This study investigates the origin of the zonal asymmetry in stratospheric ozone trends at northern high latitudes, identified in satellite limb observations over the past two decades. We use a merged dataset consisting of ozone profiles retrieved at the University of Bremen from SCIAMACHY and OMPS-LP measurements to derive ozone trends. We also use TOMCAT chemical transport model (CTM) simulations, forced by ERA5 reanalyses, to investigate the factors which determine the asymmetry observed in the long-term changes. By studying seasonally and longitudinally resolved observation-based ozone trends, we find, especially during spring, a well-pronounced asymmetry at polar latitudes, with values up to +6 % per decade over Greenland and -5 % per decade over western Russia. The control CTM simulation agrees well with these observed trends, whereas sensitivity simulations indicate that chemical mechanisms, involved in the production and removal of ozone, or their changes, are unlikely to explain the observed behaviour. The decomposition of TOMCAT ozone time series and of ERA5 geopotential height into the first two wavenumber components shows a clear correlation between the two variables in the middle stratosphere and demonstrates a weakening and a shift in the wavenumber-1 planetary wave activity over the past two decades. Finally, the analysis of the polar vortex position and strength points to a decadal oscillation with a reversal pattern at the beginning of the century, also found in the ozone trend asymmetry. This further stresses the link between changes in the polar vortex position and the identified ozone trend pattern.

We present a comparison of atmospheric transport models that simulate carbonyl sulfide (COS). This is part II of the ongoing Atmospheric Transport Model (ATM) Inter-comparison Project (TransCom–COS). Differently from part I, we focus on seven model intercomparison by transporting two recent COS inversions of NOAA surface data within TM5-4DVAR and LMDz models. The main goals of TransCom-COS part II are (a) to compare the COS simulations using the two sets of optimized fluxes with simulations that use a control scenario (part I) and (b) to evaluate the simulated tropospheric COS abundance with aircraft-based observations from various sources. The output of the seven transport models are grouped in terms of their vertical mixing strength: strong and weak mixing. The results indicate that all transport models capture the meridional distribution of COS at the surface well. Model simulations generally match the aircraft campaigns HIPPO and ATom. Comparisons to HIPPO and ATom demonstrate a gap between observed and modelled COS over the Pacific Ocean at 0–40N, indicating a potential missing source in the free troposphere. The effects of seasonal continental COS uptake by the biosphere, observed on HIPPO and ATom over oceans, is well reproduced by the simulations. We found that the strength of the vertical mixing within the column as represented in the various atmospheric transport models explains much of the model to model differences. We also found that weak-mixing models transporting the optimized flux derived from the strong-mixing TM5 model show a too strong seasonal cycle at high latitudes.

In the winter and spring of 2019/2020, the unusually cold, strong, and stable polar vortex created favorable conditions for ozone depletion in the Arctic. Chemical ozone loss started earlier than in any previous year in the satellite era, and continued until the end of March, resulting in the unprecedented reduction of the ozone column. The vortex was located above the Polar Environment Atmospheric Research Laboratory in Eureka, Canada (80 °N, 86 °W) from late February to the end of April, presenting an excellent opportunity to examine ozone loss from a single ground station. Measurements from a suite of instruments show that total column ozone in 2020 was at an all-time low in the 20-year dataset, 22 to 102 DU below previous records set in 2011. Ozone minima (<200 DU), enhanced OClO and BrO slant columns, and unusually low HCl, ClONO2 , and HNO3 columns were observed in March. Polar stratospheric clouds were present as late as 20 March, and ozonesondes show unprecedented depletion in the March and April ozone profiles (to <0.2 ppmv). While both chemical and dynamical factors lead to reduced ozone when the vortex is cold, the contribution of chemical depletion was exceptional in spring 2020 when compared to typical Arctic winters. The mean chemical ozone loss over Eureka was estimated to be 111-127 DU (27-31%) using April measurements and passive ozone from the SLIMCAT chemical transport model. While absolute ozone loss was generally smaller in 2020 than in 2011, percentage ozone loss was greater in 2020.

We use a 3-D chemical transport model and satellite observations to investigate Arctic ozone depletion in winter/spring 2019/20 and compare with earlier years. Persistently low temperatures caused extensive chlorine activation through to March. March-mean polar-cap-mean modelled chemical column ozone loss reached 78 DU (local maximum loss of ~108 DU in the vortex), similar to that in 2011. However, weak dynamical replenishment of only 59 DU from December to March was key to producing very low (<220 DU) column ozone values. The only other winter to exhibit such weak transport in the past 20 years was 2010/11, so this process is fundamental to causing such low ozone values. A model simulation with peak observed stratospheric total chlorine and bromine loading (from the mid-1990s) shows that gradual recovery of the ozone layer over the past two decades ameliorated the polar cap ozone depletion in March 2020 by ~20 DU.

Satellite observations of relevant trace gases, together with meteorological data from ERA5, were used to describe the dynamics and chemistry of the spectacular Arctic 2019/20 winter/spring season. Exceptionally low total ozone values of slightly less than 220 DU were observed in mid March within an unusually large stratospheric polar vortex. This was associated with very low temperatures and extensive polar stratospheric cloud formation, a prerequisite for substantial springtime ozone depletion. Very high OClO and very low NO2 column amounts observed by GOME-2A are indicative of unusually large active chlorine levels and significant denitrification, which likely contributed to large chemical ozone loss. Using results from the TOMCAT chemical transport model (CTM) and ozone observations from S5P/TROPOMI, GOME-2 (total column), SCIAMACHY and OMPS-LP (vertical profiles) chemical ozone loss was evaluated and compared with the previous record Arctic winter 2010/11. The polar-vortex-averaged total column ozone loss in 2019/20 reached 88 DU (23%) and 106~DU (28%) based upon observations and model, respectively, by the end of March, which was similar to that derived for 2010/11. The total column ozone loss is in agreement with OMPS-LP-derived partial column loss between 350 K and 550 K to within the uncertainty. The maximum ozone loss (~80%) observed by OMPS-LP was near the 450 K potential temperature level (~18 km altitude). Because of the larger polar vortex area in March 2020 compared to March 2011 (about 25% at 450 K), ozone mass loss was larger in Arctic winter 2019/20.

We present a comparison of atmospheric transport model simulations for carbonyl sulfide (COS), within the framework of the ongoing atmospheric tracer transport model intercomparison project “TransCom”. Seven atmospheric transport models participated in the inter-comparison experiment and provided simulations of COS mixing ratios in the troposphere over a 9-year period (2010–2018), using prescribed state-of-the-art surface fluxes for various components of the atmospheric COS budget: biospheric sink, oceanic source, sources from fire and industry. Since the biosphere is the largest sink of COS, we tested sink estimates produced by two different biosphere models. The main goals of TransCom-COS are (a) to investigate the impact of the transport uncertainty and emission distribution in simulating the spatio-temporal variability of COS mixing ratios in the troposphere, and (b) to assess the sensitivity of simulated tropospheric COS mixing ratios to the seasonal and diurnal variability of the COS biosphere fluxes. To this end, a control case with state-of-the-art seasonal fluxes of COS was constructed. Models were run with the same fluxes and without chemistry to isolate transport differences. Further, two COS flux scenarios were compared: one using a biosphere flux with a monthly time resolution and the other using a biosphere flux with a three-hourly time resolution. In addition, we investigated the sensitivity of the simulated concentrations to different biosphere fluxes and to indirect oceanic emissions through dimethylsulfide (DMS) and carbon disulfide (CS2). The modelled COS mixing ratios were assessed against in-situ observations from surface stations and aircraft.

The 2019/2020 Australian wildfires emitted large quantities of atmospheric pollutant gases and aerosols. Using state-of-the-art near-real-time satellite measurements of tropospheric composition, we present an analysis of several emitted trace gases and their long-range transport, and compare to the previous (2018/2019) fire season. Observations of carbon monoxide (CO) show that fire emissions were so intense that the distinct Australian fire plume managed to circumnavigate the Southern Hemisphere (SH) within a few weeks, with eastward propagation over the South Pacific, South America, the South Atlantic, Africa and the Indian Ocean. Elevated atmospheric methane levels were also detected in January 2020 fire plumes over the Pacific, defined using CO as a plume tracer, even though sampling was restricted spatially by aerosols and clouds. Observations also show significant enhancements of methanol from the fires, where CH3OH:CO enhancement ratios increased within the aged plume downwind over the South Pacific indicating secondary in-plume CH3OH formation.