[1] Recent satellite observations and dynamical studies have demonstrated the existence of filamentary structures in chemical tracer fields in the stratosphere. It is also evident that such features are often below the spatial resolution of the highest-resolution Eulerian models that have been used up to the present time. These observations have motivated the development of a novel Chemical Lagranigan Model of the Stratosphere (CLaMS) that is based on a Lagrangian transport of tracers. The description of CLaMS is divided into two parts: Part 1 (this paper) concentrates on the Lagrangian dynamics, i.e., on the calculation of trajectories and on a completely new mixing algorithm based on a dynamically adaptive grid, while part 2 describes the chemical integration and initialization procedure. The mixing of different air masses in CLaMS is driven by the large-scale horizontal flow deformation and takes into account the mass exchange between the nearest neighbors determined by Delaunay triangulation. Here we formulate an isentropic, i.e., two-dimensional version of the model and verify the mixing algorithm using tracer distributions measured during the space shuttle CRISTA-1 experiment where highly resolved stratospheric structures were observed in early November 1994. A comparison of the measured Southern Hemispheric N 2 O distribution with CLaMS results allows the intensity of simulated mixing to be optimized. The long-term robustness of the transport scheme is investigated in a case study of the 1996-1997 Northern Hemisphere polar vortex. This study further provides a dynamical framework for investigations of chemical arctic ozone destruction discussed in part 2.

We compare global water vapor observations from Microwave Limb Sounder (MLS) and simulations with the Lagrangian chemical transport model CLaMS (Chemical Lagrangian Model of the Stratosphere) to investigate the pathways of water vapor into the lower stratosphere during Northern Hemisphere (NH) summer. We find good agreement between the simulation and observations, with an effect of the satellite averaging kernel especially at high latitudes. The Asian and American monsoons emerge as regions of particularly high water vapor mixing ratios in the lower stratosphere during boreal summer. In NH midlatitudes and high latitudes, a clear anticorrelation between water vapor and ozone daily tendencies reveals a large region influenced by frequent horizontal transport from low latitudes, extending up to about 450K during summer and fall. Analysis of the zonal mean tracer continuity equation shows that close to the subtropics, this horizontal transport is mainly caused by the residual circulation. In contrast, at higher latitudes, poleward of about 50°N, eddy mixing dominates the horizontal water vapor transport. Model simulations with transport barriers confirm that almost the entire annual cycle of water vapor in NH midlatitudes above about 360K, with maximum mixing ratios during summer and fall, is caused by horizontal transport from low latitudes. In the model, highest water vapor mixing ratios in this region are clearly linked to horizontal transport from the subtropics.

Abstract. The impact of different boundary layer source regions in Asia on the chemical composition of the Asian monsoon anticyclone, considering its intraseasonal variability in 2012, is analysed by simulations of the Chemical Lagrangian Model of the Stratosphere (CLaMS) using artificial emission tracers. The horizontal distribution of simulated CO, O3, and artificial emission tracers for India/China are in good agreement with patterns found in satellite measurements of O3 and CO by the Aura Microwave Limb Sounder (MLS). Using in addition, correlations of artificial emission tracers with potential vorticity demonstrates that the emission tracer for India/China is a very good proxy for spatial distribution of trace gases within the Asian monsoon anticyclone. The Asian monsoon anticyclone constitutes a horizontal transport barrier for emission tracers and is highly variable in location and shape. From the end of June to early August, a northward movement of the anticyclone and, during September, a strong broadening of the spatial distribution of the emission tracer for India/China towards the tropics are found. In addition to the change of the location of the anticyclone, the contribution of different boundary source regions to the composition of the Asian monsoon anticyclone in the upper troposphere strongly depends on its intraseasonal variability and is therefore more complex than hitherto believed. The largest contributions to the composition of the air mass in the anticyclone are found from northern India and Southeast Asia at a potential temperature of 380 K. In the early (mid-June to mid-July) and late (September) period of the 2012 monsoon season, contributions of emissions from Southeast Asia are highest; in the intervening period (early August), emissions from northern India have the largest impact. Our findings show that the temporal variation of the contribution of different convective regions is imprinted in the chemical composition of the Asian monsoon anticyclone. Air masses originating in Southeast Asia are found both within and outside of the Asian monsoon anticyclone because these air masses experience, in addition to transport within the anticyclone, upward transport at the southeastern flank of the anticyclone and in the tropics. Subsequently, isentropic poleward transport of these air masses occurs at around 380 K with the result that the extratropical lowermost stratosphere in the Northern Hemisphere is flooded by the end of September with air masses originating in Southeast Asia. Even after the breakup of the anticyclonic circulation (around the end of September), significant contributions of air masses originating in India/China are still found in the upper troposphere over Asia. Our results demonstrate that emissions from India, China, and Southeast Asia have a significant impact on the chemical composition of the lowermost stratosphere of the Northern Hemisphere, in particular at the end of the monsoon season in September/October 2012.

Abstract. The Asian summer monsoon provides an important pathway of tropospheric source gases and pollution into the lower stratosphere. This transport is characterized by deep convection and steady upwelling, combined with confinement inside a large-scale anticyclonic circulation in the upper troposphere and lower stratosphere (UTLS). In this paper, we show that a barrier to horizontal transport along the 380 K isentrope in the monsoon anticyclone can be determined from a local maximum in the gradient of potential vorticity (PV), following methods developed for the polar vortex (e.g., Nash et al., 1996). The monsoon anticyclone is dynamically highly variable and the maximum in the PV gradient is weak, such that additional constraints are needed (e.g., time averaging). Nevertheless, PV contours in the monsoon anticyclone agree well with contours of trace gas mixing ratios (CO, O 3 ) and mean age from model simulations with a Lagrangian chemistry transport model (CLaMS) and satellite observations from the Microwave Limb Sounder (MLS) instrument. Hence, the PV-based transport barrier reflects the separation between air inside the core of the anticyclone and the background atmosphere well. For the summer season 2011 we find an average PV value of 3.6 PVU for the transport barrier in the anticyclone on the 380 K isentrope.

Abstract. Chemical ozone loss in the Arctic stratosphere was investigated for the twelve years between 1991 and 2003 employing the ozone-tracer correlation method. For this method, the change in the relation between ozone and a longlived tracer is considered for all twelve years over the lifetime of the polar vortex to calculate chemical ozone loss. Both the accumulated local ozone loss in the lower stratosphere and the column ozone loss were derived consistently, mainly on the basis of HALOE satellite observations. HALOE measurements do not cover the polar region homogeneously over the course of the winter. Thus, to derive an early winter reference function for each of the twelve years, all available measurements were additionally used; for two winters climatological considerations were necessary. Moreover, a detailed quantification of uncertainties was performed. This study further demonstrates the interaction between meteorology and ozone loss. The connection between temperature conditions and chlorine activation, and in turn, the connection between chlorine activation and ozone loss, becomes obvious in the HALOE HCl measurements. Additionally, the degree of homogeneity of ozone loss within the vortex was shown to depend on the meteorological conditions.Results derived here are in general agreement with the results obtained by other methods for deducing polar ozone loss. Differences occur mainly owing to different time periods considered in deriving accumulated ozone loss. However, very strong ozone losses as deduced from SAOZ for January in winters 1993-1994 and 1995-1996 cannot be identified using available HALOE observations in the early winter. In general, strong accumulated ozone loss was found to occur in conjunction with a strong cold vortex containing a large volume of possible PSC existence (V PSC ), whereas moderate ozone loss was found if the vortex was less strong and moderately warm. Hardly any ozone loss was calculated Correspondence to: S. Tilmes (simone.tilmes@t-online.de) for very warm winters with small amounts of V PSC during the entire winter. This study supports the linear relationship between V PSC and the accumulated ozone loss reported by Rex et al. (2004) if V PSC was averaged over the entire winter period. Here, further meteorological factors controlling ozone loss were additionally identified if V PSC was averaged over the same time interval as that for which the accumulated ozone loss was deduced. A significant difference in ozone loss (of ≈36 DU) was found due to the different duration of solar illumination of the polar vortex of at maximum 4 hours per day in the observed years. Further, the increased burden of aerosols in the atmosphere after the Pinatubo volcanic eruption in 1991 significantly increased the extent of chemical ozone loss.