Technical note: A stratospheric climatology for O3, H2O and CH4 derived from HALOE measurements

International audienceThe Halogen Occultation Experiment (HALOE) on board the Upper Atmosphere research satellite (UARS) has observed mixing ratios of important trace species in the stratosphere over more than a decade since 1991. Here we present a climatology for the stratosphere compiled from the HALOE data for ozone, H₂O and CH₄ for the period from 1991 to 2002. In this approach, the data are averaged over equivalent latitude instead of latitude in order to correctly reproduce the gradients at the transport barriers like the polar vortex edge. The climatology is compiled for 5 degree equivalent latitude bins. The seasonal dependence is taken into account by choosing intervals of one month. The climatology is available as an electronic supplement

Does Cosmic-Ray-Induced Heterogeneous Chemistry Influence Stratospheric Polar Ozone Loss ?

Cosmic-ray (CR) -induced heterogeneous reactions of halogenated species have been suggested to play the dominant role in causing the Antarctic ozone hole. However, measurements of total ozone in Antarctica do not show a compact and significant correlation with CR activity. Further, a substantial CR-induced heterogeneous loss of chlorofluorocarbons is incompatible with multiyear satellite observations of N2O and CFC-12. Thus, CR-induced heterogeneous reactions cannot be considered as an alternative mechanism causing the Antarctic ozone hole

Long-term changes of hydrogen-containing species in the stratosphere

Understanding the 1% per year increase of stratospheric water vapour from 1954 to 2000 is a great challenge in atmospheric science. The increase is predominantly caused by long-term changes in transport of water vapour into the stratosphere and systematic increases of tropospheric methane levels. This paper gives a review on stratospheric water vapour changes for the 1980 and 2000 time period with emphasis on the contribution of methane oxidation. Predictions for 2050 indicate that likely increases of tropospheric methane levels will lead to an increase of upper stratospheric water vapour values of about 0.4 ppmv. A similar value is predicted as an upper limit of effects of a future hydrogen economy. (c) 2006 Elsevier Ltd. All rights reserved

Stratospheric ozone chemistry in the Antarctic: what determines the lowest ozone values reached and their recovery?

Balloon-borne observations of ozone from the South Pole Station have been reported to reach ozone mixing ratios below the detection limit of about 10 ppbv at the 70 hPa level by late September. After reaching a minimum, ozone mixing ratios increase to above 1 ppmv on the 70 hPa level by late December. While the basic mechanisms causing the ozone hole have been known for more than 20 yr, the detailed chemical processes determining how low the local concentration can fall, and how it recovers from the minimum have not been explored so far. Both of these aspects are investigated here by analysing results from the Chemical Lagrangian Model of the Stratosphere (CLaMS). As ozone falls below about 0.5 ppmv, a balance is maintained by gas phase production of both HCl and HOCl followed by heterogeneous reaction between these two compounds in these simulations. Thereafter, a very rapid, irreversible chlorine deactivation into HCl can occur, either when ozone drops to values low enough for gas phase HCl production to exceed chlorine activation processes or when temperatures increase above the polar stratospheric cloud (PSC) threshold. As a consequence, the timing and mixing ratio of the minimum ozone depends sensitively on model parameters, including the ozone initialisation. The subsequent ozone increase between October and December is linked mainly to photochemical ozone production, caused by oxygen photolysis and by the oxidation of carbon monoxide and methane

The impact of mixing across the polar vortex edge on Match ozone loss estimates

The Match method for quantification of polar chemical ozone loss is investigated mainly with respect to the impact of mixing across the vortex edge onto this estimate. We show for the winter 2002/03 that significant mixing across the vortex edge occurred and was accurately modeled by the Chemical Lagrangian Model of the Stratosphere. Observations of inert tracers and ozone in-situ from HAGAR on the Geophysica aircraft and sondes and also remote from MIPAS on ENVISAT were reproduced well. The model even reproduced a small vortex remnant that was isolated until June 2003 and was observed in-situ by a balloon-borne whole air sampler. We use this CLaMS simulation to quantify the impact of cross vortex edge mixing on the results of the Match method. It is shown that a time integration of the determined vortex average ozone loss rates as performed in Match results in larger ozone loss than the polar vortex average ozone loss in CLaMS. Also, the determination of the Match ozone loss rates can be influenced by mixing. This is especially important below 430 K, where ozone outside the vortex is lower than inside and the vortex boundary is not a strong transport barrier. This effect and further sampling effects cause an offset between vortex average ozone loss rates derived from Match and deduced from CLaMS with an even sampling for the entire vortex. Both, the time-integration of ozone loss and the determination of ozone loss rates for Match are evaluated using the winter 2002/03 CLaMS simulation. These impacts can explain the differences between CLaMS and Match column ozone loss. While the investigated effects somewhat reduce the apparent discrepancy in January ozone loss rates, a discrepancy between simulations and Match remains. However, its contribution to the accumulated ozone loss over the winter is not large

A model study of the January 2006 low total ozone episode over Western Europe and comparison with ozone sonde data

Total column and stratospheric ozone levels at mid-latitudes often reveal strong fluctuations on time scales of days caused by dynamic processes. In some cases the total ozone column is distinctly reduced below climatological values. Here, a very low total ozone episode around 19 January 2006 over Western Europe is investigated when the observed total ozone column over Uccle (BE), measured by a Brewer spectrophotometer, reached a daily minimum of 200 DU, the lowest recorded value at this station. In order to investigate the mechanisms leading to the ozone minimum, the present study used data from (i) six ozone sounding stations in Western and Middle Europe, (ii) ECMWF meteorological fields, (iii) a simulation of the CLaMS model for January 2006, (iv) a multi-year run of the chemistry transport model KASIMA, and (v) a six-year run of the climate chemistry model ECHAM5/MESSy1. The ozone decrease at different heights was quantified and it was determined to what extent different transport mechanisms, and instantaneous, in-situ chemical ozone depletion contributed to the event. All three models reproduced the evolution and formation of the event. The ozone column decrease between Theta=300 and 750K was strongest at Uccle (BE) and De Bilt (NL) with 108 and 103 DU, respectively, and somewhat lower at Hohenpeissenberg (DE), Payerne (CH), Prague (CZ) and Lerwick (UK) with 85, 84, 83 and 74 DU, respectively. This analysis demonstrated that mainly the displacement of the ozone depleted polar vortex contributed to the ozone column decrease. Advection of ozone-poor low-latitude air masses was important in the UTLS region. The vertical displacement of isentropes connected with divergence of air out of the column was found to be of minor importance compared to the horizontal transport processes. Severe low total ozone episodes seem to occur when the mentioned mechanisms are superimposed. Instantaneous, in-situ chemical ozone depletion accounted for only 2+/-1% of the overall total ozone decrease at the sounding stations

The maintenance of elevated active chlorine levels in the Antarctic lower stratosphere through HCl null cycles

The Antarctic ozone hole arises from ozone destruction driven by elevated levels of ozone destroying ("active") chlorine in Antarctic spring. These elevated levels of active chlorine have to be formed first and then maintained throughout the period of ozone destruction. It is a matter of debate how this maintenance of active chlorine is brought about in Antarctic spring, when the rate of formation of HCl (considered to be the main chlorine deactivation mechanism in Antarctica) is extremely high. Here we show that in the heart of the ozone hole (16–18 km or 85–55 hPa, in the core of the vortex), high levels of active chlorine are maintained by effective chemical cycles (referred to as HCl null cycles hereafter). In these cycles, the formation of HCl is balanced by immediate reactivation, i.e. by immediate reformation of active chlorine. Under these conditions, polar stratospheric clouds sequester HNO3 and thereby cause NO2 concentrations to be low. These HCl null cycles allow active chlorine levels to be maintained in the Antarctic lower stratosphere and thus rapid ozone destruction to occur. For the observed almost complete activation of stratospheric chlorine in the lower stratosphere, the heterogeneous reaction HCl + HOCl is essential; the production of HOCl occurs via HO2 + ClO, with the HO2 resulting from CH2O photolysis. These results are important for assessing the impact of changes of the future stratospheric composition on the recovery of the ozone hole. Our simulations indicate that, in the lower stratosphere, future increased methane concentrations will not lead to enhanced chlorine deactivation (through the reaction CH4 + Cl  ⟶  HCl + CH3) and that extreme ozone destruction to levels below  ≈ 0.1 ppm will occur until mid-century

Dynamics and chemistry of vortex remnants in late Arctic spring 1997 and 2000: Simulations with the Chemical Lagrangian Model of the Stratosphere (CLaMS)

High-resolution simulations of the chemical composition of the Arctic stratosphere during late spring 1997 and 2000 were performed with the Chemical Lagrangian Model of the Stratosphere (CLaMS). The simulations were performed for the entire northern hemisphere on two isentropic levels 450 K (~18 km) and 585 K (~24 km).<br> <br> The spatial distribution and the lifetime of the vortex remnants formed after the vortex breakup in May 1997 display different behavior above and below 20 km. Above 20 km, vortex remnants propagate southward (up to 40°N) and are &quot;frozen in'' in the summer circulation without significant mixing. Below 20 km the southward propagation of the remnants is bounded by the subtropical jet. Their lifetime is shorter by a factor of 2 than that above 20 km, owing to significant stirring below this altitude. The behavior of vortex remnants formed in March 2000 is similar but, due to an earlier vortex breakup, dominated during the first 6 weeks after the vortex breakup by westerly winds, even above 20 km.<br> <br> Vortex remnants formed in May 1997 are characterized by large mixing ratios of HCl indicating negligible, halogen-induced ozone loss. In contrast, mid-latitude ozone loss in late boreal spring 2000 is dominated, until mid-April, by halogen-induced ozone destruction within the vortex remnants, and subsequent transport of the ozone-depleted polar air masses (dilution) into the mid-latitudes. By varying the intensity of mixing in CLaMS, the impact of mixing on the formation of ClONO₂ and ozone depletion is investigated. We find that the photochemical decomposition of HNO₃ and not mixing with NO_x-rich mid-latitude air is the main source of NO_x within the vortex remnants in March and April 2000. Ozone depletion in the remnants is driven by ClO_x photolytically formed from ClONO₂. At the end of May 1997, the halogen-induced ozone deficit at 450 K poleward of 30°N amounts to ~12% with ~10% in the polar vortex and ~2% in well-isolated vortex remnants after the vortex breakup

The implementation of the CLaMS Lagrangian transport core into the chemistry climate model EMAC 2.40.1: application on age of air and transport of long-lived trace species

Lagrangian transport schemes have proven to be useful tools for modelling stratospheric trace gas transport since they are less diffusive than classical Eulerian schemes and therefore especially well suited for maintaining steep tracer gradients. Here, we present the implementation of the full-Lagrangian transport core of the Chemical Lagrangian Model of the Stratosphere (CLaMS) into the ECHAM/MESSy Atmospheric Chemistry model (EMAC). We performed a ten-year time-slice simulation to evaluate the coupled model system EMAC/CLaMS. Simulated zonal mean age of air distributions are compared to age of air derived from airborne measurements, showing a good overall representation of the stratospheric circulation. Results from the new Lagrangian transport scheme are compared to tracer distributions calculated with the standard flux-form semi-Lagrangian (FFSL) transport scheme in EMAC. The differences in the resulting tracer distributions are most pronounced in the regions of strong transport barriers. The polar vortices are presented as an example and simulated trace gas distributions are compared to satellite measurements. The analysis of CFC-11, N2O, CH4, and age of air in the polar vortex regions shows that the CLaMS Lagrangian transport scheme produces a stronger, more realistic transport barrier at the edge of the polar vortex than the FFSL transport scheme of EMAC. Differences in simulated age of air range up to one year in the Arctic polar vortex in late winter/early spring. The new coupled model system EMAC/CLaMS thus constitutes a suitable tool for future model studies of stratospheric tracer transport