A reconstruction of the past trend of atmospheric CO based on firn air samples from Berkner Island, Antarctica

International audienceAlthough for several atmospheric trace gases trends over the past 100 year have been reconstructed using firn air analyses, little is known about one of the chemically most significant trace gases, namely CO. Among the 3 Antarctic drilling expeditions reported, the one from Berkner Island appears to have given results of sufficient analytical quality to warrant a modelling with the aim to reconstruct past changes in atmospheric CO. Based on our reconstructions, CO in high latitudes of the Southern Hemisphere has been increasing since beginning of the 20th century from ~38 ppbv to a recent value of about 52.5 ppbv. The increase in CO is mainly explained by the known increase in CH4, with biomass burning output being most likely responsible for an additional increase. Which, if any, role changes in OH have played cannot be derived

ATTILA 4.0: Lagrangian advective and convective transport of passive tracers within the ECHAM5/MESSy (2.53.0) chemistry–climate model

We have extended ATTILA (Atmospheric Tracer Transport in a LAgrangian model), a Lagrangian tracer transport scheme, which is online coupled to the global ECHAM/MESSy Atmospheric Chemistry (EMAC) model, with a combination of newly developed and modified physical routines and new diagnostic and infrastructure submodels. The new physical routines comprise a parameterisation for Lagrangian convection, a formulation of diabatic vertical velocity, and the new grid-point submodel LGTMIX to calculate the mixing of compounds in Lagrangian representation. The new infrastructure routines simplify the transformation between grid-point (GP) and Lagrangian (LG) space in a parallel computing environment. The new submodel LGVFLUX is a useful diagnostic tool to calculate online vertical mass fluxes through horizontal surfaces. The submodel DRADON was extended to account for emissions and changes of 222Rn on Lagrangian parcels. To evaluate the new physical routines, two simulations in free-running mode with prescribed sea surface temperatures were performed with EMAC–ATTILA in T42L47MA resolution from 1950 to 2010. The results show an improvement of the tracer transport into and within the stratosphere when the diabatic vertical velocity is used for vertical advection in ATTILA instead of the standard kinematic vertical velocity. In particular, the age-of-air distribution is more in accordance with observations. The global tropospheric distribution of 222Rn, however, is simulated in agreement with available observations and with the results from EMAC in grid space for both Lagrangian systems. Additional sensitivity studies reveal an effect of inter-parcel mixing on the age of air in the tropopause region and the stratosphere, but there is no significant effect for the troposphere.</p

Consistent simulation of bromine chemistry from the marine boundary layer to the stratosphere – Part 2: Bromocarbons

In this second part of a series of articles dedicated to a detailed analysis of bromine chemistry in the atmosphere we address one (out of two) dominant natural sources of reactive bromine. The two main source categories are the release of bromine from sea salt and the decomposition of bromocarbons by photolysis and reaction with OH. Here, we focus on C&lt;sub&gt;1&lt;/sub&gt;-bromocarbons. We show that the atmospheric chemistry general circulation model ECHAM5/MESSy realistically simulates their emission, transport and decomposition from the boundary layer up to the mesosphere. We included oceanic emission fluxes of the short-lived bromocarbons CH&lt;sub&gt;2&lt;/sub&gt;Br&lt;sub&gt;2&lt;/sub&gt;, CH&lt;sub&gt;2&lt;/sub&gt;ClBr, CHClBr&lt;sub&gt;2&lt;/sub&gt;, CHCl&lt;sub&gt;2&lt;/sub&gt;Br, CHBr&lt;sub&gt;3&lt;/sub&gt; and of CH&lt;sub&gt;3&lt;/sub&gt;Br. The vertical profiles and the surface mixing ratios of the bromocarbons are in general agreement with the (few available) observations, especially in view of the limited information available and the consequent coarseness of the emission fields. For CHBr&lt;sub&gt;3&lt;/sub&gt;, CHCl&lt;sub&gt;2&lt;/sub&gt;Br and CHClBr&lt;sub&gt;2&lt;/sub&gt; photolysis is the most important degradation process in the troposphere. In contrast to this, tropospheric CH&lt;sub&gt;2&lt;/sub&gt;Br&lt;sub&gt;2&lt;/sub&gt;, CH&lt;sub&gt;3&lt;/sub&gt;Br and CH&lt;sub&gt;2&lt;/sub&gt;ClBr are more efficiently decomposed by reaction with OH. In the free troposphere approximately 40% of the C&lt;sub&gt;1&lt;/sub&gt;-bromocarbons decompose by reaction with OH. Our results indicate that bromoform contributes substantial amounts of reactive bromine to the lower stratosphere and thus should not be neglected in stratospheric simulations

A refined method for calculating equivalent effective stratospheric chlorine

Chlorine and bromine atoms lead to catalytic depletion of ozone in the stratosphere. Therefore the use and production of ozone-depleting substances (ODSs) containing chlorine and bromine is regulated by the Montreal Protocol to protect the ozone layer. Equivalent effective stratospheric chlorine (EESC) has been adopted as an appropriate metric to describe the combined effects of chlorine and bromine released from halocarbons on stratospheric ozone. Here we revisit the concept of calculating EESC. We derive a refined formulation of EESC based on an advanced concept of ODS propagation into the stratosphere and reactive halogen release. A new transit time distribution is introduced in which the age spectrum for an inert tracer is weighted with the release function for inorganic halogen from the source gases. This distribution is termed the "release time distribution". We show that a much better agreement with inorganic halogen loading from the chemistry transport model TOMCAT is achieved compared with using the current formulation. The refined formulation shows EESC levels in the year 1980 for the mid-latitude lower stratosphere, which are significantly lower than previously calculated. The year 1980 is commonly used as a benchmark to which EESC must return in order to reach significant progress towards halogen and ozone recovery. Assuming that – under otherwise unchanged conditions – the EESC value must return to the same level in order for ozone to fully recover, we show that it will take more than 10 years longer than estimated in this region of the stratosphere with the current method for calculation of EESC. We also present a range of sensitivity studies to investigate the effect of changes and uncertainties in the fractional release factors and in the assumptions on the shape of the release time distributions. We further discuss the value of EESC as a proxy for future evolution of inorganic halogen loading under changing atmospheric dynamics using simulations from the EMAC model. We show that while the expected changes in stratospheric transport lead to significant differences between EESC and modelled inorganic halogen loading at constant mean age, EESC is a reasonable proxy for modelled inorganic halogen on a constant pressure level

Characterising the seasonal and geographical variability in tropospheric ozone, stratospheric influence and recent changes

The stratospheric contribution to tropospheric ozone (O3) has been a subject of much debate in recent decades but is known to have an important influence. Recent improvements in diagnostic and modelling tools provide new evidence that the stratosphere has a much larger influence than previously thought. This study aims to characterise the seasonal and geographical distribution of tropospheric ozone, its variability, and its changes and provide quantification of the stratospheric influence on these measures. To this end, we evaluate hindcast specified-dynamics chemistry–climate model (CCM) simulations from the European Centre for Medium-Range Weather Forecasts – Hamburg (ECHAM)/Modular Earth Submodel System (MESSy) Atmospheric Chemistry (EMAC) model and the Canadian Middle Atmosphere Model (CMAM), as contributed to the International Global Atmospheric Chemistry – Stratosphere-troposphere Processes And their Role in Climate (IGAC-SPARC) (IGAC–SPARC) Chemistry Climate Model Initiative (CCMI) activity, together with satellite observations from the Ozone Monitoring Instrument (OMI) and ozone-sonde profile measurements from the World Ozone and Ultraviolet Radiation Data Centre (WOUDC) over a period of concurrent data availability (2005–2010). An overall positive, seasonally dependent bias in 1000–450 hPa (∼0–5.5 km) sub-column ozone is found for EMAC, ranging from 2 to 8 Dobson units (DU), whereas CMAM is found to be in closer agreement with the observations, although with substantial seasonal and regional variation in the sign and magnitude of the bias (∼±4 DU). Although the application of OMI averaging kernels (AKs) improves agreement with model estimates from both EMAC and CMAM as expected, comparisons with ozone-sondes indicate a positive ozone bias in the lower stratosphere in CMAM, together with a negative bias in the troposphere resulting from a likely underestimation of photochemical ozone production. This has ramifications for diagnosing the level of model–measurement agreement. Model variability is found to be more similar in magnitude to that implied from ozone-sondes in comparison with OMI, which has significantly larger variability. Noting the overall consistency of the CCMs, the influence of the model chemistry schemes and internal dynamics is discussed in relation to the inter-model differences found. In particular, it is inferred that CMAM simulates a faster and shallower Brewer–Dobson circulation (BDC) compared to both EMAC and observational estimates, which has implications for the distribution and magnitude of the downward flux of stratospheric ozone over the most recent climatological period (1980–2010). Nonetheless, it is shown that the stratospheric influence on tropospheric ozone is significant and is estimated to exceed 50 % in the wintertime extratropics, even in the lower troposphere. Finally, long-term changes in the CCM ozone tracers are calculated for different seasons. An overall statistically significant increase in tropospheric ozone is found across much of the world but particularly in the Northern Hemisphere and in the middle to upper troposphere, where the increase is on the order of 4–6 ppbv (5 %–10 %) between 1980–1989 and 2001–2010. Our model study implies that attribution from stratosphere–troposphere exchange (STE) to such ozone changes ranges from 25 % to 30 % at the surface to as much as 50 %–80 % in the upper troposphere–lower stratosphere (UTLS) across some regions of the world, including western Eurasia, eastern North America, the South Pacific and the southern Indian Ocean. These findings highlight the importance of a well-resolved stratosphere in simulations of tropospheric ozone and its implications for the radiative forcing, air quality and oxidation capacity of the troposphere

COSMOGENIC 14CO FOR ASSESSING THE OH-BASED SELF-CLEANING CAPACITY OF THE TROPOSPHERE

An application of radiocarbon (14C) in atmospheric chemistry is reviewed. 14C produced by cosmic neutrons immediately forms 14CO, which reacts with hydroxyl radicals (OH) to 14CO2. By this the distribution and seasonality (the lifetime of 14CO is ∼1 month) of the pivotal atmospheric oxidant OH can be established. 14CO measurement is a complex but unique application which benefitted enormously from the realization of AMS, bearing in mind that 14CO abundance is of the order of merely 10 molecules per cm3 not only provides 14CO an independent measure for the OH based self-cleansing capacity of the troposphere, but also enabled detection of 14C production due to high energy solar protons in 1989. Although its production takes place throughout the atmosphere and does not have the character of a point source, transport processes in the atmosphere affect the distribution of 14CO. Vertical mixing in the troposphere renders gradients in its production rate less critical, but considerable meridional gradients exist. One question has remained open, namely confirmation of calculated 14C production by direct measurement. A new sampling method is proposed. The conclusions are a guide to future work on 14CO in relation to OH and atmospheric transport

Brominated VSLS and their influence on ozone under a changing climate

Very short-lived substances (VSLS) contribute as source gases significantly to the tropospheric and stratospheric bromine loading. At present, an estimated 25 % of stratospheric bromine is of oceanic origin. In this study, we investigate how climate change may impact the ocean–atmosphere flux of brominated VSLS, their atmospheric transport, and chemical transformations and evaluate how these changes will affect stratospheric ozone over the 21st century. Under the assumption of fixed ocean water concentrations and RCP6.0 scenario, we find an increase of the ocean–atmosphere flux of brominated VSLS of about 8–10 % by the end of the 21st century compared to present day. A decrease in the tropospheric mixing ratios of VSLS and an increase in the lower stratosphere are attributed to changes in atmospheric chemistry and transport. Our model simulations reveal that this increase is counteracted by a corresponding reduction of inorganic bromine. Therefore the total amount of bromine from VSLS in the stratosphere will not be changed by an increase in upwelling. Part of the increase of VSLS in the tropical lower stratosphere results from an increase in the corresponding tropopause height. As the depletion of stratospheric ozone due to bromine depends also on the availability of chlorine, we find the impact of bromine on stratospheric ozone at the end of the 21st century reduced compared to present day. Thus, these studies highlight the different factors influencing the role of brominated VSLS in a future climate

Description and Evaluation of the specified-dynamics experiment in the Chemistry-Climate Model Initiative

We provide an overview of the REF-C1SD specified-dynamics experiment that was conducted as part of phase 1 of the Chemistry-Climate Model Initiative (CCMI). The REF-C1SD experiment, which consisted of mainly nudged general circulation models (GCMs) constrained with (re)analysis fields, was designed to examine the influence of the large-scale circulation on past trends in atmospheric composition. The REF-C1SD simulations were produced across various model frameworks and are evaluated in terms of how well they represent different measures of the dynamical and transport circulations. In the troposphere there are large (∼40 %) differences in the climatological mean distributions, seasonal cycle amplitude, and trends of the meridional and vertical winds. In the stratosphere there are similarly large (∼50 %) differences in the magnitude, trends and seasonal cycle amplitude of the transformed Eulerian mean circulation and among various chemical and idealized tracers. At the same time, interannual variations in nearly all quantities are very well represented, compared to the underlying reanalyses. We show that the differences in magnitude, trends and seasonal cycle are not related to the use of different reanalysis products; rather, we show they are associated with how the simulations were implemented, by which we refer both to how the large-scale flow was prescribed and to biases in the underlying free-running models. In most cases these differences are shown to be as large or even larger than the differences exhibited by free-running simulations produced using the exact same models, which are also shown to be more dynamically consistent. Overall, our results suggest that care must be taken when using specified-dynamics simulations to examine the influence of large-scale dynamics on composition

Prevalences of primary headache symptoms at school-entry: a population-based epidemiological survey of preschool children in Germany

Primary headache and functional abdominal pain prevalences in an unselected populationbased sample of German preschool children and their parents (n=885) were collected in relation to health-related quality of life and sociodemographic variables. The pain symptoms were assessed according to IHS classification (2004) and Rome-II criteria (1999) during the 2004 data census. The participation rate was 62.7%, with an equal gender distribution. The focus of this paper lies on the symptom-oriented point prevalences for primary headaches of preschool children: 3.6% headache, 33.2% abdominal pain, 48.8% headache+abdominal pain and 14.4% without pain. High comorbidities for pain-affected children have been found. Pain intensities differ significantly only for abdominal pain (one-way ANOVA F=3,339, df=4/445, p=0.010*), not for headaches. However, recurrent headaches show a striking ratio in favour of boys (10:1). Children at preschool age have high quality-of-life measures, already influenced negatively by paediatric pain experiences (one-way ANOVA: F=9,193, df=4/546, p=0.000**). Headache and abdominal pain are relevant for children’s everyday life; hence, simultaneous and prospective assessment is an essential issue in public health research

Gender differences in lung cancer risk by smoking: a multicentre case-control study in Germany and Italy

Several studies in the past have shown appreciably higher lung cancer risk estimates associated with smoking exposure among men than among women, while more recent studies in the USA report just the opposite. To evaluate this topic in a European population we conducted a case-control study of lung cancer in three German and three Italian centres. Personal interviews and standardized questionnaires were used to obtain detailed life-long smoking and occupational histories from 3723 male and 900 female cases and 4075 male and 1094 female controls. Lung cancer risk comparing ever-smokers with never-smokers was higher among men (odds ratios (OR) adjusted for age and centre = 16.1, 95% confidence interval (CI) 12.8-20.3) than among women (OR = 4.2, CI 3.5-5.1). Because the smoking habits of women were different from men, we conducted more detailed analyses using comparable levels of smoking exposure. After restriction to smokers and adjustment for other smoking variables, risk estimates did not differ appreciably between genders. The analysis of duration of smoking (0-19, 20-39, 40+ years) adjusted for cigarette consumption and time since quitting smoking revealed similar risk estimates in men (OR = 1.0, 3.3 [CI 2.6-4.2], 4.1 [CI 3.1-5.6]) and women (OR = 1.0, 2.7 [CI 1.7-4.1], 3.3 [CI 1.9-5.8]). The same was true of the analysis of average or cumulative smoking consumption, and also of analyses stratified by different histological types. We conclude that for comparable exposure to tobacco smoke, the risk of lung cancer is comparable in women and men