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NASA NTRS1993

Interpretation of NO(x)/NO(y) observations from AASE-2 using a model of chemistry along trajectories

In situ measurements of NO and NO(y) are used to derive the ratio NO(x)/NO(y) along the flight track of the NASA ER-2 aircraft. Data are presented for two flights at midlatitudes in October 1991 during the Airborne Arctic Stratospheric Expedition-2 (AASE-2). Aerosol particle surface area was concurrently measured. The observations are compared with a photochemical model integrated along back trajectories from the aircraft flight track. Comparison of observations with the model run along trajectories and at a fixed position clearly and quantitatively demonstrates the importance of an air parcel's dynamic history in interpretation of local chemical observations. Comparison of the data with model runs under different assumptions regarding heterogeneous chemistry further reinforces the case for occurrence of the reaction of N2O5 + H2O on sulfate aerosol surfaces in the atmosphere. Finally, comparisons for which relative changes in the model and the data are not consistent caution that our ability to resolve all the observations is not yet complete.

Kawa, S. R.↗

NASA NTRS1993

Effects of Pinatubo aerosol on stratospheric ozone at mid-latitudes

Mid-latitude ozone data from ER-2 aircraft measurements in 1989, 1991, and 1992 were examined to determine how sulfate aerosols from the eruption of Mt. Pinatubo had affected ozone at about 18 km. N2O was used as a tracer to help distinguish between chemical and dynamical aerosol effects. At 20-45 deg N in February 1992, ozone was about 10-20% lower than February 1989 and 1991, with respect to N2O. Data from Aug. 1991 - Mar. 1992 showed changes in ozone with respect to N2O, but the magnitude of those changes was not correlated with the magnitude of the changes in aerosol surface area density.

Weaver, A.↗

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

In-situ measurements of changes in stratospheric aerosol and the N2O-aerosol relationship 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 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.

Borrmann, S.↗

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.↗

NASA NTRS1994

In situ measurements of the NO2/NO ratio for testing atmospheric photochemical models

Simultaneous in situ measurements of NO2, NO, O3, ClO, pressure and temperature have been made for the first time, presenting a unique opportunity to test our current understanding of the photochemistry of the lower stratospere. Data were collected from several flights of the ER-2 aircraft at mid-latitudes in May 1993 during NASA's Stratospheric Photochemistry, Aerosols and Dynamics Expedition (SPADE). The daytime ratio of NO2/NO remains fairly constant at 19 km with a typical value of 0.68 and standard deviation of +/- 17. The ratio observations are compared with simple steady-state calculations based on laboratory-measured reaction rates and modeled NO2 photolysis rates. At each measurement point the daytime NO2/NO with its measurements uncertainty overlap the results of steady-state caculations and associated uncertainty. Possible sources of error are examined in both model and measurements. It is shown that more accurate laboratory determinations of the NO + 03 reaction rate and of the NO2 cross-sections in the 200-220 K temperature range characteristic of the lower stratosphere would allow for a more robust test of our knowledge of NO(X) phtochemistry by reducing significant sources if uncertainties in the interpretation of statospheric measurements.

Jaegle, L.↗

NASA NTRS1994

Tracer-tracer relationships and lower stratospheric dynamics: CO2 and N2O correlations during SPADE

Simultaneous measurements of CO2 and N2O from the NASA ER-2 aircraft during SPADE deployments in November 1992, April/May 1993, and October 1993 provide new information on transport rates in the lower stratosphere. The tropospheric seasonal cycle in CO2, superimposed on the long-term trend, is observed to propagate into the statosphere. The compact correlations observed between CO2 and N2O indicate that meridional transport is sufficiently rapid to create a uniform set of relationships over the northern hemisphere up to at least 21 km even though CO2 changes significantly on a time scale of 8 to 12 weeks. the observed seasonal dependence of the correlations indicates that vertical transport above 20 km is slower in northern summer than in winter and slow throughout the year between 19 km and the tropopause. The inferred amplitude of the seasonal CO2 oscillation in the statopshere, viewed relative to N2O, places constraints on the mean latitude for air entering the statosphere.

Boering, Kristie A.↗

NASA NTRS1994

Development of Techniques for the In Situ Observation of OH and HO2 for Studies of the Impact of High-Altitude Supersonic Aircraft on the Stratosphere

This three-year project supported the construction, calibration, and deployment of a new instrument to measure the OH and HO2 radicals on the NASA ER-2 aircraft. The instrument has met and exceeded all of its design goals. The instrumentation represents a true quantum leap in performance over that achieved in previous HO(x) instruments built in our group. Sensitivity for OH was enhanced by over two orders of magnitude as the weight fell from approximately 1500 to less than 200 Kg. Reliability has been very high: HO(x) data are available for all flights during the first operational mission, the Stratospheric Photochemistry, Aerosols, and Dynamics Expedition (SPADE). The results of that experiment have been reported in the scientific literature and at conferences. Additionally, measurements of H2O and O3 were made and have been reported in the scientific literature. The measurements demonstrate the important role that OH and HO2 play in determining the concentration of ozone in the lower stratosphere. During the SPADE campaign, the measurements demonstrate that the catalytic removal is dominated by processes involving the odd-hydrogen and halogen radical extremely important constraint for photochemical models that are being used to assess the potential deleterious effects of super-sonic aircraft effluent on the burden of stratospheric ozone. A list of the papers that came from this research are included, along with a copy of the paper, 'Aircraft-borne, laser-induced fluorescence instrument for the in situ detection of hydroxyl and hydroperoxyl radicals'.

Anderson, James G.↗

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 PSC-processed air.

Webster, C. R.↗

NASA NTRS1993

Airborne Arctic Stratospheric Expedition 2: An Overview

The sudden onset of ozone depletion in the antarctic vortex set a precedent for both the time scale and the severity of global change. The Airborne Antarctic Ozone Experiment (AAOE), staged from Punta Arenas, Chile, in 1987, established that CFCs, halons, and methyl bromide, the dominant sources of chlorine and bromine radicals in the stratosphere, control the rate of ozone destruction over the Antarctic; that the vortex is depleted in reactive nitrogen and water vapor; and that diabatic cooling during the antarctic winter leads to subsidence within the vortex core, importing air from higher altitudes and lower latitudes. This last conclusion is based on observed dramatic distortion in the tracer fields, most notably N2O. In 1989, the first Airborne Arctic Stratospheric Expedition (AASE-I), staged from Stavanger, Norway, and using the same aircraft employed for AAOE (the NASA ER-2 and the NASA DC-8), discovered that while NO(x) and to some degree NO(y) were perturbed within the arctic vortex, there was little evidence for desiccation. Under these (in contrast to the antarctic) marginally perturbed conditions, however, Cl0 was found to be dramatically enhanced such that a large fraction of the available (inorganic) chlorine resided in the form of Cl0 and its dimer ClOOCl. This leaves two abiding issues for the northern hemisphere and the mission of the second Airborne Arctic Stratospheric Expedition (AASE-II): (1) Will significant ozone erosion occur within the arctic vortex in the next ten years as chlorine loading in the stratosphere exceeds four parts per billion by volume? and (2) Which mechanisms are responsible for the observed ozone erosion poleward of 30 deg N in the winter/spring northern hemisphere reported in satellite observations?

Anderson, James G.↗

NASA NTRS1993

Effects of Pinatubo Aerosol on Stratospheric Zone at Mid-Lattiudes

Mid-latitude ozone data from ER-2 aircraft measurements in 1989, 1991 and 1992 were examined to determine how sulfate aerosols from the eruption of Mt. Pinatubo had affected ozone at about 18 km. N2O was used as a tracer to help distinguish between chemical and dynamical aerosol effects. At 20-45 deg N in February 1992, ozone was about 10-20% lower than February 1989 and 1991, with respect to N2O. Data from Aug.1991 - Mar. 1992 showed changes in ozone with respect to N2O, but the magnitude of those changes was not correlated with the magnitude of the changes in aerosol surface area density.

Weaver, A.↗

NASA NTRS1993

In Situ Measurements of the ClO/HCl Ratio: Heterogeneous Processing on Sulfate Aerosols and Polar Stratospheric Clouds

Webster, C. R.↗

NASA NTRS1993

In-Situ Measurements of Changes in Stratospheric Aerosol and the N2O - Aerosol Relationship 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.

Borrmann, S.↗

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 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.

Weinheimer, A. J.↗

NASA NTRS1989

The Origins of Air Parcels Uplifted in a Two Dimensional Gravity Wave in the Tropical Upper Troposphere During the NASA Stratosphere Troposphere Exchange Project (STEP)

During January and February 1987, as part of the Stratosphere-Troposphere Exchange Project, the NASA ER-2 made 11 flights from Darwin, Australia to investigate dehydration mechanisms in the vicinity of the tropical tropopause. After the monsoon onset in the second week of January, steady easterly flow of 15-25 ms (exp -1) was established in the upper troposphere and lower stratosphere over northern Australia and adjacent seas. Penetrating into this regime were elements of the monsoon convection such as overshooting convective turrets and extensive anvils including cyclone cloud shields. In cases of the latter, the resulting flow obstructions tended to produce mesoscale gravity waves. In several instances the ER- 2 meteorological and trace constituent measurements provide a detailed description of the structure of these gravity waves. Among these was STEP Flight 6, 22-23 January. It is of particular interest to STEP because of the close proximity of ice-laden and dehydrated air on the same isentropic surfaces. Convective events inject large amounts of ice into the upper troposphere and lower stratosphere which may not be completely removed by local precipitation processes. In the present instance, a gravity wave for removed from the source region appears to induce relativity rapid upward motion in the ice-laden air and subsequent dessication. Potential mechanisms for such a localized removal process are under investigation.

Selkirk, Henry B.↗

NASA NTRS1992

Black Carbon (Soot) Aerosol in the Lower Stratosphere and Upper Troposphere

We have used two approaches to measure BCA in the stratosphere. The first method consists of collecting aerosols by impaction on quartz rods, upon which are mounted strips of polystyrene filter material. Each 25 mm by 0.5 mm filter strip is alternately masked and exposed in 5 mm long sections. After sampling, the optical density of the exposed sections is measured and compared with the optical density of the masked (unexposed) sections. The filter strip is a Lambertian collector, the scattering property of which is not affected by the deposition of liquid sulfuric acid droplets which dominate the stratospheric aerosol. Hence, all attenuation greater in the exposed than in the non-exposed sections is due to absorption by BCA or rare opaque materials such as meteoritic iron. In a second approach we expose carbon-coated gold or palladium wires to air outside the aircraft boundary layer [Farlow et al., 1979; Pueschel et al., 1989]. With a field emission scanning electron microscope we are able to characterize BCA particles in addition to the dominant sulfuric acid droplets. Typically, soot is comprised of 20 nm diameter spheres linked together as branching chains or loosely packed aggregates (Figure 1a). The microscope has a lateral image resolution of 1.5 nm and can clearly resolve individual spheres making up BCA aggregates. Their morphology is uniquely different from that of the liquid sulfuric acid-water aerosol (Figure 1b). We approximate the size of each BCA particle by that of a sphere of equivalent volume and fit a lognormal size distribution to both the BCA and H2SO4/H2O aerosols. Both sampler types have been mounted on NASA's ER-2 high-altitude research aircraft (altitude ceiling of 70,000 feet), and on NASA's DC-8 (40,000 feet ceiling) aircraft to sample aerosols from a significant portion of the atmosphere.

Pueschel, R. F.↗

NASA NTRS1994

Pinatubo Aerosol Evolution: Using Composite Data Sets to Build the Global- to Micro-Scale Picture and Assess Consistency of Different Measurements

This paper brings together experimental evidence required to build realistic models of the global evolution of physical, chemical, and optical properties of the aerosol resulting from the 1991 Pinatubo volcanic eruption. Such models are needed to compute the effects of the aerosol on atmospheric chemistry, dynamics, radiation, and temperature. Whereas there is now a large and growing body of post-Pinatubo measurements by a variety of techniques, some results are in conflict, and a self-consistent, unified picture is needed, along with an assessment of remaining uncertainties. This paper examines data from photometers, radiometers, impactors, optical counters/sizers, and lidars operated on the ground, aircraft, balloons, and spacecraft. Example data sources include: - Tracking sunphotometers and lidars at Mauna Loa Observatory (MLO) and on the DC-8 - Particle spectrometers and wire impactors on the ER-2 and DC-8 - Dustsondes (particle counters/sizers on balloons) - SAGE II, SAM II, AVHRR, CLAES, and ISAMS sensors on a variety of satellites. We assess the mutual consistency of these disparate data sets and recommend 'consensus" properties and uncertainties in the process of developing a composite data set. Recommended properties include the spatial and temporal evolution of particle chemical composition, shape, wavelength and temperature-dependent refractive index, size distribution, and optical depth spectra. Supporting references are cited and representative data shown.

Russell, P. B.↗