On the possible causes of recent increases in NH total ozone from a statistical analysis of satellite data from 1979 to 2003

International audienceGlobal total ozone measurements from various satellite instruments such as SBUV, TOMS, and GOME show an increase in zonal mean total ozone at NH mid to high latitudes since the mid-nineties. This increase could be expected from the peaking and start of decline in the effective stratospheric halogen loading, but the rather rapid increase observed in NH zonal mean total ozone suggests that another physical mechanism such as winter planetary wave activity has increased which has led to higher stratospheric Arctic temperatures. This has enhanced ozone transport into higher latitudes in recent years as part of the residual circulation and at the same time reduced the frequency of cold Arctic winters with enhanced polar ozone loss. Results from various multi-variate linear regression analyses using SBUV V8 total ozone with explanatory variables such as a linear trend or, alternatively, EESC (effective equivalent stratospheric chlorine) and on the other hand planetary wave driving (eddy heat flux) or, alternatively, polar ozone loss (PSC volume) in addition to proxies for stratospheric aerosol loading, QBO, and solar cycle, all considered to be main drivers for ozone variability, are presented. It is shown that the main contribution to the recent increase in NH total ozone is from the combined effect of rising tropospheric driven planetary wave activity associated with reduced polar ozone loss at high latitudes as well as increasing solar activity. This conclusion can be drawn regardless of the use of linear trend or EESC terms in our statistical model. It is also clear that more years of data will be needed to further improve our estimates of the relative contributions of the individual processes to decadal ozone variability. The question remains if the observed increase in planetary wave driving is part of the natural decadal atmospheric variability or will persist. If the latter is the case, it could be interpreted as a possible signature of climate change

Validation of water vapour transport in the tropical tropopause region in coupled Chemistry Climate Models

International audienceIn this study backward trajectories from the tropical lower stratosphere were calculated for the Northern Hemisphere (NH) winters 1995?1996, 1997?1998 (El Niño) and 1998?1999 (La Niña) and summers 1996, 1997 and 1999 using both ERA-40 reanalysis data of the European Centre for Medium-Range Weather Forecast (ECMWF) and coupled chemistry climate model (CCM) data. The calculated trajectories were analyzed to determine the distribution of points where individual air masses encounter the minimum temperature and thus minimum water vapour mixing ratio during their ascent through the tropical tropopause layer (TTL) into the stratosphere. The geographical distribution of these dehydration points and the local conditions there determine the overall water vapour entry into the stratosphere. Results of two CCMs are presented: the ECHAM4.L39(DLR)/CHEM (hereafter: E39/C) from the German Aerospace Center (DLR) and the Freie Universität Berlin Climate Middle Atmosphere Model with interactive chemistry (hereafter: FUB-CMAM-CHEM). In the FUB-CMAM-CHEM model the minimum temperatures are overestimated by about 7 K in Northern Hemisphere (NH) winter as well as in NH summer, resulting in too high water vapour entry values compared to ERA-40. However, the geographical distribution of dehydration points is fairly reproduced for NH winter 1995?1996 and 1998?1999 and in all boreal summers. The distribution of dehydration points suggests an influence of the Indian monsoon upon the water vapour transport. The E39/C model displays a temperature bias of about +3 K. Hence, the minimum water vapour mixing ratios are higher relative to ERA-40. The geographical distribution of dehydration points is satisfactory in NH winter 1995?1996 and 1997?1998 with respect to ERA-40. The distribution is not reproduced for the NH winter 1998?1999 (La Niña event) compared to ERA-40. There is excessive mass flux through warm regions e.g. Africa, leading to excessive water vapour flux in the NH winter and summer. The possible influence of the Indian monsoon on the transport is not seen in the boreal summer. Further, the residence times of air parcels in the TTL were derived from the trajectory calculations. The analysis of the residence times reveals that in both CCMs residence times in the TTL are underestimated compared to ERA-40 and the seasonal variation is hardly present

Variability and trends in total and vertically resolved stratospheric ozone

International audienceTrends in ozone columns and vertical distributions were calculated for the period 1979?2004 based on the three-dimensional ozone data set CATO (Candidoz Assimilated Three-dimensional Ozone) using a multiple linear regression model. CATO has been reconstructed from TOMS, GOME and SBUV total column ozone observations in an equivalent latitude and potential temperature framework and offers a pole to pole coverage of the stratosphere on 15 potential temperature levels. The regression model includes explanatory variables describing the influence of the quasi-biennial oscillation, volcanic eruptions, the solar cycle, the Brewer-Dobson circulation, Arctic ozone depletion, and the increase in stratospheric chlorine. The effects of displacements of the polar vortex and jet streams due to planetary waves, which may significantly affect trends at a given geographical latitude, are eliminated in the equivalent latitude framework. Ozone variability is largely explained by the QBO and stratospheric aerosol loading and the spatial structure of their influence is in good agreement with previous studies. The solar cycle signal peaks at about 30 to 35 km altitude which is lower than reported previously, and no negative signal is found in the tropical lower stratosphere. The Brewer-Dobson circulation shows a dominant contribution to interannual variability at both high and low latitudes and accounts for some of the ozone increase seen in the northern hemisphere since the mid-1990s. Arctic ozone depletion significantly affects the high northern latitudes between January and March and extends its influence to the mid-latitudes during later months. The vertical distribution of the ozone trend shows distinct negative trends at about 18 km in the lower stratosphere with largest declines over the poles, and above 35 km in the upper stratosphere. A narrow band of large negative trends extends into the tropical lower stratosphere. Assuming that the observed negative trend before 1995 continued to 2004 cannot explain the ozone changes since 1996. A model accounting for recent changes in EESC, aerosols and Eliassen-Palm flux, on the other hand, closely tracks ozone changes since 1995

A tropical West Pacific OH minimum and implications for stratospheric composition

Most of the short-lived biogenic and anthropogenic chemical species that are emitted into the atmosphere break down efficiently by reaction with OH and do not reach the stratosphere. Here we show the existence of a pronounced minimum in the tropospheric column of ozone over the West Pacific, the main source region for stratospheric air, and suggest a corresponding minimum of the tropospheric column of OH. This has the potential to amplify the impact of surface emissions on the stratospheric composition compared to the impact when assuming globally uniform OH conditions. Specifically, the role of emissions of biogenic halogenated species for the stratospheric halogen budget and the role of increasing emissions of SO₂ in Southeast Asia or from minor volcanic eruptions for the increasing stratospheric aerosol loading need to be reassessed in light of these findings. This is also important since climate change will further modify OH abundances and emissions of halogenated species. Our study is based on ozone sonde measurements carried out during the TransBrom cruise with the RV <i>Sonne</i> roughly along 140–150° E in October 2009 and corroborating ozone and OH measurements from satellites, aircraft campaigns and FTIR instruments. Model calculations with the GEOS-Chem Chemistry and Transport Model (CTM) and the ATLAS CTM are used to simulate the tropospheric OH distribution over the West Pacific and the transport pathways to the stratosphere. The potential effect of the OH minimum on species transported into the stratosphere is shown via modeling the transport and chemistry of CH₂Br₂ and SO₂

Uncertainties in Modelling Heterogeneous Chemistry and Arctic Ozone Depletion in the Winter 2009/2010

Stratospheric chemistry and denitrification are simulated for the Arctic winter 2009/2010 with the Lagrangian Chemistry and Transport Model ATLAS. A number of sensitivity runs is used to explore the impact of uncertainties in chlorine activation and denitrification on the model results. In particular, the efficiency of chlorine activation on different types of liquid aerosol versus activation on nitric acid trihydrate clouds is examined. Additionally, the impact of changes in reaction rate coefficients, in the particle number density of polar stratospheric clouds, in supersaturation, temperature or the extent of denitrification is investigated. Results are compared to satellite measurements of MLS and ACE-FTS and to in-situ measurements onboard the Geophysica aircraft during the RECONCILE measurement campaign. It is shown that even large changes in the underlying assumptions have only a small impact on the modelled ozone loss, even though they can cause considerable differences in chemical evolution of other species and in denitrification. Differences in column ozone between the sensitivity runs stay below 10% at the end of the winter. Chlorine activation on liquid aerosols alone is able to explain the observed magnitude and morphology of the mixing ratios of active chlorine, reservoir gases and ozone. This is even true for binary aerosols (no uptake of HNO3 from the gas-phase allowed in the model). Differences in chlorine activation between sensitivity runs are within 30 %. Current estimates of nitric acid trihydrate (NAT) number density and supersaturation imply that, at least for this winter, NAT clouds play a relatively small role compared to liquid clouds in chlorine activation. The change between different reaction rate coefficients for liquid or solid clouds has only a minor impact on ozone loss and chlorine activation in our sensitivity runs

A Lagrangian convective transport scheme including a simulation of the time air parcels spend in updrafts

Abstract. We present a Lagrangian convective transport scheme developed for Chemistry and Transport Models and ensemble trajectory simulations. Similar to existing schemes in other Lagrangian models, it is based on a statistical approach of calculating parcel displacements by convection. These schemes redistribute air parcels within a fixed time step by calculating probabilities for entrainment and the altitude of detrainment. Our scheme extends this approach by modelling vertical updraft velocities and the time that an air parcel spends inside the convective event, which is important for simulating the tropospheric chemistry of short-lived species, e.g. it determines the time available for heterogeneous processes on the surface of cloud droplets. Two different schemes for determining the vertical updraft velocities are introduced, which are based on constant or random convective area fraction profiles, respectively. SO2 is used as an example to show that there is a significant effect on species mixing ratios when modelling the time spent in convective updrafts compared to a nearly instantaneous redistribution of air parcels. The scheme is driven by convective mass fluxes and detrainment rates that originate from an external convective parameterization, which can be obtained from meteorological analysis data or General Circulation Models. Validation runs driven by ECMWF ERA Interim reanalysis data are performed with the scheme implemented into the ATLAS Chemistry and Transport Model. These include long-term global trajectory simulations of Radon-222 that are compared to measurements, and runs testing mass conservation and the reproduction of the convective mass fluxes and detrainment rates of ERA Interim. Simulated vertical updraft velocities are validated by wind profiler measurements in Darwin. </jats:p

A Lagrangian convective transport scheme including a simulation of the time air parcels spend in updrafts (LaConTra v1.0)

We present a Lagrangian convective transport scheme developed for global chemistry and transport models, which considers the variable residence time that an air parcel spends in convection. This is particularly important for accurately simulating the tropospheric chemistry of short-lived species, e.g., for determining the time available for heterogeneous chemical processes on the surface of cloud droplets. In current Lagrangian convective transport schemes air parcels are stochastically redistributed within a fixed time step according to estimated probabilities for convective entrainment as well as the altitude of detrainment. We introduce a new scheme that extends this approach by modeling the variable time that an air parcel spends in convection by estimating vertical updraft velocities. Vertical updraft velocities are obtained by combining convective mass fluxes from meteorological analysis data with a parameterization of convective area fraction profiles. We implement two different parameterizations: a parameterization using an observed constant convective area fraction profile and a parameterization that uses randomly drawn profiles to allow for variability. Our scheme is driven by convective mass fluxes and detrainment rates that originate from an external convective parameterization, which can be obtained from meteorological analysis data or from general circulation models. We study the effect of allowing for a variable time that an air parcel spends in convection by performing simulations in which our scheme is implemented into the trajectory module of the ATLAS chemistry and transport model and is driven by the ECMWF ERA-Interim reanalysis data. In particular, we show that the redistribution of air parcels in our scheme conserves the vertical mass distribution and that the scheme is able to reproduce the convective mass fluxes and detrainment rates of ERA-Interim. We further show that the estimated vertical updraft velocities of our scheme are able to reproduce wind profiler measurements performed in Darwin, Australia, for velocities larger than 0.6 m s−1. SO2 is used as an example to show that there is a significant effect on species mixing ratios when modeling the time spent in convective updrafts compared to a redistribution of air parcels in a fixed time step. Furthermore, we perform long-time global trajectory simulations of radon-222 and compare with aircraft measurements of radon activity

Reconciliation of essential process parameters for an enhanced predictability of Arctic stratospheric ozone loss and its climate interactions

Significant reductions in stratospheric ozone occur inside the polar vortices each spring when chlorine radicals produced by heterogeneous reactions on cold particle surfaces in winter destroy ozone mainly in two catalytic cycles, the ClO dimer cycle and the ClO/BrO cycle. Chlorofluorocarbons (CFCs), which are responsible for most of the chlorine currently present in the stratosphere, have been banned by the Montreal Protocol and its amendments, and the ozone layer is predicted to recover to 1980 levels within the next few decades. During the same period, however, climate change is expected to alter the temperature, circulation patterns and chemical composition in the stratosphere, and possible geo-engineering ventures to mitigate climate change may lead to additional changes. To realistically predict the response of the ozone layer to such influences requires the correct representation of all relevant processes. The European project RECONCILE has comprehensively addressed remaining questions in the context of polar ozone depletion, with the objective to quantify the rates of some of the most relevant, yet still uncertain physical and chemical processes. To this end RECONCILE used a broad approach of laboratory experiments, two field missions in the Arctic winter 2009/10 employing the high altitude research aircraft M55-Geophysica and an extensive match ozone sonde campaign, as well as microphysical and chemical transport modelling and data assimilation. Some of the main outcomes of RECONCILE are as follows: (1) vortex meteorology: the 2009/10 Arctic winter was unusually cold at stratospheric levels during the six-week period from mid-December 2009 until the end of January 2010, with reduced transport and mixing across the polar vortex edge; polar vortex stability and how it is influenced by dynamic processes in the troposphere has led to unprecedented, synoptic-scale stratospheric regions with temperatures below the frost point; in these regions stratospheric ice clouds have been observed, extending over >106km2 during more than 3 weeks. (2) Particle microphysics: heterogeneous nucleation of nitric acid trihydrate (NAT) particles in the absence of ice has been unambiguously demonstrated; conversely, the synoptic scale ice clouds also appear to nucleate heterogeneously; a variety of possible heterogeneous nuclei has been characterised by chemical analysis of the non-volatile fraction of the background aerosol; substantial formation of solid particles and denitrification via their sedimentation has been observed and model parameterizations have been improved. (3) Chemistry: strong evidence has been found for significant chlorine activation not only on polar stratospheric clouds (PSCs) but also on cold binary aerosol; laboratory experiments and field data on the ClOOCl photolysis rate and other kinetic parameters have been shown to be consistent with an adequate degree of certainty; no evidence has been found that would support the existence of yet unknown chemical mechanisms making a significant contribution to polar ozone loss. (4) Global modelling: results from process studies have been implemented in a prognostic chemistry climate model (CCM); simulations with improved parameterisations of processes relevant for polar ozone depletion are evaluated against satellite data and other long term records using data assimilation and detrended fluctuation analysis. Finally, measurements and process studies within RECONCILE were also applied to the winter 2010/11, when special meteorological conditions led to the highest chemical ozone loss ever observed in the Arctic. In addition to quantifying the 2010/11 ozone loss and to understand its causes including possible connections to climate change, its impacts were addressed, such as changes in surface ultraviolet (UV) radiation in the densely populated northern mid-latitudes

Stratospheric ozone loss in the Arctic winters between 2005 and 2013 derived with ACE-FTS measurements

Stratospheric ozone loss inside the Arctic polar vortex for the winters between 2004–2005 and 2012–2013 has been quantified using measurements from the space-borne Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS). For the first time, an evaluation has been performed of six different ozone loss estimation methods based on the same single observational dataset to determine the Arctic ozone loss (mixing ratio loss profiles and the partial-column ozone losses between 380 and 550 K). The methods used are the tracer-tracer correlation, the artificial tracer correlation, the average vortex profile descent, and the passive subtraction with model output from both Lagrangian and Eulerian chemical transport models (CTMs). For the tracer-tracer, the artificial tracer, and the average vortex profile descent approaches, various tracers have been used that are also measured by ACE-FTS. From these seven tracers investigated (CH4, N2O, HF, OCS, CFC-11, CFC-12, and CFC-113), we found that CH4, N2O, HF, and CFC-12 are the most suitable tracers for investigating polar stratospheric ozone depletion with ACE-FTS v3.5. The ozone loss estimates (in terms of the mixing ratio as well as total column ozone) are generally in good agreement between the different methods and among the different tracers. However, using the average vortex profile descent technique typically leads to smaller maximum losses (by approximately 15–30 DU) compared to all other methods. The passive subtraction method using output from CTMs generally results in slightly larger losses compared to the techniques that use ACE-FTS measurements only. The ozone loss computed, using both measurements and models, shows the greatest loss during the 2010–2011 Arctic winter. For that year, our results show that maximum ozone loss (2.1–2.7 ppmv) occurred at 460 K. The estimated partial-column ozone loss inside the polar vortex (between 380 and 550 K) using the different methods is 66–103, 61–95, 59–96, 41–89, and 85–122 DU for March 2005, 2007, 2008, 2010, and 2011, respectively. Ozone loss is difficult to diagnose for the Arctic winters during 2005–2006, 2008–2009, 2011–2012, and 2012–2013, because strong polar vortex disturbance or major sudden stratospheric warming events significantly perturbed the polar vortex, thereby limiting the number of measurements available for the analysis of ozone loss