Abstract. 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.
[1] Thirty years of balloon-borne measurements over Boulder (40 ı N, 105 ı W) are used to investigate the water vapor trend in the tropopause region. This analysis extends previously published trends, usually focusing on altitudes greater than 16 km, to lower altitudes. Two new concepts are applied: (1) Trends are presented in a thermal tropopause (TP) relative coordinate system from -2 km below to 10 km above the TP, and (2) sonde profiles are selected according to TP height. Tropical (TP z > 14 km), extratropical (TP z < 12 km), and transitional air mass types (12 km < TP z < 14 km) reveal three different water vapor reservoirs. The analysis based on these concepts reduces the dynamically induced water vapor variability at the TP and principally favors refined water vapor trend studies in the upper troposphere and lower stratosphere. Nonetheless, this study shows how uncertain trends are at altitudes -2 to +4 km around the TP. This uncertainty in turn has an influence on the uncertainty and interpretation of water vapor radiative effects at the TP, which are locally estimated for the 30 year period to be of uncertain sign. The much discussed decrease in water vapor at the beginning of 2001 is not detectable between -2 and 2 km around the TP. On lower stratospheric isentropes, the water vapor change at the beginning of 2001 is more intense for extratropical than for tropical air mass types. This suggests a possible link with changing dynamics above the jet stream such as changes in the shallow branch of the Brewer-Dobson circulation.
Laboratory and numerical experiments are reported on dye advection processes in geostrophic turbulence. The experimental setup is the classical rotating annulus with differential heating which mimics the most essential features of midlatitude atmospheric flow. The main control parameter is the temperature contrast. Fluorescent dye is used as passive tracer, and dispersion is evaluated by digital image processing. The results are compared with tracer dispersion computations which are performed by means of global reanalysis wind fields at the pressure height of 500 hPa covering a time interval of one year. Apart from initial transient periods, the characteristic behavior for intermediate time scales is ballistic dispersion in both systems, where the zonal extent of the tracer cloud increases linearly in time (Batchelor scaling). The long-time evolution cannot be followed by the experimental technique, however, the numerical tests suggest a slower diffusive dispersion (Taylor regime) after 70-80 revolutions (days), in agreement with expectations. Richardson-Obukhov scaling (superdiffusion with an exponent value of 3/2) is neither observed in the laboratory nor in the numerical tests. Our findings confirm recent experimental results on the classic prediction by Batchelor that the initial pair separation is an essential parameter of the subsequent time evolution of tracers.
We report on a detailed time series analysis of long total column ozone (TO) records based on multi-satellite observations of daily resolution. We concentrate on three geographic latitudes over and around the Antarctic area, specifically on three circles at 58.5 ∘ S, 59.5 ∘ S, and 79.5 ∘ S. Almost continuous observations are available at the two former latitudes; however, data are lacking during the polar winter periods at 79.5 ∘ S, because the measurement technique requires sunlight. The methodology is motivated by level-crossing statistics, where subsets of the records above or below particular threshold levels are evaluated. Long-term trend reversal at around the turn of the century is already detectable for low TO levels in the raw time series in the "ozone-hole" region (79.5 ∘ S). In order to overcome the apparent non-stationarities of the time series, we determined daily TO differences (ΔTO) belonging to the same geographic longitudes between the different latitudinal circles. The result is a stable, stationary behavior for small (absolute) ΔTO values in the period January-February-March without any significant detectable trends. The high absolute value ΔTO subsets (September-October-November) indicate a robust trend reversal in the middle of the 1990s. The observed trend reversal in the total column ozone time series is consistent with the temporal development of the stratospheric halogen loading. However, a close correspondence of ozone and halogen turnaround years is not expected because of the statistical uncertainties in the determination of the ozone turnaround, and the many factors contributing to ozone depletion processes.
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 >10<sup>6</sup>km<sup>2</sup> 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 exis...
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