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We show that a nighttime profile of OClO in the Arctic vortex during the winter of 2000 is overestimated, by nearly a factor of 2, using an isentropic trajectory model constrained by observed profiles of ClOx (ClO + 2 X ClOOCl) and BrO. Calculated abundances of nighttime OClO are shown to be sensitive to the abundance of BrOx (BrO + BrCl), details of the air parcel history during the most recent sunrise/sunset transitions, and the BrCl yield from the reaction BrO + ClO. Many uncertainties are considered, and the discrepancy between measured and modeled nighttime OClO appears to be robust. This discrepancy suggests that production of OClO occurs more slowly than implied by standard photochemistry. If the yield of BrCl from the reaction of BrO + ClO is increased from 7% (JPL 2002 value) to 11% (near the upper limit of the uncertainty), good agreement is found between measured and modeled nighttime OClO. This study highlights the importance of accurate knowledge of BrO + ClO reaction kinetics as well as air parcel trajectories for proper interpretation of nighttime OClO. These factors have a considerably smaller impact on the interpretation of OClO observations obtained during twilight (90(deg) <=SZA <= 92(deg)), when photolytic processes are still active.

Ozone measurements from ozonesondes, AROTAL, DIAL, and POAM III instruments during the SOLVE-2/VINTERSOL period are composited in a time-varying, flow-following quasi-conservative (PV-6) coordinate space; the resulting composites from each instrument are mapped onto the other instruments locations and times. The mapped data are then used to intercompare data from the different instruments. Overall, the four data sets are found to be in good agreement. AROTAL shows somewhat lower values below 16 km, and DIAL has a positive bias at the upper limits of its altitude range. These intercomparisons are consistent with those obtained from more conventional near-coincident profiles, where available. Although the PV-theta mapping technique entails larger uncertainties of individual profile differences compared to direct near-coincident comparisons, the ability to include much larger numbers of comparisons can make this technique advantageous.

During the winter of 1999-2000, the Sage III Ozone Loss and Validation Experiment (SOLVE) field experiment took place in Kiruna, Sweden. The purpose of SOLVE was to examine ozone depletion mechanisms in the Arctic stratosphere (from about 10 to 50 km altitude) during the winter and early spring, when a band of strong winds (the 'polar vortex') circle the pole. Measurements of stratospheric ozone were made by several different kinds of instruments in different meteorological situations. We analyzed these data using the 'quasi-conservative coordinate mapping' technique, in which the measurements are analyzed in terms of meteorological properties ('potential temperature' and 'potential vorticity') which tend not to change very much over a few days. This technique reduces or removes the changes that are associated with the polar vortex moving around. Over longer time periods, potential temperature and potential vorticity change as air cools and descends within the polar vortex. We account for these changes by calculating the trajectories of air parcels, and this enables us to extend the analysis over a ten-week period from January 10 to March 17, 2000. Using data from the NASA ER-2 aircraft, from the DIAL and AROTEL laser sounders on the NASA DC-8 aircraft, and balloon-borne ozonesondes, our analysis reveals changes in ozone which, because we have removed the effects of polar vortex motion and the descending air, indicate chemical destruction of ozone in early 2000. We find a peak decline rate of approximately 0.03 ppmv/day near 470 K of potential temperature (near 20 km) in mid-January which sinks in altitude to around 440 K (near 18 km) in mid-March.

A high-altitude aircraft flight on April 18, 1997 detected an enormous aerosol cloud at 20 km altitude near California (37 N). Not visually observed, the cloud had high concentrations of soot and sulfate aerosol, and was over 180 km in horizontal extent. The cloud was probably a large hydrocarbon fueled vehicle, most likely from rocket motors burning liquid oxygen and kerosene. One of two Russian Soyuz rockets could have produced the cloud: a launch from the Baikonur Cosmodrome, Kazakhstan on April 6; or from Plesetsk, Russia on April 9. Parcel trajectories and long-lived trace gas concentrations suggest the Baikonur launch as the cloud source. Cloud trajectories do not trace the Soyuz plume from Asia to North America, illustrating the uncertainties of point-to-point trajectories. This cloud encounter is the only stratospheric measurement of a hydrocarbon fuel powered rocket.

Ozone amounts observed at high Northern latitudes in late winter and early spring have been relatively very low in four of the last six years. On the face of it, this decline appears similar to that observed in the Antarctic in the mid-1980s in spite of the fact that the abundance of stratospheric chlorine is currently steady or decreasing. In order to predict the extent to which this change represents a trend, and to understand what combination of factors produces the low ozone, we need to accurately simulate these observations with models. In this presentation, we focus on the winter of 1999-2000, which exhibited some of the lowest ozone ever recorded in the Northern hemisphere. It also contained the largest-ever assembled set of atmospheric measurements and modeling activities in the SAGE III Ozone Loss and Validation Experiment/Third European Stratospheric Experiment on Ozone (SOLVE/THESEO). We use SOLVE/THESEO observations in comparison with the Goddard 3-D global model of stratospheric chemistry and transport to explore the model's capability to simulate the evolution of ozone and other species through the winter. We will discuss advective transport and mixing, chlorine activation, and denitrification, which are key processes to accurately simulating wintertime ozone. Preliminary results show that, although the model tracer transport and chlorine activation compare relatively well with observations, the magnitude of observed ozone loss is difficult to achieve in the model. Calculated ozone loss is sensitive to denitrification, which presents a major challenge to parameterization in a global model. Simulation requirements and uncertainties will be evaluated.

Ozone observations from ozonesondes, the DIAL and AROTEL lidars aboard the DC-8, in situ ozone measurements from the ER-2 and satellite ozone measurements from POAM were used to assess ozone loss during the SOLVE 1999-2000 campaign. We compare three different methods of computing the ozone loss. The first method simply compares the time sequence of ozonesondes taken at the same station inside the vortex from December through the end of March. In the second method, ozonesondes from a variety of stations are compared using a variant on the Match technique. This method uses short (approx. 5-10 day) forward diabatic trajectories to connect various sonde launches. In the third method, the measurements are simply injected into a diabatic trajectory model and carried forward in time from December 1 to March 16. Over 60,000 individual measurements were used in the last calculation. Again, ozone loss is estimated by comparing vortex interior measurements made early in the campaign with those made later in the campaign. The diabatic nature of the second and third methods calculation presumably corrects for the normal increase in ozone within the vortex due to downward advection. The three methods agree that the largest ozone loss occurs between 400 and 460 K potential temperatures (approx. 16-20 km) with slightly over 1.5 ppmv lost over the winter period. Between 460 K and 500 K (approx. 22 km) net ozone loss is less than 0.8 ppmv. From 500K to 600K (26 km) net loss is less than 0.5 ppmv.

During a routine ER-2 aircraft high-altitude test flight on April 18, 1997, an unusual aerosol cloud was detected at 20 km altitude near the California coast at about 370 degrees N latitude. Not visually observed by the ER-2 pilot, the cloud was characterized bv high concentration of soot and sulfate aerosol in a region over 100 km in horizontal extent indicating that the source of the plume was a large hydrocarbon fueled vehicle, most likely a launch vehicle powered only by rocket motors burning liquid oxygen and kerosene. Two Russian Soyuz rockets could conceivably have produced the plume. The first was launched from the Baikonur Cosmodrome, Kazakhstan on April 6th; the second was launched from Plesetsk, Russia on April 9. Air parcel trajectory calculations and long-lived tracer gas concentrations in the cloud indicate that the Baikonur rocket launch is the most probable source of the plume. The parcel trajectory calculations do not unambiguously trace the transport of the Soyuz plume from Asia to North America, illustrating serious flaws in the point-to-point trajectory calculations. This chance encounter represents the only measurement of the stratospheric effects of emissions from a rocket powered exclusively with hydrocarbon fuel.

Dehydration of more than 0.5 ppmv water was observed between 18 and 19 km (0-450-465 K) at the edge of the Arctic polar vortex on February 1, 1996. More than half the reactive nitrogen (NO(y)) had also been removed, with layers of enhanced NO(y) at lower altitudes. Back trajectory calculations show that air parcels sampled inside the vortex had experienced temperatures as low as 188 K within the previous 12 days, consistent with a small amount of dehydration. The depth of the dehydrated layer (approximately 1 km) and the fact that trajectories passed through the region of ice saturation in one day imply selective growth of a small fraction of particles to sizes large enough (>10 microns) to be irreversibly removed on this timescale. Over 25% of the Arctic vortex in a 20-30 K range of 0 is estimated to have been dehydrated in this event.

The poleward transport of tropical air in the lower stratosphere during the winter period of the second Airborne Arctic Stratospheric Expedition (AASE 2) (December 1991-March 1992) is examined using contour advection calcutions. These calculations show that filaments of tropical air extend into mid-latitudes, and are wrapped around the equatorward edge of the polar jet. Simultaneously filaments are drawn from the polar vortex and are intermingled with the filaments of tropical air. The tropical filaments are consistent with measurements of chemical tracers taken aboard the ER-2 and DC-8 aircraft which show localized regions, in mid-latitudes, of air with the characteristics of tropical air.

A technique based on conservative properties of certain meteorological fields is used to compare ozone measurements from the Microwave Limb Sounder (MLS) on the Upper Atmosphere Research Satellite (UARS) with soundings from a lidar system operated at midlatitudes by the University of L'Aquila, Italy. A few typical cases are analyzed in connection with the position of the vortex relative to the observing station, and it is shown that in general lidar observations taken within the vortex compare well with the UARS data, regardless of whether they are coincident with a satellite overpass. It is shown that such analysis may be useful for comparing measurements of the same quantity taken at different sites using different measurement techniques.

The fine-scale structure in lower stratospheric tracer transport during the period of the two Arctic Airborne Stratospheric Expeditions (January and February 1989; December 1991 to March 1992) is investigated using contour advection with surgery calculations. These calculations show that Rossby wave breaking is an ongoing occurrence during these periods and that air is ejected from the polar vortex in the form of long filamentary structures. There is good qualitative agreement between these filaments and measurements of chemical tracers taken aboard the NASA ER-2 aircraft. The ejected air generally remains filamentary and is stretched and mixed with midlatitude air as it is wrapped around the vortex. This process transfers vortex air into midlatitudes and also produces a narrow region of fine-scale filaments surrounding the polar vortex. Among other things, this makes it difficult to define a vortex edge. The calculations also show that strong stirring can occur inside as well as outside the vortex.

Investigations of the kinematics of the lower stratospheric Arctic vortex during the winter of 1991-1992 using the contour advection with surgery technique reveal three distinct events in which there was substantial intrusion of midlatitude air into the vortex, in apparent contradiction of the view that the polar vortex constitutes an isolated air mass. Two of these events, in late January and mid-February, were well documented. They were predicted in high-resolution forecasts by the European Centre for Medium-Range Weather Forecasts, most clearly in experimental forecasts with reduced diffusion. Direct confirmation of the presence of the intrusions and of their calculated locations was provided by aerosol observations from the airborne differential absorption laser lidar aboard the NASA DC-8, taken as part of the second Airborne Arctic Stratospheric Expedition campaign; aerosol-rich air of midlatitude origin was seen in the expected position of the intrusions. The reality of the February event was also confirmed by in situ measurements from the NASA ER-2. Such events may be significant for the chemical processes taking place within the winter vortex. The intrusions were evidently related to the meteorology of the northern stratosphere during this winter and in particular to persistent tropospheric blocking over the northeastern Atlantic Ocean and western Europe and concomitant ridging into the lower stratospheric vortex in this region. Nevertheless, preliminary investigations have indicated that such events are not uncommon in other northern hemisphere winters, although no such events were found in the southern hemisphere during the Antarctic winter of 1987.

Analysis of Upper Altmosphere Research Satellite (UARS) Microwave Limb Sounder (MLS) observations in early January 1992 shows a clear relationship between predicted polar stratospheric cloud formation along the back trajectory and elevated ClO amounts. These findings are in good agreement with aircraft observations. The MLS observed variation of ClO amounts within the vortex also fits the pattern of ClO change as a result of air parcel solar exposure and nitric acid photolysis. Outside the polar vortex, the occasional highly elevated ClO appear statistically consistent with MLS measurement noise.

In January and March 1992, DC-8-measured stratospheric particle optical depth spectra, tau(sub p)(lambda), peaked broadly at midvisible or longer wavelengths. At mid-to-high northern latitudes outside the vortex, tau(sub p)(526 nm) nm) above about 11 km was as large as 0.22 in both January and March, reflecting continued Pinatubo volcanic influence. In both months, in-vortex tau(sub p)(lambda) above 11 km was smaller than outside-vortex values by a factor of two or more, and in January a strong anticorrelation was observed between tau(sub p)(lambda) and HF column content (an indicator of vortex penetration). In late January at 18-20S, near the edge of the southern subtropical jet, tau(sub p)(526 nm) above 12 km was only about 0.07-0.09, with a flatter spectral shape than northern mid- to high-latitude measurements in both January and March. Occasional high-latitude vertical profiles indicate 6-11-km slab optical depths, Delta tau(sub p)(526 nm), of 0.05 to 0.1, which should be added to the above-11-km values to yield values above 6 km.

Back trajectory analysis of Arctic and Antarctic aircraft data reveals that high ClO concentrations are associated with predicted polar stratospheric cloud (PSCs) encounters. The ClO concentrations within the Arctic and Antarctic polar vortices vary widely but appear to be inversely related to parcel solar exposure since the last PSC interaction. These results imply that production of NO(x) from HNO3 photolysis and reaction with OH is the mechanism for the loss of chlorine radicals through the reformation of chlorine nitrate. Highly denitrified air parcels show no change in ClO with solar exposure. The recovery process is quantitatively duplicated using a model of chemistry along trajectories. Although PSC processing is the primary mechanism for producing elevated ClO amounts, back trajectories apparently unperturbed by PSC's also show slightly elevated ClO levels in 1992 compared to Arctic 1989 and Antarctic 1987 measurements presumably due to the presence of Pinatubo aerosol.

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.

During the Airborne Arctic Stratospheric Expedition II (AASE II), September 1991 through March 1992, in situ measurements of reactive nitrogen (NO(y)) and N2O were made in the Northern Hemisphere lower stratosphere. We present an analysis of this new data and compare it with results from similar data taken during AASE in the winter of 1989. In the Northern Hemisphere there is a consistent linear correlation of N2O and NO(y) which shows no interannual variation. Cases of departure from a linear correlation are examined and classified as being due to denitrification (NO(y) loss) or sampling air from a region where the photochemical lifetime of NO(y) is decreased. The latter case was observed for the first time in the winter of 1992.

Simultaneous measurements of the stratospheric burdens of CO2, HCN, N2O, CH4, OCS, CF2Cl2, CFCl3, CHF2Cl and HF were made by the Jet propulsion Laboratory MkIV interferometer on board the NASA DC-8 aircraft during January and early February 1989 as part of the Airborne Arctic Stratosphere Experiment. Data were acquired on 11 flights at altitudes of up to 12 km over a geographic region covering the NE Atlantic Ocean, Iceland and Greenland. The results obtained show large variations in the burdens of these tracers due to the effects of transport. The tropospheric source gas burdens were reduced inside the polar vortex, suggesting that the air had subsided with respect to the surrounding midlatitude air. Increased HF burdens inside the vortex support this interpretation. The results obtained from the different tracers are highly consistent with each other and indicate that in the 15- to 20-km altitude range inside the vortex, surfaces of constant volume mixing ratio were located some 5-6 km lower in absolute altitude than outside the vortex. The results also indicate that the magnitude of this subsidence increases with altitude. These conclusions are consistent with other measurements.

This lecture describes a technique by which atmospheric measurements of trace species with medium to long lifetimes can be 'coincidentally' compared and validated even though measurements are taken at different locations and different times In other words, the method, under suitable counditions, can remove a large amount of the natural meteorological variability. The technique involves the use of quasi-Lagrangian or conservative coordinates - air parcel tags which are invariant or nearly invariant under the motion of the parcel. The technique is called 'reconstruction', since measurements taken at one location can be reconstructed at different locations. In order to do this, the data are transformed into the conservative coordinates and accumulated. Within the conservative reference frame, much of the meteorological variability is removed. Once enough data are obtained within the system, the observations can be tranformed back into physical space at any location and compared with other measurements. The method by which the trace species data are obtained makes no difference; satellite, balloon, rocket, aircraft and ground-based data all become equivalent and can be intercompared. The conservative-coordinate system not only allows for intercomparison of data, but shows how data can be taken in such a way as to maximize the physical scope of the information. In other words, the method automatically suggests when conditions might be suitable to obtain information with different environmental situations. It also allows for the forecast of constituent fields using only the meteorological forecasts and limited observational data.