Abstract. Three types of reference simulations, as recommended by the Chemistry-Climate Model Initiative (CCMI), have been performed with version 2.51 of the European Centre for Medium-Range Weather Forecasts -Hamburg (ECHAM)/Modular Earth Submodel System (MESSy) Atmospheric Chemistry (EMAC) model: hindcast simulations , hindcast simulations with specified dynamics , i.e. nudged towards ERA-Interim reanalysis data, and combined hindcast and projection simulations . The manuscript summarizes the updates of the model system and details the different model set-ups used, including the on-line calculated diagnostics. Simulations have been performed with two different nudging setups, with and without interactive tropospheric aerosol, and with and without a coupled ocean model. Two different vertical resolutions have been applied. The on-line calculated sources and sinks of reactive species are quantified and a first evaluation of the simulation results from a global perspective is provided as a quality check of the data. The focus is on the intercomparison of the different model set-ups. The simulation data will become publicly available via CCMI and the Climate and Environmental Retrieval and Archive (CERA) database of the German Climate Computing Centre (DKRZ). This manuscript is intended to serve as an extensive reference for further analyses of the Earth System Chemistry integrated Modelling (ESCiMo) simulations.

We present version 4.0 of the atmospheric chemistry box model CAABA/MECCA that now includes a number of new features: (i) skeletal mechanism reduction, (ii) the Mainz Organic Mechanism (MOM) chemical mechanism for volatile organic compounds, (iii) an option to include reactions from the Master Chemical Mechanism (MCM) and other chemical mechanisms, (iv) updated isotope tagging, and (v) improved and new photolysis modules (JVAL, RAD-JIMT, DISSOC). Further, when MECCA is connected to a global model, the new feature of coexisting multiple chemistry mechanisms (PolyMECCA/CHEMGLUE) can be used. Additional changes have been implemented to make the code more user-friendly and to facilitate the analysis of the model results. Like earlier versions, CAABA/MECCA-4.0 is a community model published under the GNU General Public License.

Abstract. Four simulations with the ECHAM/MESSy Atmospheric Chemistry (EMAC) model have been evaluated with the Earth System Model Validation Tool (ESMValTool) to identify differences in simulated ozone and selected climate parameters that resulted from (i) different setups of the EMAC model (nudged vs. free-running) and (ii) different boundary conditions (emissions, sea surface temperatures (SSTs) and sea ice concentrations (SICs)). To assess the relative performance of the simulations, quantitative performance metrics are calculated consistently for the climate parameters and ozone. This is important for the interpretation of the evaluation results since biases in climate can impact on biases in chemistry and vice versa. The observational data sets used for the evaluation include ozonesonde and aircraft data, meteorological reanalyses and satellite measurements. The results from a previous EMAC evaluation of a model simulation with nudging towards realistic meteorology in the troposphere have been compared to new simulations with different model setups and updated emission data sets in free-running time slice and nudged quasi chemistrytransport model (QCTM) mode. The latter two configurations are particularly important for chemistry-climate projections and for the quantification of individual sources (e.g., the transport sector) that lead to small chemical perturbations of the climate system, respectively. With the exception of some specific features which are detailed in this study, no large differences that could be related to the different setups (nudged vs. free-running) of the EMAC simulations were found, which offers the possibility to evaluate and improve the overall model with the help of shorter nudged simulations. The main differences between the two setups is a better representation of the tropospheric and stratospheric temperature in the nudged simulations, which also better reproduce stratospheric water vapor concentrations, due to the improved simulation of the temperature in the tropical tropopause layer. Ozone and ozone precursor concentrations, on the other hand, are very similar in the different model setups, if similar boundary conditions are used. Different boundary conditions however lead to relevant differences in the four simulations. Biases which are common to all simulations are the underestimation of the ozone hole and the overestimation of tropospheric column ozone, the latter being significantly reduced when lower lightning emissions of nitrogen oxides are used. To further investigate possible other reasons for such bias, two sensitivity simulations with an updated scavenging routine and the addition of a newly proposed HNO 3 -forming channel of the HO 2 + NO reaction were performed. The update in the scavenging routine resulted in a slightly better representation of ozone compared to the reference simulation. The introduction of the new HNO 3 -forming channel significantly reduces the overestimation of tropospheric ozone. Therefore, including the new reaction rate could potentially...

Abstract. Methane (CH4) is the second-most important directly emitted greenhouse gas, the atmospheric concentration of which is influenced by human activities. In this study, numerical simulations with the chemistry–climate model (CCM) EMAC are performed, aiming to assess possible consequences of significantly enhanced CH4 concentrations in the Earth's atmosphere for the climate. We analyse experiments with 2×CH4 and 5×CH4 present-day (2010) mixing ratio and its quasi-instantaneous chemical impact on the atmosphere. The massive increase in CH4 strongly influences the tropospheric chemistry by reducing the OH abundance and thereby extending the CH4 lifetime as well as the residence time of other chemical substances. The region above the tropopause is impacted by a substantial rise in stratospheric water vapour (SWV). The stratospheric ozone (O3) column increases overall, but SWV-induced stratospheric cooling also leads to a enhanced ozone depletion in the Antarctic lower stratosphere. Regional patterns of ozone change are affected by modification of stratospheric dynamics, i.e. increased tropical upwelling and stronger meridional transport towards the polar regions. We calculate the net radiative impact (RI) of the 2×CH4 experiment to be 0.69 W m−2, and for the 5×CH4 experiment to be 1.79 W m−2. A substantial part of the RH is contributed by chemically induced O3 and SWV changes, in line with previous radiative forcing estimates. To our knowledge this is the first numerical study using a CCM with respect to 2- and 5-fold CH4 concentrations and it is therefore an overdue analysis as it emphasizes the impact of possible strong future CH4 emissions on atmospheric chemistry and its feedback on climate.

Three types of reference simulations, as recommended by the Chemistry–Climate Model Initiative (CCMI), have been performed with version 2.51 of the European Centre for Medium-Range Weather Forecasts – Hamburg (ECHAM)/Modular Earth Submodel System (MESSy) Atmospheric Chemistry (EMAC) model: hindcast simulations (1950–2011), hindcast simulations with specified dynamics (1979–2013), i.e. nudged towards ERA-Interim reanalysis data, and combined hindcast and projection simulations (1950–2100). The manuscript summarizes the updates of the model system and details the different model set-ups used, including the on-line calculated diagnostics. Simulations have been performed with two different nudging setups, with and without interactive tropospheric aerosol, and with and without a coupled ocean model. Two different ver- tical resolutions have been applied. The on-line calculated sources and sinks of reactive species are quantified and a first evaluation of the simulation results from a global perspective is provided as a quality check of the data. The focus is on the intercomparison of the different model set-ups. The simulation data will become publicly available via CCMI and the Climate and Environmental Retrieval and Archive (CERA) database of the German Climate Computing Centre (DKRZ). This manuscript is intended to serve as an extensive reference for further analyses of the Earth System Chemistry integrated Modelling (ESCiMo) simulations