Reconciling modelled and observed age of air through SF6 sinks

Author(s):  
Sheena Loeffel ◽  
Roland Eichinger ◽  
Hella Garny ◽  
Thomas Reddmann ◽  
Stefan Versick ◽  
...  

<p>Mean age of air (AoA) is a common diagnostic for the stratospheric overturning circulation in both climate models and observations. Observations of AoA mostly base on measurements of SF6, which is an almost ideal AoA tracer because its emssions across the recent decades increased nearly linearly and it is fairly stable in the troposphere and stratosphere. Over the last ten years, however, researchers were puzzled as to why AoA climatologies and trends of model simulations and observational data do not coincide. AoA in climate models is generally much lower than in observations and models show a clear decrease of AoA over time while measurements show a non-significant increase.</p><p>What is commonly not considered in the models is that SF6 has chemical sinks in the mesosphere, and these lead to apparently older air in the stratosphere. In our experiment, we explicitely calculate SF6 sinks based on physical processes in simulations with the global chemistry-climate model EMAC (ECHAM MESSy Atmospheric Chemistry). We show that considering the SF6 removal reactions strongly increases stratospheric AoA and leads to much better agreement between the climatologies of EMAC and MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) satellite observations. Moreover, the stratospheric AoA trend over the recent decades reverses sign when we derive it from SF6 with sinks. This means that the trend can such be reconciled with the trend that has been derived from long-term balloon-borne measurements. Our specifically designed sensitivity studies moreover reveal that this positive trend results neither from circulation changes, nor from variations of the reactive species involved in mesospheric SF6 depletion. Instead, it is generated through the temporally growing influence of the SF6 sinks themselves, an effect that overcompensates the negative trend resulting from the accelerating stratospheric overturning circulation.</p>

2021 ◽  
Author(s):  
Ramiro Checa-Garcia ◽  
Didier Didier Hauglustaine ◽  
Yves Balkanski ◽  
Paola Formenti

<p>Glyoxal (GL) and methylglyoxal (MGL) are the smallest di-carbonyls present in the atmosphere. They hydrate easily, a process that is followed by an oligomerisation. As a consequence, it is considered that they participate actively in the formation of secondary organic aerosols (SOA) and therefore, they are being introduced in the current climate models with interactive chemistry to assess their importance on atmospheric chemistry. In our study we present the introduction of glyoxal in the INCA global model. A new closed set of gas-phase  reactions is analysed first with a box model. Then the simulated global distribution of glyoxal by the global climate model is compared with satellite observations. We show that the oxidation of volatile organic compounds and acetylene, together with the photolysis of more complex di-carbonyls allows us to reproduce well glyoxal seasonal cycle in the tropics but it requires an additional sink in several northern hemispheric regions. Additional sensitivity studies are being conducted by introducing  GL and MGL interactions with dust and SOA according to new uptake  coefficients obtained by dedicated experiments in the CESAM instrument (Chamber of Experimental Simulation of Atmospheric Multiphases). The effects of these heterogeneous chemistry processes will be quantified in the light of the new chamber measurements  and also evaluated in terms of optical properties of aged dust aerosol  and the changes in direct radiative effects  of the involved aerosol species.</p>


2017 ◽  
Author(s):  
Gerald Wetzel ◽  
Hermann Oelhaf ◽  
Michael Höpfner ◽  
Felix Friedl-Vallon ◽  
Andreas Ebersoldt ◽  
...  

Abstract. The first stratospheric measurements of the diurnal variation of the inorganic bromine (Bry) reservoir species BrONO2 around sunrise and sunset are reported. Arctic flights of the balloon-borne Michelson Interferometer for Passive Atmospheric Sounding (MIPAS-B) were carried out from Kiruna (68°N, Sweden) in January 2010 and March 2011 inside the stratospheric polar vortices where diurnal variations of BrONO2 around sunrise have been observed. High nighttime BrONO2 volume mixing ratios of up to 21 parts per trillion by volume (pptv) were detected in the late winter 2011 in the absence of polar stratospheric clouds (PSCs). In contrast, the amount of measured BrONO2 was significantly lower in January 2010 due to low available NO2 amounts (for the build-up of BrONO2), heterogeneous destruction of BrONO2 on PSC particles, and the gas-phase interaction of BrO (the source to form BrONO2) with ClO. A further balloon flight took place at mid-latitudes from Timmins (49°N, Canada) in September 2014. Mean BrONO2 mixing ratios of 22 pptv were observed after sunset in the altitude region between 21 and 29 km. Measurements are compared and discussed with the results of a multi-year simulation performed with the chemistry climate model ECHAM5/MESSy Atmospheric Chemistry (EMAC). The calculated temporal variation of BrONO2 is in principal agreement with the balloon-borne observations. Using the nighttime simulated ratio between BrONO2 and Bry, the amount of Bry observed by MIPAS-B was estimated to about 21–25 pptv in the lower stratosphere.


2021 ◽  
Author(s):  
Cyril Caram ◽  
Sophie Szopa ◽  
Anne Cozic ◽  
Slimane Bekki ◽  
Carlos Cuevas ◽  
...  

Abstract. The atmospheric chemistry of halogenated species (Cl, Br, I) participates in the global chemical sink of tropospheric ozone and perturbs the oxidizing capacity of the troposphere, notably influencing the atmospheric lifetime of methane. Global chemistry-climate models are commonly used to assess the global budget of ozone, its sensitivity to emissions of its precursors, and to project its long-term evolution. Here, we report on the implementation of tropospheric halogens chemistry in the chemistry-climate model LMDZ-INCA and its effects on the tropospheric ozone budget. Overall, the results show that the model simulates satisfactorily the impact of halogens on the photooxidizing system in the troposphere, in particular in the marine boundary layer. To elucidate the mechanisms and quantify the effects, standard metrics representative of the behavior of the tropospheric chemical system (Ox, HOx, NOx, CH4, and NMVOCs) are computed with and without halogen chemistry. Tropospheric halogens in the LMDZ-INCA model lead to a decrease of 22 % in the ozone burden, 8 % in OH, and 33 % in NOx. Additional sensitivity simulations show that the inclusion of halogens chemistry makes ozone more sensitive to perturbations in CH4, NOx, and NMVOCs. Consistent with other global model studies, the sensitivity of the tropospheric ozone burden to changes from pre-industrial to present-day emissions is found to be ~20 % lower when tropospheric halogens are taken into account.


2017 ◽  
Vol 17 (23) ◽  
pp. 14631-14643
Author(s):  
Gerald Wetzel ◽  
Hermann Oelhaf ◽  
Michael Höpfner ◽  
Felix Friedl-Vallon ◽  
Andreas Ebersoldt ◽  
...  

Abstract. The first stratospheric measurements of the diurnal variation in the inorganic bromine (Bry) reservoir species BrONO2 around sunrise and sunset are reported. Arctic flights of the balloon-borne Michelson Interferometer for Passive Atmospheric Sounding (MIPAS-B) were carried out from Kiruna (68° N, Sweden) in January 2010 and March 2011 inside the stratospheric polar vortices where diurnal variations of BrONO2 around sunrise have been observed. High nighttime BrONO2 volume mixing ratios of up to 21 pptv (parts per trillion by volume) were detected in late winter 2011 in the absence of polar stratospheric clouds (PSCs). In contrast, the amount of measured BrONO2 was significantly lower in January 2010 due to low available NO2 amounts (for the build-up of BrONO2), the heterogeneous destruction of BrONO2 on PSC particles, and the gas-phase interaction of BrO (the source to form BrONO2) with ClO. A further balloon flight took place at midlatitudes from Timmins (49° N, Canada) in September 2014. Mean BrONO2 mixing ratios of 22 pptv were observed after sunset in the altitude region between 21 and 29 km. Measurements are compared and discussed with the results of a multi-year simulation performed with the chemistry climate model ECHAM5/MESSy Atmospheric Chemistry (EMAC). The calculated temporal variation in BrONO2 largely reproduces the balloon-borne observations. Using the nighttime simulated ratio between BrONO2 and Bry, the amount of Bry observed by MIPAS-B was estimated to be about 21–25 pptv in the lower stratosphere.


2017 ◽  
Vol 17 (18) ◽  
pp. 11521-11539 ◽  
Author(s):  
Stefan Lossow ◽  
Hella Garny ◽  
Patrick Jöckel

Abstract. The amplitude of the annual variation in water vapour exhibits a distinct isolated maximum in the middle and upper stratosphere in the southern tropics and subtropics, peaking typically around 15° S in latitude and close to 3 hPa (∼  40.5 km) in altitude. This enhanced annual variation is primarily related to the Brewer–Dobson circulation and hence also visible in other trace gases. So far this feature has not gained much attention in the literature and the present work aims to add more prominence. Using Envisat/MIPAS (Environmental Satellite/Michelson Interferometer for Passive Atmospheric Sounding) observations and ECHAM/MESSy (European Centre for Medium-Range Weather Forecasts Hamburg/Modular Earth Submodel System) Atmospheric Chemistry (EMAC) simulations we provide a dedicated illustration and a full account of the reasons for this enhanced annual variation.


2018 ◽  
Vol 11 (6) ◽  
pp. 2033-2048 ◽  
Author(s):  
Richard Hyde ◽  
Ryan Hossaini ◽  
Amber A. Leeson

Abstract. Clustering – the automated grouping of similar data – can provide powerful and unique insight into large and complex data sets, in a fast and computationally efficient manner. While clustering has been used in a variety of fields (from medical image processing to economics), its application within atmospheric science has been fairly limited to date, and the potential benefits of the application of advanced clustering techniques to climate data (both model output and observations) has yet to be fully realised. In this paper, we explore the specific application of clustering to a multi-model climate ensemble. We hypothesise that clustering techniques can provide (a) a flexible, data-driven method of testing model–observation agreement and (b) a mechanism with which to identify model development priorities. We focus our analysis on chemistry–climate model (CCM) output of tropospheric ozone – an important greenhouse gas – from the recent Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). Tropospheric column ozone from the ACCMIP ensemble was clustered using the Data Density based Clustering (DDC) algorithm. We find that a multi-model mean (MMM) calculated using members of the most-populous cluster identified at each location offers a reduction of up to ∼ 20 % in the global absolute mean bias between the MMM and an observed satellite-based tropospheric ozone climatology, with respect to a simple, all-model MMM. On a spatial basis, the bias is reduced at ∼ 62 % of all locations, with the largest bias reductions occurring in the Northern Hemisphere – where ozone concentrations are relatively large. However, the bias is unchanged at 9 % of all locations and increases at 29 %, particularly in the Southern Hemisphere. The latter demonstrates that although cluster-based subsampling acts to remove outlier model data, such data may in fact be closer to observed values in some locations. We further demonstrate that clustering can provide a viable and useful framework in which to assess and visualise model spread, offering insight into geographical areas of agreement among models and a measure of diversity across an ensemble. Finally, we discuss caveats of the clustering techniques and note that while we have focused on tropospheric ozone, the principles underlying the cluster-based MMMs are applicable to other prognostic variables from climate models.


2021 ◽  
Author(s):  
Gunter Stober ◽  
Ales Kuchar ◽  
Dimitry Pokhotelov ◽  
Huixin Liu ◽  
Han-Li Liu ◽  
...  

Abstract. Long-term and continuous observations of mesospheric/lower thermospheric winds are rare, but they are important to investigate climatological changes at these altitudes on time scales of several years, covering a solar cycle and longer. Such long time series are a natural heritage of the mesosphere/lower thermosphere climate, and they are valuable to compare climate models or long term runs of general circulation models (GCMs). Here we present a climatological comparison of wind observations from six meteor radars at two conjugate latitudes to validate the corresponding mean winds and atmospheric diurnal and semidiurnal tides from three GCMs, namely Ground-to-Topside Model of Atmosphere and Ionosphere for Aeronomy (GAIA), Whole Atmosphere Community Climate Model Extension (Specified Dynamics) (WACCM-X(SD)) and Upper Atmosphere ICOsahedral Non-hydrostatic (UA-ICON) model. Our results indicate that there are interhemispheric differences in the seasonal characteristics of the diurnal and semidiurnal tide. There also are some differences in the mean wind climatologies of the models and the observations. Our results indicate that GAIA shows a reasonable agreement with the meteor radar observations during the winter season, whereas WACCM-X(SD) shows a better agreement with the radars for the hemispheric zonal summer wind reversal, which is more consistent with the meteor radar observations. The free running UA-ICON tends to show similar winds and tides compared to WACCM-X(SD).


2018 ◽  
Vol 31 (12) ◽  
pp. 4727-4743 ◽  
Author(s):  
Wei Liu ◽  
Jian Lu ◽  
Shang-Ping Xie ◽  
Alexey Fedorov

Climate models show that most of the anthropogenic heat resulting from increased atmospheric CO2 enters the Southern Ocean near 60°S and is stored around 45°S. This heat is transported to the ocean interior by the meridional overturning circulation (MOC) with wind changes playing an important role in the process. To isolate and quantify the latter effect, we apply an overriding technique to a climate model and decompose the total ocean response to CO2 increase into two major components: one due to wind changes and the other due to direct CO2 effect. We find that the poleward-intensified zonal surface winds tend to shift and strengthen the ocean Deacon cell and hence the residual MOC, leading to anomalous divergence of ocean meridional heat transport around 60°S coupled to a surface heat flux increase. In contrast, at 45°S we see anomalous convergence of ocean heat transport and heat loss at the surface. As a result, the wind-induced ocean heat storage (OHS) peaks at 46°S at a rate of 0.07 ZJ yr−1 (° lat)−1 (1 ZJ = 1021 J), contributing 20% to the total OHS maximum. The direct CO2 effect, on the other hand, very slightly alters the residual MOC but primarily warms the ocean. It induces a small but nonnegligible change in eddy heat transport and causes OHS to peak at 42°S at a rate of 0.30 ZJ yr−1 (° lat)−1, accounting for 80% of the OHS maximum. We also find that the eddy-induced MOC weakens, primarily caused by a buoyancy flux change as a result of the direct CO2 effect, and does not compensate the intensified Deacon cell.


2019 ◽  
Vol 19 (19) ◽  
pp. 12309-12324 ◽  
Author(s):  
Maxime Prignon ◽  
Simon Chabrillat ◽  
Daniele Minganti ◽  
Simon O'Doherty ◽  
Christian Servais ◽  
...  

Abstract. Hydrochlorofluorocarbons (HCFCs) are the first, but temporary, substitution products for the strong ozone-depleting chlorofluorocarbons (CFCs). HCFC consumption and production are currently regulated under the Montreal Protocol on Substances that Deplete the Ozone Layer and their emissions have started to stabilize or even decrease. As HCFC-22 (CHClF2) is by far the most abundant HCFC in today's atmosphere, it is crucial to continue to monitor the evolution of its atmospheric concentration. In this study, we describe an improved HCFC-22 retrieval strategy from ground-based high-resolution Fourier transform infrared (FTIR) solar spectra recorded at the high-altitude scientific station of Jungfraujoch, the Swiss Alps, 3580 m a.m.s.l. (above mean sea level). This new strategy distinguishes tropospheric and lower-stratospheric partial columns. Comparisons with independent datasets, such as the Advanced Global Atmospheric Gases Experiment (AGAGE) and the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS), supported by models, such as the Belgian Assimilation System for Chemical ObErvation (BASCOE) and the Whole Atmosphere Community Climate Model (WACCM), demonstrate the validity of our tropospheric and lower-stratospheric long-term time series. A trend analysis on the datasets used here, now spanning 30 years, confirms the last decade's decline in the HCFC-22 growth rate. This updated retrieval strategy can be adapted for other ozone-depleting substances (ODSs), such as CFC-12. Measuring or retrieving ODS atmospheric concentrations is essential for scrutinizing the fulfilment of the globally ratified Montreal Protocol.


Geosciences ◽  
2019 ◽  
Vol 9 (6) ◽  
pp. 255 ◽  
Author(s):  
Thomas J. Bracegirdle ◽  
Florence Colleoni ◽  
Nerilie J. Abram ◽  
Nancy A. N. Bertler ◽  
Daniel A. Dixon ◽  
...  

Quantitative estimates of future Antarctic climate change are derived from numerical global climate models. Evaluation of the reliability of climate model projections involves many lines of evidence on past performance combined with knowledge of the processes that need to be represented. Routine model evaluation is mainly based on the modern observational period, which started with the establishment of a network of Antarctic weather stations in 1957/58. This period is too short to evaluate many fundamental aspects of the Antarctic and Southern Ocean climate system, such as decadal-to-century time-scale climate variability and trends. To help address this gap, we present a new evaluation of potential ways in which long-term observational and paleo-proxy reconstructions may be used, with a particular focus on improving projections. A wide range of data sources and time periods is included, ranging from ship observations of the early 20th century to ice core records spanning hundreds to hundreds of thousands of years to sediment records dating back 34 million years. We conclude that paleo-proxy records and long-term observational datasets are an underused resource in terms of strategies for improving Antarctic climate projections for the 21st century and beyond. We identify priorities and suggest next steps to addressing this.


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