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 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

Validation of OMI-TOMS and OMI-DOAS total ozone column using five Brewer spectroradiometers at the Iberian peninsula

This article focuses on the comparison of the total ozone column data from the Ozone Monitoring Instrument (OMI) flying aboard the NASA EOS-Aura satellite platform with ground-based measurement recorded by Brewer spectroradiometers located at five Spanish remote sensing ground stations between January 2005 and December 2007. The satellite data are derived from two algorithms: OMI Total Ozone Mapping Spectrometer (OMI-TOMS) and OMI Differential Optical Absorption Spectroscopy (OMI-DOAS). The largest relative differences between these OMI total ozone column estimates reach 5% with a significant seasonal dependence. The agreement between OMI ozone data and Brewer measurements is excellent. Total ozone columns from OMI-TOMS are on average a mere 2.0% lower than Brewer data. For OMI-DOAS data the bias is a mere 1.4%. However, the relative difference between OMI-TOMS and Brewer measurements shows a notably lower seasonal dependence and variability than the differences between OMI-DOAS and ground-based data. For both OMI ozone data products these relative differences show significant dependence on the satellite ground pixel solar zenith angle for cloud-free cases as well as for cloudy conditions. However, the OMI ozone data products are shown to reveal opposite behavior with respect to the two antagonistic sky conditions. No significant dependency of the ground-based to satellite-based differences with respect to the satellite cross-track position is seen for either OMI retrieval algorithm.This work was partially supported by Ministerio de Educación y Ciencia under Project CGL2005-05693-C03-03/CLI and by Ministerio de Ciencia e Innovación under project CGL2008-05939-C03-02/CLI

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

Reconciliation of essential process parameters for an enhanced predictability of Arctic stratospheric ozone loss and its climate interactions : (RECONCILE) ; activities and results

The international research project RECONCILE has addressed central questions regarding polar ozone depletion, with the objective to quantify some of the most relevant yet still uncertain physical and chemical processes and thereby improve prognostic modelling capabilities to realistically predict the response of the ozone layer to climate change. This overview paper outlines the scope and the general approach of RECONCILE, and it provides a summary of observations and modelling in 2010 and 2011 that have generated an in many respects unprecedented dataset to study processes in the Arctic winter stratosphere. Principally, it summarises important outcomes of RECONCILE including (i) better constraints and enhanced consistency on the set of parameters governing catalytic ozone destruction cycles, (ii) a better understanding of the role of cold binary aerosols in heterogeneous chlorine activation, (iii) an improved scheme of polar stratospheric cloud (PSC) processes that includes heterogeneous nucleation of nitric acid trihydrate (NAT) and ice on non-volatile background aerosol leading to better model parameterisations with respect to denitrification, and (iv) long transient simulations with a chemistry-climate model (CCM) updated based on the results of RECONCILE that better reproduce past ozone trends in Antarctica and are deemed to produce more reliable predictions of future ozone trends. The process studies and the global simulations conducted in RECONCILE show that in the Arctic, ozone depletion uncertainties in the chemical and microphysical processes are now clearly smaller than the sensitivity to dynamic variability

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

Evaluation of the inter-annual variability of stratospheric chemical composition in chemistry-climate models using ground-based multi species time series

The variability of stratospheric chemical composition occurs on a broad spectrum of timescales, ranging from day to decades. A large part of the variability appears to be driven by external forcings such as volcanic aerosols, solar activity, halogen loading, levels of greenhouse gases (GHG), and modes of climate variability (quasi-biennial oscillation (QBO), El Niño-Southern Oscillation (ENSO)). We estimate the contributions of different external forcings to the interannual variability of stratospheric chemical composition and evaluate how well 3-D chemistry-climate models (CCMs) can reproduce the observed response-forcing relationships. We carry out multivariate regression analyses on long time series of observed and simulated time series of several traces gases in order to estimate the contributions of individual forcings and unforced variability to their internannual variability. The observations are typically decadal time series of ground-based data from the international Network for the Detection of Atmospheric Composition Change (NDACC) and the CCM simulations are taken from the CCMVal-2 REF-B1 simulations database. The chemical species considered are column O3, HCl, NO2, and N2O. We check the consistency between observations and model simulations in terms of the forced and internal components of the total interannual variability (externally forced variability and internal variability) and identify the driving factors in the interannual variations of stratospheric chemical composition over NDACC measurement sites. Overall, there is a reasonably good agreement between regression results from models and observations regarding the externally forced interannual variability. A much larger fraction of the observed and modelled interannual variability is explained by external forcings in the tropics than in the extratropics, notably in polar regions. CCMs are able to reproduce the amplitudes of responses in chemical composition to specific external forcings. However, CCMs tend to underestimate very substantially the internal variability and hence the total interannual variability for almost all species considered. This lack of internal variability in CCMs might partly originate from the surface forcing of these CCMs by analysed SSTs. The results illustrate the potential of NDACC ground-based observations for evaluating CCMs