The Mediterranean troposphere exhibits a marked and localised summertime ozone maximum, which has the potential to strongly impact regional air quality and radiative forcing. The Mediterranean region can be perturbed by long-range pollution import from Northern Europe, North America and Asia, in addition to local emissions, which may all contribute to regional ozone enhancements. We exploit ozone profile observations from the Tropospheric Emission Spectrometer (TES) and the Global Ozone Monitoring Experiment-2 (GOME-2) satellite instruments, and an offline 3-D global chemical transport model (TOMCAT) to investigate the geographical and vertical structure of the summertime tropospheric ozone maximum over the Mediterranean region. We show that both TES and GOME-2 are able to detect enhanced levels of ozone in the lower troposphere over the region during the summer. These observations, together with surface measurements, are used to evaluate the TOMCAT model's ability to capture the observed ozone enhancement. The model is used to quantify sensitivities of the ozone maximum to anthropogenic and natural volatile organic compound (VOC) emissions, anthropogenic NOx emissions, wildfire emissions and long-range import of ozone and precursors. Our results show a dominant sensitivity to natural VOC emissions in the Mediterranean basin over anthropogenic VOC emissions. However, local anthropogenic NOx emissions are result in the overall largest sensitivity in near-surface ozone. We also show that in the lower troposphere, global VOC emissions account for 40% of the ozone sensitivity to VOC emissions in the region, whereas, for NOx the ozone sensitivity to local sources is 9 times greater than that for global emissions at these altitudes. However, in the mid and upper troposphere ozone is most sensitive to non-local emission sources. In terms of radiative effects on regional climate, ozone contributions from non-local emission sources are more important, as these have a larger impact on ozone in the upper troposphere where its radiative effects are larger, with Asian monsoon outflow having the greatest impact. Our results allow improved understanding of the large-scale processes controlling air quality and climate in the region of the Mediterranean basin
Background: Mediation studies test the mechanisms by which interventions produce clinical outcomes. Consistent positive mediation results have previously been evidenced (Hayes et al., 2006) for the putative processes that compromise the psychological flexibility model of acceptance and commitment therapy (ACT). Aims: The present review aimed to update and extend the ACT mediation evidence base by reviewing mediation studies published since the review of Hayes et al. (2006). Method: ACT mediation studies published between 2006 and 2015 were systematically collated, synthesized and quality assessed. Results: Twelve studies met inclusion criteria and findings were synthesized by (a) the putative processes under investigation, and (b) the outcomes on which processes were tested for mediation. Mediation results were found to be generally consistent with the psychological flexibility model of ACT. However, studies were limited in methodological quality and were overly focused on a small number of putative processes. Conclusions: Further research is required that addresses the identified methodological limitations and also examines currently under-researched putative processes.
Abstract. This paper describes and assesses the performance of the RAL (Rutherford Appleton Laboratory) ozone profile retrieval scheme for the Global Ozone Monitoring Experiment 2 (GOME-2) with a focus on tropospheric ozone. Developments to the scheme since its application to GOME-1 measurements are outlined. These include the approaches developed to account sufficiently for UV radiometric degradation in the Hartley band and for inadequacies in knowledge of instrumental parameters in the Huggins bands to achieve the high-precision spectral fit required to extract information on tropospheric ozone.The assessment includes a validation against ozonesondes (sondes) sampled worldwide over 2 years (2007)(2008). Standard deviations of the ensemble with respect to the sondes are considerably lower for the retrieved profiles than for the a priori, with the exception of the lowest subcolumn. Once retrieval vertical smoothing (averaging kernels) has been applied to the sonde profiles there is a retrieval bias of 6 % (1.5 DU) in the lower troposphere, with smaller biases in the subcolumns above. The bias in the troposphere varies with latitude. The retrieval underestimates lower tropospheric ozone in the Southern Hemisphere (SH) (15-20 % or ∼ 1-3 DU) and overestimates it in the Northern Hemisphere (NH) (10 % or 2 DU).The ability of the retrieval to reflect the geographical distribution of lower tropospheric ozone, globally (rather than just ozonesonde launch sites) is demonstrated by comparison with the chemistry transport model TOMCAT. For a monthly mean of cloud-cleared GOME-2 pixels, a correlation of 0.66 is found between the retrieval and TOMCAT sampled accordingly, with a bias of 0.7 Dobson Units. GOME-2 estimates higher concentrations in NH pollution centres but lower ozone in the Southern Ocean and South Pacific, which is consistent with the comparison to ozonesondes.
Abstract.A methodology for the round-robin evaluation and the geophysical validation of ozone profile data retrieved from nadir UV backscatter satellite measurements is detailed and discussed, consisting of data set content studies, information content studies, co-location studies, and comparisons with reference measurements. Within the European Space Agency's Climate Change Initiative on ozone (Ozone_cci project), the proposed round-robin procedure is applied to two nadir ozone profile data sets retrieved at the Royal Netherlands Meteorological Institute (KNMI) and the Rutherford Appleton Laboratory (RAL, United Kingdom), using their respective OPERA v1.26 and RAL v2
Abstract. This paper documents the tropospheric chemical mechanism scheme used in the TOMCAT 3-D chemical transport model. The current scheme includes a more detailed representation of hydrocarbon chemistry than previously included in the model, with the inclusion of the emission and oxidation of ethene, propene, butane, toluene and monoterpenes. The model is evaluated against a range of surface, balloon, aircraft and satellite measurements. The model is generally able to capture the main spatial and seasonal features of high and low concentrations of carbon monoxide (CO), ozone (O 3 ), volatile organic compounds (VOCs) and reactive nitrogen. However, model biases are found in some species, some of which are common to chemistry models and some that are specific to TOMCAT and warrant further investigation. The most notable of these biases are (1) a negative bias in Northern Hemisphere (NH) winter and spring CO and a positive bias in Southern Hemisphere (SH) CO throughout the year, (2) a positive bias in NH O 3 in summer and a negative bias at high latitudes during SH winter and (3) a negative bias in NH winter C 2 and C 3 alkanes and alkenes. TOMCAT global mean tropospheric hydroxyl radical (OH) concentrations are higher than estimates inferred from observations of methyl chloroform but similar to, or lower than, multi-model mean concentrations reported in recent model intercomparison studies. TOMCAT shows peak OH concentrations in the tropical lower troposphere, unlike other models which show peak concentrations in the tropical upper troposphere. This is likely to affect the lifetime and transport of important trace gases and warrants further investigation.
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