Abstract. Stratosphere–troposphere exchange within extratropical cyclones provides the potential for anthropogenic and natural surface emissions to rapidly reach the stratosphere as well as for ozone from the stratosphere to penetrate deep into the troposphere, even down into the boundary layer. The efficiency of this process directly influences the surface climate, the chemistry in the stratosphere, the chemical composition of the extratropical transition layer, and surface pollution levels. Here, we present evidence for a mixing process within extratropical cyclones which has gained only a small amount of attention so far and which fosters the transport of tropospheric air masses into the stratosphere in ridges of baroclinic waves. We analyzed airborne measurement data from a research flight of the WISE (Wave-driven ISentropic Exchange) campaign over the North Atlantic in autumn 2017, supported by forecasts from a numerical weather prediction model and trajectory calculations. Further detailed process understanding is obtained from experiments of idealized baroclinic life cycles. The major outcome of this analysis is that air masses mix in the region of the tropopause and potentially enter the stratosphere in ridges of baroclinic waves at the anticyclonic side of the jet without changing their potential temperature drastically. This quasi-isentropic exchange occurs above the outflow of warm conveyor belts, in regions which exhibit enhanced static stability in the lower stratosphere and a Kelvin–Helmholtz instability across the tropopause. The enhanced static stability is related to radiative cooling below the tropopause and the presence of small-scale waves. The Kelvin–Helmholtz instability is related to vertical shear of the horizontal wind associated with small-scale waves at the upper edge of the jet stream. The instability leads to the occurrence of turbulence and consequent mixing of trace gases in the tropopause region. While the overall relevance of this process has yet to be assessed, it has the potential to significantly modify the chemical composition of the extratropical transition layer in the lowermost stratosphere in regions which have previously gained a small amount of attention in terms of mixing in baroclinic waves.

Abstract. Stratospheric inorganic chlorine (Cly) is predominantly released from long-lived chlorinated source gases and, to a small extent, very short-lived chlorinated substances. Cly includes the reservoir species (HCl and ClONO2) and active chlorine species (i.e., ClOx). The active chlorine species drive catalytic cycles that deplete ozone in the polar winter stratosphere. This work presents calculations of inorganic chlorine (Cly) derived from chlorinated source gas measurements on board the High Altitude and Long Range Research Aircraft (HALO) during the Southern Hemisphere Transport, Dynamic and Chemistry (SouthTRAC) campaign in austral late winter and early spring 2019. Results are compared to Cly in the Northern Hemisphere derived from measurements of the POLSTRACC-GW-LCYCLE-SALSA (PGS) campaign in the Arctic winter of 2015/2016. A scaled correlation was used for PGS data, since not all source gases were measured. Using the SouthTRAC data, Cly from a scaled correlation was compared to directly determined Cly and agreed well. An air mass classification based on in situ N2O measurements allocates the measurements to the vortex, the vortex boundary region, and midlatitudes. Although the Antarctic vortex was weakened in 2019 compared to previous years, Cly reached 1687±19 ppt at 385 K; therefore, up to around 50 % of total chlorine was found in inorganic form inside the Antarctic vortex, whereas only 15 % of total chlorine was found in inorganic form in the southern midlatitudes. In contrast, only 40 % of total chlorine was found in inorganic form in the Arctic vortex during PGS, and roughly 20 % was found in inorganic form in the northern midlatitudes. Differences inside the two vortices reach as much as 540 ppt, with more Cly in the Antarctic vortex in 2019 than in the Arctic vortex in 2016 (at comparable distance to the local tropopause). To our knowledge, this is the first comparison of inorganic chlorine within the Antarctic and Arctic polar vortices. Based on the results of these two campaigns, the differences in Cly inside the two vortices are substantial and larger than the inter-annual variations previously reported for the Antarctic.

<p>The tropopause acts as a transport barrier between the upper troposphere and the lower stratosphere. Non-conservative (i.e. PV changing) processes are required to overcome this barrier. Orographically generated gravity waves (i.e. mountain waves) can potentially lead to cross-isentropic fluxes of trace gases via the generation of turbulence. Thus they may alter the isentropic gradient of these trace species across the tropopause.<br>The specific goal of this study is to identify cross-isentropic mixing processes at the tropopause based on the distribution of trace gases (i.e. tracer-tracer correlations). Based on airborne in-situ trace gas measurements of CO and N<sub>2</sub>O during the DEEPWAVE (Deep Propagating Gravity Wave Experiment) campaign in July 2014 we identified mixing regions above the Southern Alps during periods of gravity wave activity. These in-situ data show that the composition of the air above the Southern Alps change from the upstream to the leeward side of the mountains indicating cross isentropic mixing of trace gases in the region of gravity wave activity.<br>We complement our analysis of the measurement data with high resolution operational analysis data from the ECMWF (European Centre for Medium-Range Weather Forecasts). Furthermore, using potential vorticity and stability parameters.<br>Using 3D wind fields, data form Graphical Turbulence Guidance (GTG) system and in-situ measurements of the vertical wind we identify occurrence of turbulence in the region of mixing events. Using wavelet analysis, we could identify the spatial and temporal scales of local trace gas fluxes. We also give estimates of cross-isentropic flux, i.e. we want to quantify the mixing in terms of exchange.</p>

Abstract. Orographic gravity waves (i.e., mountain waves) can potentially lead to cross-isentropic fluxes of trace gases via the generation of turbulence. During the DEEPWAVE (Deep Propagating Gravity Wave Experiment) campaign in July 2014, we performed tracer measurements of carbon monoxide (CO) and nitrous oxide (N2O) above the Southern Alps during periods of gravity wave activity. The measurements were taken along two stacked levels at 7.9 km in the troposphere and 10.9 km in the stratosphere. A detailed analysis of the observed wind components shows that both flight legs were affected by vertically propagating gravity waves with momentum deposition and energy dissipation between the two legs. Corresponding tracer measurements indicate turbulent mixing in the region of gravity wave occurrence. For the stratospheric data, we identified mixing leading to a change of the cross-isentropic tracer gradient of N2O from the upstream to the downstream region of the Southern Alps. Based on the quasi-inert tracer N2O, we identified two distinct layers in the stratosphere with different chemical composition on different isentropes as given by constant potential temperature Θ. The CO–N2O relationship clearly indicates that irreversible mixing between these two layers occurred. Further, we found a significant change of the vertical profiles of N2O with respect to Θ from the upstream to the downstream side above the Southern Alps just above the tropopause. A scale-dependent gradient analysis reveals that this cross-isentropic gradient change of N2O is triggered in the region of gravity wave occurrence. The power spectra of the in situ measured vertical wind, Θ, and N2O indicate the occurrence of turbulence above the mountains associated with the gravity waves in the stratosphere. The estimated eddy dissipation rate (EDR) based on the measured three-dimensional wind indicates a weak intensity of turbulence in the stratosphere above the mountain ridge. The Θ–N2O relation downwind of the Alps modified by the gravity wave activity provides clear evidence that trace gas fluxes, which were deduced from wavelet co-spectra of vertical wind and N2O, are at least in part cross-isentropic. Our findings thus indicate that orographic waves led to turbulent mixing on both flight legs in the troposphere and in the stratosphere. Despite only weak turbulence during the stratospheric leg, the cross-isentropic gradient and the related composition change on isentropic surfaces from upstream to downstream of the mountain unambiguously conserves the effect of turbulent mixing by gravity wave activity on the trace gas distribution prior to the measurements. This finally leads to irreversible trace gas fluxes across isentropes and thus has a persistent effect on the upper troposphere and lower stratosphere (UTLS) trace gas composition.

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