Organic and inorganic bromine measurements around the extratropical tropopause and lowermost stratosphere (Ex-LMS): Insights into transport pathways and total bromine

<p>We report on measurements of total bromine (Br<sup>tot</sup>) in the upper troposphere and lower stratosphere (UTLS) taken from the German High Altitude and LOng range research aircraft (HALO) over the North Atlantic, Norwegian Sea and north-western Europe in September/ October 2017 during the WISE (Wave-driven ISentropic Exchange) research campaign. Br<sup>tot</sup> is calculated from measured total organic bromine (Br<sup>org</sup>) (i.e., the sum of bromine contained in CH<sub>3</sub>Br, the halons and the major very short-lived brominated substances) added to inorganic bromine (Br<sub>y</sub><sup>inorg</sup>), evaluated from measured BrO and photochemical modelling. Combining these data, the weighted mean [Br<sup>tot</sup>] is 19.2 ± 1.2 ppt in the extratropical lower stratosphere (Ex-LS) of the northern hemisphere. The inferred average Br<sup>tot</sup> for the Ex-LS is slightly smaller than expected for the middle stratosphere in 2016 (~19.6 ppt (ranging from 19-20 ppt) as reported by the WMO/UNEP Assessment (2018)). However, it reflects the expected variability in Br<sup>tot</sup> in the Ex-LS due to influxes of shorter lived brominated source and product gases from different regions of entry. A closer look into Br<sup>org</sup> and Br<sub>y</sub><sup>inorg</sup> as well as simultaneously measured transport tracers (CO, N<sub>2</sub>O, ...) and an air mass lag-time tracer (SF<sub>6</sub>), suggests that a filament of air with elevated Br<sup>tot</sup> protruded into the extratropical lowermost stratosphere (Ex-LMS) from 350-385 K and between equivalent latitudes of 55-80˚N (high bromine filament – HBrF). Lagrangian transport modelling shows the multi-pathway contributions to Ex-LMS bromine. According to CLaMS air mass origin simulations, contributions to the HBrF consist of predominantly isentropic transport from the tropical troposphere (also with elevated [Br<sup>tot</sup>] = 21.6 ± 0.7 ppt) as well as a smaller contribution from an exchange across the extratropical tropopause which are mixed into the stratospheric background air. In contrast, the surrounding LS above and below the HBrF has less tropical tropospheric air, but instead additional stratospheric background air. Of the tropical tropospheric air in the HBrF, the majority is from the outflow of the Asian monsoon anticyclone and the adjacent tropical regions, which greatly influences concentrations of trace gases transported into the Ex-LMS in boreal summer and fall. The resulting increase of Br<sup>tot</sup> in the Ex-LMS and its consequences for ozone is investigated through the TOMCAT/SLIMCAT model simulations. However, more extensive monitoring of total stratospheric bromine in more aged air (i.e., in the middle stratosphere) as well as globally and seasonally is required in addition to model simulations to fully understand its impact on Ex-LMS ozone and the radiative forcing of climate.</p>

The leading modes of NH extratropical tropopause variability and their connection with stratosphere-troposphere variability

The leading modes of Northern Hemisphere tropopause variability for November–April (1979/1980–2018/2019) and the associated stratosphere-troposphere variability were analyzed based on the NCEP and ERA interim reanalysis products. For this, cyclostationary empirical orthogonal function technique is employed. The first two modes feature the intraseasonal evolution of tropopause pressure anomalies over the Arctic, which respond directly to stratospheric temperature fluctuations in association with stratospheric polar vortex variations. These two modes reflect the link between stratospheric polar vortex strength and high-latitude tropospheric circulation. The first mode represents a single-phase fluctuation of the stratospheric polar vortex from winter to early spring. The second mode describes a two-phase fluctuation of the stratospheric vortex with opposite signs in winter and in spring. Tropopause pressure anomalies near the mid-latitude tropospheric jet regions exhibit significant zonal variation. In the first mode, in particular, these mid-latitude tropopause anomalies are linked to asymmetric jet variations in the Atlantic and the Pacific regions. In regard to the Northern Annular mode, distinct vertical evolution structures of the two modes are practically related to the varying evolutionary structure of extreme vortex events with relatively long persistence.

Variations in the Frequency of Stratospheric Sudden Warmings in CMIP5 and CMIP6 and Possible Causes

The climatological frequency of stratospheric sudden warming events (SSWs) is an important dynamical characteristic of the extratropical stratosphere. However, modern climate models have difficulties in simulating this frequency, with many models either considerably under- or overestimating the observational estimates. Past research has found that models with a higher upper lid tend to simulate a higher and more realistic number of SSWs. The present study revisits this issue and investigates causes for biases in the simulated SSW frequency from the CMIP5 and CMIP6 models. It is found that variations in the frequency are closely related to 1) the strength of the polar vortex and 2) the upward-propagating wave activity in the stratosphere. While it is difficult to explain the variations in the polar vortex strength from the available model output, the stratospheric wave activity is influenced by different aspects of the climatological mean state of the atmosphere in the lower stratosphere. We further find that models with a finer vertical resolution in the stratosphere are overall more realistic: vertical resolution is associated with a smaller cold bias above the extratropical tropopause, more upward-propagating wave activity in the lower stratosphere, and a higher frequency of SSWs. We conclude that not only a high model lid but also a fine vertical resolution in the stratosphere is important for simulating the dynamical variability of the stratosphere.

A convolution of observational and model data to estimate age of air spectra in the northern hemispheric lower stratosphere

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.

Bromine from short-lived source gases in the extratropical northern hemispheric upper troposphere and lower stratosphere (UTLS)

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.

Characterizing Extratropical Tropopause Bimodality and its Relationship to the Occurrence of Double Tropopauses Using COSMIC GPS Radio Occultation Observations

Lapse rate tropopause (LRT) heights in the extratropics have been shown to display a bimodal distribution, with one modal maxima above 15 km (typical of the tropical tropopause) and the other below 13 km (typical of the extratropical tropopause). The climatology of the tropopause is studied by characterizing tropopause bimodality and how it relates to the occurrence of double tropopauses (DTs). LRT heights are derived from Constellation Observing System for Meteorology, Ionosphere, and Climate (COSMIC) GPS Radio Occultation temperature profiles from 2006 to 2017. Tropopause bimodality occurs most frequently within a subtropical band (20°–40°) in both hemispheres. A distinct seasonality is observed as bimodality occurs most frequently in winter except for another local maximum along the northern edge of the Asian summer monsoon. The regions with a bimodal height distribution nearly overlap the regions that experience a high frequency of DTs. DTs occur most frequently in winter (50%–70% of the time) along the poleward edge of the bimodal band, and most LRT heights are within the extratropical mode (>80%), whereas DT occurrence decreases quickly toward the equatorward edge (<20%) along with fewer LRT heights in the extratropical mode (<50%). These results indicate that LRT height bimodality occurs along the equatorward edge due to the occurrences of double tropopauses, while the poleward edge is due to single tropopause profiles that are more tropical in nature.

A convolution of observational and model data to estimate age of air spectra in the northern hemispheric lower stratosphere

Derivation of mean age of air (AoA) and age spectra from atmospheric measurements remains a challenge and often requires data from atmospheric models. This study tries to minimize the direct influence of model data 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 ten 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 scale. 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/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 extratropical and tropical tropopause has peaked prior to both campaigns, but with lower mean AoA for WISE than PGS data. For a full assessment the ratio of moments for all retrieved age spectra is evaluated and found to range between 0.52 years and 2.81 years for PGS and WISE. It is concluded 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.

Variations in The Frequency of Sudden Stratospheric Warmings in CMIP5 and CMIP6

&lt;p&gt;The frequency of sudden stratospheric warming events (SSWs) is an essential characteristic of the coupled stratosphere-troposphere system. This study is motivated by the fact that many of the CMIP5 and CMIP6 climate models considerably over- or underestimate the observed SSW frequency. The goal is to understand the causes for the large intermodel spread in the number of SSWs and relate it to specific model configurations. To this end, various dynamical quantities associated with the simulation of SSWs are investigated. It is found that variations in the SSW frequency are closely related to the strength of the polar vortex and the stratospheric wave activity. While it is difficult to explain the variations in the strength of the polar vortex, the stratospheric wave activity is strongly influenced by the background state (i.e., zonal wind and index of refraction) of the lower stratosphere. An important regulator for the background is the extratropical tropopause temperature, which in turn is associated with the vertical model resolution. Low-resolution models tend to have large biases in simulating the location and temperature of the extratropical tropopause. The results indicate that the simulated SSW frequency is a useful metric for model performance, as the frequency is highly sensitive to a number of stratospheric and tropospheric factors.&lt;/p&gt;

Inorganic and organic bromine measurements around the extra-tropical tropopause: Insights into total stratospheric bromine

&lt;p&gt;Bromine greatly influences the UT/LS ozone concentrations, however the transport of bromine across the tropical tropopause layer and in particular across the extratropical tropopause is not well quantified. Air-borne measurements of atmospheric trace gases such as organic and inorganic bromine along the tropopause are studied during the WISE (Wave-driven ISentropic Exchange) research campaign over the northern Atlantic and western Europe from September 13 - October 21, 2017. The remote sensing instrument mini-DOAS (Differential Optical Absorption Spectroscopy) is mounted on the HALO (High Altitude and LOng range) aircraft and measures BrO (O&lt;sub&gt;3&lt;/sub&gt;, NO&lt;sub&gt;2&lt;/sub&gt; among other trace gases). The novel scaling method is applied to infer the target gas BrO mixing ratios from slant column densities using in-situ O&lt;sub&gt;3&lt;/sub&gt; measurements from the FAIRO instrument (operated by KIT) as the scaling gas. For each flight, the inferred mixing ratios are directly compared with CLaMS (Chemical Lagrangian Model of the Stratosphere) simulated curtains of the trace gases along the flight path. The partitioning coefficient of inorganic bromine from CLaMS and all relevant organic halogen species and air mass ages (SF&lt;sub&gt;6&lt;/sub&gt;, CO&lt;sub&gt;2&lt;/sub&gt;) from the GhOST-MS instrument (operated by UFra) are used to determine the total bromine budget along the UT/LS. A climatology of organic, inorganic and total bromine is constructed with respect to the extratropical tropopause as well as the air mass ages. This indicates the interplay of bromine transport across the extratropical tropopause and of the transport of air via the lower branch from the tropics as well as potential losses of inorganic bromine by uptake onto and sedimentation of ice particles.&lt;/p&gt;

Static Stability Associated with Southern Hemisphere Blocking Onsets

&lt;p&gt;The horizontal and temporal variation of static stability prior to blocking onset is characterized through composite analysis of blocking events in the Southern Hemisphere. It is found that a local minimum of static stability in the upper troposphere and on the tropopause is achieved over the block-onset region when blocking onset takes place. From the perspective of isentropic potential vorticity, blocking onset is accompanied by extratropical tropopause elevation and a local low isentropic potential vorticity anomaly that is formed right under the elevated tropopause. This low isentropic potential vorticity anomaly is coincident with a local minimum of static stability over the block-onset region. In addition, based on static stability budget analysis, it revealed that the decrease of static stability in the upper troposphere and on the tropopuase prior to blocking onset is attributable to horizontal advection of low static stability from subtropics to midlatitude as well as the stretching effect associated with upper-level convergence, with the horizontal advection forcing being the primary contributor. On the other hand, the vertical advection of static stability tends to oppose the decreasing static stability through advecting more stable air downward such that it stabilizes the local air over the block-onset region. Furthermore, the indirect and direct effect of latent heat to the local change of static stability over the block-onset region are also discussed, respectively.&lt;/p&gt;