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While observed mesospheric polar nitric acid enhancements have been attributed to energetic particle precipitation through ion cluster chemistry in the past, this phenomenon is not reproduced in current whole-atmosphere chemistry-climate models. We investigate such nitric acid enhancements resulting from energetic electron precipitation events using a recently developed variant of the Whole Atmosphere Community Climate Model (WACCM) that includes a sophisticated ion chemistry tailored for the D-layer of the ionosphere (50–90 km), namely, WACCM-D. Using the specified dynamics mode, that is, nudging dynamics in the troposphere and stratosphere to meteorological reanalyses, we perform a 1-year-long simulation (July 2009–June 2010) and contrast WACCM-D with the standard WACCM. Both WACCM and WACCM-D simulations are performed with and without forcing from medium-to-high energy electron precipitation, allowing a better representation of the energetic electrons penetrating into the mesosphere. We demonstrate the effects of the strong particle precipitation events which occurred during April and May 2010 on nitric acid and on key ion cluster species, as well as other relevant species of the nitrogen family. The 1-year-long simulation allows the event-related changes in neutral and ionic species to be placed in the context of their annual cycle. We especially highlight the role played by medium-to-high energy electrons in triggering ion cluster chemistry and ion-ion recombinations in the mesosphere and lower thermosphere during the precipitation event, leading to enhanced production of nitric acid and raising its abundance by 2 orders of magnitude from 10−4 to a few 10−2 ppb.

Southern summer low-ozone events (LOEs) are examined using Met Office ozone analyses for 2005–2007. At 31 hPa, tongues of low-ozone air are pulled out of the polar region and extend to lower latitudes. Low tongues are also seen at 100 hPa, but there the low ozone is transported from low to high latitudes. These low tongues are frequently superimposed on one another, meaning that there are often also reductions in total ozone. What is striking is that at high latitudes, summer total ozone is typically lower over the Weddell Sea than at other longitudes. The low-ozone tongues at 31 and 100 hPa are consistent with transport associated with planetary waves. Daily geopotential height fields show a poleward and westward wave tilt with height, indicating the presence of baroclinic waves. The tilt enables the superimposition of the low-ozone tongues at 100 and 31 hPa. Filtered geopotential height anomalies reveal the presence of waves reported in other studies and indicate the connection between tropospheric and stratospheric wave dynamics in driving the LOEs. There is also a high connection between the LOEs and ultraviolet (UV) Index. The Weddell Sea region gets up to 20–30% more UV than the zonal mean, and the tip of South America gets about 10–25% more. There have been numerous studies of the impacts of increased UV on the Antarctic marine ecosystem during the springtime ozone hole, and our results indicate there is a case for these studies being extended to the summer LOEs.

We use observations of N2O and mean age to identify realistic transport in models in order to explain their ozone predictions. The results are applied to 15 chemistry climate models (CCMs) participating in the 2010 World Meteorological Organization ozone assessment. Comparison of the observed and simulated N2O, mean age and their compact correlation identifies models with fast or slow circulations and reveals details of model ascent and tropical isolation. This process-oriented diagnostic is more useful than mean age alone because it identifies models with compensating transport deficiencies that produce fortuitous agreement with mean age. The diagnosed model transport behavior is related to a model's ability to produce realistic lower stratosphere (LS) O3 profiles. Models with the greatest tropical transport problems compare poorly with O3 observations. Models with the most realistic LS transport agree more closely with LS observations and each other. We incorporate the results of the chemistry evaluations in the Stratospheric Processes and their Role in Climate (SPARC) CCMVal Report to explain the range of CCM predictions for the return-to-1980 dates for global (60°S–60°N) and Antarctic column ozone. Antarctic O3 return dates are generally correlated with vortex Cly levels, and vortex Cly is generally correlated with the model's circulation, although model Cl chemistry and conservation problems also have a significant effect on return date. In both regions, models with good LS transport and chemistry produce a smaller range of predictions for the return-to-1980 ozone values. This study suggests that the current range of predicted return dates is unnecessarily broad due to identifiable model deficiencies.

We have developed a 5.5 year climatology of atmospheric transport into the Antarctic troposphere, which uses the same data set and methods as described in a recent study for the Arctic. This allows direct comparisons of transport properties for the two polar regions. The climatology is based on a simulation with the Lagrangian particle dispersion model FLEXPART, where the model atmosphere was globally filled with particles. Transport characteristics as well as emission sensitivities were derived from 6 hourly particle positions. We found that the probability for near-surface air to originate from the stratosphere on a time scale of 10 days is an order of magnitude higher near the South Pole than near the North Pole, a result of higher topography and descent that partly compensates for the flow of air down the Antarctic Plateau with the katabatic winds. The stratospheric influence is largest in fall, which is opposite to the seasonality in the Arctic. Stratospheric influence is much smaller over the shelf ice regions and in a band around Antarctica. The average time for which air near the surface has been exposed to continuous darkness in July (continuous light in January) is longest over the Ronne Ice Shelf and Ross Ice Shelf at ∼11 days (20 days). We calculated how sensitive Antarctic air masses are to emission input up to 30 days before arriving in Antarctica if removal processes are ignored. The emission sensitivity shows strong meridional gradients and, as a result, is generally low over South America, Africa, and Australia. For a 10 day time scale, the largest emission sensitivities over these continents are 1–2 orders of magnitude smaller than over Eurasia for transport to the Arctic, showing that foreign continents have a much smaller potential to pollute the Antarctic than the Arctic troposphere. Emission sensitivities and derived black carbon (BC) source contributions over South America, Africa, and Australia are substantially (a factor 10 for Africa) larger in winter than in summer. In winter, biomass burning contributes more BC than anthropogenic sources. For typical aerosol lifetimes of 5–10 days, ship emissions south of 60°S account for half of the total BC concentrations in the lowest 1000 m of the atmosphere south of 70°S in December. The increasing number of tourists visiting Antarctica and fishing vessels operating close to Antarctica are, therefore, a matter of concern.

An evaluation is made of ozone profiles retrieved from measurements of the nadir-viewing Global Ozone Monitoring Experiment (GOME) instrument. Currently, four different approaches are used to retrieve ozone profile information from GOME measurements, which differ in the use of external information and a priori constraints. In total nine different algorithms will be evaluated exploiting the optimal estimation (Royal Netherlands Meteorological Institute, Rutherford Appleton Laboratory, University of Bremen, National Oceanic and Atmospheric Administration, Smithsonian Astrophysical Observatory), Phillips-Tikhonov regularization (Space Research Organization Netherlands), neural network (Center for Solar Energy and Hydrogen Research, Tor Vergata University), and data assimilation (German Aerospace Center) approaches. Analysis tools are used to interpret data sets that provide averaging kernels. In the interpretation of these data, the focus is on the vertical resolution, the indicative altitude of the retrieved value, and the fraction of a priori information. The evaluation is completed with a comparison of the results to lidar data from the Network for Detection of Stratospheric Change stations in Andoya (Norway), Observatoire Haute Provence (France), Mauna Loa (Hawaii), Lauder (New Zealand), and Dumont d'Urville (Antarctic) for the years 1997–1999. In total, the comparison involves nearly 1000 ozone profiles and allows the analysis of GOME data measured in different global regions and hence observational circumstances. The main conclusion of this paper is that unambiguous information on the ozone profile can at best be retrieved in the altitude range 15–48 km with a vertical resolution of 10 to 15 km, precision of 5–10%, and a bias up to 5% or 20% depending on the success of recalibration of the input spectra. The sensitivity of retrievals to ozone at lower altitudes varies from scheme to scheme and includes significant influence from a priori assumptions.

A solar occultation sensor, the Improved Limb Atmospheric Spectrometer (ILAS)-II, measured 5890 vertical profiles of ozone concentrations in the stratosphere and lower mesosphere and of other species from January to October 2003. The measurement latitude coverage was 54–71°N and 64–88°S, which is similar to the coverage of ILAS (November 1996 to June 1997). One purpose of the ILAS-II measurements was to continue such high-latitude measurements of ozone and its related chemical species in order to help accurately determine their trends. The present paper assesses the quality of ozone data in the version 1.4 retrieval algorithm, through comparisons with results obtained from comprehensive ozonesonde measurements and four satellite-borne solar occultation sensors. In the Northern Hemisphere (NH), the ILAS-II ozone data agree with the other data within ±10% (in terms of the absolute difference divided by its mean value) at altitudes between 11 and 40 km, with the median coincident ILAS-II profiles being systematically up to 10% higher below 20 km and up to 10% lower between 21 and 40 km after screening possible suspicious retrievals. Above 41 km, the negative bias between the NH ILAS-II ozone data and the other data increases with increasing altitude and reaches 30% at 61–65 km. In the Southern Hemisphere, the ILAS-II ozone data agree with the other data within ±10% in the altitude range of 11–60 km, with the median coincident profiles being on average up to 10% higher below 20 km and up to 10% lower above 20 km. Considering the accuracy of the other data used for this comparative study, the version 1.4 ozone data are suitably used for quantitative analyses in the high-latitude stratosphere in both the Northern and Southern Hemisphere and in the lower mesosphere in the Southern Hemisphere.

The 2002 Southern Hemisphere final warming occurred early, following an unusually active winter and the first recorded major warming in the Antarctic. The breakdown of the stratospheric polar vortex in October and November 2002 is examined using new satellite observations from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument aboard the European Space Agency (ESA) Environment Satellite (ENVISA7-) and meteorological analyses, both high-resolution fields from the European Centre for Medium-Rangc Weather Forecasts and the coarser Met Office analyses. The results derived from MIPAS observations are compared to measurements and inferences from well-validated solar occultation satellite instruments [Halogen Occultation Experiment (HALOE), Polar Ozone and Aerosol Measurement lit (POAM III), and Stratospheric Aerosol and Gas Experiments II and III (SAGE II and III)] and to finescale tracer fields reconstructed by transporting trace gases based oil MIPAS or climatological data using a reverse-trajectory method. These comparisons confirm the features in the MIPAS data and the interpretation of the evolution of the flow during the vortex decay revealed by those features. Mapped ozone and water vapor from MIPAS and the analyzed isentropic potential vorticity vividly display the vortex breakdown, which occurred earlier than usual. A large tongue of vortex air was pulled out westward and coiled up in an anticyclone, while the vortex core remnant shrank and drifted eastward and equatorward over the South Atlantic. By roughly mid-November, the vortex remnant at 10 mb had shrunk below scales resolved by the satellite observations, while a vortex core remained in the lower stratosphere.

In March 2002 the European Space Agency (ESA) launched the polar-orbiting environmental satellite Envisat. One of its nine instruments is the Global Ozone Monitoring by Occultation of Stars (GOMOS) instrument, which is a medium-resolution stellar occultation spectrometer measuring vertical profiles of ozone. In the first year after launch a large group of scientists performed additional measurements and validation activities to assess the quality of Envisat observations. In this paper, we present validation results of GOMOS ozone profiles from comparisons to microwave radiometer, balloon ozonesonde, and lidar measurements worldwide. Thirty-one instruments/launch sites at twenty-five stations ranging from the Arctic to the Antarctic joined in this activity. We identified 6747 collocated observations that were performed within an 800-km radius and a maximum 20-hour time difference of a satellite observation, for the period between 1 July 2002 and 1 April 2003. The GOMOS data analyzed here have been generated with a prototype processor that corresponds to version 4.02 of the operational GOMOS processor. The GOMOS data initially contained many obviously unrealistic values, most of which were successfully removed by imposing data quality criteria. Analyzing the effect of these criteria indicated, among other things, that for some specific stars, only less than 10% of their occultations yield an acceptable profile. The total number of useful collocated observations was reduced to 2502 because of GOMOS data unavailability, the imposed data quality criteria, and lack of altitude overlap. These collocated profiles were compared, and the results were analyzed for possible dependencies on several geophysical (e.g., latitude) and GOMOS observational (e.g., star characteristics) parameters. We find that GOMOS data quality is strongly dependent on the illumination of the limb through which the star is observed. Data measured under bright limb conditions, and to a certain extent also in twilight limb, should be used with caution, as their usability is doubtful. In dark limb the GOMOS data agree very well with the correlative data, and between 14- and 64-km altitude their differences only show a small (2.5–7.5%) insignificant negative bias with a standard deviation of 11–16% (19–63 km). This conclusion was demonstrated to be independent of the star temperature and magnitude and the latitudinal region of the GOMOS observation, with the exception of a slightly larger bias in the polar regions at altitudes between 35 and 45 km.

To improve our understanding of wintertime polar ozone losses, two ozonesonde Match campaigns were performed. The first one was carried out in the Arctic winter 2002/03. About 450 coordinated ozonesondes were launched from late November 2002 to March 2003. Temperatures low enough for the formation of polar stratospheric clouds (PSC) occurred already in the second half of November. At 475 K the Match analysis shows increasing ozone loss rates from early December until the second half of January with peaking loss rates of 35 ppbv/day. Afterwards the rate of ozone loss decreased and stopped after a month. Throughout the whole winter we find accumulated ozone loss of about 1.5 ppmv at the 500 K isentrope and approximately 60 DU in the total ozone column, which is about half of the maximum loss found in past winters. From June to October 2003 an Antarctic Match campaign was carried out for the first time. About 400 sondes were launched by 9 stations. Ozone loss rates of up to 75 ppbv/day were found inside the polar vortex at the 475 K potential temperature level during the first half of September. The timing of the fastest ozone loss coincides with the return of sunlight to the vortex after the Antarctic winter. During the whole time period temperatures were low enough for PSCs, including ice clouds, to form. Results for the potential temperature range between 400 K and 550 K will be presented.

Ground-based zenith sky UV–visible measurements of stratospheric bromine monoxide (BrO) slant column densities are compared with simulations from the SLIMCAT three-dimensional chemical transport model. The observations have been obtained from a network of 11 sites, covering high and midlatitudes of both hemispheres. This data set gives for the first time a near-global picture of the distribution of stratospheric BrO from ground-based observations and is used to test our current understanding of stratospheric bromine chemistry. In order to allow a direct comparison between observations and model calculations, a radiative transfer model has been coupled to the chemical model to calculate simulated slant column densities. The model reproduces the observations in general very well. The absolute amount of the BrO slant columns is consistent with a total stratospheric bromine loading of 20 ± 4 ppt for the period 1998–2000, in agreement with previous estimates. The seasonal and latitudinal variations of BrO are well reproduced by the model. In particular, the good agreement between the observed and modeled diurnal variation provides strong evidence that the BrO-related bromine chemistry is correctly modeled. A discrepancy between observed and modeled BrO at high latitudes during events of chlorine activation can be resolved by increasing the rate constant for the reaction BrO + ClO → BrCl + O2 to the upper limit of current recommendations. However, other possible causes of the discrepancy at high latitudes cannot be ruled out.

The altitude dependent variability of ozone in the polar stratosphere is regularly observed by balloon-borne ozonesonde observations at Neumayer Station (70°S) in the Antarctic and at Koldewey Station (79°N) in the Arctic. The reasons for observed seasonal and interannual variability and long-term changes are discussed. Differences between the hemispheres are identified and discussed in light of differing dynamical and chemical conditions. Since the mid- 1980s, rapid chemical ozone loss has been recorded in the lower Antarctic stratosphere during the spring season. Using coordinated ozone soundings in some Arctic winters, similar chemical ozone loss rates have been detected related to periods of low temperatures. The currently observed cooling trend of the stratosphere, potentially caused by the increase of anthropogenic greenhouse gases, may further strengthen chemical ozone removal in the Arctic. However, the role of internal climate oscillations in observed temperature trends is still uncertain. First results of a 10000 year integration of a low order climate model indicate significant internal climate variability. on decadal time scales, that may alter the effect of increasing levels of greenhouse gases in the polar stratosphere.

The paper presents a new global modeling tool, Stratospheric Chemical Transport Model 2. It has been developed for effective three-dimensional multiyear stratospheric chemistry studies, featuring an extensive chemistry scheme, heterogeneous processing on sulfate aerosols, and some polar stratospheric cloud processes. The transport algorithm maintains sub-grid-scale distributions and connects vertically the stratospheric layers, even in a coarse vertical grid. The model has been integrated for 49 months, recycling 1 year of precalculated transport from a middle atmosphere general circulation model. One year of daily National Centers for Environmental Prediction global analyses are used as temperatures. Diurnal cycles of photolysis rates are recalculated every 7 days to give interaction with ozone changes. The model is able to describe most of the geographical and seasonal ozone variability and the meridional distributions of ozone, reactive nitrogen, chlorine, and bromine. Stratospheric diurnal cycles for nitrogen, hydrogen, chlorine, and bromine species are captured in detail. The upper stratosphere ozone deficiency, typical to models, is large. Its sensitivity to different ways of tuning are explored. Midlatitude, rather than polar, wintertime processes have so far been the focus in this model tool. The present transport and grid resolution are not suited for realistic simulations at high latitudes. As there is only a limited inclusion of polar stratospheric cloud (PSC) microphysics, chemical processing in the cold polar lower stratosphere also cannot be well simulated. For example, the Antarctic ozone hole is not simulated, but the modeled chemistry should be suitable for warm Arctic winters when type II PSCs and particle sedimentation do not occur.

Comparisons of total column ozone measurements from Dobson, Brewer and SAOZ instruments are presented for the period 1990 to 1995 at seven stations covering the mid- and the high northern latitudes, as well as the Antarctic region. The main purpose of these comparisons is to assess, by reference to the well established Dobson network, the accuracy of the zenith-sky visible spectroscopy for the measurement of total ozone. The strengths and present limitations of this latter technique are investigated. As a general result, the different instruments are found to agree within a few percent at all stations, the best agreement being obtained at mid-latitudes. On average, for the mid-latitudes, SAOZ O3 measurements are approximately 2% higher than Dobson ones, with a scatter of about 5%. At higher latitudes, both scatter and systematic deviation tend to increase. In all cases, the relative differences between SAOZ and Dobson or Brewer column ozone are characterised by a significant seasonal signal, the amplitude of which increases from about 2.5% at mid-latitude to a maximum of 7.5% at Faraday, Antarctica. Although it introduces a significant contribution to the seasonality at high latitude, the temperature sensitivity of the O3 absorption coefficients of the Dobson and Brewer instruments is shown to be too small to account for the observed SAOZ/Dobson differences. Except for Faraday, these differences can however be largely reduced if SAOZ AMFs are calculated with realistic climatological profiles of ozone, pressure and temperature. Other sources of uncertainties that might affect the comparison are investigated. Evidence is found that the differences in the air masses sampled by the SAOZ and the other instruments contribute significantly to the scatter, and the impact of the tropospheric clouds on SAOZ measurements is displayed.