeter (determined from in situ melting and evaporation on a surface collector), the 1.0 g per meter corresponding mass of cloud ice ranged between 0.27 and 2.7 g per kilograms yielding horizontal fluxes between 8.1 and 81 g per square meters per second. The outflow ice was concentrated in crystals of a modal size of 190 micrometers. The particle size distributions were heavily skewed toward sizes with 98% of all cirrus particles smaller than the modal size comprising, however, only 20% of the mass. Thus the smaller than modal size particles dominantly affected the optical/radiative characteristics of the cloud, whereas the larger than modal size crystals determined the ice mass, hence dominated latent heating. Questions to be addressed relate to the origin of individual ice particles as the hurricane evolved and the likelihood of pristine and aggregate particle formation under the complicated conditions of rotation and outflow in the eyewall.

A significant increase in sulfuric acid aerosol concentration was detected above 10 km pressure altitude during a cross-corridor flight out of Shannon, Ireland, on October 23, 1997.

A significant increase in sulfuric acid aerosol concentration was detected above 10 km pressure altitude during a cross-corridor flight out of Shannon on October 23, 1997. The source of this aerosol is ascribed to commercial aircraft operations in flight corridors above 10 km, because (1) a stable atmosphere prevented vertical air mass exchanges and thus eliminated surface sources, (2) air mass back trajectories documented the absence of remote continental sources, and (3) temperature profiler data showed the tropopause at least one kilometers above flight altitude throughout the flight. Particle volatility identified 70% H2SO4, 20% (NH4)2SO4 and 10% nonvolatile aerosol in the proximity of flight corridors, and (10-30)% H2SO4, up to 50% (NH4)2SO4, and (40-60)% nonvolatile aerosols in air that was not affected by aircraft operations below 10 km. Only a very small fraction of the nonvolatile particles (determined with a condensation nucleus counter) could be morphologically identified as soot aerosol (validated by scanning electron microscopy of wire impactor samples). The newly formed H2SO4 particles did not measurably affect surface area and volume of the background aerosol due to their small size, hence did not affect radiative transfer directly.

Aerosol from aircraft can affect the environment in three ways: First, soot aerosol has been implicated to cause Icing-tern ozone depletion at mid-latitudes in the lower stratosphere at a rate of approx. 5% per decade. This effect is in addition and unrelated to the polar ozone holes which are strongly influenced by heterogeneous chemistry on polar stratospheric clouds. Second, the most obvious effect of jet aircraft is the formation of visible contrails in the upper troposphere. The Salt Lake City region experienced an 8% increase in cirrus cloud cover over a 15-year period which covariates with an increase in regional commercial air traffic. If soot particles act as freezing nuclei to cause contrail formation heterogeneously, they would be linked to a secondary effect to cloud modification that very likely is climatologically important. Third, a buildup of soot aerosol could reduce the single scatter albedo of stratospheric aerosol from 0.993+0.004 to 0.98, a critical value that has been postulated to separate stratospheric cooling from warming. Thus arises an important question: Do aircraft emit sufficient amounts of soot to have detrimental effects and warrant emission controls? During the 1996 SUCCESS field campaign, we sampled aerosols in the exhaust wake of a Boeing 757 aircraft and determined emission indices for sulfuric acid (EI(sub H2SO4) = 9.0E-2 and 5.0E-1 g/kg (sub FUEL) for 75 and 675 ppm fuel-sulfur, respectively) and soot aerosol (2.2E-3 less than EI(sub SOOT) = l.lE-2 g/kg (sub FUEL)). The soot particle analysis accounted for their fractal nature, determined electron-microscopically, which enhanced the surface area by a factor of 26 and the volume 11-fold over equivalent-volume spheres. The corresponding fuel-sulfur to H2SO4 conversion efficiency was 10% (for 675 ppmm fuel-S) and 37% (for 75 ppmm fuel-S). Applying the H2SO4 emission index to the 1990 fuel use by the worlds commercial fleets of 1.3E11 kg, a conversion efficiency of 30% of 500 ppmm fuel-S would have led to an annual contribution to the atmospheric sulfur budget by aircraft of 2.E7 kg H2SO4. This is about one part in 1.E4 of anthropogenic sulfate from other sources. The soot emission index given above yielded a 1990 injection of soot aerosol by aircraft of 1.E6 kg. Thus, soot amounts to only five percent of the aerosol generated by aircraft. Its reactivity with ozone would have to be 20 times that of sulfuric acid particles to make it chemically significant. Nevertheless, the findings, of stratospheric soot loadings commensurate with aircraft fuel consumption, based on the emission index given above and the assumption of stratospheric residence times of the order of one year implicate aircraft as stratospheric polluters. A trend similar to soot of H2SO4 aerosol loading could not be deciphered, neither from in situ measurements nor SAGE II satellite extinction, against the "noise" due to volcanic eruptions. Observation of soot particles at 20 km altitude which, if emitted by aircraft were generated at 10-12 km altitude, suggests a displacement of those particles against gravity. Because eddy mixing is virtually absent in the lower stratosphere and isentropic mixing explains lofting to only about 15 km, radiometric forces acting on morphologically and chemically asymmetric soot particles must be considered a possibility. The consequence could be an extended residence time of soot against that of sulfuric acid aerosol that would lower the single scatter albedo with time.

The light absorption coefficient, Beta(a) of the stratospheric aerosol is an important quantity that determines its radiative effects. When combined with the aerosol scattering coefficient, Beta(a) it becomes possible to evaluate the aerosol single scatter albedo, omega = Beta(s)/(Beta(s) + Beta(a)) which is essential for modeling the overall radiative effects of the stratospheric aerosol. Pollack1 determined that omega = 0.98 is a critical value that separates stratospheric cooling from warming.

A combination of CN counts, Ames wire impactor size analyses and optical particle counter data in aircraft exhaust results in a continuous particle size distribution between 0.01 micrometer and 1 micrometer particle radius sampled in the exhaust of a Boeing 757 research aircraft. The two orders of magnitude size range covered by the measurements correspond to 6-7 orders of magnitude particle concentration. CN counts and small particle wire impactor data determine a nucleation mode, composed of aircraft-emitted sulfuric acid aerosol, that contributes between 62% and 85% to the total aerosol surface area and between 31% and 34% to its volume. Soot aerosol comprises 0.5% of the surface area of the sulfuric acid aerosol. Emission indices are: EIH2SO4 = 0.05 g/kgFUEL and (0.2-0.5) g/kgFUEL (for 75 ppmm and 675 ppmm fuel-S, respectively), 2.5E4

Aircraft have become the fastest, fairly convenient and, in most cases of long-distance travel, most economical mode of travel. This is reflected in the increase of commercial air traffic at a rate of 6% per year since 1978. Future annual growth rates of passenger miles of 4% for domestic and 6% for international routes are projected. A still larger annual increase of 8.5% is expected for the Asia/Pacific region. To meet that growth, Boeing predicts the addition of 15,900 new aircraft to the world's fleets, valued at more than $1.1 trillion, within the next 20 years. The largest concern of environmental consequences of aircraft emissions deals with ozone (O3), because: (1) the O3 layer protects the blaspheme from short-ultraviolet radiation that can cause damage to human, animal and plant life, and possibly affect agricultural production and the marine food chain; (2) O3 is important for the production of the hydroxyl radical (OH) which, in turn, is responsible for the destruction of other greenhouse gases, e.g., methane (CH4) and for the removal of other pollutants, and (3) O3 is a greenhouse gas. Additional information is contained in the original extended abstract.

A focused cavity aerosol spectrometer aboard a NASA ER-2 high-altitude aircraft provided high-resolution measurements of the size of the stratospheric particles in the 0.06-2.0-micrometer-diameter range in flights following the eruption of Mount Pinatubo in 1991. Effects of anisokinetic sampling and evaporation in the sampling system were accounted for by means adapted and specifically developed for this instrument. Calibrations with monodisperse aerosol particles provided the instrument's response matrix, which upon inversion during data reduction yielded the particle size distributions. The resultant dataset is internally consistent and generally shows agreement to within a factor of 2 with comparable measurements simultaneously obtained by a condensation nuclei counter, a forward-scattering spectrometer probe, and aerosol particle impactors, as well as with nearby extinction profiles obtained by satellite measurements and with lidar measurements of backscatter.

The distribution of black carbon (soot) aerosol (BCA) in the atmosphere is of interest for several reasons: (1) Because BCA has the highest absorption cross section of any compound known, it can absorb solar radiation to cause atmospheric warming. (2) Because it is a strong adsorber of gases, it can catalyze heterogeneous reactions to change the chemical composition of the atmosphere.(3) If aircraft are a major source of BCA, it is an important tracer of aircraft emissions. Analysis for BCA of impactor samples from Arctic and Antarctic deployments, utilizing particle morphology of scanning electron microscopy images, permits the following conclusions: (1) The BCA concentration in the northern stratosphere varies between 0 and 2.6 ng m-3 averaging 0.6 ng/cu m. (2) This BCA loading is commensurate with estimated fuel consumptions in the stratosphere by the current commercial fleet and an emission index E=0.03 g BCA per kg fuel burnt which was measured in jet exhaust at al titude.Thus, most stratospheric BCA in the northern stratosphere results from aircraft emissions. The background BCA concentration in the southern stratosphere varies between 0 and 0.6 ng cu m averaging 0.1 ng/cu m. This strong meridional gradient implies that stratospheric BCA residence time- is shorter than are mixing times between hemispheres. Projected annual fuel consumption of a future supersonic commercial fleet is 7E13 g. This fleet would increase stratospheric BCA loadings by a factor of 2-3, because almost all fuel would be burnt above the tropopause. An improved EI(BCA) by a factor of ten would result in an increase of stratospheric BCA loadings by approximately 50 %.

Interest in the distribution of black carbon (soot) aerosol (BCA) in the atmosphere is warranted for the following reasons: (1) BCA has the highest absorption cross section of any compound known, thus it can absorb solar radiation to cause atmospheric warming; (2) BCA is a strong adsorber of gases, thus it can catalyze heterogeneous chemical reactions to modify the chemical composition of the atmosphere; (3) If aircraft emission is the major source of atmospheric BCA, it can serve as an atmospheric tracer of aircraft exhaust. We collect BCA particles greater than or equal to 0.02 micrometer diameter by wires mounted on both the DC-8 and ER-2 aircraft. After return to the laboratory, the wires are examined with a field emission scanning electron microscope to identify BCA particles by their characteristic morphology. Typically, BCA exists in the atmosphere as small particles of complex morphology. The particle sizes at the source are measured in tens of Angstrom units; after a short residence time in the atmosphere, individual particles coalesce to loosely packed agglomerates of typical dimensions 0.01 to 0.1 micrometer. We approximate the size of each BCA aggregate by that of a sphere of equivalent volume. This is done by computing the volume of a sphere whose diameter is the mean between averaged minimum and maximum dimensions of the BCA particle. While this procedure probably underestimates the actual surface area, it permits us to compare BCA size distributions among themselves and with other types of aerosols. When statistically justified, we fit lognormal distributions to the data points to determine number concentrations, geometric mean radii, standard deviations, BCA surface areas and volumes. Results to date permit the following conclusions: (1) BCA concentration in the northern stratosphere averages 0.6 ng per cubic meters. This amount is one part in 10(exp 4) after a volcanic eruption (e.g., Pinatubo) increasing to about one percent during volcanic quiescence. In the northern troposphere, BCA concentration averages 3.2 ng per cubic meters, or 0.3 percent of the background aerosol. (2) Applying an BCA emission index EI(BCA)=5 x 10(exp -5), measured in the exhaust wake of a Concorde supersonic jet aircraft, to realistic estimates of fuel burnt by the current and projected fleets permits us to conclude that: (i) Most BCA in the northern stratosphere results from aircraft emissions; (ii) Most BCA in the northern troposphere results from other sources than aircraft; (iii) A projected supersonic fleet will increase the northern stratospheric BCA concentration by one order of magnitude, unless the emission index is substantially reduced. (3) A strong gradient between the northern and southern hemispheres indicates that mixing across the equator is greatly inhibited in relation to atmospheric residence times of BCA. (4) The single scatter albedo of BCA/"background" aerosol mixtures suggests a cooling effect for most of the globe; an exemption is the Arctic because of the high surface albedo of the snow/ice covered earth's surface.

Interest in the distribution of black carbon (soot) aerosol (BCA) in the atmosphere is based on the following: (1) Because BCA has the highest absorption cross section of any compound know, it can absorb solar radiation to cause atmospheric warming; (2) Because BCA is a strong adsorber of gases, it can catalyze heterogeneous chemical reactions to modify the chemical composition of the atmosphere; (3) If aircraft emission is the major source of BCA, it can serve as an atmospheric tracer of aircraft exhaust. We collect BCA particles as small as 0.02 micrometers by wires mounted on both the DC-8 and ER-2 aircraft. After return to the laboratory, the wires are examined with a field emission scanning electron microscope to identify BCA particles by their characteristics morphology, Typically, BCA exists in the atmosphere as small particles of complex morphology. The particle sizes at the source are measured in tens of Angstrom units; after a short residence time in the atmosphere, individual particles coalesce to loosely packed agglomerates of typical dimensions 0.01 to 0.1 micrometer. We approximate the size of each BCA aggregate by that of a sphere of equivalent volume. This is done by computing the volume of a sphere whose diameter is the mean between averaged minimum and maximum dimensions of the BCA particle. While this procedure probably underestimates the actual surface area, it permits us to compare BCA size distributions among themselves and with other types of aerosols.

On February 8, 1993, the NASA DC-8 aircraft profiled from 10,000 to 37,000 feet (3.1-11.3 km) pressure altitude in a stratified section of tropical cyclone "Oliver" over the Coral Sea northeast of Australia. Size, shape and phase of cloud and precipitation particles were measured with a 2-D Greyscale probe. Cloud/precipitation particles changed from liquid to ice as soon as the freezing level was reached near 17,000 feet (5.2 km) pressure altitude. The cloud was completely glaciated at -5 C. There was no correlation between ice particle habit and ambient temperature. In the liquid phase, the precipitation-cloud drop concentration was 4.0 x 10(exp 3)/cu m, the geometric mean diameter D(sub g) = 0.5-0.7 mm, and the liquid water content 0.7-1.9 g m(exp-3). The largest particles anywhere in the cloud, dominated by fused dendrites at concentrations similar to that of raindrops (2.5 x 10(exp 3) m(exp -3)) but a higher condensed water content(5.4 g/cu m estimated) were found in the mixed phase; condensed water is removed very effectively from the mixed layer due to high settling velocities of the large mixed particles. The highest number concentration (4.9 x 10(exp 4)/cu m, smallest size (D(sub g) = 0.3-0.4 mm), largest surface area (up to 2.6 x 10 (exp 2) sq cm/cu m at 0.4- 1.0 g/cu m of condensate) existed in the ice phase at the coldest temperature (- 40 C) at 35,000 feet ( 10.7 km). Each cloud contained aerosol (haze particles) in addition to cloud particles. The aerosol total surface area exceeded that of the cirrus particles at the coldest temperature. Thus, aerosols must play a significant role in the upscattering of solar radiation. Light extinction (6.2/km) and backscatter (0.8/sr/km) was highest in the coldest portion of the cirrus cloud at the highest altitude.

Whether cirrus clouds heat or cool the Earth-atmosphere system depends on the relative importance of the cloud shortwave albedo effect and the cloud thermal greenhouse effect. Both an determined by the distribution of ice condensate with cloud particle size. The microphysics instrument package flown aboard the DC-8 In TOGA/COARE included an ice crystal replicator, a 2D Greyscale Cloud Particle Probe and a Forward Scattering Spectrometer Aerosol Probe. In combination. these instruments permitted particle size measurements between 0.5 micrometers and 2.6 mm diameter. Ice crystal replicas were used to validate signals from the electro-optical instruments. Typical results show a prevalence in tropical cirrus clouds of micron-sized particles, in addition to cloud particles that exceed 100 micrometer radius. The mechanism of their formation is growth of (hygroscopic, possibly ocean-derived) aerosol particles along the Kohler curves. The concentration of small particles is higher and less variable in space and time, and their tropospheric residence time is longer, than those of large cloud particles because of lower sedimentation velocities. Small particles shift effective cloud particle radii to sizes much smaller than the mean diameter of the cloud particles. This causes an increase in shortwave reflectivity and IR emissivity. and a decrease in transmissivity. In the cirrus outflow of tropical cyclone Oliver on 8 February, 1993, the reflectivity increases with altitude (decreasing temperature) stronger than does cloud emissivity, yielding enhanced radiative cooling at higher altitudes.

As determined in situ by impactor samplers flown on an ER-2 at 16.5- to 20.7-km pressure altitude and on a DC-8 at 9.5- to 12.6-km pressure altitudes, the 1991 Pinatubo volcanic eruption increased the particle surface area of stratospheric aerosols up to 50-fold and the particle volume up to 2 orders of magnitude. Particle composition was typical of a sulfuric acid-water mixture at ER-2 altitudes. Ash particles coated with sulfuric acid comprised a significant fraction of aerosol at DC-8 altitudes. Mie-computed light extinction increased up to 20-fold at midvisible and greater than 100-fold at near-IR wavelengths. The optical thickness measured through the aerosol layer by an autotracking Sun photometer aboard a DC-8 aircraft at 10.7- to 11.3-km pressure altitudes shows a spectral shape that is similar to the Mie-calculated spectral extinction at ER-2 altitudes. Surface area distributions calculated by inversion of spectral optical depth measurements show characteristics that are similar to the mean surface area distribution resulting from 35 in situ measurements.

Stratospheric aerosols, collected near 19 km altitude on wire impactors over western North America from August 20, 1991 to May 11, 1993, show strong influence of the June 1991 Mt. Pinatubo eruption. Lognormal size distributions are bimodal; each of the mode radii increases and reaches maximum value at about 15 months after eruption. The second (large particle) mode becomes well developed then, and about 40% of the droplets are larger than 0.4 micron radius. The eruption of Mt. Spurr (Alaska) may also have contributed to this. Sulfate mass loading decays exponentially (e-folding 216 days), similar to El Chichon. Silicates are present in samples only immediately after eruption. Two years after eruption, sulfate mass loading is about 0.4 micrograms/cu m, about an order of magnitude higher than background pre-volcanic values. Aerosol size distributions are still bimodal with a very well-defined large droplet mode.

During NASA's Global Backscatter Experiment (GLOBE) mission flights in November 1989 and May 1990, a DC-8 research aircraft probed the Pacific Basin free troposphere for about 90 flight hours in each month between +72 and -62 degrees latitude, +130 and -120 degrees longitude, and up to 39,000 feet pressure altitudes. Aerosols were sampled continuously in situ by optical particle counters to measure concentration and particle size, and during 48 10-min intervals during each mission by wire impactors for concentration, size, composition, phase and shape analyses. The optical particle counters cover a particle diameter range between 0.3 and 20 microns; wire impactors extend the range down to 0.03 microns. Results of particle number, size, shape, together with the assumption of a refractive index corresponding to (NH4)2SO4 to account for the prevalence of aerosol sulfur, were utilized in a Mie algorithm to calculate aerosol extinction and backscatter for a range of wavelengths (0.385 less than lambda less than 10.64 microns). Computations for 22 randomly selected size distributions yield coefficients of extinction E(0.525) = (2.03 +/- 1.20) x 10(exp -4) km(exp -1) and backscatter beta(0.525) = (6.45 +/- 3.49) x 10(exp -6) km(exp -1) sr(exp -1) in the visible, and E(10.64) = (8.13 +/- 6.47) x 10(exp -6) km(exp -1) and beta(10.64) = (9.98 +/- 10.69) x 10(exp -8) km(exp -1) sr(exp -1) in the infrared, respectively. Large particles (D greater than 0.3 microns) contribute two-thirds to the total extinction in the visible (lambda = 0.525 microns), and almost 100% in the infrared (lambda = 10.64 microns). These results have been used to define an IR optical aerosol climatology of the Pacific Basin free troposphere, from which it follows that the infrared backscatter coefficient at lambda = 9.25 microns wavelength fluctuates between 5.0 x 10(exp -10) and 2.0 x 10(exp -7) km(exp -1) sr(exp -1) with a modal value 2.0 x 10(exp -8) km(exp -1) sr(exp -1).

During the Coupled Ocean-Atmosphere Response Experiment (COARE) of the Tropical Ocean and the Global Atmosphere (TOGA) program we measured cloud and aerosol particles aboard the NASA DC-8 over the warm pool of the western Pacific. Instruments on the aircraft included a condensation nuclei counter, optical particle counters, two-dimensional shadow probes and an ice crystal replicator. The size range covered by these instruments was from =0.01 micron to 6.4 mm diameter; particle shapes were determined for particles of sizes D greater than 1 micron.

Two optical particle counters on the ER-2, together covering a particle size diameter range from 0.1 microns to 23 microns, were used to measure the aerosol bulk quantities integral number, aerosol surface and volume, as well as detailed size distributions inside and outside of the polar vortex in the lower stratosphere. While AAES I (Arctic Airborne Stratospheric Expedition, (Dec. 88 - Feb. 89) was conducted in a period of relative volcanic quiescence, enhancements in aerosol number, surface and volume of factors around 10, 25 and 100 were observed during AASE 2 (Aug. 91 - Mar. 92) due to the eruption of Mt. Pinatubo. The changes in these bulk quantities as well as in the size distributions measured both outside and inside the polar vortex are presented and compared with those obtained in polar stratospheric cloud events (AASE I). Except for a shift towards larger aerosol mixing ratios the general shape of correlograms between the measured N2O and particle mixing ratios remain similar before and after the eruption. Similar correlograms are used to interpret data from vertical profiles inside and outside of the polar vortex.

Two optical particle counters on the ER-2, together covering a particle size diameter range from 0.1 micrometers to 23 micrometers, were used to measure the aerosol bulk quantities integral number, aerosol surface and volume, as well as detailed size distributions inside and outside of the polar vortex in the lower stratosphere. While AASE I (Arctic Airborne Stratospheric Expedition, (Dec. 1988 - Feb. 1989) was conducted in a period of relative volcanic quiescence, enhancements in aerosol number, surface and volume of factors around 10, 25 and 100 were observed during AASE II (Aug. 1991 - Mar. 1992) due to the eruption of Mt. Pinatubo. The changes in these bulk quantities as well as in the size distributions measured both outside and inside the the polar vortex are presented and compared with those obtained in polar stratospheric cloud events (AASE I). Except for a shift towards larger aerosol mixing ratios the general shape of correlograms between the measured N2O and particle mixing ratios remain similar before and after the eruption. Similar correlograms are used to interpret data from vertical profiles inside and outside of the polar vortex.

The NASA ER-2 aircraft flew on January 24, 1989, from Stavanger to Spitsbergen, Norway, at the 430-440 K potential temperature surface (19.2-19.8 km pressure altitude). Aerosols were sampled continuously by an optical particle counter (PMS-FSSP300) for concentration and size analyses, and during five 10-min intervals by four wire and one replicator impactor for concentration, size, composition, and phase analysis. During sampling, the air saturation of H2O with respect to ice changed from 20 to 100 percent, and of HNO3 with respect to nitric acid trihydrate (NAT) from subsaturation to supersaturation. Data from both instruments indicate a condensation of hydrochloric acid and, later, nitric acid on the background aerosol particles as the ambient temperature decreases along the flight track. This heterogeneous nucleation mechanism generates type I polar stratospheric cloud particles of 10-fold enhanced optical depth, which could play a role in stratospheric ozone depletion.

The paper uses particle size and volume measurements obtained with the forward scattering spectrometer probe model 300 during January and February 1989 in the Airborne Arctic Stratospheric Experiment to investigate processes important in the formation and growth of polar stratospheric cloud (PSC) particles. It is suggested on the basis of comparisons of the observations with expected sulfuric acid droplet deliquescence that in the Arctic a major fraction of the sulfuric acid droplets remain liquid until temperatures at least as low as 193 K. It is proposed that homogeneous freezing of the sulfuric acid droplets might occur near 190 K and might play a role in the formation of PSCs.

In situ aircraft measurements in the lower stratosphere are used to investigate the reactive nitrogen, NO(y), total water, and particle components of the polar stratospheric cloud (PSC) aerosol in the Arctic. The results are compared to findings from the Antarctic derived using similar measurements and interpretive techniques. The Arctic data show that particle volume well above background values is present at temperatures above the frostpoint, confirming the result from the Antarctic that the observed PSCs are not water ice particles. NO(y) measurements inside a PSC are enhanced above ambient values consistent with anisokinetic sampling of particles containing NO(y). In the Arctic data over long segments of several flights, calculations show saturation with respect to nitric acid trihydrate without significant PSC particle growth above background.

Measurements were made of stratospheric sulfate aerosols using a passive cavity aerosol spectrometer and a condensation nucleus counter on a NASA ER-2 aircraft in the Airborne Arctic Stratospheric Experiment of 1989. The problems of representative and accurate sampling and particle evaporation were explicitly addressed in the design of the inlets and reduction of the data. The measurements suggest that the sulfate aerosol is bimodal in the polar vortex above the mass mixing ratio maximum in the sulfate layer. It appears that a nuclei mode of small, newly formed particles exists in this region. A stronger case is made for a nuclei mode in the upper few kilometers of the troposphere and in the lower few kilometers of the stratosphere. This mode is probably a global phenomenon occurring in all seasons. Comparison of denitrified and nondenitrified air suggests that denitrification removes some of the larger sulfate particles.

Report dicusses nitrate, sulfate, and chloride contents of stratospheric aerosols during 1987 Airborne Antarctic Ozone Experiment. Emphasizes growth of HNO3*3H2O particles in polar stratospheric clouds. Important in testing theories concerning Antarctic "ozone hole".

Representative measurement of aerosol from aircraft-aspirated systems requires special efforts in order to maintain near isokinetic sampling conditions, estimate aerosol losses in the sample system, and obtain a measurement of sufficient duration to be statistically significant for all sizes of interest. This last point is especially critical for aircraft measurements which typically require fast response times while sampling in clean remote regions. This paper presents size-resolved tests, intercomparisons, and analysis of aerosol inlet performance as determined by a custom laser optical particle counter. Measurements discussed here took place during the Global Backscatter Experiment (1988-1989) and the Central Pacific Atmospheric Chemistry Experiment (1988). System configurations are discussed including (1) nozzle design and performance, (2) system transmission efficiency, (3) nonadiabatic effects in the sample line and its effect on the sample-line relative humidity, and (4) the use and calibration of a virtual impactor.

Stratospheric aerosol collections by wire impactors, taken mainly over the western U.S. from early 1984 to late 1986, show the diminishing effects of El Chichon's 1982 eruption, and provide a set of data for judging subsequent volcanic effects. Decrease in sulfate burden during the study time is due to preferential gravitational settling-out of large (above 0.5-micron diameter) sulfate aerosol droplets. As a result of settling from higher levels, lower altitude (12.2-15.2 km) air early in 1984 tends to contain more sulfate than higher level (19.8-21.3 km) air. As of late 1986, however, high- and low-altitude sulfate contents have decreased and are similar, suggesting large-particle settling has been completed. The later sulfate collection size distributions resemble unimodal background spectra, whereas earlier ones are bimodal. Average sulfate load for all altitudes decreases during the period of study from 0.4 to 0.08 microgram/cu m. The latter value is somewhat higher than a volcanically unenriched pre-El Chichon level, suggesting that even as of 1987, stratospheric background had not been obtained.

Particle-size distributions measured from the NASA ER-2 with the new Forward Scattering Spectrometer Probe 300 in a type I polar stratospheric cloud (PSC) on January 24, 1989 show a volume mode near 0.8 micron in diameter. The large increase in particle concentration and volume after cloud entry did not occur until the apparent saturation ratio of nitric acid with respect to nitric acid trihydrate reached 10, but at ratios near 1 subtle changes in the size distribution suggest some type I particles were present. Particle concentrations in cloud of 15-17/cu cm were greater than the CN concentrations of 5-7/cu cm just outside of cloud, suggesting nucleation on more than just sulfate particles. Some particles greater than 4 microns in diameter were observed in a region which was saturated with respect to ice.

The ER-2 Condensation Nucleus Counter (ER-2 CNC) was operated in the Airborne Arctic Stratospheric Expedition (AASE) in January and February 1989. The ER-2 CNC measures the mixing ratio of particles, CN, with diameters from approximately 0.02 to approximately 1 micron. The spatial distribution of CN in the Arctic polar vortex was found to resemble that measured in the Antarctic in the Spring of 1987. The vertical profile of CN in the vortex was lowered by subsidence. At altitudes above the minimum in the CN mixing ratio profile, CN mixing ratios correlated negatively with that of N2O, demonstrating new particle production. CN serve as nuclei in the formation of Polar Stratospheric Clouds (PSCs) and the concentration of CN can affect PSC properties.

In-situ particle measurements made aboard the NASA ER-2 in the Arctic on 890130 (YYMMDD) show Type 1 PSC particles over much of the flight, with instances of embedded Type 2 PSCs. The Type 2 particles were observed at temperatures warmer than the local frost-point temperature of water; extended up to the upper size cutoff of the instrument (about 24-micron diameter); and are shown to contain too large a volume to be primarily NAT. Based on measured vertical temperature profiles, it is concluded that the Type 2 particles observed on this day were formed above the aircraft in a region where saturation with respect to ice was achieved and were sufficiently large to have fallen into the path of the ER-2. Although the amount of material in the particles, expressed as water, is small by comparison to the total (vapor + aerosol) water concentration, the flux of water from the falling particles is of sufficient magnitude, if sustained, to lead to dehydration of the source region. These observations verify the mechanism for dehydration of polar vortex air masses by precipitation of ice particles.

A new instrument, the Forward Scattering Spectrometer Probe (FSSP) 300, was used on the NASA ER-2 during the Airborne Arctic Stratospheric Expedition (AASE) to count and size particles in the size range 0.4-24 microns in diameter. A brief description of the instrument is presented, and observations for each ER-2 flight are summarized. Measurements were made in both type I and type II polar stratospheric clouds as well as in the background sulfuric-acid particles. Total particle concentrations up to 16/cu cm with total particle volumes up to 10 cubic micron/cu cm were observed in some of the polar-stratospheric-cloud events.

Polar stratospheric cloud (PSC) particles are collected on impactors and studied with regard to physical and chemical properties to help explain the importance of heterogeneous chemical reactions for stratospheric ozone depletion. The nitric, hydrochloric, and sulfuric acid content of stratospheric aerosol particles collected at 18 km altitude was determined. It is suggested that nitric acid is a component of polar stratospheric clouds. This is important for two reasons: (1) it proves that chlorine activation takes place at the surface of PSC particles by converting chemically inert chlorine nitrate to chlorine radicals that can react with ozone; and (2) if the PSC particles are large enough to settle out from the stratosphere, the possibility of nitric acid removal can result in the denitrification of the stratosphere.

Results from the flight on January 24, 1989 of the Airborne Arctic Stratospheric Experiment during which the ER-2 aircraft transitioned from unsaturated to ice saturated air at 20 km altitude are presented. Aerosol particles were sampled by wire impactors and examined for number density as a function of particle size by taking photomicrographs in a scanning electron microscope and visually sizing and counting the particles. Differences in the chemical, physical and optical properties of stratospheric aerosol between ice-saturated and nonsaturated air are described.

The use of the active scattering spectrometer probe (ASAS-X) to measure sulfuric acid aerosols on U-2 and ER-2 research aircraft has yielded results that are at times ambiguous due to the dependence of particles' optical signatures on refractive index as well as physical dimensions. The calibration correction of the ASAS-X optical spectrometer probe for stratospheric aerosol studies is validated through an independent and simultaneous sampling of the particles with impactors; sizing and counting of particles on SEM images yields total particle areas and volumes. Upon correction of calibration in light of these data, spectrometer results averaged over four size distributions are found to agree with similarly averaged impactor results to within a few percent: indicating that the optical properties or chemical composition of the sample aerosol must be known in order to achieve accurate optical aerosol spectrometer size analysis.

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.