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The modeling study presented here aims to estimate how uncertainties in global hydroxyl radical (OH) distributions, variability, and trends may contribute to resolving discrepancies between simulated and observed methane (CH4) changes since 2000. A multi-model ensemble of 14 OH fields was analyzed and aggregated into 64 scenarios to force the offline atmospheric chemistry transport model LMDz (Laboratoire de Meteorologie Dynamique) with a standard CH4 emission scenario over the period 2000–2016. The multi-model simulated global volume-weighted tropospheric mean OH concentration ([OH]) averaged over 2000–2010 ranges between 8.7×105 and 12.8×105 molec cm−3. The inter-model differences in tropospheric OH burden and vertical distributions are mainly determined by the differences in the nitrogen oxide (NO) distributions, while the spatial discrepancies between OH fields are mostly due to differences in natural emissions and volatile organic compound (VOC) chemistry. From 2000 to 2010, most simulated OH fields show an increase of 0.1–0.3×105 molec cm−3 in the tropospheric mean [OH], with year-to-year variations much smaller than during the historical period 1960–2000. Once ingested into the LMDz model, these OH changes translated into a 5 to 15 ppbv reduction in the CH4 mixing ratio in 2010, which represents 7 %–20 % of the model-simulated CH4 increase due to surface emissions. Between 2010 and 2016, the ensemble of simulations showed that OH changes could lead to a CH4 mixing ratio uncertainty of >±30 ppbv. Over the full 2000–2016 time period, using a common state-of-the-art but nonoptimized emission scenario, the impact of [OH] changes tested here can explain up to 54 % of the gap between model simulations and observations. This result emphasizes the importance of better representing OH abundance and variations in CH4 forward simulations and emission optimizations performed by atmospheric inversions., Atmospheric Chemistry and Physics, 19 (21), ISSN:1680-7375, ISSN:1680-7367

o estimate the impact of emissions by road, aircraft and ship traffic on ozone and OH in the present-day atmosphere six different atmospheric chemistry models have been used. Based on newly developed global emission inventories for road, ship and aircraft emission data sets each model performed sensitivity simulations reducing the emissions of each transport sector by 5%. The model results indicate that on global annual average lower tropospheric ozone responds most sensitive to ship emissions (50.6%±10.9% of the total traffic induced perturbation), followed by road (36.7%±9.3%) and aircraft exhausts (12.7%±2.9%), respectively. In the northern upper troposphere between 200–300 hPa at 30–60° N the maximum impact from road and ship are 93% and 73% of the maximum effect of aircraft, respectively. The latter is 0.185 ppbv for ozone (for the 5% case) or 3.69 ppbv when scaling to 100%. On the global average the impact of road even dominates in the UTLS-region. The sensitivity of ozone formation per NOx molecule emitted is highest for aircraft exhausts. The local maximum effect of the summed traffic emissions on the ozone column predicted by the models is 0.2 DU and occurs over the northern subtropical Atlantic extending to central Europe. Below 800 hPa both ozone and OH respond most sensitively to ship emissions in the marine lower troposphere over the Atlantic. Based on the 5% perturbation the effect on ozone can exceed 0.6% close to the marine surface (global zonal mean) which is 80% of the total traffic induced ozone perturbation. In the southern hemisphere ship emissions contribute relatively strongly to the total ozone perturbation by 60%–80% throughout the year. Methane lifetime changes against OH are affected strongest by ship emissions up to 0.21 (± 0.05)%, followed by road (0.08 (±0.01)%) and air traffic (0.05 (± 0.02)%). Based on the full scale ozone and methane perturbations positive radiative forcings were calculated for road emissions (7.3±6.2 mWm−2) and for aviation (2.9±2.3 mWm−2). Ship induced methane lifetime changes dominate over the ozone forcing and therefore lead to a net negative forcing (−25.5±13.2 mWm−2)., Atmospheric Chemistry and Physics, 9 (9), ISSN:1680-7375, ISSN:1680-7367

This is the second part of a rigorous model evaluation study involving five global Chemistry-Transport and two Chemistry-Climate Models operated by different groups in Europe. Simulated trace gas fields were interpolated to the exact times and positions of the observations to account for the actual weather conditions and hence for the specific histories of the sampled air masses. In this part of the study we focus on a detailed comparison with two selected campaigns, PEM-Tropics A and SONEX, contrasting the clean environment of the tropical Pacific with the more polluted North Atlantic region. The study highlights the different strengths and weaknesses of the models in accurately simulating key processes in the UT/LS region including stratosphere-troposphere-exchange, rapid convective transport, lightning emissions, radical chemistry and ozone production. Model simulated Radon, which was used as an idealized tracer for continental influence, was occasionally much better correlated with measured CO than simulated CO pointing towards deficiencies in the used biomass burning emission fields. The abundance and variability of HOx radicals is in general well represented in the models as inferred directly from the comparison with measured OH and HO2 and indirectly from the comparison with hydrogen peroxide concentrations. Components of the NOy family such as PAN, HNO3 and NO were found to compare less favorably. Interestingly, models showing good agreement with observations in the case of PEM-Tropics A often failed in the case of SONEX and vice versa. A better description of NOx and NOy emissions, chemistry and sinks is thought to be key to future model improvements with respect to the representation of chemistry in the UT/LS region., Atmospheric Chemistry and Physics, 5 (1), ISSN:1680-7375, ISSN:1680-7367

A rigorous evaluation of five global Chemistry-Transport and two Chemistry-Climate Models operated by several different groups in Europe, was performed. Comparisons were made of the models with trace gas observations from a number of research aircraft measurement campaigns during the four-year period 1995-1998. Whenever possible the models were run over the same four-year period and at each simulation time step the instantaneous tracer fields were interpolated to all coinciding observation points. This approach allows for a very close comparison with observations and fully accounts for the specific meteorological conditions during the measurement flights. This is important considering the often limited availability and representativity of such trace gas measurements. A new extensive database including all major research and commercial aircraft measurements between 1995 and 1998, as well as ozone soundings, was established specifically to support this type of direct comparison. Quantitative methods were applied to judge model performance including the calculation of average concentration biases and the visualization of correlations and RMS errors in the form of so-called Taylor diagrams. We present the general concepts applied, the structure and content of the database, and an overall analysis of model skills over four distinct regions. These regions were selected to represent various atmospheric conditions and to cover large geographical domains such that sufficient observations are available for comparison. The comparison of model results with the observations revealed specific problems for each individual model. This study suggests the further improvements needed and serves as a benchmark for re-evaluations of such improvements. In general all models show deficiencies with respect to both mean concentrations and vertical gradients of important trace gases. These include ozone, CO and NOx at the tropopause. Too strong two-way mixing across the tropopause is suggested to be the main reason for differences between simulated and observed CO and ozone values. The generally poor correlations between simulated and measured NOx values suggest that in particular the NOx input by lightning and the convective transport from the polluted boundary layer are still not well described by current parameterizations, which may lead to significant differences in the spatial and seasonal distribution of NOx in the models. Simulated OH concentrations, on the other hand, were found to be in surprisingly good agreement with measured values., Atmospheric Chemistry and Physics, 3 (5), ISSN:1680-7375, ISSN:1680-7367