Abstract. Analysis of stratospheric transport from an observational point of view is frequently realized by evaluation of the mean age of air values from long-lived trace gases. However, this provides more insight into general transport strength and less into its mechanism. Deriving complete transit time distributions (age spectra) is desirable, but their deduction from direct measurements is difficult. It is so far primarily based on model work. This paper introduces a modified version of an inverse method to infer age spectra from mixing ratios of short-lived trace gases and investigates its basic principle in an idealized model simulation. For a full description of transport seasonality the method includes an imposed seasonal cycle to gain multimodal spectra. An ECHAM/MESSy Atmospheric Chemistry (EMAC) model simulation is utilized for a general proof of concept of the method and features an idealized dataset of 40 radioactive trace gases with different chemical lifetimes as well as 40 chemically inert pulsed trace gases to calculate pulse age spectra. It is assessed whether the modified inverse method in combination with the seasonal cycle can provide matching age spectra when chemistry is well-known. Annual and seasonal mean inverse spectra are compared to pulse spectra including first and second moments as well as the ratio between them to assess the performance on these timescales. Results indicate that the modified inverse age spectra match the annual and seasonal pulse age spectra well on global scale beyond 1.5 years of mean age of air. The imposed seasonal cycle emerges as a reliable tool to include transport seasonality in the age spectra. Below 1.5 years of mean age of air, tropospheric influence intensifies and breaks the assumption of single entry through the tropical tropopause, leading to inaccurate spectra, in particular in the Northern Hemisphere. The imposed seasonal cycle wrongly prescribes seasonal entry in this lower region and does not lead to a better agreement between inverse and pulse age spectra without further improvement. Tests with a focus on future application to observational data imply that subsets of trace gases with 5 to 10 species are sufficient for deriving well-matching age spectra. These subsets can also compensate for an average uncertainty of up to ±20 % in the knowledge of chemical lifetime if a deviation of circa ±10 % in modal age and amplitude of the resulting spectra is tolerated.

Abstract. We present novel measurements of five short-lived brominated source gases (CH2Br2, CHBr3, CH2ClBr, CHCl2Br and CHClBr2). These rather short-lived gases are an important source of bromine to the stratosphere, where they can lead to depletion of ozone. The measurements have been obtained using an in situ gas chromatography and mass spectrometry (GC–MS) system on board the High Altitude and Long Range Research Aircraft (HALO). The instrument is extremely sensitive due to the use of chemical ionization, allowing detection limits in the lower parts per quadrillion (ppq, 10−15) range. Data from three campaigns using HALO are presented, where the upper troposphere and lower stratosphere (UTLS) of the northern hemispheric mid-to-high latitudes were sampled during winter and during late summer to early fall. We show that an observed decrease with altitude in the stratosphere is consistent with the relative lifetimes of the different compounds. Distributions of the five source gases and total organic bromine just below the tropopause show an increase in mixing ratio with latitude, in particular during polar winter. This increase in mixing ratio is explained by increasing lifetimes at higher latitudes during winter. As the mixing ratios at the extratropical tropopause are generally higher than those derived for the tropical tropopause, extratropical troposphere-to-stratosphere transport will result in elevated levels of organic bromine in comparison to air transported over the tropical tropopause. The observations are compared to model estimates using different emission scenarios. A scenario with emissions mainly confined to low latitudes cannot reproduce the observed latitudinal distributions and will tend to overestimate organic bromine input through the tropical tropopause from CH2Br2 and CHBr3. Consequently, the scenario also overestimates the amount of brominated organic gases in the stratosphere. The two scenarios with the highest overall emissions of CH2Br2 tend to overestimate mixing ratios at the tropical tropopause, but they are in much better agreement with extratropical tropopause mixing ratios. This shows that not only total emissions but also latitudinal distributions in the emissions are of importance. While an increase in tropopause mixing ratios with latitude is reproduced with all emission scenarios during winter, the simulated extratropical tropopause mixing ratios are on average lower than the observations during late summer to fall. We show that a good knowledge of the latitudinal distribution of tropopause mixing ratios and of the fractional contributions of tropical and extratropical air is needed to derive stratospheric inorganic bromine in the lowermost stratosphere from observations. In a sensitivity study we find maximum differences of a factor 2 in inorganic bromine in the lowermost stratosphere from source gas injection derived from observations and model outputs. The discrepancies depend on the emission scenarios and the assumed contributions from different source regions. Using better emission scenarios and reasonable assumptions on fractional contribution from the different source regions, the differences in inorganic bromine from source gas injection between model and observations is usually on the order of 1 ppt or less. We conclude that a good representation of the contributions of different source regions is required in models for a robust assessment of the role of short-lived halogen source gases on ozone depletion in the UTLS.

Abstract. Derivation of mean age of air (AoA) and age spectra from atmospheric measurements remains a challenge and often requires output from atmospheric models. This study tries to minimize the direct influence of model output and presents an extension and application of a previously established inversion method to derive age spectra from mixing ratios of long- and short-lived trace gases. For a precise description of cross-tropopause transport processes, the inverse method is extended to incorporate air entrainment into the stratosphere across the tropical and extratropical tropopause. We first use simulations with the Chemical Lagrangian Model of the Stratosphere (CLaMS) to provide a general proof of concept of the extended principle in a controllable and consistent environment, where the method is applied to an idealized set of 10 trace gases with predefined constant lifetimes and compared to reference model age spectra. In the second part of the study we apply the extended inverse method to atmospheric measurements of multiple long- and short-lived trace gases measured aboard the High Altitude and Long Range (HALO) research aircraft during the two research campaigns POLSTRACC–GW-LCYCLE–SALSA (PGS) and Wave-driven Isentropic Exchange (WISE). As some of the observed species undergo significant loss processes in the stratosphere, a Monte Carlo simulation is introduced to retrieve age spectra and chemical lifetimes in stepwise fashion and to account for the large uncertainties. Results show that in the idealized model scenario the inverse method retrieves age spectra robustly on annual and seasonal scales. The extension to multiple entry regions proves reasonable as our CLaMS simulations reveal that in the model between 50 % and 70 % of air in the lowermost stratosphere has entered through the extratropical tropopause (30–90∘ N and S) on annual average. When applied to observational data of PGS and WISE, the method derives age spectra and mean AoA with meaningful spatial distributions and quantitative range, yet large uncertainties. Results indicate that entrainment of fresh tropospheric air across both the extratropical and tropical tropopause peaked prior to both campaigns, but with lower mean AoA for WISE than PGS data. The ratio of moments for all retrieved age spectra for PGS and WISE is found to range between 0.52 and 2.81 years. We conclude that the method derives reasonable and consistent age spectra using observations of chemically active trace gases. Our findings might contribute to an improved assessment of transport with age spectra in future studies.

Abstract. Inter-hemispheric transport may strongly affect the trace gas composition of the atmosphere, especially in relation to anthropogenic emissions which originate mainly in the Northern Hemisphere. This study investigates the transport from the boundary surface layer of the Northern Hemispheric (NH) extratropics (30–90° N), Southern Hemispheric (SH) extratropics (30–90° S), and tropics (30° S–30° N) into the global upper troposphere and lower stratosphere (UTLS) using simulations with the Chemical Lagrangian Model of the Stratosphere (CLaMS). In particular, we diagnose inter-hemispheric transport in terms of the air mass fractions (AMF), age spectra, and the mean age of air (AoA) calculated for these three source regions. We find that the AMFs from the NH extratropics to the UTLS are about five times larger than the corresponding contributions from the SH extratropics and almost twenty times smaller than those from the tropics. The amplitude of the AMF seasonal variability originating from the NH extratropics is comparable to that from the tropics. The NH and SH extratropics age spectra show much stronger seasonality compared to the seasonality of the tropical age spectra. The transit time of NH extratropical origin air to the SH extratropics is longer than vice versa. The asymmetry of the inter-hemispheric transport is mainly driven by the Asian summer monsoon (ASM). Both ASM and westerly ducts affect the cross hemispheric transport of the NH extratropical air to the SH, and it is an interplay between the ASM and westerly ducts which triggers such cross-equator transport from boreal summer to fall, mainly westerly ducts over the eastern Atlantic.

Abstract. Inter-hemispheric transport may strongly affect the trace gas composition of the atmosphere, especially in relation to anthropogenic emissions, which originate mainly in the Northern Hemisphere. This study investigates the transport from the boundary surface layer of the northern hemispheric (NH) extratropics (30–90∘ N), southern hemispheric (SH) extratropics (30–90∘ S), and tropics (30∘ S–30∘ N) into the global upper troposphere and lower stratosphere (UTLS) using simulations with the Chemical Lagrangian Model of the Stratosphere (CLaMS). In particular, we diagnose inter-hemispheric transport in terms of the air mass fractions (AMFs), age spectra, and the mean age of air (AoA) calculated for these three source regions. We find that the AMFs from the NH extratropics to the UTLS are about 5 times larger than the corresponding contributions from the SH extratropics and almost 20 times smaller than those from the tropics. The amplitude of the AMF seasonal variability originating from the NH extratropics is comparable to that from the tropics. The NH and SH extratropical age spectra show much stronger seasonality compared to the seasonality of the tropical age spectra. The transit time of NH-extratropical-origin air to the SH extratropics is longer than vice versa. The asymmetry of the inter-hemispheric transport is mainly driven by the Asian summer monsoon (ASM). We confirm the important role of ASM and westerly ducts in the inter-hemispheric transport from the NH extratropics to the SH. Furthermore, we find that it is an interplay between the ASM and westerly ducts which triggers such cross-Equator transport from boreal summer to fall in the UTLS between 350 and 370 K.