[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 European Centre for Medium-Range Weather Forecasts' (ECMWF's) next-generation reanalysis ERA5 provides many improvements, but it also confronts the community with a “big data” challenge. Data storage requirements for ERA5 increase by a factor of ∼80 compared with the ERA-Interim reanalysis, introduced a decade ago. Considering the significant increase in resources required for working with the new ERA5 data set, it is important to assess its impact on Lagrangian transport simulations. To quantify the differences between transport simulations using ERA5 and ERA-Interim data, we analyzed comprehensive global sets of 10-day forward trajectories for the free troposphere and the stratosphere for the year 2017. The new ERA5 data have a considerable impact on the simulations. Spatial transport deviations between ERA5 and ERA-Interim trajectories are up to an order of magnitude larger than those caused by parameterized diffusion and subgrid-scale wind fluctuations after 1 day and still up to a factor of 2–3 larger after 10 days. Depending on the height range, the spatial differences between the trajectories map into deviations as large as 3 K in temperature, 30 % in specific humidity, 1.8 % in potential temperature, and 50 % in potential vorticity after 1 day. Part of the differences between ERA5 and ERA-Interim is attributed to the better spatial and temporal resolution of the ERA5 reanalysis, which allows for a better representation of convective updrafts, gravity waves, tropical cyclones, and other meso- to synoptic-scale features of the atmosphere. Another important finding is that ERA5 trajectories exhibit significantly improved conservation of potential temperature in the stratosphere, pointing to an improved consistency of ECMWF's forecast model and observations that leads to smaller data assimilation increments. We conducted a number of downsampling experiments with the ERA5 data, in which we reduced the numbers of meteorological time steps, vertical levels, and horizontal grid points. Significant differences remain present in the transport simulations, if we downsample the ERA5 data to a resolution similar to ERA-Interim. This points to substantial changes of the forecast model, observations, and assimilation system of ERA5 in addition to improved resolution. A comparison of two Lagrangian trajectory models allowed us to assess the readiness of the codes and workflows to handle the comprehensive ERA5 data and to demonstrate the consistency of the simulation results. Our results will help to guide future Lagrangian transport studies attempting to navigate the increased computational complexity and leverage the considerable benefits and improvements of ECMWF's new ERA5 data set.

[1] To assess the impact of the vertical velocity scheme on modeling transport in the tropical tropopause layer (TTL), 3 month backward trajectories are initialized in the TTL for boreal winter and summer 2002. The calculations are done in either a kinematic scenario with pressure tendency as the vertical velocity or in a diabatic scenario with cross-isentropic velocity deduced from various diabatic heating rates due to radiation (clear sky, all sky) and latent, diffusive and turbulent heating. This work provides a guideline for assessing the sensitivity of trajectory and chemical transport model (CTM) results on the choice of the vertical velocity scheme. We find that many transport characteristics, such as time scales, pathways and dispersion, crucially depend on the vertical velocity scheme. The strongest tropical upwelling results from the operational European Centre for Medium-Range Weather Forecasts kinematic scenario with the time scale for ascending from 340 to 400 K of 1 month. For the ERA-Interim kinematic and total diabatic scenarios, this time scale is about 2 months, and for the all-sky scenario it is as long as 2.5 months. In a diabatic scenario, the whole TTL exhibits mean upward motion, whereas in a kinematic scenario, regions of subsidence occur in the upper TTL. However, some transport characteristics robustly emerge from the different scenarios, such as an enhancement of residence times between 350 and 380 K and a strong impact of meridional in-mixing from the extratropics on the composition of the TTL. Moreover, an increase of meridionally transported air from the summer hemisphere into the TTL (maximum for boreal summer) is found as an invariant feature among all the scenarios.

Abstract. Variations in the mixing ratio of trace gases of tropospheric origin entering the stratosphere in the tropics are of interest for assessing both troposphere to stratosphere transport fluxes in the tropics and the impact of these transport fluxes on the composition of the tropical lower stratosphere. Anomaly patterns of carbon monoxide (CO) and long-lived tracers in the lower tropical stratosphere allow conclusions about the rate and the variability of tropical upwelling to be drawn. Here, we present a simplified chemistry scheme for the Chemical Lagrangian Model of the Stratosphere (CLaMS) for the simulation, at comparatively low numerical cost, of CO, ozone, and long-lived trace substances (CH4, N2O, CCl3F (CFC-11), CCl2F2 (CFC-12), and CO2) in the lower tropical stratosphere. For the long-lived trace substances, the boundary conditions at the surface are prescribed based on ground-based measurements in the lowest model level. The boundary condition for CO in the lower troposphere (below about 4 km) is deduced from MOPITT measurements. Due to the lack of a specific representation of mixing and convective uplift in the troposphere in this model version, enhanced CO values, in particular those resulting from convective outflow are underestimated. However, in the tropical tropopause layer and the lower tropical stratosphere, there is relatively good agreement of simulated CO with in situ measurements (with the exception of the TROCCINOX campaign, where CO in the simulation is biased low ≈10–15 ppbv). Further, the model results (and therefore also the ERA-Interim winds, on which the transport in the model is based) are of sufficient quality to describe large scale anomaly patterns of CO in the lower stratosphere. In particular, the zonally averaged tropical CO anomaly patterns (the so called "tape recorder" patterns) simulated by this model version of CLaMS are in good agreement with observations, although the simulations show a too rapid upwelling compared to observations as a consequence of the overestimated vertical velocities in the ERA-Interim reanalysis data set. Moreover, the simulated tropical anomaly patterns of N2O are in good agreement with observations. In the simulations, anomaly patterns of CH4 and CFC-11 were found to be very similar to those of N2O; for all long-lived tracers, positive anomalies are simulated because of the enhanced tropical upwelling in the easterly shear phase of the quasi-biennial oscillation.

Abstract. During the second part of the TROCCINOX campaign that took place in Brazil in early 2005, chemical species were measured on-board the high-altitude research aircraft Geophysica (ozone, water vapor, NO, NO y , CH 4 and CO) in the altitude range up to 20 km (or up to 450 K potential temperature), i.e. spanning the entire TTL region roughly extending between 350 and 420 K.Here, analysis of transport across the TTL is performed using a new version of the Chemical Lagrangian Model of the Stratosphere (CLaMS). In this new version, the stratospheric model has been extended to the earth surface. Above the tropopause, the isentropic and cross-isentropic advection in CLaMS is driven by meteorological analysis winds and heating/cooling rates derived from a radiation calculation. Below the tropopause, the model smoothly transforms from the isentropic to the hybrid-pressure coordinate and, in this way, takes into account the effect of large-scale convective transport as implemented in the vertical wind of the meteorological analysis. As in previous CLaMS simulations, the irreversible transport, i.e. mixing, is controlled by the local horizontal strain and vertical shear rates.Stratospheric and tropospheric signatures in the TTL can be seen both in the observations and in the model. The composition of air above ≈350 K is mainly controlled by mixing on a time scale of weeks or even months. Based on CLaMS transport studies where mixing can be completely switched off, we deduce that vertical mixing, mainly driven by the vertical shear in the tropical flanks of the subtropical jets and, Correspondence to: P. Konopka (p.konopka@fz-juelich.de) to some extent, in the the outflow regions of the large-scale convection, offers an explanation for the upward transport of trace species from the main convective outflow at around 350 K up to the tropical tropopause around 380 K.

Abstract. Enhanced tropospheric trace gases such as CO, CH4 and H2O and reduced stratospheric O3 were measured in situ in the lowermost stratosphere over northern Europe on 26 September 2012 during the TACTS aircraft campaign. The measurements indicate that these air masses clearly differ from the stratospheric background. The calculation of 40-day backward trajectories with the trajectory module of the CLaMS model shows that these air masses are affected by the Asian monsoon anticyclone. Some air masses originate from the boundary layer in Southeast Asia/West Pacific and are rapidly lifted (1–2 days) within a typhoon up to the outer edge of the Asian monsoon anticyclone. Afterwards, the air parcels are entrained by the anticyclonic circulation of the Asian monsoon. The subsequent long-range transport (8–14 days) of enhanced water vapour and pollutants to the lowermost stratosphere in northern Europe is driven by eastward transport of tropospheric air from the Asian monsoon anticyclone caused by an eddy shedding event. We found that the combination of rapid uplift by a typhoon and eastward eddy shedding from the Asian monsoon anticyclone is a novel fast transport pathway that may carry boundary emissions from Southeast Asia/West Pacific within approximately 5 weeks to the lowermost stratosphere in northern Europe.