Sensitivity of age of air trends to the derivation method for non-linear increasing inert SF6

Mean age of air (AoA) is a diagnostic of transport along the stratospheric Brewer–Dobson circulation. While models consistently show negative trends, long-term time series (1975–2016) of AoA derived from observations show non-significant positive trends in mean AoA in the Northern Hemisphere. This discrepancy between observed and modelled mean AoA trends is still not resolved. There are uncertainties and assumptions required when deriving AoA from trace gas observations. At the same time, AoA from climate models is subject to uncertainties, too. In this paper, we focus on the uncertainties due to the parameter selection in the method that is used to derive mean AoA from SF$_{6}$ measurements in Engel et al. (2009, 2017). To correct for the non-linear increase in SF$_{6}$ concentrations, a quadratic fit to the time series at the reference location, i.e. the tropical surface, is used. For this derivation, the width of the AoA distribution (age spectrum) has to be assumed. In addition, to choose the number of years the quadratic fit is performed for, the fraction of the age spectrum to be considered has to be assumed. Even though the uncertainty range due to all different aspects has already been taken into account for the total errors in the AoA values, the systematic influence of the parameter selection on AoA trends is described for the first time in the present study. For this, we use the EMAC (ECHAM MESSy Atmospheric Chemistry) climate model as a test bed, where AoA derived from a linear tracer is available as a reference and modelled age spectra exist to diagnose the actual spatial age spectra widths. The comparison of mean AoA from the linear tracer with mean AoA from a SF$_{6}$ tracer shows systematic deviations specifically in the trends due to the selection of the parameters. However, for an appropriate parameter selection, good agreement for both mean AoA and its trend can be found, with deviations of about 1 % in mean AoA and 12 % in AoA trend. In addition, a method to derive mean AoA is evaluated that applies a convolution to the reference time series. The resulting mean AoA and its trend only depend on an assumption about the ratio of moments. Also in that case, it is found that the larger the ratio of moments, the more the AoA trend gravitates towards the negative. The linear tracer and SF$_{6}$ AoA are found to agree within 0.3 % in the mean and 6 % in the trend. The different methods and parameter selections were then applied to the balloon-borne SF$_{6}$ and CO$_{2}$ observations. We found the same systematic changes in mean AoA trend dependent on the specific selection. When applying a parameter choice that is suggested by the model results, the AoA trend is reduced from 0.15 to 0.07 years per decade. It illustrates that correctly constraining those parameters is crucial for correct mean AoA and trend estimates and still remains a challenge in the real atmosphere

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

Modelling marine emissions and atmospheric distributions of halocarbons and dimethyl sulfide: the influence of prescribed water concentration vs. prescribed emissions

Marine-produced short-lived trace gases such as dibromomethane (CH2Br2), bromoform (CHBr3), methyliodide (CH3I) and dimethyl sulfide (DMS) significantly impact tropospheric and stratospheric chemistry. Describing their marine emissions in atmospheric chemistry models as accurately as possible is necessary to quantify their impact on ozone depletion and Earth's radiative budget. So far, marine emissions of trace gases have mainly been prescribed from emission climatologies, thus lacking the interaction between the actual state of the atmosphere and the ocean. Here we present simulations with the chemistry climate model EMAC (ECHAM5/MESSy Atmospheric Chemistry) with online calculation of emissions based on surface water concentrations, in contrast to directly prescribed emissions. Considering the actual state of the model atmosphere results in a concentration gradient consistent with model real-time conditions at the ocean surface and in the atmosphere, which determine the direction and magnitude of the computed flux. This method has a number of conceptual and practical benefits, as the modelled emission can respond consistently to changes in sea surface temperature, surface wind speed, sea ice cover and especially atmospheric mixing ratio. This online calculation could enhance, dampen or even invert the fluxes (i.e. deposition instead of emissions) of very short-lived substances (VSLS). We show that differences between prescribing emissions and prescribing concentrations (−28 % for CH2Br2 to +11 % for CHBr3) result mainly from consideration of the actual, time-varying state of the atmosphere. The absolute magnitude of the differences depends mainly on the surface ocean saturation of each particular gas. Comparison to observations from aircraft, ships and ground stations reveals that computing the air–sea flux interactively leads in most of the cases to more accurate atmospheric mixing ratios in the model compared to the computation from prescribed emissions. Calculating emissions online also enables effective testing of different air–sea transfer velocity (k) parameterizations, which was performed here for eight different parameterizations. The testing of these different k values is of special interest for DMS, as recently published parameterizations derived by direct flux measurements using eddy covariance measurements suggest decreasing k values at high wind speeds or a linear relationship with wind speed. Implementing these parameterizations reduces discrepancies in modelled DMS atmospheric mixing ratios and observations by a factor of 1.5 compared to parameterizations with a quadratic or cubic relationship to wind spee

Archiving and referencing source code with Software Heritage

Software, and software source code in particular, is widely used in modern research. It must be properly archived, referenced, described and cited in order to build a stable and long lasting corpus of scientic knowledge. In this article we show how the Software Heritage universal source code archive provides a means to fully address the first two concerns, by archiving seamlessly all publicly available software source code, and by providing intrinsic persistent identifiers that allow to reference it at various granularities in a way that is at the same time convenient and effective. We call upon the research community to adopt widely this approach.Comment: arXiv admin note: substantial text overlap with arXiv:1909.1076

Depletion of Ozone and Reservoir Species of Chlorine and Nitrogen Oxide in the Lower Antarctic Polar Vortex Measured from Aircraft

Novel airborne in situ measurements of inorganic chlorine, nitrogen oxide species, and ozone were performed inside the lower Antarctic polar vortex and at its edge in September 2012. We focus on one flight during the Transport and Composition of the LMS/Earth System Model Validation (TACTS/ESMVal) campaign with the German research aircraft HALO (High-Altitude LOng range research aircraft), reaching latitudes of 65°S and potential temperatures up to 405 K. Using the early winter correlations of reactive trace gases with N2O from the Atmospheric Chemistry Experiment-Fourier Transform Spectrometer (ACE-FTS), we find high depletion of chlorine reservoir gases up to ∼40% (0.8 ppbv) at 12 km to 14 km altitude in the vortex and 0.4 ppbv at the edge in subsided stratospheric air with mean ages up to 4.5 years. We observe denitrification of up to 4 ppbv, while ozone was depleted by 1.2 ppmv at potential temperatures as low as 380 K. The advanced instrumentation aboard HALO enables high-resolution measurements with implications for the oxidation capacity of the lowermost stratosphere. ©2017. American Geophysical Union

Modelling marine emissions and atmospheric distributions of halocarbons and dimethyl sulfide: The influence of prescribed water concentration vs. prescribed emissions

Marine-produced short-lived trace gases such as dibromomethane (CH$_{2}$Br$_{2}$), bromoform (CHBr$_{3}$), methyliodide (CH$_{3}$I) and dimethyl sulfide (DMS) significantly impact tropospheric and stratospheric chemistry. Describing their marine emissions in atmospheric chemistry models as accurately as possible is necessary to quantify their impact on ozone depletion and Earth’s radiative budget. So far, marine emissions of trace gases have mainly been prescribed from emission climatologies, thus lacking the interaction between the actual state of the atmosphere and the ocean. Here we present simulations with the chemistry climate model EMAC (ECHAM5/MESSy Atmospheric Chemistry) with online calculation of emissions based on surface water concentrations, in contrast to directly prescribed emissions. Considering the actual state of the model atmosphere results in a concentration gradient consistent with model realtime conditions at the ocean surface and in the atmosphere, which determine the direction and magnitude of the computed flux. This method has a number of conceptual and practical benefits, as the modelled emission can respond consistently to changes in sea surface temperature, surface wind speed, sea ice cover and especially atmospheric mixing ratio. This online calculation could enhance, dampen or even invert the fluxes (i.e. deposition instead of emissions) of very short-lived substances (VSLS). We show that differences between prescribing emissions and prescribing concentrations (-28%for CH$_{2}$Br$_{2}$ to +11%for CHBr$_{3}$) result mainly from consideration of the actual, time-varying state of the atmosphere. The absolute magnitude of the differences depends mainly on the surface ocean saturation of each particular gas. Comparison to observations from aircraft, ships and ground stations reveals that computing the air–sea flux interactively leads in most of the cases to more accurate atmospheric mixing ratios in the model compared to the computation from prescribed emissions. Calculating emissions online also enables effective testing of different air–sea transfer velocity (k) parameterizations, which was performed here for eight different parameterizations. The testing of these different k values is of special interest for DMS, as recently published parameterizations derived by direct flux measurements using eddy covariance measurements suggest decreasing k values at high wind speeds or a linear relationship with wind speed. Implementing these parameterizations reduces discrepancies in modelled DMS atmospheric mixing ratios and observations by a factor of 1.5 compared to parameterizations with a quadratic or cubic relationship to wind speed

Dynamical Gauge Symmetry Breaking in SU(3)L⊗U(1)XSU(3)_L\otimes U(1)_X Extension of the Standard Model

We study the $SU(3)_L\otimes U(1)_X$ extension of the Standard model with a strong U(1) coupling. We argue that current experiments limit this coupling to be relatively large. The model is dynamically broken to the Standard $SU(2)_L \otimes U(1)$ model at the scale of a few TeV with all the extra gauge bosons and the exotic quarks acquiring masses much larger than the scale of electroweak symmetry breaking. Furthermore we find that the model leads to large dynamical mass of the top quark and hence also breaks the electroweak gauge symmetry. It therefore leads to large dynamical effects within the Standard model and can partially replace the Higgs interactions.Comment: 4 pages, revtex, no figures; revised version predicting realistic mass spectru

Mercury distribution in the upper troposphere and lowermost stratosphere according to measurements by the IAGOS-CARIBIC observatory: 2014-2016

Mercury was measured onboard the IAGOSCARIBIC passenger aircraft from May 2005 until February 2016 during near monthly sequences of mostly four intercontinental flights from Germany to destinations in North and South America, Africa and South and East Asia. Most of these mercury data were obtained using an internal default signal integration procedure of the Tekran instrument but since April 2014 more precise and accurate data were obtained using post-flight manual integration of the instrument raw signal. In this paper we use the latter data. Increased upper tropospheric total mercury (TM) concentrations due to large scale biomass burning were observed in the upper troposphere (UT) at the equator and southern latitudes during the flights to Latin America and South Africa in boreal autumn (SON) and boreal winter (DJF). TM concentrations in the lowermost stratosphere (LMS) decrease with altitude above the thermal tropopause but the gradient is less steep than reported before. Seasonal variation of the vertical TM distribution in the UT and LMS is similar to that of other trace gases with surface sources and stratospheric sinks. Speciation experiments suggest comparable TM and gaseous elementary mercury (GEM) concentrations at and below the tropopause leaving little space for Hg2+ (TM-GEM) being the dominating component of TM here. In the stratosphere significant GEM concentrations were found to exist up to 4 km altitude above the thermal tropopause. Correlations with N2O as a reference tracer suggest stratospheric lifetimes of 72 ± 37 and 74 ± 27 years for TM and GEM, respectively, comparable to the stratospheric lifetime of COS. This coincidence, combined with pieces of evidence from us and other researchers, corroborates the hypothesis that Hg2+ formed by oxidation in the stratosphere attaches to sulfate particles formed mainly by oxidation of COS and is removed with them from the stratosphere by air mass exchange, gravitational sedimentation and cloud scavenging processes

The Collider Phenomenology of Technihadrons in the Technicolor Straw Man Model

We discuss the phenomenology of the lightest SU(3)_C singlet and non-singlet technihadrons in the Straw Man Model of low-scale technicolor (TCSM). The technihadrons are assumed to be those arising in topcolor--assisted technicolor models in which topcolor is broken by technifermion condensates. We improve upon the description of the color--singlet sector presented in our earlier paper introducing the TCSM (hep-ph/9903369). These improvements are most important for subprocess energies well below the masses of the technirho and techniomega, and, therefore, apply especially to e+e- colliders such as LEP and a low--energy linear collider. In the color--octet sector, we consider mixing of the gluon, the coloron V_8 from topcolor breaking, and four isosinglet color--octet technirho mesons. We assume, as expected in walking technicolor, that these technirhos decay into qbar-q, gg, and g-technipion final states, but not into technipion pairs. All the TCSM production and decay processes discussed here are included in the event generator Pythia. We present several simulations appropriate for the Tevatron Collider, and suggest benchmark model lines for further experimental investigation.Comment: 42 pages, 7 figure

Evaluation of stratospheric age of air from CF4_{4}, C2_{2}F6_{6}, C3_{3}F8_{8}, CHF3_{3}, HFC-125, HFC-227ea and SF6_{6}; Implications for the calculations of halocarbon lifetimes, fractional release factors and ozone depletion potentials

In a changing climate, potential stratospheric circulation changes require long-term monitoring. Stratospheric trace gas measurements are often used as a proxy for stratospheric circulation changes via the “mean age of air” values derived from them. In this study, we investigated five potential age of air tracers – the perfluorocarbons CF4, C2F6 and C3F8 and the hydrofluorocarbons CHF3 (HFC-23) and HFC-125 – and compare them to the traditional tracer SF6 and a (relatively) shorter-lived species, HFC-227ea. A detailed uncertainty analysis was performed on mean ages derived from these “new” tracers to allow us to confidently compare their efficacy as age tracers to the existing tracer, SF6. Our results showed that uncertainties associated with the mean age derived from these new age tracers are similar to those derived from SF6, suggesting that these alternative compounds are suitable in this respect for use as age tracers. Independent verification of the suitability of these age tracers is provided by a comparison between samples analysed at the University of East Anglia and the Scripps Institution of Oceanography. All five tracers give younger mean ages than SF6, a discrepancy that increases with increasing mean age. Our findings qualitatively support recent work that suggests that the stratospheric lifetime of SF6 is significantly less than the previous estimate of 3200 years. The impact of these younger mean ages on three policy-relevant parameters – stratospheric lifetimes, fractional release factors (FRFs) and ozone depletion potentials – is investigated in combination with a recently improved methodology to calculate FRFs. Updates to previous estimations for these parameters are provided