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All sourcesNASA NTRSDOE OSTI
NASA NTRS1991

Aircraft laser infrared absorption spectrometer (ALIAS) for polar ozone studies

The ALIAS instrument is a very high resolution (0.0003/cm) scanning, tunable diode laser spectrometer designed to make direct, simultaneous measurements of NO2, HNO3, HCl, CH4, and either O3 or N2O (including vertical profiles of CH4 and N2O) in the polar stratosphere at sub-part-per-billion level sensitivities over integration times from 3 to 30 s. Unique features include a sample inlet/throttle system designed to achieve near-isokinetic sampling, in PSC events, an in-flight wavelength reference cell rack, mechanical fringe-spoilers, a four-laser/four-detector dewar with 24-hr hold-time operating at a fixed temperature without electrical regulation, and in-flight fast correlation routines for spectral drift compensation prior to spectral addition. Instrument design and test flight results are discussed in the light of ALIAS's role in the Winter 1991 Arctic aircraft stratospheric ozone campaigns out of Fairbanks, Alaska, and Bangor, Maine.

Webster, C. R.↗
NASA NTRS1993

Heterogeneous chemistry on Antarctic polar stratospheric clouds - A microphysical estimate of the extent of chemical processing

A detailed model of polar stratospheric clouds (PSCs), which includes nucleation, condensational growth. and sedimentation processes, has been applied to the study of heterogeneous chemical reactions. For the first time, the extent of chemical processing during a polar winter has been estimated for an idealized air parcel in the Antarctic vortex by calculating in detail the rates of heterogeneous reactions on PSC particles. The resulting active chlorine and NO(x) concentrations at first sunrise are analyzed with respect to their influence upon the Antarctic ozone hole using a photochemical model. It is found that the species present at sunrise are primarily influenced by the relative values of the heterogeneous reaction rate constants and the initial gas concentrations. However, the extent of chlorine activation is also influenced by whether N2O5 is removed by reaction with HCl or H2O. The reaction of N2O5 with HCl, which occurs rapidly on type 1 PSCs, activates the chlorine contained in the reservoir species HCl. Hence the presence and surface area of type 1 PSCs early in the winter are crucial in determining ozone depletion.

Drdla, K.↗
NASA NTRS1993

Fourier transform infrared studies of the interaction of HCl with model polar stratospheric cloud films

Heterogeneous reactions involving hydrochloric acid adsorbed on the surfaces of polar stratospheric clouds (PSCs) are postulated to contribute to polar ozone loss. Using FTIR spectroscopy to probe the condensed phase, we have examined the interaction of HCl with ice and nitric acid trihydrate (NAT) films representative of types II and I PSCs, respectively. For HCl pressures in the range of 10 exp -7 to 10 exp -5 Torr, our FTIR studies show that a small amount of crystalline HCl-6H2O formed on or in ice at 155 K. However, for higher HCl pressures, we observed that the entire film of ice rapidly converted into an amorphous 4:1 H2O:HCl mixture. From HCl-uptake experiments with P(HCl) = 8 x 10 exp -7 Torr, we estimate roughly that the diffusion coefficient of HCl in ice is around 2 x 10 exp -12 sq cm/s at 158 K. For higher temperatures more closely approximating those found in the stratosphere, we were unable to detect bulk HCl uptake by ice. Indirect evidence suggests that HCl adsorption onto the surface of model PSC films inhibited the evaporation of both ice and NAT by 3-5 K.

Koehler, Birgit G.↗
NASA NTRS1993

Spectroscopic studies of model polar stratospheric cloud films

Fourier transform infrared (FTIR) spectroscopy has been used to study nitric-acid/ice films representative of type I polar stratospheric clouds (PSCs). These studies reveal that in addition to amorphous nitric acid/ice mixtures, there are three stable stoichiometric hydrates of nitric acid: nitric-acid monohydrate (NAM), dihydrate (NAD), and trihydrate (NAT). We also observe two distinct crystalline forms of the trihydrate, which we denote alpha- and beta-NAT. These two forms appear to differ in their concentration of crystalline defects, but not in their chemical composition. In addition to probing the composition of type I PSCs, we have also used FTIR spectroscopy to study the interaction of HCl with model PSC films. In this work we find that for HCl pressures in the range 10 exp -5 to 10 exp -7 Torr, HCl is taken up by ice at 155 K to form a thin layer of HCl.6H2O. At 193 K, the uptake of HCl by ice was consistent with less than or equal to monolayer coverage. Uptake of HCl by alpha and beta-NAT at 175 K was also consistent with less than or equal to monolayer coverage.

Tolbert, Margaret A.↗
NASA NTRS1993

Physical chemistry of the H2SO4/HNO3/H2O system - Implications for polar stratospheric clouds

Polar stratospheric clouds (PSCs) play a key role in stratospheric ozone depletion. Surface-catalyzed reactions on PSC particles generate chlorine compounds that photolyze readily to yield chlorine radicals, which in turn destroy ozone very efficiently. The most prevalent PSCs form at temperatures several degrees above the ice frost point and are believed to consist of HNO3 hydrates; however, their formation mechanism is unclear. Results of laboratory experiments are presented which indicate that the background stratospheric H2SO4/H2O aerosols provide an essential link in this mechanism: These liquid aerosols absorb significant amounts of HNO3 vapor, leading most likely to the crystallization of nitric acid trihydrate (NAT). The frozen particles then grow to form PSCs by condensation of additional amounts of HNO3 and H2O vapor. Furthermore, reaction probability measurements reveal that the chlorine radical precursors are formed readily at polar stratospheric temperatures not just on NAT and ice crystals, but also on liquid H2SO4 solutions and on solid H2SO4 hydrates. These results imply that the chlorine activation efficiency of the aerosol particles increases rapidly as the temperature approaches the ice frost point regardless of the phase or composition of the particles.

Molina, M. J.↗
NASA NTRS1993

Studies of dynamical processes affecting the distribution of stratospheric ozone

The purpose of the research was to understand large-scale tracer transport processes in the stratosphere. Two approaches were taken. The first is analysis of tracer observations, especially satellite observations of ozone concentration and total column ozone. The second is numerical simulation of tracer transport processes. Topics researched include: quasi-biennial oscillation (QBO) and stratospheric ozone; mixing in the polar vortices; polar stratospheric clouds (PSC) properties from Antarctic lidar data; and statistical methods for numerical experiments.

Bowman, Kenneth P.↗
NASA NTRS1993

Stratospheric aircraft exhaust plume and wake chemistry

Progress to date in an ongoing study to analyze and model emissions leaving a proposed High Speed Civil Transport (HSCT) from when the exhaust gases leave the engine until they are deposited at atmospheric scales in the stratosphere is documented. A kinetic condensation model was implemented to predict heterogeneous condensation in the plume regime behind an HSCT flying in the lower stratosphere. Simulations were performed to illustrate the parametric dependence of contrail droplet growth on the exhaust condensation nuclei number density and size distribution. Model results indicate that the condensation of water vapor is strongly dependent on the number density of activated CN. Incorporation of estimates for dilution factors into a Lagrangian box model of the far-wake regime with scale-dependent diffusion indicates negligible decrease in ozone and enhancement of water concentrations of 6-13 times background, which decrease rapidly over 1-3 days. Radiative calculations indicate a net differential cooling rate of the plume about 3K/day at the beginning of the wake regime, with a total subsidence ranging between 0.4 and 1 km. Results from the Lagrangian plume model were used to estimate the effect of repeated superposition of aircraft plumes on the concentrations of water and NO(y) along a flight corridor. Results of laboratory studies of heterogeneous chemistry are also described. Kinetics of HCl, N2O5 and ClONO2 uptake on liquid sulfuric acid were measured as a function of composition and temperature. Refined measurements of the thermodynamics of nitric acid hydrates indicate that metastable dihydrate may play a role in the nucleation of more stable trihydrates PSC's.

Miake-Lye, R. C.↗
NASA NTRS1994

Stratospheric minor species vertical distributions during polar winter by balloon borne UV-Vis spectrometry

A light, relatively cheap and easy to operate balloonborne UV-visible spectrometer was designed for investigating ozone photochemistry in the Arctic winter. The instrument was flown 11 times during the European Arctic Stratospheric Ozone Experiment (EASOE) in winter 1991-92 in Northern Scandinavia. The first simultaneous measurements of vertical distributions of aerosols, PSC's, O3, NO2 and OClO inside the vortex during flight no. 6 on 16 January, in cold conditions are reported, which show that nitrogen oxides were almost absent (lower than 100 ppt) in the stratosphere below 22 km, while a layer of relatively large OClO concentration (15 ppt) was present at the altitude of the minimum temperature.

Pommereau, J. P.↗
NASA NTRS1994

Measurements of the vertical profile, diurnal variation, and secular change of ClO in the stratosphere over Thule, Greenland, February-March, 1992

We report observations of stratospheric chlorine monoxide over the altitude range approx. 16 to 50 km at Thule, Greenland from Feb. 8 to Mar. 24, 1992. A new, more sensitive ground-based mm-wave spectrometer was employed for these measurements, similar in principle to that used earlier for the discovery of low altitude ClO in the Antarctic springtime. In this report, we discuss different aspects of vertical distribution, secular trends, and diurnal variation of ClO in the Arctic stratosphere, based on a preliminary analysis of our Thule data. We see no evidence for large (approx. 1.2-1.5 ppb) amounts of ClO in the lower stratosphere at any time during February or March, in agreement with UARS-MLS findings for this period, and in marked contrast to findings reported for the Arctic in January. We have some evidence for small enhancements (approx. 0.2-0.5 ppb) in the 18-30 km range in late February-early March, which might be associated with volcanic aerosol, rather than PSC, processing.

Dezafra, Robert L.↗
NASA NTRS1994

Ozone, aerosols and polar stratospheric clouds measurements during the EASOE Campaign

Preliminary results are presented of observations obtained during the EASOE campaign, with an airborne backscatter lidar and a ground-based DIAL ozone lidar system. Although the main signature observed on the lidar signals was due to the Pinatubo cloud which erupted in June 1991, distinct PSC events were detected on several occasions by the airborne lidar often in relation with orographic wave activity over the norvegian mountains. The ozone profiles obtained in Sodankyla with the ground based lidar are locally perturbed by the presence of the volcanic cloud. After a first correction of the aerosols effect, they present however a reasonably good agreement with the ozone sondes profiles performed on the same site.

Godin, S.↗
NASA NTRS1994

Observation of ozone and aerosols in the Antarctic ozone hole of 1991 under the Polar Patrol Balloon (PPB) Project. Preliminary result

We present preliminary results for the PPB (Polar Patrol Balloon) experiment. The balloon was launched at 07:55 UT on 23 September and dropped at 21 UT on 28 September 1991. During the period, ozone and aerosol concentrations were measured correspondingly along the track. During the Lagrangian type observation, drastic change of ozone concentration in 'same air mass' and positive correlation between ozone concentration and sulfate aerosol amount were obtained at the level within 80-78 hPa. During the descent motion at 80 deg S active PSC's (type-1 and -2) were observed from 200 hPa to 80 hPa.

Hayashi, Masahiko↗
NASA NTRS1995

Nucleation and growth of crystals under cirrus and polar stratospheric cloud conditions

Laboratory studies examine phase changes of hygroscopic substances which occur as aerosol in stratosphere and troposphere (sodium chloride, ammonium sulfate, ammonium bisulfate, nitric acid, sulfuric acid), under controlled conditions, in samples volume 1 to 10(exp -4) ml. Crystallization of salts from supersaturated solutions is examined by slowly evaporating a solution drop on a substrate, under controlled relative humidity, until self nucleation occurs; controlled nucleation of ice in a mm capillary U-tube gives a measured ice crystallization velocity at known supercooling. Two states of crystallization occur for regions where hydrates exist. It is inferred that all of the materials readily exist as supersaturated/supercooled solutions; the degree of metastability appears to be slightly enhanced by inclusion of aircraft produced soot. The crystallization velocity is taken as a measure of viscosity. Results suggest an approach to a glass transition at high molality, supersaturation and/or supercooling within the range of atmospheric interest. It is hypothesized that surface reactions occur more readily on solidified particles - either crystalline or glass, whereas volume reactions are more important on droplets with sufficiently low viscosity and volume diffusivity. Implications are examined for optical properties of such particles in the atmosphere. In a separate experiment, crystal growth was examined in a modified thermal vapor diffusion chamber over the range of cirrus temperature (-30 to -70 C) and under controlled supersaturation and air pressure. The crystals grew at a velocity of 1-2 microns/s, thickness 60-70 micron, in the form of thin column crystals. Design criteria are given for a system to investigate particle growth down to -100 C, (PSC temperatures) where nitric acid particles can be grown under similar control and in the form of hydrate crystals.

Hallett, John↗
NASA NTRS1995

Minimum fan turbine inlet temperature mode evaluation

Measured reductions in turbine temperature which resulted from the application of the F-15 performance seeking control (PSC) minimum fan turbine inlet temperature (FTIT) mode during the dual-engine test phase is presented as a function of net propulsive force and flight condition. Data were collected at altitudes of 30,000 and 45,000 feet at military and partial afterburning power settings. The FTIT reductions for the supersonic tests are less than at subsonic Mach numbers because of the increased modeling and control complexity. In addition, the propulsion system was designed to be optimized at the mid supersonic Mach number range. Subsonically at military power, FTIT reductions were above 70 R for either the left or right engines, and repeatable for the right engine. At partial afterburner and supersonic conditions, the level of FTIT reductions were at least 25 R and as much as 55 R. Considering that the turbine operates at or very near its temperature limit at these high power settings, these seemingly small temperature reductions may significantly lengthen the life of the turbine. In general, the minimum FTIT mode has performed well, demonstrating significant temperature reductions at military and partial afterburner power. Decreases of over 100 R at cruise flight conditions were identified. Temperature reductions of this magnitude could significantly extend turbine life and reduce replacement costs.

Orme, John S.↗
NASA NTRS1994

Growth of nitric acid hydrates on thin sulfuric acid films

Type I polar stratospheric clouds (PSCs) are thought to nucleate and grow on stratospheric sulfate aerosols (SSAs). To model this system, thin sulfuric acid films were exposed to water and nitric acid vapors (1-3 x 10(exp -4) Torr H2O and 1-2.5 x 10(exp -6) Torr HNO3) and subjected to cooling and heating cycles. Fourier Transform Infrared (FTIR) spectroscopy was used to probe the phase of the sulfuric acid and to identify the HNO3/H2O films that condensed. Nitric acid trihydrate (NAT) was observed to grow on crystalline sulfuric acid tetrahydrate (SAT) films. NAT also condensed in/on supercooled H2SO4 films without causing crystallization of the sulfuric acid. This growth is consistent with NAT nucleation from ternary solutions as the first step in PSC formation.

Iraci, Laura T.↗
NASA NTRS1993

In situ measurements of the ClO/HCl ratio: Heterogeneous processing on sulfate aerosols and polar stratospheric clouds

Simultaneous in situ measurements of stratospheric ClO and HCl have been made for the first time, during numerous flights of the ER-2 aircraft covering latitudes 24-90 deg N from October 1991 through March 1992. The ClO/HCl ratio is identified as a key indicator of heterogeneous processing both outside and within the Arctic polar vortex. For ClO mixing ratios below about 120 pptv, remarkably constant ClO/HCl values of about 15% characterize the lower stratosphere. The observed values are significantly higher than those derived from a 2-D model using either gas phase photochemistry alone (2%), or including heterogeneous sulfate chemistry (5-10%). During the Arctic early spring, after conversion of HCl into reactive chlorine has taken place, the vortex edge is poorly defined by ClO levels. Loss of HCl and its slow recovery following low-temperature polar heterogeneous chemistry distinguishes HCl as a new and unique dynamical tracer of polar stratospheric clouds (PSC)-processed air.

Webster, C. R.↗
NASA NTRS1993

A case study of the mountain lee wave event of January 6, 1992

A mountain wave event, observed at the southern tip of Greenland on January 6, 1992, was corroborated by three experiments: the Meteorological Measurement System (MMS), the Microwave Temperature Profiler (MTP), and the Reactive Nitrogen Instrument (NO/NO(y)). Gravity wave signatures with classical phase relationship between wind and temperature were observed on both the outbound and inbound legs at different altitudes. The waves showed both vertically propagating and evanescent properties. Characteristics of the dominant wave mode are: wavelength about = 35 km; vertical displacement about = 0.8 km, and peak-to-peak vertical wind about = 6/ms. With the prevailing wind at about = 37/ms, the stratospheric temperature was reduced by 6K to 195.5 K within 8 minutes. The implication and potential impact of mountain lee waves on the formation of polar stratospheric clouds (PSC's) are discussed.

Chan, K. R.↗
NASA NTRS1993

Stratospheric NO(y) measurements on the NASA DC-8 during AASE 2

We survey measurements of stratospheric NO(y) on the NASA DC-8 during AASE 2 in early 1992. Emphasis is on correlations with other long-lived species: O3, N2O, and CH4. No cases of extremely high NO(y)/O3 ratios were seen in 1992. This suggests that denitrification at higher altitudes was less pervasive than in 1989. Values of NO(y)/O3 in 1992 are comparable to, though perhaps lower than, those measured in 1989. The correlation of NO(y) with N2O changes over the course of the mission. Relative to the correlation for the whole season, low values of NO(y) occur in February, most notably on the 22nd. The reason for the low NO(y) is unknown. It is generally too warm at DC-8 altitudes for the presence of Polar Stratospheric Cloud (PSC) particles, but denitrification at higher altitudes, followed by descent, might account for the low values seen on 22 February. However, this may be unlikely since the NASA ER-2, flying during the same period, saw no evidence of denitrification at higher altitudes (Loewenstein et al., 1993).

Weinheimer, A. J.↗
NASA NTRS1994

Analysis of the physical state of one Arctic polar stratospheric cloud based on observations

During the Arctic Airborne Stratospheric Expedition (AASE) simultaneous measurements of aerosol size distribution and NO(y)(HN03 + NO + NO2 + 2(N205)) were made along ER-2 flight paths. The flow characteristics of the NO(y) instrument allow us to derive the condensed NO(y) amount (assumed to be HN03) present during polar stratospheric cloud (PSC) events. Analysis of the January 24th flight indicates that this condensed HN03 amount does not agree well with the aerosol volume if the observed PSCs are composed of solid nitric acid trihydrate (NAT), as is generally assumed. However, the composition agrees well with that predicted for liquid H2S04/HN03/H20 solution droplets using a new Aerosol Physical Chemistry Model (APCM). The agreement corresponds in detail to variations in temperature and humidity. The weight percentages of H2SO4, HN03, and H2O derived from the measurements all correspond to those predicted for ternary, liquid solutions.

Drdla, K.↗