European Stratospheric Experiment Research Articles

Mountain Wave–Induced Polar Stratospheric Cloud Forecasts for Aircraft Science Flights during SOLVE/THESEO 2000

Abstract The results of a multimodel forecasting effort to predict mountain wave–induced polar stratospheric clouds (PSCs) for airborne science during the third Stratospheric Aerosol and Gas Experiment (SAGE III) Ozone Loss and Validation Experiment (SOLVE)/Third European Stratospheric Experiment on Ozone (THESEO 2000) Arctic ozone campaign are assessed. The focus is on forecasts for five flights of NASA's instrumented DC-8 research aircraft in which PSCs observed by onboard aerosol lidars were identified as wave related. Aircraft PSC measurements over northern Scandinavia on 25–27 January 2000 were accurately forecast by the mountain wave models several days in advance, permitting coordinated quasi-Lagrangian flights that measured their composition and structure in unprecedented detail. On 23 January 2000 mountain wave ice PSCs were forecast over eastern Greenland. Thick layers of wave-induced ice PSC were measured by DC-8 aerosol lidars in regions along the flight track where the forecasts predicted enhanced stratospheric mountain wave amplitudes. The data from these flights, which were planned using this forecast guidance, have substantially improved the overall understanding of PSC microphysics within mountain waves. Observations of PSCs south of the DC-8 flight track on 30 November 1999 are consistent with forecasts of mountain wave–induced ice clouds over southern Scandinavia, and are validated locally using radiosonde data. On the remaining two flights wavelike PSCs were reported in regions where no mountain wave PSCs were forecast. For 10 December 1999, it is shown that locally generated mountain waves could not have propagated into the stratosphere where the PSCs were observed, confirming conclusions of other recent studies. For the PSC observed on 14 January 2000 over northern Greenland, recent work indicates that nonorographic gravity waves radiated from the jet stream produced this PSC, confirming the original forecast of no mountain wave influence. This forecast is validated further by comparing with a nearby ER-2 flight segment to the south of the DC-8, which intercepted and measured local stratospheric mountain waves with properties similar to those predicted. In total, the original forecast guidance proves to be consistent with PSC data acquired from all five of these DC-8 flights. The work discussed herein highlights areas where improvements can be made in future wave PSC forecasting campaigns, such as use of anelastic rather than Boussinesq linearized gridpoint models and a need to forecast stratospheric gravity waves from sources other than mountains.

The APE-THESEO Tropical Campaign: An Overview

The APE-THESEO campaign was held from 15 February to 15 March 1999 from the Seychelles in the western Indian Ocean. APE-THESEO stands for Airborne Platform for Earth observation — (contribution to) the Third European Stratospheric Experiment on Ozone. The campaign aimed to study processes controlling the low water content of the stratosphere, including the mechanisms of cloud formation in the tropical tropopause region, and transport processes, studied using measurements of long-lived trace gases and ozone. Two aircraft were used: the high-altitude research aircraft, M-55 Geophysica, which can fly up to 21 km, and the Falcon of the Deutsches Zentrum fur Luft- und Raumfahrt, a tropospheric aircraft. Seven flights were performed, including the first simultaneous in situ and remote sensing of sub-visible cirrus clouds, the first interception of sub-visible cirrus using in-flight guidance from a path-finding aircraft, and guided descent of a high-altitude research aircraft into the anvil cloud at the top of a tropical cyclone. In this paper we describe the payload used, the objectives for each flight, and the meteorological conditions encountered. First results show that a new type of cloud, which we have dubbed ultra-thin tropical tropopause cloud (UTTC), has been observed frequently, and observed to cover areas of 105 km2. The frequent coincidence of the tropopause and hygropause implies that the western Indian Ocean played an important role in the dehydration of the lower tropical stratosphere during the season of the mission. UTTCs, sub-visible cirrus, and visible cirrus, have all been implicated in the observed dehydration. Tracer measurements indicate little mixing of stratospheric air into the upper tropical troposphere.

Measurements of large stratospheric particles in the Arctic polar vortex

During the SAGE III Ozone Loss and Validation Experiment/Third European Stratospheric Experiment on Ozone 2000 mission, the Multiangle Aerosol Spectrometer Probe (MASP) was flown aboard the ER‐2 aircraft sampling the Arctic polar vortex. On several of the flights the ER‐2 flew directly through polar stratospheric clouds (PSCs), and on six of these flights the MASP sampled large particles (2–22 μm diameter). MASP large particle observations are correlated in time with the large particle signal from the NOAA NOy measurements. This is direct evidence supporting the inference of particle size made by the NOy instrument. On 20 January 2000, the day of the most intense PSC encounter, the shapes of the large particle size distributions above 9 μm observed by the MASP and simulated based on the NOy instruments are in reasonable agreement. The MASP observations show a dramatic increase in large particle volume as the temperature approaches the nitric acid trihydrate equilibrium temperature. Our study suggests that large particles containing nitric acid are present in the Arctic polar stratosphere and may lead to denitrification.

Estimation of Arctic polar vortex ozone loss during the winter of 1999–2000 using vortex‐averaged airborne differential absorption lidar ozone measurements referenced to N2O isopleths

The NASA Langley UV differential absorption lidar (DIAL) system flew on the NASA DC‐8 aircraft during the Stratospheric Aerosol and Gas Experiment (SAGE) III Ozone Loss and Validation Experiment/Third European Stratospheric Experiment on Ozone 2000 (SOLVE/THESEO 2000) mission from 30 November 1999 to 15 March 2000. The UV DIAL system measured ozone (O3) profiles at altitudes from about 1 km above the aircraft up to about 26 km with a vertical resolution of 750 m and a horizontal resolution of 70 km below 19 km and 140 km above 19 km. In comparison with electrochemical concentration cell ozonesonde profiles, the UV DIAL O3 measurements agreed to within 5% up to 20 km and 10% from 20 to 25 km. Ozone loss during the season was determined using the UV DIAL O3 data along with air mass subsidence determined using N2O as a conservative tracer at five levels from 50 to 250 ppbv [Greenblatt et al., 2002]. O3 mixing ratios were determined inside the polar vortex, away from the collar region along these five levels during the mission. The maximum O3 loss determined from 30 November to 12 March was 1.55 ± 0.3 ppmv at the 440–450 K potential temperature (Θ) level, while the loss there between 20 January and 15 March was 1.3 ± 0.3 ppmv. These results are comparable to many of the other reported losses for these periods, but lower than several. Some of the determinations of higher losses used a different method to determine descent during the season. These results indicate that a series of vertical profiles of O3 that sample much of the vortex during the winter, along with determinations of the descent of air masses inside the vortex, can give a reasonable estimate of the O3 changes during the season.

In situ observations of ClO near the winter polar tropopause

Significant abundances of chlorine oxide (ClO) were observed throughout the lowermost stratosphere at high latitudes during winter from the NASA DC‐8 aircraft during the SAGE III—Ozone Loss and Validation Experiment and Third European Stratospheric Experiment on Ozone 2000 (SOLVE/THESEO 2000) campaign. Mixing ratios of ClO averaging 15–20 parts per trillion by volume (pptv) were observed near the tropopause, a region where ClO abundances are usually only a pptv or less at lower latitudes. The ratio of ClO to inferred inorganic chlorine ([ClO]/[Cly]) was found to be largest (∼7%) in air characterized by low abundances of ozone (∼100–250 parts per billion by volume (ppbv)). This was the region where cirrus clouds were also observed occasionally during the measurement period, although abundances of ClO directly within cirrus clouds were not significantly different than background abundances. Nonzero instrument signals during darkness are attributed to detection of ∼5–15 pptv of OClO. BrO mixing ratios between 2 and 4 pptv are sufficient to produce these amounts of OClO, assuming daytime mixing ratios of ClO between 15 and 20 pptv. At these levels of ClO and BrO, approximately 10% of the ozone at these altitudes is chemically destroyed per month in springtime by reactions of ClO and BrO, representing an effective loss process for ozone near the high‐latitude tropopause.

Lidar observations of equatorial cirrus clouds at Mahé Seychelles

In February–March 1999, nocturnal observations with a ground‐based backscatter/depolarization lidar were conducted during the Airborne Platform for Earth Observation–Third European Stratospheric Experiment on Ozone (APE‐THESEO) campaign at Mahé, Seychelles (4.4°S, 55.3°E). Upper tropospheric cirrus clouds were a common feature in the lidar echoes; they were detected for about 67 hours out of a total measurement time of 125 hours. Optical and geometrical characteristics of the clouds detected at altitudes above 9 km throughout the campaign are derived and discussed. Cirri above 14.5 km present a layered structure and appear more persistent and thinner than cirri at lower altitudes. The behavior of average optical and geometrical depths, integrated depolarization, backscatter‐to‐extinction ratio, integrated backscatter, and extinction coefficient is studied as a function of midcloud temperature and is compared with results from previous measurements and models. The estimated cloud backscatter‐to‐extinction ratio ranges from 0.01 to 0.2 sr−1, with an average value of 0.051 ± 0.030 sr−1. In the temperature range between 200 and 240 K the integrated depolarization ranges between 0.27 and 0.19 and appears lower than that for midlatitude cirri. In a single night, very high values of the integrated depolarization for a layered cirrus at 16 km could be related to outflow from an active convective cell. The two highest and coldest (temperature around 188 K) layers show values of optical and geometrical depth and integrated depolarization lower than for cirri at temperatures between 190 and 200 K. The optical characteristics of the clouds decrease for temperatures from 190 to 200 K, possibly indicating different evolution phases of the clouds.

Polar stratospheric cloud microphysical properties measured by the microRADIBAL instrument on 25 January 2000 above Esrange and modeling interpretation

The balloonborne microRADIBAL instrument is a radiometer that measures the radiance and polarization of the sunlight scattered by the atmosphere, gas, and aerosols in a horizontal plane in the near‐infrared range. It was launched from Esrange, Sweden, on 25 January 2000 in the framework of the Third European Stratospheric Experiment on Ozone (THESEO) 2000 campaign, and performed measurements in the vicinity of a large polar stratospheric cloud (PSC). The measurements provide diagrams of the radiance versus scattering angle at several altitudes. The aerosol signature, derived from the radiance measurements, has been modeled via Mie theory and the T‐Matrix code. Three different size distributions of aerosols have been tested: monomodal and bimodal size distributions of spherical particles, and bimodal size distributions including a mode of spherical and a mode of nonspherical particles. The best agreement between the measured and modeled signatures is obtained considering a bimodal size distribution composed by a mode of medium spherical particles (median radius about 0.15 μm) and a second mode of larger nonspherical particles (median radius about 1.1 μm, aspect ratio about 0.6). Concentrations and surface densities of the PSC particles have been estimated. The existence of such particles has been tentatively explained using the Lagrangian Microphysical and Photochemical Lagrangian Stratospheric Model of Ozone (MiPLaSMO) model. On 25 January 2000 the polar stratospheric cloud detected by microRADIBAL is associated with a lee‐wave event. Temperature perturbations due to lee‐wave events were calculated using the National Research Laboratory Mountain Wave Forecast Model (MWFM) and have been included along trajectories. They are localized in a large region between the Norwegian mountains and Esrange. Their amplitude varies from 3 to 7 K. Detailed comparisons between measured and modeled surfaces and dimensional distributions of PSCs' particles are achieved. The two modes of particles detected by microRADIBAL can be interpreted from MiPLaSMO results considering different air masses located along the lines of sight. The air masses are characterized by two different temperature perturbations due to lee‐wave events. With a small temperature perturbation (∼3 K) that occurred just before the time of the measurement, supercooled ternary solution particles are predicted, and with a strong temperature perturbation (∼6 K) that occurred four hours before the measurement, nitric acid trihydate particles are formed.

N2O and NOy observations in the 1999/2000 Arctic polar vortex: Implications for transport processes in a CTM

We compare the evolution of simulated NOy and N2O with observations made during the 1999/2000 NASA Stratospheric Aerosol and Gas Experiment (SAGE) III Ozone Loss and Validation Experiment/Third European Stratospheric Experiment on Ozone‐2000 to understand the different effects of transport on these two species and evaluate model transport processes in the Arctic lower stratosphere during mid to late winter. The simulations were made with the Goddard Space Flight Center chemistry and transport model, driven by meteorological analyses from the Goddard Data Assimilation Office. In January, model NOy and N2O distributions agree well with observations, provided a substantial loss of NOy due to polar stratospheric cloud sedimentation is included in the model simulation. In late winter, model NOy is ∼2–3 times larger than observed, despite the continued reasonable agreement of N2O. Anomalously large vertical transport of NOy due to overly vigorous descent in the CTM is primarily responsible for the large late winter NOy mixing ratios. However, the rapid descent is not apparent in the evolution of modeled N2O and presumably other similar species due to compensating horizontal transport of N2O across the vortex edge, which results in the reasonable agreement between modeled and measured N2O at ER‐2 altitudes throughout the winter. The need to properly represent the seasonal evolution of NOy when studying lower stratospheric polar wintertime photochemistry places strong constraints on the meteorological data used to drive global chemistry and transport models.

Clouds at the tropical tropopause: A case study during the APE‐THESEO campaign over the western Indian Ocean

In this paper, we report a detailed description of a thin cirrus at the tropopause above a cumulonimbus (Cb) convective cluster observed during the Airborne Platform for Earth Observation–Third European Stratospheric Experiment for Ozone (APE‐THESEO) campaign in February–March 1999 in the western Indian Ocean. The thin cirrus (Ci) has an optical depth at 532 nm below 0.1, with extended subvisible stretches, and is located directly below the tropopause, which was supersaturated with respect to ice. A direct comparison between the optical depth retrieved by Meteosat and that obtained by means of the hygrometers installed on the M55‐Geophysica aircraft is discussed showing discrepancies ranging from 10 to 20%. Combining satellite and aircraft data, we show that the observed Ci is not due to cirrus outflow from Cb anvils. In the absence of any deeply convective clouds reaching altitudes above 15 km, we propose a possible mechanism of Ci formation based on a net mesoscale transport of water vapor from altitudes above 16 km to the tropopause region around 18 km. This transport could be driven by the critical layer and turbulence induced by gravity waves that could have been generated by lower level Cb cluster activity. The proposed mechanism for high‐altitude Ci formation corroborates the new paradigm of a tropical tropopause layer (TTL) or “substratosphere,” several kilometers thick, which is decoupled from the convection‐dominated lower troposphere.

In situ measurements of background aerosol and subvisible cirrus in the tropical tropopause region

In situ aerosol measurements were performed in the Indian Ocean Intertropical Convergence Zone (ITCZ) region during the Airborne Polar Experiment‐Third European Stratospheric Experiment on Ozone (APE‐THESEO) field campaign based in Mahé, Seychelles between 24 February and 6 March 1999. These are measurements of particle size distributions with a laser optical particle counter of the Forward Scattering Spectrometer Probe (FSSP)‐300 type operated on the Russian M‐55 high‐altitude research aircraft Geophysica in the tropical upper troposphere and lower stratosphere up to altitudes of 21 km. On 24 and 27 February 1999, ultrathin layers of cirrus clouds were penetrated by Geophysica directly beneath the tropical tropopause at 17 km pressure altitude and temperatures below 190 K. These layers also were concurrently observed by the Ozone Lidar Experiment (OLEX) lidar operating on the lower‐flying German DLR Falcon research aircraft. The encountered ultrathin subvisual cloud layers can be characterized as (1) horizontally extending over several hundred kilometers, (2) persisting for at least 3 hours (but most likely much longer), and (3) having geometrical thicknesses of 100–400 m. These cloud layers belong to the geometrically and optically thinnest ever observed. In situ particle size distributions covering diameters between 0.4 and 23 μm obtained from these layers are juxtaposed with those obtained inside cloud veils around cumulonimbus (Cb) anvils and also with background aerosol measurements in the vicinity of the clouds. A significant number of particles with size diameters around 10 μm were detected inside these ultrathin subvisible cloud layers. The cloud particle size distribution closely resembles a background aerosol onto which a modal peak between 2 and 17 μm is superimposed. Measurements of particles with sizes above 23 μm could not be obtained since no suitable instrument was available on Geophysica. During the flight of 6 March 1999, upper tropospheric and lower stratospheric background aerosol was measured in the latitude band between 4°S and 19°S latitude. The resulting particle number densities along the 56th meridian exhibit very little latitudinal variation. The concentrations for particles with sizes above 0.5 μm encountered under these background conditions varied between 0.1 and 0.3 particles/cm3 of air in altitudes between 17 and 21 km.

An overview of the SOLVE/THESEO 2000 campaign

Between November 1999 and April 2000, two major field experiments, the Stratospheric Aerosol and Gas Experiment (SAGE) III Ozone Loss and Validation Experiment (SOLVE) and the Third European Stratospheric Experiment on Ozone (THESEO 2000), collaborated to form the largest field campaign yet mounted to study Arctic ozone loss. This international campaign involved more than 500 scientists from over 20 countries. These scientists made measurements across the high and middle latitudes of the Northern Hemisphere. The main scientific aims of SOLVE/THESEO 2000 were to study (1) the processes leading to ozone loss in the Arctic vortex and (2) the effect on ozone amounts over northern midlatitudes. The campaign included satellites, research balloons, six aircraft, ground stations, and scores of ozonesondes. Campaign activities were principally conducted in three intensive measurement phases centered on early December 1999, late January 2000, and early March 2000. Observations made during the campaign showed that temperatures were below normal in the polar lower stratosphere over the course of the 1999–2000 winter. Because of these low temperatures, extensive polar stratospheric clouds (PSC) formed across the Arctic. Large particles containing nitric acid trihydrate were observed for the first time, showing that denitrification can occur without the formation of ice particles. Heterogeneous chemical reactions on the surfaces of the PSC particles produced high levels of reactive chlorine within the polar vortex by early January. This reactive chlorine catalytically destroyed about 60% of the ozone in a layer near 20 km between late January and mid‐March 2000, with good agreement being found between a number of empirical and modeling studies. The measurements made during SOLVE/THESEO 2000 have improved our understanding of key photochemical parameters and the evolution of ozone‐destroying forms of chlorine.

Photochemical ozone loss in the Arctic as determined by MSX/UVISI stellar occultation observations during the 1999/2000 winter

The combined SAGE III Ozone Loss and Validation Experiment and Third European Stratospheric Experiment on Ozone 2000 (SOLVE/THESEO 2000) campaign during winter 1999/2000 sought, in part, to quantify ozone loss within the Arctic polar vortex using a variety of aircraft‐, balloon‐, ground‐, and space‐based instrument platforms. The Midcourse Space Experiment/Ultraviolet and Visible Imagers and Spectrographic Imagers (MSX/UVISI) suite of instruments performed 31 stellar occultation observations from 23 January through 4 March 2000 in and near the Arctic polar vortex. Using a newly developed combined extinctive‐refractive algorithm, ozone mixing ratio profiles, along with profiles of total density, pressure, and temperature, were retrieved. Retrieved temperature and ozone profiles are shown to agree well with other measurements. Diabatic trajectory calculations are used to remove the effects of subsidence within the vortex, allowing photochemical ozone loss to be inferred from these occultation measurements. A maximum ozone loss of about 1 ppmv is found at 400–500 K (∼16–21 km) during the 41‐day period for which occultation data are available, in agreement with several other ozone loss analyses of the campaign. This corresponds to an average daily loss rate of ∼0.024 ppmv/day. The combined extinctive‐refractive stellar occultation technique is demonstrated to accurately measure stratospheric ozone loss during polar winter.

In situ observations of gravity waves and comparisons with numerical simulations during the SOLVE/THESEO 2000 campaign

This article presents observational and numerical results on gravity waves in the Arctic polar vortex during the SAGE III—Ozone Loss and Validation Experiment and Third European Stratospheric Experiment on Ozone 2000 (SOLVE/THESEO) campaign. Long‐duration balloons that were launched from Kiruna, Sweden, on 18 February 2000 provided in situ meteorological measurements for several weeks in the lower stratosphere. A strong gravity wave event was observed above southern Scandinavia on 2 March 2000. The main characteristics (amplitude of disturbances, frequency, and wavelengths) are reported, and it is shown that the wave induced mesoscale temperature fluctuations were large (18 K peak to peak). Furthermore, it is found that the gravity wave was most likely generated by flow across the Norwegian mountains. The observations are compared with results of numerical simulations. In particular, the mesoscale and ray‐tracing simulations reproduced some features of the observed wave packet. However, the fluctuations induced by the wave were significantly underestimated in the general circulation model of the European Center for Medium‐Range Weather Forecasting. Finally, the overall gravity wave activity during the flight is analyzed and is found to be relatively small.

Discriminating Types Ia and Ib polar stratospheric clouds in POAM satellite data

A method for discriminating Types Ia and Ib Polar Stratospheric Clouds (PSCs) from Polar Ozone and Aerosol Measurement (POAM) satellite occultation measurements of aerosol extinction coefficient is described. The method has been validated by applying several statistical tests to the results and by using Differential Absorption Lidar (DIAL) and Ozone Lidar Experiment (OLEX) lidar observations made during Stratospheric Aerosol and Gas Experiment (SAGE) III Ozone Loss and Validation Experiment/Third European Stratospheric Experiment on Ozone II (SOLVE/THESEO 2000). Type Ia PSCs are believed to be composed of large nitric‐acid‐containing particles that will sediment out of the stratosphere, causing denitrification and facilitating ozone depletion. Type Ib PSCs are believed to be much smaller and will not sediment out of the stratosphere. Discriminating between these two types of PSCs is significant because it will permit a better understanding of ozone depletion today and predict the fate and effect of PSCs using the more continuous temporal coverage and larger areal coverage that can be obtained from satellites. The method is made possible by the character of POAM observations when plotted as normalized extinction versus wavelength dependence. As the extinction increases, observations of Types Ia and Ib PSCs bifurcate. This behavior is also observed in idealized simulations of the formation of Supercooled Ternary Solutions (STS) and nitric acid trihydrate (NAT) particles, which are believed to make up Types Ib and Ia PSCs, respectively. Analysis of POAM observations from the 1999/2000 Arctic winter using the PSC discrimination algorithm revealed that the number of PSC observations peaked in January. In November, December, and January, the ratio of Type Ia to Ib PSCs was about 3. In February and March, this ratio was about 0.3. The average altitude of Type Ia PSCs descended more than the Type Ib, especially in the spring where the Type Ia observations were 2–3 km below the Type Ib observations. This is consistent with observations of denitrification during the 1999/2000 winter. The PSC discrimination algorithm is applicable to previous winters in both hemispheres and will work with SAGE III observations as well. This will permit a more extensive study of the statistical significance of some features of the PSCs observed during the 1999/2000 Arctic winter. It is our belief that the present method of analyzing satellite data to discriminate Type I PSCs will be of great utility in the study of PSCs and ozone depletion.

Ozone depletion observed by the Airborne Submillimeter Radiometer (ASUR) during the Arctic winter 1999/2000

In the winter 1999/2000 the Airborne Submillimeter Radiometer (ASUR) participated in the Stratospheric Aerosol and Gas Experiment III Ozone Loss and Validation Experiment/Third European Stratospheric Experiment on Ozone project on board the NASA research aircraft DC‐8. During three deployments in early December 1999, late January, and early March 2000, the ASUR instrument took various measurements of ozone and key species related to stratospheric ozone chemistry. After the sunlight reached the vortex region in January 2000 peak values of about 1.8 ppb ClO were measured by ASUR. There was nearly no ozone destruction observed during the period between mid December 1999 and late January 2000. As expected from ASUR observation of high chlorine activation and continuously low temperatures until mid March, significant ozone depletion was observed between late January and mid March 2000. In order to determine ozone loss it is important to separate dynamical and chemical effects. Since N2O is a good tracer due to its chemical stability in the lower stratosphere for determining ozone changes due to descent of air, ozone loss can be estimated from simultaneous measurements of ozone and N2O by ASUR. Between mid December 1999 and mid March 2000 a chemical ozone loss of about 30% (eq 1.1 ppm) in the altitude range between 19.0 and 22.2 km and of about 40% (eq 1.15 ppm) between 16.0 and 18.1 km was observed. The air masses subsided 2.1–3.2 km in the lower stratosphere due to diabatic descent in the period from mid December 1999 to mid March 2000 as derived from ASUR N2O measurements. Vortex‐averaged ASUR measurements of ozone are systematical greater than results from the Global Ozone Monitoring Experiment (GOME) which has a similar vertical resolution than ASUR. This, however, has little impact on the determination of delta ozone and chemical loss estimates.

Ozone loss from quasi‐conservative coordinate mapping during the 1999–2000 SOLVE/THESEO 2000 campaigns

Ozone observations made by the Airborne Raman Ozone, Temperature, and Aerosol Lidar (AROTEL) and Differential Absorption Lidar (DIAL) on board the NASA DC‐8 aircraft, the NOAA in situ instrument on board the NASA ER‐2 aircraft, and Third European Stratospheric Experiment on Ozone 2000 (THESEO 2000) ozonesondes are analyzed by applying a quasi‐conservative coordinate mapping technique. Measurements from the late winter/early spring SAGE III Ozone Loss and Validation Experiment (SOLVE) period (January through March 2000) are incorporated into a time‐varying composite field in a potential vorticity‐potential temperature coordinate space; ozone loss rates are calculated both with and without diabatic effects. The average loss rate from mid‐January to mid‐March near the 450 K isentropic surface in the polar vortex is found to be approximately 0.03 ppmv/d.

Diagnosis of mixing between middle latitudes and the polar vortex from tracer‐tracer correlations

A method is introduced for diagnosing mixing between the polar vortex and midlatitudes from tracer data. Tracers with different photochemical activities and lifetimes usually exhibit curved tracer‐tracer correlation functions on an isentropic surface. The effect of mixing events is to populate the inner side of such a curve. Using simultaneous measurements of trace gases or model results, we exploit this process to calculate the distribution of recent origins in tracer space prior to such a mixing event. The method relies on both hemispheric and local data and is applicable to situations where mixing is nonlocal in tracer space. It is applied to measurements taken during the Stratospheric Aerosol and Gas Experiment (SAGE) III Ozone Loss and Validation Experiment/Third European Stratospheric Experiment on Ozone 2000 (SOLVE/THESEO 2000) winter campaign and to a chemical transport model simulation covering the same winter. In one of the cases studied, a vortex breakup and subsequent remerger of the vortex fragments in March 2000 results in significant diagnosed mixing. In a further example, an elongated filament shed off the polar vortex is characterized by anomalous composition. For the two high‐altitude aircraft flights of the SOLVE campaign that probe the vortex boundary, a correspondence is found for mixing diagnosed in the measurements and in the model. Mixing timescales considered here are given by the life span of planetary waves, up to a few weeks.

POAM III observations of arctic ozone loss for the 1999/2000 winter

During the Stratospheric Aerosol and Gas Experiment (SAGE) III Ozone Loss and Validation Experiment (SOLVE)/Third European Stratospheric Experiment on Ozone (THESEO) campaign, Polar Ozone and Aerosol Measurement (POAM) III sampled in the vortex core, on the vortex edge, and outside the vortex on a near‐daily basis from December 1999 through mid‐March 2000. During this period, POAM observed a substantial amount of ozone decline. For example, ozone mixing ratios in the core of the vortex dropped from about 3.5 ppmv in mid‐January to about 2 ppmv by mid‐March at 500 K. The ozone chemical loss indicated by these measurements is assessed using two methodologies. First, the POAM data is used to construct vortex‐averaged ozone profiles, which are advected downward using vortex average descent rates. The maximum ozone loss (1 January to 15 March) is found to be about 1.8 ppmv. In a second approach, the REPROBUS 3‐D CTM is used to specify the passive ozone distribution throughout the winter. The chemical loss in the vortex is estimated by performing a point‐by‐point subtraction of the POAM measurements inside the vortex from the model passive ozone evaluated at the time and location of the POAM measurements. Both ozone loss estimates are in general agreement and they agree well with published loss estimates from ER2 and ozonesonde measurements.

Intercomparison of BrO measurements from ERS-2 GOME, ground-based and balloon platforms

The consistency of BrO column amounts derived from GOME spectra and from correlative ground-based and balloon measurements performed in 1998-1999 during the Third European Stratospheric Experiment on Ozone (THESEO) has been investigated. The study relies on UV-visible observations at several mid- and high latitude ground-based stations in both hemispheres, complemented by balloon-borne solar occultation profile measurements and 3D chemical transport model simulations. Previous investigations have reported GOME BrO columns systematically larger than those deduced from balloon, suggesting BrO being present, possibly ubiquitously, in the free troposphere. The robustness of this hypothesis has been further tested based on the presently available correlative data set. It is shown that when accounting for the BrO diurnal variation and the solar zenith angle dependency of the sensitivity of correlative data to the troposphere, measurements from all platforms are consistent with the presence of a tropospheric BrO background of 1–3 ×10 13 molec/cm 2 extending over mid- and high latitudes.

Modeling the effect of denitrification on Arctic ozone depletion during winter 1999/2000

We have used the SLIMCAT three‐dimensional chemical transport model together with observations from the Stratospheric Aerosol and Gas Experiment (SAGE III) Ozone Loss and Validation Experiment (SOLVE) and the Third European Stratospheric Experiment on Ozone (THESEO 2000) to quantify the effect of denitrification on Arctic ozone loss. We have used two different denitrification schemes in the model: one based on the sedimentation of ice particles containing cocondensed nitric acid trihydrate (NAT) and the other based on large NAT particles. The model was forced using both UK Meteorological Office (UKMO) and European Centre for Medium‐Range Weather Forecasts (ECMWF) analyses. In the Arctic lower stratosphere the UKMO analyzed temperatures are similar to the ECMWF, except at temperatures near the ice point where the UKMO analyses are colder by over 2 K. Consequently, the UKMO analyses predicted large regions of ice clouds, in contrast to the ECMWF. The denitrification scheme based on large NAT particles gives the best agreement with ER‐2 NOy observations for both sets of meteorological analyses. Although the ice scheme and UKMO analyses also produce denitrification, the vertical extent of denitrification and renitrification does not agree as well with the observed NOy. Uncertainties in the budget of ClOy observations from the ER‐2 prevent an indirect validation of the best model denitrification scheme based on these data. The denitrified model runs give the best agreement with the observed HCl and ClONO2 reservoirs in mid March. However, UKMO‐forced runs generally overestimate the observed ClOx during the same period. The denitrified model runs indicate that by late March 56–74% O3 loss had occurred at 460 K and that denitrification contributed 21–30% of this loss. The model runs showing the largest O3 depletion (forced by UKMO analyses) agree well with ER‐2 and ozone sonde data, although these runs overestimated ClOx.