What does the global mean OH concentration tell us?

International audienceThe global mean OH concentration ([OH]GM ) has been used as an indicator of the atmospheric oxidizing efficiency or its changes over time. It is also used for evaluating the performance of atmospheric chemistry models by comparing with other models or with observationally-based reference [OH]GM levels. We contend that the treatment of this quantity in the recent literature renders it problematic for either of these pur-poses. Several different methods have historically been used to compute [OH]GM: weighting by atmospheric mass or volume, or by the reaction with CH4 or CH3CCl3. In addition, these have been applied over different domains to represent the troposphere. While it is clear that this can lead to inconsistent [OH]GM values, to date there has been no careful assessment of the differences expected when [OH]GM is computed using various weightings and domains. Here these differences are considered using four different 3D OH distributions, along with the weightings mentioned above applied over various atmospheric domains. We find that the [OH]GM values computed based on a given distribution but using different domains for the troposphere can result in differences of 10% or more, while different weightings can lead to differences of up to 30%, comparable to the uncertainty which is commonly stated for [OH]GM or its trend. Thus, at present comparing [OH]GM values or trends from different studies does not provide clearly interpretable information about whether the OH amounts are actually similar or not, except in the few cases where the same weighting and domain have been used in both studies. Furthermore, we find that the only direct indicator of the global atmospheric oxidizing efficiency of OH with respect to a particular gas (e.g. CH4 or CH3CCl3 ) is the [OH]GM value weighted by the reaction with that gas; the mass-weighted and volume-weighted [OH]GM values, in contrast, are generally poor indicators of the atmospheric oxidizing efficiency on a global basis (regionally they are better). We recommend that in future studies the [OH]GM value weighted by the reaction with CH4 , along with the CH4 turnover time, be given as the primary indicators of the atmospheric oxidizing efficiency, and that serious evaluations of modeled OH concentrations be done with air mass weighted [OH]GM broken down into atmospheric sub-compartments, especially focusing on the tropics, where the atmospheric oxidizing efficiency is greatest

Missing Heritability in the Tails of Quantitative Traits? A Simulation Study on the Impact of Slightly Altered True Genetic Models

Objective: Genome-wide association studies have identified robust associations between single nucleotide polymorphisms and complex traits. As the proportion of phenotypic variance explained is still limited for most of the traits, larger and larger meta-analyses are being conducted to detect additional associations. Here we investigate the impact of the study design and the underlying assumption about the true genetic effect in a bimodal mixture situation on the power to detect associations. Methods: We performed simulations of quantitative phenotypes analysed by standard linear regression and dichotomized case-control data sets from the extremes of the quantitative trait analysed by standard logistic regression. Results: Using linear regression, markers with an effect in the extremes of the traits were almost undetectable, whereas analysing extremes by case-control design had superior power even for much smaller sample sizes. Two real data examples are provided to support our theoretical findings and to explore our mixture and parameter assumption. Conclusions: Our findings support the idea to re-analyse the available meta-analysis data sets to detect new loci in the extremes. Moreover, our investigation offers an explanation for discrepant findings when analysing quantitative traits in the general population and in the extremes. Copyright (C) 2011 S. Karger AG, Base

Will climate change increase ozone depletion from low-energy-electron precipitation?

We investigate the effects of a strengthened stratospheric/mesospheric residual circulation on the transport of nitric oxide (NO) produced by energetic particle precipitation. During periods of high geomagnetic activity, energetic electron precipitation (EEP) is responsible for winter time ozone loss in the polar middle atmosphere between 1 and 6 hPa. However, as climate change is expected to increase the strength of the Brewer-Dobson circulation including extratropical downwelling, the enhancements of EEP NO<sub>x</sub> concentrations are expected to be transported to lower altitudes in extratropical regions, becoming more significant in the ozone budget. Changes in the mesospheric residual circulation are also considered. We use simulations with the chemistry climate model system EMAC to compare present day effects of EEP NO<sub>x</sub> with expected effects in a climate change scenario for the year 2100. In years of strong geomagnetic activity, similar to that observed in 2003, an additional polar ozone loss of up to 0.4 μmol/mol at 5 hPa is found in the Southern Hemisphere. However, this would be approximately compensated by an ozone enhancement originating from a stronger poleward transport of ozone from lower latitudes caused by a strengthened Brewer-Dobson circulation, as well as by slower photochemical ozone loss reactions in a stratosphere cooled by risen greenhouse gas concentrations. In the Northern Hemisphere the EEP NO<sub>x</sub> effect appears to lose importance due to the different nature of the climate-change induced circulation changes

Corrigendum to "Geomagnetic activity related NOx enhancements and polar surface air temperature variability in a chemistry climate model: modulation of the NAM index" published in Atmos. Chem. Phys., 11, 4521–4531, 2011

No abstract available

A discussion on the determination of atmospheric OH and its trends

The oxidation efficiency of the troposphere is largely determined by the hydroxyl radical and its global distribution. Its presence limits the lifetime of most trace gases. Because of the great importance of several of these gases for climate, ozone budget and OH itself, it is of fundamental importance to acquire knowledge about atmospheric OH and possible trends in its concentrations. In the past, average concentrations of OH and trends were largely derived using industrially produced CH₃CCl₃ as a chemical tracer. The analyses have given valuable, but also rather uncertain results. In this paper we describe an idealized computer aided tracer experiment which has as one of its goals to derive tracer concentration weighted, global average <<i>k</i>(OH)>, where the temporal and spatial OH distribution is prescribed and <i>k</i> is the reaction rate coefficient of OH with a hitherto never produced (Gedanken) tracer, which is injected at a number of surface sites in the atmosphere in well known amounts over a given time period. Using a three-dimensional (3-D) time-dependent chemistry transport model, <<i>k</i>(OH)> can be accurately determined from the calculated 3-D tracer distribution. It is next explored how well <<i>k</i>(OH)> can be retrieved solely from tracer measurements at a limited number of surface sites. The results from this analysis are encouraging enough to actually think about the feasibility to carry out a global dedicated tracer experiment to derive <<i>k</i>(OH)> and its temporal trends. However, before that, we propose to test the methods that are used to derive <<i>k</i>(OH)>, so far largely using CH₃CCl₃, with an idealized tracer experiment, in which a global chemistry transport model is used to calculate the ``Gedanken'' tracer distribution, representing the real 3-D world, from which <<i>k</i>(OH)> is derived, using only the tracer information from a limited set of surface sites. We propose here that research groups which are, or will be, involved in global average OH studies to participate in such an inter-comparison of methods, organized and over-seen by a committee appointed by the International Global Atmospheric Chemistry (IGAC) program

A climatology of surface ozone in the extra tropics: cluster analysis of observations and model results

Important aspects of the seasonal variations of surface ozone are discussed. The underlying analysis is based on the long-term (1990&amp;ndash;2004) ozone records of the Co-operative Programme for Monitoring and Evaluation of the Long-range Transmission of Air Pollutants in Europe (EMEP) and the World Data Centre of Greenhouse Gases, which provide data mostly for the Northern Hemisphere. Seasonal variations are pronounced at most of the 114 locations at all times of the day. A seasonal-diurnal variations classification using hierarchical agglomeration clustering reveals 6 distinct clusters: clean background, rural, semi-polluted non-elevated, semi-polluted semi-elevated, elevated and polar/remote marine. For the &quot;clean background&quot; cluster the seasonal maximum is observed in March-April, both for night and day. For those sites with a double maximum or a wide spring-summer maximum, the spring maximum appears both for day and night, while the summer maximum is more pronounced for daytime and hence can be attributed to photochemical processes. The spring maximum is more likely caused by dynamical/transport processes than by photochemistry as it is observed in spring for all times of the day. We compare the identified clusters with corresponding data from the 3-D atmospheric chemistry general circulation model ECHAM5/MESSy1 covering the period of 1998&amp;ndash;2005. For the model output as for the measurements 6 clusters are considered. The simulation shows at most of the sites a spring seasonal maximum or a broad spring-summer maximum (with higher summer mixing ratios). For southern hemispheric and polar remote locations the seasonal maximum in the simulation is shifted to spring, while the absolute mixing ratios are in good agreement with the measurements. The seasonality in the model cluster covering background locations is characterized by a pronounced spring (April&amp;ndash;May) maximum. For the model clusters which cover rural and semi-polluted sites the role of the photochemical production/destruction seems to be overestimated. Taking into consideration the differences in the data sampling procedure, the comparison demonstrates the ability of the model to reproduce the main regimes of surface ozone variations quite well

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

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

Global Atmospheric Aerosol Modeling

Global aerosol models are used to study the distribution and properties of atmospheric aerosol particles as well as their effects on clouds, atmospheric chemistry, radiation, and climate. The present article provides an overview of the basic concepts of global atmospheric aerosol modeling and shows some examples from a global aerosol simulation. Particular emphasis is placed on the simulation of aerosol particles and their effects within global climate models