Geosci. Model Dev., 7, 2435?2475, 2014 www.geosci-model-dev.net/7/2435/2014/ doi:10.5194/gmd-7-2435-2014 ? Author(s) 2014. CC Attribution 3.0 License. Simulation of tropospheric chemistry and aerosols with the climate model EC-Earth T. P. C. van Noije1, P. Le Sager1, A. J. Segers2, P. F. J. van Velthoven1, M. C. Krol3,4, W. Hazeleger1,3, A. G. Williams5, and S. D. Chambers5 1Royal Netherlands Meteorological Institute, De Bilt, the Netherlands 2Netherlands Organisation for Applied Scientific Research (TNO), Utrecht, the Netherlands 3Wageningen University, Wageningen, the Netherlands 4Institute for Marine and Atmospheric Research Utrecht, Utrecht University, Utrecht, the Netherlands 5Institute for Environmental Research, Australian Nuclear Science and Technology Organisation, Lucas Heights, Australia Correspondence to: T. P. C. van Noije (noije@knmi.nl) Received: 20 February 2014 ? Published in Geosci. Model Dev. Discuss.: 25 March 2014 Revised: 1 September 2014 ? Accepted: 15 September 2014 ? Published: 22 October 2014 Abstract. We have integrated the atmospheric chemistry and transport model TM5 into the global climate model EC-Earth version 2.4. We present an overview of the TM5 model and the two-way data exchange between TM5 and the IFS model from the European Centre for Medium-Range Weather Forecasts (ECMWF), the atmospheric general cir- culation model of EC-Earth. In this paper we evaluate the simulation of tropospheric chemistry and aerosols in a one- way coupled configuration. We have carried out a decadal simulation for present-day conditions and calculated chem- ical budgets and climatologies of tracer concentrations and aerosol optical depth. For comparison we have also per- formed offline simulations driven by meteorological fields from ECMWF?s ERA-Interim reanalysis and output from the EC-Earth model itself. Compared to the offline simula- tions, the online-coupled system produces more efficient ver- tical mixing in the troposphere, which reflects an improve- ment of the treatment of cumulus convection. The chem- istry in the EC-Earth simulations is affected by the fact that the current version of EC-Earth produces a cold bias with too dry air in large parts of the troposphere. Compared to the ERA-Interim driven simulation, the oxidizing capacity in EC-Earth is lower in the tropics and higher in the extrat- ropics. The atmospheric lifetime of methane in EC-Earth is 9.4 years, which is 7 % longer than the lifetime obtained with ERA-Interim but remains well within the range reported in the literature. We further evaluate the model by comparing the simulated climatologies of surface radon-222 and carbon monoxide, tropospheric and surface ozone, and aerosol opti- cal depth against observational data. The work presented in this study is the first step in the development of EC-Earth into an Earth system model with fully interactive atmospheric chemistry and aerosols. 1 Introduction Chemically reactive gases and aerosols play important roles in the climate system. They affect the Earth?s energy balance by direct interaction with radiation and in various indirect ways. Ozone (O3) absorbs both solar (shortwave) and terrestrial (longwave) radiation. The absorption of ultraviolet and vis- ible radiation by ozone causes solar heating in the strato- sphere, and the absorption of thermal infrared radiation makes ozone an important greenhouse gas. Depletion of stratospheric ozone has been the main cause for the observed cooling of the lower stratosphere since the 1980s (Forster et al., 2011). Although the impact on the global radiation balance of the troposphere is thought to be relatively small (Myhre et al., 2013b), stratospheric ozone depletion has been identified as an important driver of tro- pospheric circulation changes in the Southern Hemisphere (e.g. Gillett and Thompson, 2003; Arblaster and Meehl, 2006; Polvani et al., 2011) and of circulation changes in the Southern Ocean (Sigmond et al., 2011). This may also have Published by Copernicus Publications on behalf of the European Geosciences Union. 2436 T. P. C. van Noije et al.: Simulation of chemistry and aerosols with EC-Earth reduced the uptake of carbon dioxide (CO2) by the Southern Ocean (Lenton et al., 2009). It is anticipated that the expected recovery of the ozone layer in the coming decades will tend to reverse these trends (Perlwitz et al., 2008; Son et al., 2008; Sigmond et al., 2011). Ozone is not directly emitted into the atmosphere. In the troposphere it is produced by oxidation of carbon monoxide (CO), methane (CH4), and other volatile organic compounds (VOCs), in the presence of nitrogen oxides (NOx =NO+NO2). Increases in tropospheric ozone since the preindustrial era have contributed substantially to global warming by direct radiative effects (Stevenson et al., 2013; Myhre et al., 2013b), especially in the Northern Hemisphere (Mickley et al., 2004; Shindell et al., 2006a). Moreover, in- creases in ground-level ozone may have contributed to global warming by reducing the CO2 uptake by vegetation (Felzer et al., 2005; Sitch et al., 2007; Arneth et al., 2013), but the im- portance of this effect is still uncertain (Myhre et al., 2013b). Methane itself strongly absorbs thermal infrared radiation and is therefore a very potent greenhouse gas. Methane is also important as a precursor of stratospheric water vapour. Increases in methane concentrations have contributed sub- stantially to global warming, and increases in the anthro- pogenic methane emissions even more so (Shindell et al., 2009; Myhre et al., 2013b). Aerosols affect the Earth?s radiation budget by scattering and absorption of sunlight, by absorption of thermal infrared radiation, and by interactions with clouds. Scattering tends to increase the planetary albedo and has a cooling effect. Absorption, on the other hand, causes warming in the atmo- sphere. The importance of scattering versus absorption de- pends on the chemical composition, mixing state, size distri- bution, particle shapes, and vertical distribution of the aerosol mixture, as well as on the presence of clouds and the surface albedo. Absorption of infrared radiation mainly takes place through coarse-mode aerosols, and is most relevant for stratospheric aerosols resulting from large volcanic eruptions (Arfeuille et al., 2013), and for tropospheric aerosols contain- ing mineral dust or sea salt (Jacobson, 2001). The shortwave radiative effects of aerosols are generally considered to be more important for the climate (Myhre et al., 2013a, b). Black carbon (Petzold et al., 2013) strongly absorbs sun- light, which makes it an important warming agent (Bond et al., 2013). Sulfate, nitrate, and sea salt only weakly absorb sunlight and are mainly scattering. Mineral dust and organic aerosols vary from weakly to strongly absorbing, depending on their composition and the wavelength of the light. Light absorbing aerosols such as black carbon and mineral dust also have a warming effect when deposited on snow or ice (Myhre et al., 2013b). Aerosol?cloud interactions include the effects of aerosols on the albedo and the lifetime of clouds (Boucher et al., 2013). Overall, aerosol?cloud interactions are thought to have a cooling effect (Myhre et al., 2013b). Due to the difficulty of characterizing the concentrations and properties of aerosols and the complexities involved in the processes that determine their effects on the climate, aerosols still are a major source of uncertainty in our un- derstanding of climate change. It is generally believed that increases in anthropogenic aerosols since the preindustrial era have slowed down global warming, but it is highly un- certain by how much (Myhre et al., 2013b). Moreover, the cooling effect of increases in sulfate and other weakly ab- sorbing aerosols, such as organic aerosols and nitrate, has been largely compensated by a substantial warming effect due to increases in black carbon (Bond et al., 2013). Aerosols and chemically reactive gases are coupled in var- ious ways. Many aerosol components are produced from gaseous precursors by chemical reactions and nucleation or condensation processes in the atmosphere. Sulfate (SO4), ni- trate (NO3) and ammonium (NH4) result from emissions of sulfur dioxide (SO2), dimethyl sulfide (DMS), NOx, and am- monia (NH3), and secondary organic aerosols (SOA) from emissions of VOCs. Nitrate, ammonium and many organic aerosol components are semi-volatile and exist in equilib- rium with their gas-phase counterparts. Moreover, aerosols have an influence on photolysis rates by scattering and ab- sorption of ultraviolet light and by their impacts on clouds. They also provide particle surfaces on which heterogeneous chemical reactions can take place. Deposition of chemically reactive gases and aerosols from the atmosphere is a source of nutrients to the terrestrial and marine biosphere. The biogeochemical cycles of nitrogen and carbon are tightly coupled, and it is likely that the avail- ability of reactive nitrogen will be a limiting factor for the land carbon sink in the twenty-first century (Ciais et al., 2013). Despite the important role aerosols and chemically re- active gases play in the climate system, the description of atmospheric chemistry and aerosols varies strongly among climate models. Most global models that participated in the recent Coupled Model Intercomparison Project Phase 5 (CMIP5) (Taylor et al., 2012) did not include atmospheric chemistry and many did not have fully interactive aerosols (Flato et al., 2013). Even so, atmospheric or atmosphere? ocean general circulation models (GCMs) are increasingly being transformed into chemistry-climate models (CCMs) with interactive representations of chemistry and aerosols (e.g. Zhang, 2008; Dameris and J?ckel, 2013; Lamarque et al., 2012). The work presented in this paper is the first step in the de- velopment of an interactive chemistry module in the global climate model EC-Earth (Hazeleger et al., 2010, 2012). EC-Earth is a relatively new climate model that has been developed in recent years by a consortium of partner in- stitutes from currently ten European countries, consisting of the national meteorological services of Denmark, Ire- land, the Netherlands, Portugal, Spain and Sweden, uni- versities, high-performance computing centres, and other Geosci. Model Dev., 7, 2435?2475, 2014 www.geosci-model-dev.net/7/2435/2014/ T. P. C. van Noije et al.: Simulation of chemistry and aerosols with EC-Earth 2437 research institutes. The atmospheric GCM of EC-Earth is based on the Integrated Forecasting System (IFS) model from the European Centre for Medium-Range Weather Fore- casts (ECMWF). EC-Earth is used for seasonal to decadal predictions as well as for long-term climate simulations (see Hazeleger et al., 2010). The chemistry module of EC-Earth is based on the chem- istry and transport model TM5 (Krol et al., 2005; Huijnen et al., 2010; Aan de Brugh et al., 2011). We have integrated TM5 into EC-Earth by coupling it online to IFS. The model allows for two-way exchange of fields between TM5 and IFS, but in this paper we focus on the impact of the online integra- tion on the performance of TM5, without feedbacks to IFS. To this end, we have carried out a decadal simulation of tropospheric chemistry and aerosols for present-day condi- tions, and calculated seasonal climatologies of concentration fields and chemical budgets for various tracers. For compari- son, we have repeated this simulation with the stand-alone version of TM5 driven by meteorological fields from the ECMWF ERA-Interim reanalysis (Dee et al., 2011). We have evaluated the results from both simulations against a number of observational data sets. In Sect. 2 we briefly introduce the EC-Earth model and describe the most important aspects of TM5 and the data ex- change between TM5 and IFS. In Sect. 3 we describe the set-up of the online and offline simulations. An evaluation of the results is presented in Sect. 4. We end with a discussion and conclusions in Sect. 5. 2 Model description 2.1 EC-Earth version 2.3 The atmosphere?ocean GCM applied in this study is EC- Earth version 2.3. It consists of an atmospheric GCM based on the IFS model cycle 31r1 with the H-TESSEL land- surface scheme, and an ocean GCM from the Nucleus for Eu- ropean Modelling of the Ocean (NEMO) version 2 with the Louvain-la-Neuve sea ice model (LIM) version 2. The ex- change of two-dimensional fields between IFS?H-TESSEL and NEMO?LIM takes place through the OASIS3 coupler (Ocean Atmosphere Sea Ice Soil version 3). A description of these components and the coupling interface is given by Hazeleger et al. (2010, 2012). A number of improvements in physical parameterizations have been included from more recent cycles of IFS (see Hazeleger et al., 2012). In particular, the convection scheme has been updated to the formulation of cycle 32r3. A detailed description of the changes that are involved in this update is given by Bechtold et al. (2008). It has been shown that the new convection scheme produces higher and more realistic levels of convective activity over land, and leads to improve- ments in tropical precipitation patterns and extratropical circulation characteristics (Bechtold et al., 2008; Jung et al., 2010). EC-Earth version 2.3 has been used for CMIP5. Com- pared to the version described by Hazeleger et al. (2012), the aerosol forcings have been improved and made consis- tent with the CMIP5 recommendations (Taylor et al., 2012). In this study, we applied the same configuration as for the CMIP5 long-term simulations, using the T159 spectral res- olution (corresponding to 1.125?) with 62 vertical levels for the atmosphere and the ORCA1 grid (about 1? horizontal res- olution and 42 layers) for the ocean. 2.2 TM5 We have extended the atmosphere?ocean GCM version of EC-Earth with a module for simulating atmospheric chem- istry and transport, the Tracer Model 5 (TM5). The new model configuration with TM5 has been released as part of EC-Earth version 2.4. TM5 can be used for non-reactive greenhouse gases like CO2 (Peters et al., 2010) and sul- fur hexafluoride (SF6) (Peters et al., 2004), for diagnos- tic radioactive tracers like radon-222 (222Rn) and lead-210 (210Pb), as well as for chemically reactive gases and aerosols. The version used in this study is based on the tropospheric chemistry version documented by Huijnen et al. (2010), extended with the aerosol microphysics and optics mod- ules described by Aan de Brugh et al. (2011) and Aan de Brugh (2013). In this section we will give an overview of the main characteristics of this TM5 model version and briefly describe the most important modifications and improvements compared to these earlier publications. 2.2.1 Resolution The global atmospheric domain of TM5 is discretized on a regular latitude?longitude grid. To limit the computational costs, this grid will typically have a coarser resolution than the grid used in IFS. In this study a horizontal resolution of 3??2? (longitude?latitude) is used. Zoom regions with higher horizontal resolutions can be defined and nested into the global domain (Krol et al., 2005), but this option is not used in EC-Earth. To avoid the use of very short time steps near the poles, the number of grid cells in the zonal direc- tion is gradually reduced in the polar regions. Dry deposi- tion velocities and surface emission fluxes that depend on lo- cal meteorological conditions and/or other surface variables are calculated on a higher-resolution surface grid and subse- quently coarsened to the atmospheric grid. The resolution of the surface grid is currently 1??1?. In the vertical direction TM5 uses the same hybrid sigma- pressure levels as used in the IFS model version to which it is coupled, or a subset thereof. In the EC-Earth configuration applied in this study a selection of 31 levels is made out of the 62 levels used in IFS. Because of the relatively poor vertical resolution of the 62-level version of IFS in the upper part of www.geosci-model-dev.net/7/2435/2014/ Geosci. Model Dev., 7, 2435?2475, 2014 2438 T. P. C. van Noije et al.: Simulation of chemistry and aerosols with EC-Earth the domain (e.g. compared to the 60- or 91-level versions), no merging of levels is applied above ?100 hPa. The top of the model is at 5 hPa. 2.2.2 Data exchange and transformations As for the exchange between IFS and NEMO, the data ex- change between IFS and TM5 takes place through OASIS3 (Valcke, 2013). To prevent the different components having to wait for each other, IFS runs one exchange time interval ahead of the other modules. In the current configuration, the interval for the data exchange between TM5 and IFS is set to 6 h. A more frequent exchange will be applied in future versions of the model. Since OASIS3 can only deal with two-dimensional (2-D) fields, three-dimensional (3-D) fields are transferred layer by layer. The layers that are transferred from IFS to TM5 and vice versa correspond to the full vertical resolution of IFS. The required merging of the layers and interpolation of the data in the vertical direction is performed on the TM5 side. TM5 receives both meteorological data and surface prop- erty fields from IFS. The data sets employed in the chemistry version of TM5 used in this study are listed in Table 1. They include instantaneous, time-averaged, and constant fields. Most fields are interpolated by OASIS to TM5?s regu- lar latitude?longitude atmospheric or higher-resolution sur- face grid. However, to avoid unnecessary interpolations of the wind fields, the wind divergence and vorticity fields and the concurrent surface pressure field are received in their na- tive spectral representation and transformed into gridded air mass fluxes following the procedure of Segers et al. (2002). Here the vertical mass fluxes are calculated directly from the spectral fields, and the local mass balance over the exchange interval is closed by slightly adjusting the horizontal mass fluxes. This method has been shown to lead to superior chem- istry simulations compared to methods that make use of in- terpolated wind fields (Bregman et al., 2003). Most instantaneous fields transferred from IFS to TM5, including the spectral fields mentioned above, are valid for the middle of the exchange interval. However, for closing the mass balance the surface pressure is also required at the be- ginning and at the end of the interval. This is achieved by reading the initial surface pressure field from the TM5 restart file, and including an additional (gridded) surface pressure field valid for the end of the interval in the transfer. The system has also been prepared for data transfer in the other direction. The fields that can currently be transferred from TM5 to IFS are the ozone and methane concentra- tions, the particle number and component-specific mass con- centrations in the different aerosol modes (see below), and aerosol optical property fields (extinction, single-scattering albedo and asymmetry factor) at the wavelengths used in the IFS shortwave radiation scheme. Because IFS runs ahead of TM5, these forcing fields are applied with some delay in IFS. To minimize this delay, they are treated as instantaneous fields calculated at the end of the exchange interval. This re- duces the delay to half an exchange time step on average. In this paper we first evaluate the one-way coupled simula- tion of chemistry and aerosols. In a forthcoming publication two-way coupling will be applied, including feedbacks of the TM5 forcing fields to the radiation and cloud scheme of IFS. 2.2.3 Transport Tracers in TM5 are moved around by advection, cumulus convection, and vertical diffusion. Tracer advection is de- scribed using either the first-order moments (slopes) algo- rithm developed by Russell and Lerner (1981) or the second- order moments scheme by Prather (1986). Both schemes are conserving the mass of the advected tracers. This is an im- portant requirement especially for chemistry-climate simula- tions, where the tracer concentrations are not constrained by assimilation. The default option is to use the slopes scheme, which is used in the simulations presented in this study. Convective tracer transport in TM5 is described using a bulk mass flux approach, in which clouds are represented by a single pair of entraining and detraining plumes describing the updraft and downdraft motions. The meteorological fields involved in the calculation are the vertical air mass fluxes and the entrainment and detrainment rates in the updrafts and downdrafts. In EC-Earth the mass fluxes and detrain- ment rates are taken from IFS. The corresponding entrain- ment rates follow from mass conservation. Thus, the descrip- tion of convective tracer transport in TM5 is fully consistent with the representation of convection in IFS. Vertical diffusion of tracers in TM5 is described with a first-order closure scheme, where the diffusion coefficient is assumed to be the same as for heat (Olivi? et al., 2004a). In the free troposphere it is computed based on wind shear and static stability following Louis (1979). In the bound- ary layer it is based on the revised Louis?Tiedtke?Geleyn (LTG) scheme of Holtslag and Boville (1993). The bound- ary layer height is calculated following Vogelezang and Holt- slag (1996). Details are given in Olivi? et al. (2004a). 2.2.4 Chemistry The TM5 version applied in this study is designed to sim- ulate the concentrations of reactive gases and aerosols in the troposphere and their deposition to the Earth?s surface. The model?s gas-phase, aqueous-phase, and heterogeneous chemistry schemes are described by Huijnen et al. (2010). Details on the aqueous-phase chemistry can be found in Roelofs (1992) and Feichter et al. (1996). The gas-phase reaction scheme, representing the oxidation of CO, CH4, and non-methane volatile organic compounds (NMVOCs) in the presence of NOx, is based on the Carbon Bond Mechanism 4 (CBM4). It utilizes a structural-lumping technique in which organic species are grouped into one or more surrogate categories according to the carbon bond types Geosci. Model Dev., 7, 2435?2475, 2014 www.geosci-model-dev.net/7/2435/2014/ T. P. C. van Noije et al.: Simulation of chemistry and aerosols with EC-Earth 2439 Table 1. Meteorological data and surface property fields transferred from IFS to TM5. Field Type Three-dimensional Wind divergence/vorticity Instantaneous Temperature Instantaneous Specific humidity Instantaneous Cloud liquid/ice water content Instantaneous Cloud fraction Instantaneous Overhead/underfoot cloud fraction Instantaneous Updraught/downdraught convective air mass flux Average Updraught/downdraught convective air mass detrainment rate Average Two-dimensional Surface pressure Instantaneous 10 m wind (west?east/south?north components) Instantaneous 2 m temperature Instantaneous 2 m dew point temperature Instantaneous Surface east?west/north?south momentum stress Average Surface sensible/latent heat flux Average Surface solar radiation Average Stratiform precipitation as rain Average Convective precipitation as rain Average Skin reservoir water content Instantaneous Snow depth Instantaneous Soil wetness in top soil layer Instantaneous Low/high vegetation cover fractions Instantaneous Vegetation type fractions Instantaneous Surface roughness Instantaneous Surface orography Constant Land/sea fraction Constant Sea-ice fraction Instantaneous present in the molecule. CBM4 was originally developed for simulating urban and regional photochemistry (Gery et al., 1989), and was later extended to the global scale by including reactions important under background conditions (Houwel- ing et al., 1998). Since then, reaction rates and product dis- tributions have been updated (see Huijnen et al., 2010). In addition to CBM4, the gas-phase chemistry scheme in TM5 also includes reactions for the oxidation of SO2, DMS, and NH3. Photolysis rates are calculated based on the parameteriza- tion of Landgraf and Crutzen (1998), using seven wavelength bands between 202.0 and 752.5 nm. Variations due to the ef- fects of clouds, overhead ozone, and surface albedo are in- cluded following Krol and van Weele (1997). Aqueous-phase chemistry in clouds is included for the ox- idation of total dissolved sulfur dioxide, S(IV), by dissolved hydrogen peroxide (H2O2) and O3, depending on the acid- ity of the droplets. The sulfate production rates due to the oxidation of S(IV) by H2O2 and O3 are calculated follow- ing Martin and Damschen (1981), with a temperature depen- dence from Nair and Peters (1989), and Maahs (1983), re- spectively. The representation of heterogeneous chemistry is currently limited to the reactive uptake of dinitrogen pentox- ide (N2O5) at the surface of cloud droplets, cirrus particles, and aerosols, which produces nitric acid (HNO3) (Dentener and Crutzen, 1993). 2.2.5 Aerosols Aerosols are represented in the model as described by Aan de Brugh et al. (2011). Sulfate, black carbon (BC), organic carbon (OC), sea salt and mineral dust are described with the size-resolved modal microphysics scheme M7 (Vignati et al., 2004). It uses seven log-normal size distributions or modes with predefined geometric standard deviations. There are four water-soluble modes (nucleation, Aitken, accumula- tion, and coarse) and three insoluble modes (Aitken, accumu- lation and coarse). The nucleation mode contains only SO4 particles with dry diameters smaller than 10 nm. The Aitken, accumulation, and coarse modes represent particles with dry diameters in the range 10?100 nm, 100 nm?1 ?m, and larger than 1 ?m, respectively. The insoluble Aitken mode consists of internally mixed particles of BC and OC, while the larger insoluble modes contain only dust particles. The soluble www.geosci-model-dev.net/7/2435/2014/ Geosci. Model Dev., 7, 2435?2475, 2014 2440 T. P. C. van Noije et al.: Simulation of chemistry and aerosols with EC-Earth Aitken mode represents internal mixtures of sulfate, BC, and OC, while the larger soluble modes also contain sea salt and dust in the mixture. Each mode is characterized by the total particle number and the mass of each component. With this the total number of aerosol tracers in M7 amounts to 25. The microphysical processes included in M7 are the formation of new SO4 particles by nucleation from gaseous sulfuric acid (H2SO4), condensation of H2SO4 onto existing particles, wa- ter uptake, and intramodal and intermodal coagulation. Of organic aerosols (OA), also known as particulate or- ganic matter (POM), only the carbon component is included in M7. To account for the other components that may be present, in TM5 the dry mass of organic aerosols is assumed to be 40 % higher than the OC mass (e.g. Dentener et al., 2006; Kinne et al., 2006). The current chemistry scheme does not describe the for- mation of secondary organic aerosols. An additional source of organic aerosols is therefore included near the sur- face over land, representing SOA formation from biogenic NMVOCs (mainly mono-terpenes) on timescales of a few hours. The total mass of SOA being formed is prescribed us- ing monthly fields from Dentener et al. (2006), which amount to 19.1 Tg POM year?1. The freshly formed SOA particles are assumed soluble and are added to the soluble Aitken mode, as in Aan de Brugh et al. (2011). The other aerosol components included in the model are nitrate, ammonium, and methane sulfonic acid (MSA), which is produced in the oxidation of DMS. These are repre- sented by their total mass, i.e. using a bulk aerosol approach. The gas?aerosol partitioning of the semi-volatile inorganic species (i.e. the ratios between HNO3 and nitrate aerosol and between NH3 and NH4) is described with the thermo- dynamic equilibrium model EQSAM (Metzger et al., 2002). The optical properties of the aerosol mixtures are calcu- lated as a function of wavelength based on Mie theory, using a look-up table (Aan de Brugh et al., 2011; Aan de Brugh, 2013). The optical effects of nitrate aerosol are included by assuming that the ammonium nitrate and the water absorbed by it are present in the soluble accumulation mode (Aan de Brugh et al., 2011). Effective-medium approximations are applied to calculate the refractive indices of the internally mixed modes. Sulfate, nitrate, OC, sea salt, and water are treated as homogeneous mixtures described by the Brugge- man mixing rule. When BC and/or dust are present in the mix, these are treated as inclusions in a homogeneous back- ground medium, using the Maxwell?Garnett mixing rule. A more detailed description of the optics module of TM5 is given by Aan de Brugh (2013). 2.2.6 Radioactive tracers In addition to reactive gases and aerosols, the model also in- cludes the diagnostic radioactive tracers radon-222 and lead- 210. Radon-222 is chemically inert and insoluble in water. It is emitted at a relatively uniform rate from the continental crust and decays with a half-life of 3.8 days into lead-210. Because of its short lifetime, radon-222 can be used to study rapid vertical exchange from the continental boundary layer to the free troposphere and further transport to more remote parts of the atmosphere (see reviews in Zahorowski et al., 2004; Williams et al., 2011). Lead-210 has a much longer half-life (22.3 years). After being formed, it rapidly attaches to submicron aerosol particles. As a consequence, lead-210 is mainly removed from the atmosphere by wet deposition and can be used to diagnose the wet scavenging processes in the model. 2.2.7 Dry and wet deposition Dry deposition of gases and aerosols to the Earth?s surface in TM5 is described using a standard resistance approach (e.g. Seinfeld and Pandis, 2006). Dry deposition velocities of gaseous species are calculated as the inverse of the sum of an aerodynamic resistance, a quasi-laminar sublayer resis- tance and a surface resistance. The surface resistance is cal- culated following the method of Wesely (1989), which dis- tinguishes between deposition to vegetation, bare soils, wa- ter or wet surfaces, and snow or ice, and combines the vari- ous deposition pathways into a total surface resistance. The gas-phase deposition scheme is described in more detail by Ganzeveld and Lelieveld (1995) and Ganzeveld et al. (1998). An overview is given in Huijnen et al. (2010). Dry deposition velocities of aerosols are determined by the aerodynamic resistance and a quasi-laminar sublayer re- sistance, enhanced by sedimentation of particles by gravi- tational settling. The quasi-laminar sublayer resistance de- pends on particle size and is calculated for land and sea sur- faces following Slinn (1976) and Slinn and Slinn (1980), respectively. The implementation for the M7 modes is de- scribed by Aan de Brugh et al. (2011). The wet deposition scheme in TM5 describes the removal of gases and aerosols from the atmosphere by raining clouds, and distinguishes between convective and large-scale strati- form precipitation. Scavenging by precipitation formation in convective clouds is included in the convective mass trans- port operator as part of the mass fluxes entrained in the cu- mulus updrafts (Balkansi et al., 1993; Guelle et al., 1998). Aerosols and irreversibly soluble gases are assumed to be completely scavenged in vigorous convective updrafts, while the removal efficiencies of other gases are reduced depend- ing on their solubility. Resolution dependencies are reduced by scaling down the convective scavenging rates for all trac- ers, depending on the grid-cell mean convective precipitation at the surface (see Vignati et al., 2010a). For stratiform precipitation both in-cloud and below-cloud scavenging of gases and aerosols are considered as de- scribed by Roelofs and Lelieveld (1995) and Jeuken et al. (2001). Scavenging by precipitation formation inside stratiform clouds is assumed to be five times less effective for ice particles than for liquid droplets. In-cloud scavenging Geosci. Model Dev., 7, 2435?2475, 2014 www.geosci-model-dev.net/7/2435/2014/ T. P. C. van Noije et al.: Simulation of chemistry and aerosols with EC-Earth 2441 of aerosols is included only for the soluble accumulation and coarse modes, and for bulk aerosols like ammonium, nitrate, MSA, and lead-210. The in-cloud scavenging coefficients for the soluble accumulation and coarse modes are assumed to be equal to the values for irreversibly soluble gases, while for bulk aerosols they are reduced by 30 % to account for the presence of interstitial aerosols (Vignati et al., 2010a). Below-cloud scavenging of aerosols is modelled using es- timates of bulk washout coefficients for the various modes based on Dana and Hales (1976). Resolution dependencies in wet removal by stratiform precipitation are reduced by the introduction of a mixing timescale, which delays the subgrid- scale mixing between cloudy and cloud-free regions (see Vignati et al., 2010a). 2.2.8 Boundary conditions A detailed description of stratospheric chemistry is not in- cluded in the model. To simulate stratospheric ozone chem- istry a parameterized linear chemistry scheme can be used (Cariolle and Teyss?dre, 2007; McLinden et al., 2000; Van Noije et al., 2004, 2006). Alternatively, the O3 concentrations in the stratosphere can simply be relaxed towards observa- tional values, as described in Huijnen et al. (2010). In the current relaxation scheme, total O3 column estimates from a multi-sensor reanalysis (van der A et al., 2010) are com- bined with a climatological data set of vertical profiles con- structed from sonde and satellite observations (Fortuin and Kelder, 1998). A similar relaxation procedure is applied to the CH4 concentrations in the stratosphere, while HNO3 is constrained by prescribing the concentration ratio of HNO3 over O3 at 10 hPa. These stratospheric boundary conditions are primarily based on satellite data (see Huijnen et al., 2010). This is adequate for the present-day decadal simula- tions presented in this study, but additional data sets based on output from stratospheric chemistry models are needed for representing the longer-term trends and variability in simu- lations that start in the pre-satellite era or continue into the future. Because of the relatively long lifetime of CH4, an ad- ditional constraint can be imposed on the CH4 concentra- tions at the surface. This is common practice in chemistry models in which the CH4 lifetime, which is mainly deter- mined by the amount and distribution of the hydroxyl radical (OH) in the troposphere, is not prescribed or tuned. It pre- vents drifts and/or biases in the global CH4 concentration, which would otherwise result from inconsistencies between the CH4 sources and sinks. This constraint can be imposed by relaxing the zonal mean surface concentrations of CH4 to values consistent with observations, while at the same time including the location dependent emissions of CH4. Alter- natively, the CH4 concentrations at the surface can be pre- scribed using zonal and monthly mean fields based on ob- served values. In both cases, future concentration scenarios may be imposed by scaling the target concentration fields based on the projected evolution of the global mean concen- tration. 2.2.9 Emissions Emissions from anthropogenic activities and biomass burn- ing are taken from the data set provided for the Atmospheric Chemistry and Climate Model Intercomparison Project (AC- CMIP), which was also used in CMIP5. The historical part of this data set covers the period 1850?2000 (Lamarque et al., 2010). The estimates for the year 2000 are based on a combi- nation of regional and global inventories for the various sec- tors. The reconstruction for earlier decades is forced to agree with these estimates. For the 21st century emission projec- tions from the representative concentration pathways (RCPs) are used (Van Vuuren et al., 2011). The RCP emissions start from the historical inventory in 2000. The RCP emissions are provided as monthly emissions for the years 2000, 2005, 2010, 2020, etc. A linear interpolation of the seasonal cycle is applied to obtain the emissions in the intermediate years. Oceanic emissions of DMS and NOx production by light- ning are calculated online as in Huijnen et al. (2010). Terres- trial DMS emissions from soils and vegetation are prescribed following Spiro et al. (1992). Sea salt emissions are calcu- lated online as in Vignati et al. (2010b), based on the param- eterization by Gong (2003). The emission rate is assumed to depend on the 10 m wind speed as a power law with expo- nent 3.41 (Monahan and Muircheartaigh, 1980). Emissions of mineral dust can either be calculated online based on the parameterization by Tegen et al. (2002) or be prescribed us- ing the monthly data set for the year 2000 from the AeroCom project, described by Dentener et al. (2006). Natural emissions of CO, NMVOCs, NOx, NH3, and SO2 are prescribed using a monthly varying data set compiled for the Monitoring Atmospheric Composition and Climate (MACC) project. It includes (1) biogenic emissions of iso- prene and a number of other NMVOC species as well as CO from vegetation based on the Model of Emissions of Gases and Aerosols from Nature (MEGAN) version 2.1 (Guenther et al., 2012) for the year 2000; (2) biogenic emissions of NOx from soils based on Yienger and Levy (1995); (3) oceanic emissions of CO and NMVOCs from Olivier et al. (2003); (4) biogenic emissions of NH3 from soils under natural veg- etation and oceanic emissions of NH3 from Bouwman et al. (1997); and (5) SO2 fluxes from continuously emitting volcanoes from Andres and Kasgnoc (1998). The emissions of radon-222 are prescribed as in Dentener et al. (1999). Fol- lowing the recommendations of Rasch et al. (2000), the emis- sion flux density is set at 1.0 atoms cm?2 s?1 for all land ar- eas between 60?S and 60?N and to 0.5 atoms cm?2 s?1 for land areas between 60 and 70?N, except in Greenland. Emis- sions in Greenland and other parts of the world are assumed to be zero. As in Huijnen et al. (2010), a diurnal cycle is applied to the isoprene emissions from vegetation on top of the monthly www.geosci-model-dev.net/7/2435/2014/ Geosci. Model Dev., 7, 2435?2475, 2014 2442 T. P. C. van Noije et al.: Simulation of chemistry and aerosols with EC-Earth estimates provided in the data set. To account for SO4 forma- tion in sub-grid plumes, 2.5 % of the sulfur in the SO2 emis- sions provided for the various sources is assumed to be emit- ted in the form of SO4 (Huijnen et al., 2010; Aan de Brugh et al., 2011). The size distributions assumed for the differ- ent particulate emission sources are listed in Aan de Brugh et al. (2011). The implementation of emission heights has been revised compared to the description in Huijnen et al. (2010), based on estimates from several studies (Dentener et al., 2006; De Meij et al., 2006; Bieser et al., 2011; Simpson et al., 2012). The vertical distributions applied to the different emission sources are given in Table A1. 3 Simulations In this study we present results from decadal simulations for the years 2000?2009, using 1999 as a spin-up year for the chemistry. The various simulations that were carried out are listed in Table 2. In the atmosphere?ocean GCM simulation of EC-Earth, the historical part extends up to 2005 and is continued by a simulation based on scenario assumptions, in accordance with the CMIP5 experimental design for long-term climate simulations. As a future scenario, we adopt the RCP4.5 (Thomson et al., 2011), one of the stabilization scenarios of the representative concentration pathways. Please note that for the period considered the simulated climate will not be sensitive to the chosen scenario. The atmosphere? ocean GCM was initialized on 1 January 1999 from one of the CMIP5 20th century simulations performed by the EC- Earth consortium. To be precise, the first ensemble member (SHC1) provided by the Swedish Meteorological and Hydro- logical Institute (SMHI) was used. In TM5 the stratospheric O3 concentrations were relaxed as described in Sect. 2.2.8, using total column estimates for the years 2000?2009. Also, the surface CH4 concentrations were prescribed according to observations for those years. Emissions of CH4 were therefore not applied in these simu- lations. Simulations were carried out both with and without yearly changes in the emissions from anthropogenic activities and biomass burning in TM5. In the reference EC-Earth simu- lation these emissions were fixed to their 2000 values. This reference simulation is compared with a corresponding TM5 simulation driven by meteorological data from the ECMWF reanalysis ERA-Interim (Dee et al., 2011). Both simula- tions are also evaluated against observational data. To esti- mate the impact of possible trends in the emissions, an ad- ditional ERA-Interim simulation is used with anthropogenic and biomass burning emissions varying between 2000 and 2009. In this simulation the anthropogenic and biomass burn- ing emissions were prescribed according to the RCP4.5 sce- nario, consistent with the set-up of the atmosphere?ocean GCM. Please note, however, that during the RCP develop- ment process a harmonization procedure has been applied to ensure that the emissions in the four different RCPs are still nearly identical in 2005. As a consequence the choice of the RCP will only have some albeit small effect on the chemistry during the second half of the simulation. Results from the ERA-Interim simulation with varying emissions have also been provided to the second phase of the AeroCom project. Aerosol concentrations and optical property fields from that simulation have been evaluated within that project (see http://aerocom.met.no). In all simulations, the emissions of mineral dust were prescribed using the AeroCom data set for the year 2000 (see Sect. 2.2.9). The ERA-Interim input fields for TM5 have been created from the original ECMWF data during a pre-processing stage (see Krol et al., 2005). In this process the required meteoro- logical and surface property fields are retrieved at a spec- tral resolution of T255 (corresponding to about 0.7?) and converted into TM5 input fields at a 1??1? horizontal res- olution, keeping the full 60-level vertical resolution of the original data. The ERA-Interim simulation was carried out at the same 3??2? horizontal resolution as used in EC-Earth. However, because of the different vertical resolutions of the ERA-Interim data set and the CMIP5 EC-Earth simulations, the vertical grid is different. The ERA-Interim simulation was carried out using the same selection of 34 levels out of the original 60 levels of ERA-Interim as used in Huijnen et al. (2010). The treatment of the meteorological fields in the temporal dimension is also slightly different. In the ERA- Interim simulation most meteorological fields are updated at a 3-hourly frequency (see Huijnen et al., 2010) and a linear interpolation is applied to the instantaneous fields. Another difference relates to the representation of the tracer transport by cumulus convection. Historically, the re- quired convective air mass fluxes and entrainment and de- trainment rates were not archived in the meteorological data sets used to drive TM5. In the stand-alone version of TM5 these fields are therefore calculated diagnostically. This is done in a pre-processing step according to the parameter- ization of Tiedtke (1989). This scheme was introduced in ECMWF?s operational forecast model in 1989. As the more recent schemes used in later IFS cycles, the original Tiedtke scheme already distinguished between deep, shallow and mid-level convection. To estimate the impact of using diagnostically calculated convective mass fluxes and entrainment and detrainment rates, an additional decadal simulation was performed with the stand-alone version of TM5, but now driven by meteo- rological output from EC-Earth. The radon-222 concentra- tions from this offline simulation are compared with the re- sults from the reference EC-Earth simulation, in which the data transfer from IFS to TM5 is done online through OA- SIS. For the offline EC-Earth simulation the driving meteo- rological fields for the years 1999?2005 were taken from the CMIP5 set of long-term historical simulations, which also Geosci. Model Dev., 7, 2435?2475, 2014 www.geosci-model-dev.net/7/2435/2014/ T. P. C. van Noije et al.: Simulation of chemistry and aerosols with EC-Earth 2443 Table 2. Overview of the decadal simulations used in this study. Simulation Focus Emissionsfrom anthropogenic activitiesand biomassburning Numberof vertical levelsinTM5/IFS Highestupdate frequency of mete- orologicalfields inTM5 Temporal interpolationof instantaneous meteorological fieldsinTM5 Convective fields EC-Earth Chemistryand aerosols,radon-222 Year2000 31/62 6 hourly No ReceivedfromIFS ERA-Interim Chemistryand aerosols Year2000 34/60 3 hourly Linear Diagnosedoffline ERA-Interim, varyingemissions Chemistryand aerosols 2000?2009 34/60 3 hourly Linear Diagnosedoffline OfflineEC-Earth Radon-222 ? 31/62 6 hourly Linear Diagnosedoffline provided the start fields for the online EC-Earth simulation. From this ensemble the first simulation provided by the Irish National Meteorological Service (MEI1) was selected. For the years 2006?2009 the corresponding member (ME41) of the ensemble of RCP4.5 simulations was used. As for ERA- Interim, a pre-processing step was required to convert the IFS output into input fields for TM5. The online and offline EC- Earth simulation were performed at the same horizontal and vertical resolutions. Also, the meteorological fields are up- dated with the same 6-hourly frequency. The remaining mi- nor difference between the two simulations is that in the of- fline simulation a linear temporal interpolation is applied to the instantaneous meteorological fields, which is not possible in the online simulation (see Table 2). The inclusion of atmospheric chemistry and aerosols sub- stantially increases the computational burden of the simu- lations. In the configuration described above with 47 pro- cessors used for IFS and 32 for NEMO, the atmosphere? ocean version of EC-Earth simulates one year within less than 2 h on the ECMWF IBM POWER7 high-performance computer facility. Adding 45 processors for TM5 slows down the model by almost a factor 9. We like to point out that the performance of the online-coupled IFS-NEMO-TM5 system is similar to that of the stand-alone version of TM5, when the same number of processors is used for TM5. 4 Evaluation In this section an evaluation is presented of some impor- tant aspects of the atmospheric chemistry simulation with EC-Earth. With this objective monthly, seasonal, and/or an- nual mean 10 year climatologies from the reference EC-Earth simulation are compared with the corresponding climatolo- gies from the ERA-Interim and offline EC-Earth simulations and/or with observational data sets. The variables of inter- est for which this has been done include temperature, humid- ity, the concentrations of various tracers, aerosol burdens and optical depth, and some important chemical budget terms. When comparing the climatologies from the different simu- lations and observational data sets, the interannual variability in the underlying data is used to calculate standard devia- tions and to determine the statistical significance of the dif- ferences. Regions where the differences are not statistically significant at the 5 % level are indicated by the stippled areas in the figures. When evaluating the model with ground-based observa- tion from a particular station, we linearly interpolate the grid- cell values from the model to the location of the station. The station height is used to estimate the corresponding pressure level based on a standard atmospheric profile (US Standard Atmosphere, 1976). 4.1 Physical climate An evaluation of the physical climate of EC-Earth version 2.2 is presented by Hazeleger et al. (2012). In general the large- scale structures of the atmosphere, ocean, and sea ice are well simulated and the main patterns of interannual climate vari- ability are well represented. The climate of EC-Earth version 2.3 has qualitatively similar characteristics. In particular, the model has a cold bias in most of the troposphere through- out the year. A warm bias is found over the Southern Ocean, over the stratocumulus regions west of the continents in the subtropics, and over parts of the Northern Hemisphere (NH) extratropics, but only in the lower troposphere or near the sur- face. The middle and upper troposphere as well as the tropics and most of the Arctic are on average up to 3?4?C too cold (see Fig. 1, top panels). Consequently, the specific humid- ity is also biased low in most of the troposphere, in partic- ular in the tropics (Fig. 1, bottom panels). According to the Clausius?Clapeyron relation, the saturation vapour pressure in the lower troposphere decreases by about 7 % per degree temperature decrease (Held and Soden, 2006). Assuming that the relative humidity is insensitive to the temperature bias, a cold bias of 1?C would result in a local decrease in the spe- cific humidity of about 7 %. Such a response of specific hu- midity to the temperature bias combined with a subsequent redistribution of the resulting local humidity bias due to hor- izontal and vertical transport can explain a large part of the observed bias in the humidity field in EC-Earth compared to ERA-Interim. www.geosci-model-dev.net/7/2435/2014/ Geosci. Model Dev., 7, 2435?2475, 2014 2444 T. P. C. van Noije et al.: Simulation of chemistry and aerosols with EC-Earth EC-Earth - ERA-Interim, DJF -5 -4 -3 -2 -1 0 1 2 3 45 Temperature Difference ( o C) -90 -60 -30 0 30 60 90 Latitude (deg) 1000 900 800 700 600 500 400 300 200 100 1 0009008007 006005004 003002 001 00 Pressure (hPa) EC-Earth - ERA-Interim, JJA -5 -4 -3 -2 -1 0 1 2 3 45 Temperature Difference ( o C) -90 -60 -30 0 30 60 90 Latitude (deg) 1000 900 800 700 600 500 400 300 200 100 1 0009008007 006005004 003002 001 00 Pressure (hPa) EC-Earth - ERA-Interim, DJF -2 -1.5 -1 -0.5 -0.2 -0.1 0 0.1 0.2 0.5 1 1.5 2 Specific Humidity Difference (g/kg) -90 -60 -30 0 30 60 90 Latitude (deg) 1000 900 800 700 600 500 400 300 200 100 1 0009008007 006005004 003002 001 00 Pressure (hPa) EC-Earth - ERA-Interim, JJA -2 -1.5 -1 -0.5 -0.2 -0.1 0 0.1 0.2 0.5 1 1.5 2 Specific Humidity Difference (g/kg) -90 -60 -30 0 30 60 90 Latitude (deg) 1000 900 800 700 600 500 400 300 200 100 1 0009008007 006005004 003002 001 00 Pressure (hPa) Figure 1. Zonal mean bias in temperature (top) and specific humidity (bottom) in EC-Earth compared to ERA-Interim for boreal win- ter (December?February, left) and boreal summer (June?August, right) for the period 2000?2009. Regions where the differences are not significant at the 5 % level are indicated by the stippled areas. Various aspects of the temperature and humidity biases in EC-Earth are also found in other climate models (see, e.g. Tian et al., 2013; Flato et al., 2013; Lamarque et al., 2013a). In particular, the CMIP5 model ensemble also produces a cold bias in most of the troposphere and a similar warm and wet bias over the Southern Ocean (Tian et al., 2013). The CMIP5 multi-model mean bias in annual mean temperature maximizes at about 2?C in the extratropical upper tropo- sphere. This is somewhat lower than the cold bias produced by EC-Earth in this region, which goes up to about 3?C in the NH. Moreover, EC-Earth produces a stronger cold bias in the tropical troposphere than the CMIP5 model ensemble. As a consequence, the wet bias in the tropical lower troposphere is substantially stronger in EC-Earth. Finally, we note that the spatial distribution of surface temperature biases is quali- tatively very similar for EC-Earth and the CMIP5 ensemble, at least in the annual mean (Flato et al., 2013). 4.2 Radon-222 Simulated radon-222 concentrations provide information about transport in the different model configurations, in par- ticular transport from the continental boundary layer to the free troposphere and more remote regions. Differences be- tween the reference, online EC-Earth simulation, and the ERA-Interim simulation are caused by a combination of factors: most significantly, (1) biases in the EC-Earth cli- mate, (2) the different treatment of cumulus convection in EC-Earth, and (3) the 6-hourly update of the meteorologi- cal fields in EC-Earth (see Table 2). The effect of treating convection differently is evident in the comparison between radon concentrations from the online and offline EC-Earth simulations (see Sect. 3). Figure 2 shows winter and summer zonal mean radon concentrations from the online EC-Earth simulation. Radon concentrations are highest over the continents, where the emissions take place. The highest zonal mean concentrations overall are simulated in the NH lower troposphere during bo- real winter, when the boundary layer is most stable. For both hemispheres the concentrations in the upper troposphere are highest in summer, when the convective activity is strongest. Compared to both offline simulations, the online EC-Earth simulation produces higher radon concentrations in large parts of the upper troposphere, extending from the tropics to mid-latitudes, and, during boreal winter, in the middle tropo- sphere (above about 600 hPa) at northern mid-latitudes. The online simulation generally gives lower concentrations near the surface and in the lower troposphere, especially at north- ern mid-latitudes during winter. These features are due to the different treatment of convection and are in line with the fact that the updated convection scheme produces more intense Geosci. Model Dev., 7, 2435?2475, 2014 www.geosci-model-dev.net/7/2435/2014/ T. P. C. van Noije et al.: Simulation of chemistry and aerosols with EC-Earth 2445 EC-Earth, DJF 0 0.1 0.2 0.3 0.4 0.5 0.6 0.8 1 1.2 1.4 1.6 Rn-222 (Bq/m 3 (STP)) -90 -60 -30 0 30 60 90 Latitude (deg) 1000 900 800 700 600 500 400 300 200 100 1 0009008007 006005004 003002 001 00 Pressure (hPa) EC-Earth, JJA 0 0.1 0.2 0.3 0.4 0.5 0.6 0.8 1 1.2 1.4 1.6 Rn-222 (Bq/m 3 (STP)) -90 -60 -30 0 30 60 90 Latitude (deg) 1000 900 800 700 600 500 400 300 200 100 1 0009008007 006005004 003002 001 00 Pressure (hPa) EC-Earth - ERA-Interim, DJF -0.25 -0.2 -0.15 -0.1 -0.05 0 0.05 0.1 0.15 0.2 0.25 Rn-222 Difference (Bq/m 3 (STP)) -90 -60 -30 0 30 60 90 Latitude (deg) 1000 900 800 700 600 500 400 300 200 100 1 0009008007 006005004 003002 001 00 Pressure (hPa) EC-Earth - ERA-Interim, JJA -0.25 -0.2 -0.15 -0.1 -0.05 0 0.05 0.1 0.15 0.2 0.25 Rn-222 Difference (Bq/m 3 (STP)) -90 -60 -30 0 30 60 90 Latitude (deg) 1000 900 800 700 600 500 400 300 200 100 1 0009008007 006005004 003002 001 00 Pressure (hPa) Offline EC-Earth - ERA-Interim, JJA -0.25 -0.2 -0.15 -0.1 -0.05 0 0.05 0.1 0.15 0.2 0.25 Rn-222 Difference (Bq/m 3 (STP)) -90 -60 -30 0 30 60 90 Latitude (deg) 1000 900 800 700 600 500 400 300 200 100 1 0009008007 006005004 003002 001 00 Pressure (hPa) Offline EC-Earth - ERA-Interim, DJF -0.25 -0.2 -0.15 -0.1 -0.05 0 0.05 0.1 0.15 0.2 0.25 Rn-222 Difference (Bq/m 3 (STP)) -90 -60 -30 0 30 60 90 Latitude (deg) 1000 900 800 700 600 500 400 300 200 100 1 0009008007 006005004 003002 001 00 Pressure (hPa) Figure 2. Zonal mean radon-222 concentrations in the online EC-Earth simulation (top) and the differences compared to the ERA-Interim (middle) and offline EC-Earth (bottom) simulations for boreal winter (left) and boreal summer (right). continental convection and stronger upper-level convective detrainment (Bechtold et al., 2008). Close to the equator both EC-Earth simulations produce higher zonal mean concentrations than the ERA-Interim sim- ulation in the lower troposphere (up to about 700?600 hPa) and lower concentrations at higher altitudes up to about 200 hPa. The fact that this feature is common to both EC- Earth simulations indicates that it is the result of biases in the EC-Earth climate and/or the 6-hourly update frequency of the meteorological fields. The 6 h update frequency may not always be sufficient to capture the development of convective boundary layers over continental areas, which may lead to an overestimation of radon concentrations near the surface (Krol et al., 2005). The offline EC-Earth simulation indeed produces higher concen- trations than the ERA-Interim simulation in parts of the lower troposphere and at higher latitudes, especially during sum- mer in the NH. However, the online EC-Earth simulations give lower concentrations than the ERA-Interim simulation in these regions due to the opposing effect of stronger verti- cal transport resulting from the different treatment of convec- tion. The update frequency will be reduced in future versions of the model. We finish this section with a comparison between monthly radon concentrations from the simulations and ground-based observations. We present results for six stations, including two coastal sites (Cape Grim and Richmond, both in Aus- tralia), three island sites (Mauna Loa; Gosan on Jeju Island, www.geosci-model-dev.net/7/2435/2014/ Geosci. Model Dev., 7, 2435?2475, 2014 2446 T. P. C. van Noije et al.: Simulation of chemistry and aerosols with EC-Earth South Korea; and Sado Island, Japan) and one continen- tal site (Hohenpeissenberg, Germany). Data for Hohenpeis- senberg have been taken from the World Data Centre for Greenhouse Gases (WDCGG); data for the other stations have been provided by the Australian Nuclear Science and Technology Organisation (ANSTO). All selected stations provide multi-annual data sets of hourly radon measurements (see Table A2). We calculated monthly climatologies based on the full period of available measurements, and compare these with the 10 year climatologies from the simulations. The resulting observed and simulated seasonal cycles at the selected stations are shown in Fig. 3. Following earlier studies in which ground-based radon observations were used for evaluating global models (Dentener et al., 1999; Taguchi et al., 2002; Zahorowski et al., 2004), we applied a diurnal sampling window to the observations. The applied window is site specific (see Table A2), and is chosen to minimize contributions from small-scale effects not well resolved by the models. This is most relevant for sites like Richmond, where global models underestimate the trapping of radon in the nocturnal boundary layer, and mountainous and island sites like Mauna Loa, Gosan, and Sado, where models under- estimate the influence of local emissions for various reasons (Zahorowski et al., 2005; Chambers et al., 2013). Application of a diurnal sampling window vastly improves comparisons with the simulated results for these stations (see Fig. 3). The resulting annual mean biases, root mean square errors, and correlation coefficients between the observed and simulated seasonal cycles are given in Table A2. Many of the discrepancies between the modelled and ob- served radon seasonal cycles in Fig. 3 have also been found in other global modelling studies. Using the same radon emission fluxes as applied in our simulations, Dentener et al. (1999), Tagushi et al. (2002), and Zhang et al. (2011) reported underestimates for Mauna Loa all year round, and overestimates for Cape Grim during the austral summer. Moreover, the simulations reported by Zhang et al. (2008) also failed to reproduce the concentration increase measured at Hohenpeissenberg during boreal summer. Discrepancies may be partially related to inaccuracies in assumed emission fluxes. For example, emissions in continental Asia have been estimated to be higher than previously thought (Williams et al., 2009). Except during the summer monsoon season, higher Asian emissions estimates would substantially in- crease the simulated concentrations at Gosan and Sado Is- land (Chambers et al., 2009). Zhang et al. (2011) also ob- tained better agreements at Mauna Loa and Cape Grim using improved emissions estimates. It is important to note that discrepancies between simu- lated and observed radon concentrations are generally larger than the differences amongst the three simulations. In order to use radon observations to evaluate the differences in the simulated transport, in particular the impacts of the different treatment of convection in the online EC-Earth simulation, it will be necessary to improve the set-up of the simulations using more accurate estimates of the spatially heterogeneous and seasonally varying radon emission fluxes (Zhang et al., 2011). 4.3 Oxidizing capacity and methane lifetime The oxidizing capacity of the atmosphere is determined by the abundance and distribution of the hydroxyl radical (OH) in the troposphere. OH is highly reactive and initiates most of the photochemical reaction chains that oxidize reactive gases in the atmosphere (Levy, 1971; Lelieveld et al., 2002, 2004). The production of OH in the troposphere is mainly governed by the photolysis of O3, O3 +h? ? O(1D)+O2, followed by the reaction of the excited oxygen atom, O(1D), with a water molecule: O(1D)+H2O ? 2H. The second step is limited by the availability of water molecules in the gas phase. On average only a few percent of the O(1D) atoms produced in the first reaction step will encounter a water molecule to react with and produce OH (Lelieveld et al., 2002). As a consequence, OH production rates are highest in the tropical lower and middle tropo- sphere, due to the relatively high amounts of both sunlight and water vapour in those regions. The zonal mean OH concentrations from the reference EC-Earth simulation for winter and summer are presented in the top panels of Fig. 4. Compared to the monthly cli- matology presented by Spivakovsky et al. (2000), the region of high OH concentrations extends more towards the sur- face. In other respects, the large-scale features of the spa- tial distributions are very similar in all seasons. The peak concentrations in the tropics and subtropics are substantially lower in EC-Earth, especially in boreal winter and the transi- tion seasons. However, based on simulations of methyl chlo- roform, it has been concluded that the OH concentrations from Spivakovsky et al. (2000) are likely too high. A better correspondence with the observed decay of methyl chloro- form concentrations was obtained by reducing the climatol- ogy of Spivakovsky et al. (2000) by 8 % (see Huijnen et al., 2010). Compared to the optimized climatology thus obtained (shown in the middle panels of Fig. 4), the peak concentra- tions from the EC-Earth simulation are quantitatively similar in boreal summer, but at least 20 % lower in the other sea- sons. Compared to the ERA-Interim simulation, EC-Earth pro- duces lower OH concentrations in large parts of the tropical and subtropical troposphere. As shown in the bottom panels of Fig. 4, the zonal mean concentrations are lower in a region extending from close to the surface to about 200 hPa. The lower OH concentrations in this region are mainly caused by lower temperatures, resulting in lower specific humidi- ties. Because there is less water vapour available to react with Geosci. Model Dev., 7, 2435?2475, 2014 www.geosci-model-dev.net/7/2435/2014/ T. P. C. van Noije et al.: Simulation of chemistry and aerosols with EC-Earth 2447 Cape Grim Station, Tasmania JanFebMarApr May Jun Jul AugSep Oct NovDec 0.0 0.5 1.0 1.5 2.0 0 . 00 . 51. 01. 52. 0 Rn-222 Concentration (Bq/m 3 ) Mauna Loa Station, Hawaii JanFebMarApr May Jun Jul AugSep Oct NovDec 0.00 0.05 0.10 0.15 0.20 0.25 0 . 000 . 050 .1 00 .1 50 .2 00 .2 5 Rn-222 Concentration (Bq/m 3 ) Obse rv at i o n s, win do w edObse rv at i o n sERA-In te rimE C -E a r t h , o fflin eE C -E a r t h , o nlin e Observations, windowed Observations ERA-Interim EC-Earth, offline EC-Earth, online Richmond Station, Australia JanFebMarApr May Jun Jul AugSep Oct NovDec 0 5 10 15 051 01 5 Rn-222 Concentration (Bq/m 3 ) Sado Island Station, Japan JanFebMarApr May Jun Jul AugSep Oct NovDec 0 1 2 3 4 01234 Rn-222 Concentration (Bq/m 3 ) Gosan Station, Jeju Island, Korea JanFebMarApr May Jun Jul AugSep Oct NovDec 0 1 2 3 4 01234 Rn-222 Concentration (Bq/m 3 ) Hohenpeissenberg Station, Germany JanFebMarApr May Jun Jul AugSep Oct NovDec 0 1 2 3 4 5 6 7 8 012345678 Rn-222 Concentration (Bq/m 3 ) Figure 3. Comparison of monthly mean surface radon-222 concentrations from the online and offline EC-Earth simulations (solid red and orange lines, respectively) and the ERA-Interim simulation (solid blue lines) against surface measurements (black lines). The observational means shown by the dashed lines only include the measurements made within a certain station dependent diurnal window (see Table A2). Table 3. Contributions to the chemical production of OH in the troposphere (Tg OH year?1) for the reference EC-Earth simula- tion and the corresponding ERA-Interim simulation. The contribu- tions from 90?30? S, 30? S?30? N, and 30?90? N are given by the numbers between parentheses. Results have been obtained from a monthly analysis with a fixed tropopause level, set to the uppermost model layer for which the monthly mean O3 mixing ratio is below 150 ppbv. Standard deviations are based on the simulated interan- nual variability. Reaction EC-Earth ERA-Interim O(1D) + H2O 1432 1554 (112/1120/199) (102/1243/208) NO + HO2 994 1002 (81/649/264) (65/682/255) O3+ HO2 393 393 (42/249/102) (37/263/93) H2O2 +h? 197 230 (18/149/29) (20/175/34) Other 168 176 (12/139/17) (13/144/18) Total 3184?20 3355?30 (266/2307/611) (238/2508/608) O(1D), the production of OH via the reaction path described above is lower than in the ERA-Interim simulation (see Ta- ble 3). At higher latitudes, the OH concentrations from EC-Earth are generally higher than in the ERA-Interim simulation. As will be shown in Sect. 4.5, EC-Earth produces higher O3 concentrations in most of the lower and middle troposphere, especially in the extratropics. This increases the O(1D) pro- duction rates, especially in the summer hemisphere. In the Southern Hemisphere (SH) extratropical lower troposphere the difference in the OH concentrations between the EC- Earth and ERA-Interim simulations is further enhanced by the higher levels of humidity in EC-Earth associated with the warm bias over the Southern Ocean. In the tropical upper troposphere (above about 200 hPa), the OH concentrations in EC-Earth are also higher than in the ERA-Interim simulation. This is likely related to the fact that some of the tracers involved in the other reactions that produce OH (see Table 3) are more efficiently transported to higher altitudes by deep convection (see Sect. 4.2). Differences in the amount and distribution of the NOx production by lightning also affect the distribution of OH. The global production of NOx by lightning is significantly higher in EC-Earth than in the ERA-Interim simulation (see Table A3); the production in EC-Earth is 0.84 and 0.51 Tg N year?1 higher in the NH and SH extratropics, re- spectively, while it is 0.74 Tg N year?1 lower in the tropics (30? S?30? N). The lower OH concentrations in the tropical and sub- tropical lower and middle troposphere lead to a slower re- moval of CH4 from the atmosphere. The average chemical lifetime of CH4 against reaction with tropospheric OH is 10.9 years in the EC-Earth simulation and 10.1 years in the ERA-Interim simulation. Both values are within the multi- model ranges of 9.7?1.7, 10.2?1.7, and 9.7?1.5 years estimated by Shindell et al. (2006b), Fiore et al. (2009), and Naik et al. (2013), respectively, from simulations for present-day conditions (2000 or 2001). Assuming a lifetime of 120 and 160 years, respectively, for the chemical loss in the stratosphere and the soil sink (Ehhalt et al., 2001), the at- mospheric lifetime of CH4 is 9.4 years in the EC-Earth sim- ulations. This is 7 % longer than the atmospheric lifetime of www.geosci-model-dev.net/7/2435/2014/ Geosci. Model Dev., 7, 2435?2475, 2014 2448 T. P. C. van Noije et al.: Simulation of chemistry and aerosols with EC-Earth EC-Earth, DJF 0 0.1 0.2 0.5 1 2 5 10 15 20 25 OH (10 5 molec/cm 3 ) -90 -60 -30 0 30 60 90 Latitude (deg) 1000 900 800 700 600 500 400 300 200 100 1 0009008007 006005004 003002 001 00 Pressure (hPa) EC-Earth, JJA 0 0.1 0.2 0.5 1 2 5 10 15 20 25 OH (10 5 molec/cm 3 ) -90 -60 -30 0 30 60 90 Latitude (deg) 1000 900 800 700 600 500 400 300 200 100 1 0009008007 006005004 003002 001 00 Pressure (hPa) Spivakovsky, DJF 0 0.1 0.2 0.5 1 2 5 10 15 20 25 OH (10 5 molec/cm 3 ) -90 -60 -30 0 30 60 90 Latitude (deg) 1000 900 800 700 600 500 400 300 200 100 1 0009008007 006005004 003002 001 00 Pressure (hPa) Spivakovsky, JJA 0 0.1 0.2 0.5 1 2 5 10 15 20 25 OH (10 5 molec/cm 3 ) -90 -60 -30 0 30 60 90 Latitude (deg) 1000 900 800 700 600 500 400 300 200 100 1 0009008007 006005004 003002 001 00 Pressure (hPa) EC-Earth - ERA-Interim, DJF -4 -3 -2 -1 -0.5 -0.2 0 0.2 0.5 1 2 34 OH Difference (10 5 molec/cm 3 ) -90 -60 -30 0 30 60 90 Latitude (deg) 1000 900 800 700 600 500 400 300 200 100 1 0009008007 006005004 003002 001 00 Pressure (hPa) EC-Earth - ERA-Interim, JJA -4 -3 -2 -1 -0.5 -0.2 0 0.2 0.5 1 2 34 OH Difference (10 5 molec/cm 3 ) -90 -60 -30 0 30 60 90 Latitude (deg) 1000 900 800 700 600 500 400 300 200 100 1 0009008007 006005004 003002 001 00 Pressure (hPa) Figure 4. Zonal mean OH concentrations in the reference EC-Earth simulation (top), the climatology of Spivakovsky et al. (2000) reduced by 8 % (middle), and the differences between the reference EC-Earth simulation and the corresponding ERA-Interim simulation (bottom) for boreal winter (left) and boreal summer (right). 8.8 years obtained in the ERA-Interim simulation. Prather et al. (2012) recently estimated from methyl chloroform obser- vations that the present-day atmospheric lifetime of CH4 is in the range 9.1?0.9 years. The values obtained in the EC- Earth and ERA-Interim simulations are both well within this range. 4.4 Carbon monoxide Carbon monoxide is emitted into the atmosphere by an- thropogenic and natural sources and is chemically produced in the atmosphere by oxidation of CH4 and NMVOCs and by photolysis of certain NMVOCs. The oxidation of CH4 and many other hydrocarbons proceeds via the formation of formaldehyde (CH2O), which is subsequently converted to CO by photolysis or oxidation, mostly by reaction with OH. CO is removed from the atmosphere by reaction with OH and by dry deposition at the surface. The various contribu- tions to the atmospheric budget of CO in the EC-Earth and ERA-Interim simulations are given in Table 4. The average lifetime of CO in the atmosphere (total burden divided by total loss) is 54.6 days in EC-Earth compared to 52.5 days with ERA-Interim. The slightly longer lifetime in EC-Earth is a result of a slower chemical destruction due to the lower OH concentrations in the tropical and subtropical troposphere. In contrast, OH levels in EC-Earth are higher in Geosci. Model Dev., 7, 2435?2475, 2014 www.geosci-model-dev.net/7/2435/2014/ T. P. C. van Noije et al.: Simulation of chemistry and aerosols with EC-Earth 2449 Table 4. Contributions to the budget of CO in the atmosphere (Tg CO year?1), together with the tropospheric and atmospheric burdens of CO (Tg CO), and the atmospheric lifetime of CO (days) for the reference EC-Earth simulation and the corresponding ERA-Interim simulation. The contributions from 90?30? S, 30? S?30? N, and 30?90? N are given by the numbers between parentheses. Results have been obtained from a monthly analysis with a fixed tropopause level, set to the uppermost model layer for which the monthly mean O3 mixing ratio is below 150 ppbv. Standard deviations are based on the simulated interannual variability. EC-Earth ERA-Interim Emissions 1166 1166 (23/762/381) (23/762/381) Tropospheric chemical production 1105 1170 (81/838/186) (76/905/189) Total gain? 2284 2351 (107/1606/572) (102/1674/574) Dry deposition 173?1.0 180?1.5 (6/107/60) (6/105/69) Tropospheric chemical destruction 2065 2129 (191/1447/427) (166/1541/422) Total loss? 2284 2352 (208/1570/506) (184/1662/506) Tropospheric burden 316?2.0 317?3.3 (53/179/84) (53/175/88) Atmospheric burden 341?2.5 338?3.7 (61/185/95) (59/181/97) Atmospheric lifetime 54.6 52.5 ? The total gain and loss also include small contributions from, respectively, chemical production and destruction in the stratosphere. the extratropics, causing a more efficient removal of CO at higher latitudes, especially in the SH. Also the production of CO in the tropics and the subtropics is lower in EC-Earth. This is a direct consequence of a lower yield from the oxidation of CH4, caused by the lower OH concentrations in the tropics and subtropics. In order words, to obtain the same CH4 concentrations lower effective CH4 emissions are needed in EC-Earth, resulting in a lower pro- duction of CO. The total chemical production of CO in both simulations is lower than the range of model estimates re- ported by Shindell et al. (2006b). This is likely due to an underestimation of the CO production from NMVOCs in the CBM4 chemistry scheme. The global tropospheric burden of CO is similar in both simulations (Table 4). EC-Earth produces a lower burden in the tropics and a higher burden in the NH extratropics, but the differences are only a few percent. Compared to the ERA-Interim simulation, EC-Earth gives higher CO concen- trations in the tropical upper troposphere and in the lower stratosphere (Fig. 5), mostly due to more efficient transport of CO by deep convection into the tropical upper troposphere. In the tropical lower and middle troposphere both higher and lower concentrations are observed depending on the location and the season. The concentrations in EC-Earth are lower in the NH extratropics, due to the faster chemical destruc- tion. They are also somewhat lower in the SH extratropics in austral summer and, in the middle and upper troposphere, in austral winter. The simulated surface mixing ratios of CO have been eval- uated against monthly averages from the network of sur- face flask sampling of NOAA?s Earth System Research Lab- oratory (ESRL) Global Monitoring Division (GMD). The decadal monthly mean mixing ratios from the simulations are compared with the flask measurements in Fig. 6. Since in the reference EC-Earth simulation and the corresponding ERA-Interim simulation the emissions from anthropogenic activities and biomass burning were fixed to their values for the year 2000, we have also included the results from the ERA-Interim simulation with emissions varying from year to year (see Table 2). The two ERA-Interim simulations give very similar decadal mean CO concentrations at the stations used in the evaluation (see Table A4 for a complete list). Thus, also the simulations with fixed emissions can be di- rectly compared with the measurements. At the measurement locations the concentration differ- ences between the EC-Earth and ERA-Interim simulation are generally small in the SH and in the tropics and be- come larger in the NH extratropics (see Fig. 6 and Ta- ble A2). For the majority of stations the seasonal cycle is very well simulated, as expressed by a high correlation be- tween the simulated and the measured monthly values. The simulated CO concentrations are generally in good quanti- tative agreement with the measurements in the SH. At the tropical stations in the NH both simulations underestimate the measurements by about equal amounts. At northern mid- latitudes, both simulations underestimate the measurements, www.geosci-model-dev.net/7/2435/2014/ Geosci. Model Dev., 7, 2435?2475, 2014 2450 T. P. C. van Noije et al.: Simulation of chemistry and aerosols with EC-Earth EC-Earth, DJF 0 10 20 30 40 50 60 70 80 90 100 110 120 CO (ppbv) -90 -60 -30 0 30 60 90 Latitude (deg) 1000 900 800 700 600 500 400 300 200 100 1 0009008007 006005004 003002 001 00 Pressure (hPa) EC-Earth, JJA 0 10 20 30 40 50 60 70 80 90 100 110 120 CO (ppbv) -90 -60 -30 0 30 60 90 Latitude (deg) 1000 900 800 700 600 500 400 300 200 100 1 0009008007 006005004 003002 001 00 Pressure (hPa) EC-Earth - ERA-Interim, DJF -15 -10 -5 -2 -1 0 1 2 5 10 15 CO Difference (ppbv) -90 -60 -30 0 30 60 90 Latitude (deg) 1000 900 800 700 600 500 400 300 200 100 1 0009008007 006005004 003002 001 00 Pressure (hPa) EC-Earth - ERA-Interim, JJA -15 -10 -5 -2 -1 0 1 2 5 10 15 CO Difference (ppbv) -90 -60 -30 0 30 60 90 Latitude (deg) 1000 900 800 700 600 500 400 300 200 100 1 0009008007 006005004 003002 001 00 Pressure (hPa) Figure 5. Zonal mean CO mixing ratios in the reference EC-Earth simulation (top) and the differences compared to the corresponding ERA-Interim simulation (bottom) for boreal winter (left) and boreal summer (right). but the concentrations in EC-Earth are lower than with ERA- Interim, especially outside of the summer season. In the an- nual mean the difference can be up to about 11 ppbv. The dif- ferences between the two simulations are generally smaller than the amounts by which the measurements are underes- timated. We note that other modelling studies have shown similar CO biases in the NH, using identical anthropogenic and biomass burning emissions (Lamarque et al., 2010; Naik et al., 2013). 4.5 Ozone The sources of ozone in the troposphere are chemical produc- tion by the oxidation of CO, CH4, and NMVOCs in the pres- ence of NOx, and net transport from the stratosphere. Ozone is removed from the troposphere by chemical destruction and by dry deposition at land surfaces. The chemical destruction of tropospheric O3 occurs mainly through the photolysis of O3 followed by the reaction of the produced excited oxy- gen atom with a water molecule (see Sect. 4.3) and through the reaction of O3 with the peroxy radical (HO2) and with OH. The main contributions to the tropospheric O3 budget in the EC-Earth and ERA-Interim simulations are given in Ta- ble 5. These numbers can be directly compared with the AC- CENT and ACCMIP multi-model results for the present day reported by Stevenson et al. (2006) and Young et al. (2013), who use a similar method for defining the tropopause. Note that Stevenson et al. (2006) give ranges based on the full en- semble of models participating in that study as well as on a subset of models that were selected based on criteria related to the simulation of O3 and the CH4 lifetime for the present day. In EC-Earth the average lifetime of tropospheric O3 is 25.5 days, which is outside the ranges 22.3?2.0 days and 22.2?2.2 days estimated by Stevenson et al. (2006) for the full ensemble of ACCENT models and a subset of models, respectively, and corresponds to the highest value out of the six individual model results reported by Young et al. (2013). With ERA-Interim a lifetime of 23.9 days is obtained, which is within the ranges reported by these authors. The longer lifetime in EC-Earth is caused by a slower chemical destruc- tion. The cold bias that exists in most of the troposphere slows down the destruction of O3 by photolysis because of the lower specific humidity. Lower concentrations of OH and HO2 in large parts of the tropical and subtropical troposphere (see Sect. 4.3) further slow down the destruction of O3. EC-Earth produces a tropospheric O3 burden of 327 Tg, which is well within the ranges 344?39 Tg and 336?27 Tg reported by Stevenson et al. (2006) and the range 337?23 Tg reported by Young et al. (2013). With ERA- Interim a tropospheric burden of 309 Tg is obtained, which is at the low side of the ranges estimated by Stevenson et al. (2006) and below the range estimated by Young et Geosci. Model Dev., 7, 2435?2475, 2014 www.geosci-model-dev.net/7/2435/2014/ T. P. C. van Noije et al.: Simulation of chemistry and aerosols with EC-Earth 2451 Mauna Loa Station, Hawaii JanFebMarApr May Jun Jul AugSep Oct NovDec 0 20 40 60 80 100 120 140 160 180 200 02 04 060801 0012 014 01 601 802 00 CO Mixing Ratio (ppbv) Terceira Island Station, Azores JanFebMarApr May Jun Jul AugSep Oct NovDec 0 20 40 60 80 100 120 140 160 180 200 02 04 060801 0012 014 01 601 802 00 CO Mixing Ratio (ppbv) Ragged Point Station, Barbados JanFebMarApr May Jun Jul AugSep Oct NovDec 0 20 40 60 80 100 120 140 160 180 200 02 04 060801 0012 014 01 601 802 00 CO Mixing Ratio (ppbv) Tutuila Station, American Samoa JanFebMarApr May Jun Jul AugSep Oct NovDec 0 20 40 60 80 100 120 140 160 180 200 02 04 060801 0012 014 01 601 802 00 CO Mixing Ratio (ppbv) South Pole Station JanFebMarApr May Jun Jul AugSep Oct NovDec 0 20 40 60 80 100 120 140 160 180 200 02 04 060801 0012 014 01 601 802 00 CO Mixing Ratio (ppbv) Obse rv at i o n sERA-In te rim , v a r. e mi s .ERA-In te rimE C -E a r t h Observations ERA-Interim, var. emis. ERA-Interim EC-Earth Cape Grim Station, Tasmania JanFebMarApr May Jun Jul AugSep Oct NovDec 0 20 40 60 80 100 120 140 160 180 200 02 04 060801 0012 014 01 601 802 00 CO Mixing Ratio (ppbv) Mace Head Station, Ireland JanFebMarApr May Jun Jul AugSep Oct NovDec 0 20 40 60 80 100 120 140 160 180 200 02 04 060801 0012 014 01 601 802 00 CO Mixing Ratio (ppbv) Alert Station, Canada JanFebMarApr May Jun Jul AugSep Oct NovDec 0 20 40 60 80 100 120 140 160 180 200 02 04 060801 0012 014 01 601 802 00 CO Mixing Ratio (ppbv) Storhofdi Station, Iceland JanFebMarApr May Jun Jul AugSep Oct NovDec 0 20 40 60 80 100 120 140 160 180 200 02 04 060801 0012 014 01 601 802 00 CO Mixing Ratio (ppbv) Figure 6. Comparison of monthly mean surface CO mixing ratios from the reference EC-Earth simulation (solid red lines) and the two ERA- Interim simulations (solid and dotted blue lines) against flask measurements at a number of stations selected from the NOAA GMD network. The results from the ERA-Interim simulation with interannual variations in the emissions from anthropogenic activities and biomass burning (dotted blue lines) nearly coincide with those from the ERA-Interim simulation where these emissions are fixed to their values for the year 2000 (solid blue lines). Table 5. Contributions to the budget of O3 in the troposphere (Tg O3 year?1), together with the tropospheric O3 burden (Tg O3), and the tropospheric O3 lifetime (days) for the reference EC-Earth simulation and the corresponding ERA-Interim simulation. The contributions from 90?30? S, 30? S?30? N, and 30?90? N are given by the numbers between parentheses. Results have been obtained from a monthly analysis with a fixed tropopause level, set to the uppermost model layer for which the monthly mean O3 mixing ratio is below 150 ppbv. Standard deviations are based on the simulated interannual variability. EC-Earth ERA-Interim Chemical production 4328?17 4419?38 (339/2890/1099) (278/3070/1071) Chemical destruction 3698?24 3873?39 (327/2656/714) (291/2896/687) Dry deposition 978?3.2 851?4.1 (115/471/392) (84/425/341) Stratosphere?troposphere exchange 349?10 306?15 Burden 327?1.3 309?1.7 (66/161/100) (59/162/88) Lifetime 25.5 23.9 al. (2013). The higher burden in EC-Earth compared to the ERA-Interim simulation is mainly due to the slower chemical destruction of O3 in the troposphere and a higher net influx of O3 from the stratosphere. The influx from the stratosphere is 349 Tg year?1 in EC-Earth compared to 306 Tg year?1 with ERA-Interim. Both values are below the ranges 552?168 Tg year?1 and 556?154 Tg year?1 esti- mated by Stevenson et al. (2006) and the model results reported by Young et al. (2013). Other model studies of stratosphere?troposphere exchange also found the net O3 www.geosci-model-dev.net/7/2435/2014/ Geosci. Model Dev., 7, 2435?2475, 2014 2452 T. P. C. van Noije et al.: Simulation of chemistry and aerosols with EC-Earth flux to be higher than about 400 Tg year?1, in line with esti- mates based on observations (Olsen et al., 2004; Hsu et al., 2005). Thus, compared to the ERA-Interim simulation, the higher net stratosphere?troposphere exchange flux simulated in EC-Earth is likely an improvement. Overall, the total chemical destruction of O3 in the tropo- sphere is lower in EC-Earth than in the ERA-Interim sim- ulation. The chemical production of O3 in the troposphere is also somewhat lower, but the net chemical production of O3 in the troposphere is still higher in EC-Earth. Combined with the higher net influx from the stratosphere this is con- sistent with a higher deposition of O3. The total deposition is 978 Tg year?1 in EC-Earth, while 851 Tg year?1 is obtained in the ERA-Interim simulation. Both results are within the ranges 1003?200 Tg year?1 and 953?154 Tg year?1 esti- mated by Stevenson et al. (2006) and the model results re- ported by Young et al. (2013); however, the higher value ob- tained with EC-Earth is closer to the central estimates ob- tained by these authors. EC-Earth produces higher zonal mean O3 concentrations than the ERA-Interim simulation in large parts of the tropo- sphere, including most of the NH and the lower and middle parts of the SH (Fig. 7). Lower zonal mean concentrations are simulated in the tropical and subtropical upper troposphere and parts of the tropical and subtropical middle troposphere, and in parts of the lower stratosphere of the SH. Differences in the contribution from O3 originating from the stratosphere explain part of the differences in the sim- ulated O3 concentrations in the troposphere (compare the lower and middle panels of Fig. 7). This contribution was di- agnosed using a stratospheric O3 tracer, O3S. As in Lelieveld and Dentener (2000), O3S is subject to the same strato- spheric boundary conditions and removal processes as reg- ular O3, but is not produced below a certain pressure level, ?140 hPa in our model set-up. Since only small amounts of O3 are produced in the region between this level and the tropopause, effectively the chemical production is switched off in the troposphere. The O3S tracer therefore provides a robust method for estimating the contribution of O3 pro- duced in the stratosphere to the tropospheric budget. The to- tal chemical destruction and deposition of O3S in the tropo- sphere is 351 Tg year?1 in EC-Earth and 305 Tg year?1, very close to the estimates of the net stratosphere?troposphere ex- change flux quoted above, which were obtained by closing the tropospheric budget of O3. EC-Earth gives higher O3 concentrations than the ERA- Interim simulation in the lowermost stratosphere at high northern latitudes (Fig. 7); this, combined with the slower chemical destruction in the troposphere, leads to higher O3S concentrations in most of the NH. In the SH, the lower zonal mean O3 concentrations simulated with EC-Earth in the sub- tropical upper and middle troposphere are partly due to a lower contribution from O3S, especially in austral winter. At higher latitudes, on the other hand, the contribution from O3S in the troposphere is higher than in the ERA-Interim simulation. Concentration differences in the lower strato- sphere between the EC-Earth and ERA-Interim simulations are the combined effect of differences in the large-scale stratospheric circulation, stratosphere?troposphere exchange and vertical resolution. The slower chemical destruction due to the cold bias in EC-Earth increases the lifetime of O3 in the troposphere, and tends to increase the concentration of both O3S and O3. The resulting concentration increase is larger for O3 than for O3S, but the increase in the O3 concentration is partly compen- sated by a reduced chemical production in the troposphere. Differences in vertical exchange are also important to ex- plain the differences in the O3 concentrations between the two simulations. The different treatment of convection in EC- Earth leads to more efficient convection to the upper parts of the tropical troposphere (see Sect. 4.2). This tends to de- crease the O3 concentrations in the tropical and subtropical upper troposphere. In the extratropics enhanced vertical mix- ing in EC-Earth tends to increase the O3 concentrations in the lower parts of the troposphere by bringing down more O3 from higher altitudes. Enhanced mixing similarly tends to increase the O3S concentrations in the lower extratropical troposphere. The latter effects are unique features of the on- line EC-Earth simulation, which are not reproduced in the offline EC-Earth simulation (not shown). The simulated O3 concentrations have been evaluated against a vertically resolved, zonal, and monthly mean data set based on the O3 profile measurements from the Binary DataBase of Profiles (BDBP) of Hassler et al. (2008), which includes both satellite observations and ozonesondes. The data set used in the evaluation was constructed for the years 1979?2007 by Bodeker Scientific (www.bodekerscientific. com) in a similar way as described in Hassler et al. (2009). In addition, the monthly mean O3 data set from Cionni et al. (2011) was included in the evaluation. This data set provided the O3 distribution for the CMIP5 climate models that did not calculate O3 interactively. The historical part of this data set extends to 2009. In the stratosphere it consists of zonal mean fields derived from a multiple linear regres- sion analysis of satellite observations and polar ozonesonde data. In the troposphere it is based on simulations with the chemistry-climate models CAM3.5 (Lamarque et al., 2010) and GISS-PUCCINI (Shindell et al., 2006c) with prescribed sea surface temperatures. The anthropogenic and biomass burning emissions used in these simulations are the same as in the simulations presented here, and are also kept constant from 2000 to 2009. In Figs. 8 and 9 the monthly mean O3 mixing ratios from the EC-Earth and ERA-Interim simulations are compared with the observational and CMIP5 data sets in latitude bands of 30? at 750, 500, and 250 hPa. In these figures, the 2000? 2009 means from the simulations are compared with the 2000?2007 means from the observational data set and the 2000?2009 means from the CMIP5 data set. Geosci. Model Dev., 7, 2435?2475, 2014 www.geosci-model-dev.net/7/2435/2014/ T. P. C. van Noije et al.: Simulation of chemistry and aerosols with EC-Earth 2453 EC-Earth, DJF 0 10 20 30 40 50 60 70 80 90 100 150 Ozone (ppbv) -90 -60 -30 0 30 60 90 Latitude (deg) 1000 900 800 700 600 500 400 300 200 100 1 0009008007 006005004 003002 001 00 Pressure (hPa) EC-Earth, JJA 0 10 20 30 40 50 60 70 80 90 100 150 Ozone (ppbv) -90 -60 -30 0 30 60 90 Latitude (deg) 1000 900 800 700 600 500 400 300 200 100 1 0009008007 006005004 003002 001 00 Pressure (hPa) EC-Earth - ERA-Interim, DJF -25 -20 -15 -10 -5 -2 0 2 5 10 15 20 25 Ozone Difference (ppbv) -90 -60 -30 0 30 60 90 Latitude (deg) 1000 900 800 700 600 500 400 300 200 100 1 0009008007 006005004 003002 001 00 Pressure (hPa) EC-Earth - ERA-Interim, JJA -25 -20 -15 -10 -5 -2 0 2 5 10 15 20 25 Ozone Difference (ppbv) -90 -60 -30 0 30 60 90 Latitude (deg) 1000 900 800 700 600 500 400 300 200 100 1 0009008007 006005004 003002 001 00 Pressure (hPa) EC-Earth - ERA-Interim, DJF -25 -20 -15 -10 -5 -2 0 2 5 10 15 20 25 O 3S Difference (ppbv) -90 -60 -30 0 30 60 90 Latitude (deg) 1000 900 800 700 600 500 400 300 200 100 1 0009008007 006005004 003002 001 00 Pressure (hPa) EC-Earth - ERA-Interim, JJA -25 -20 -15 -10 -5 -2 0 2 5 10 15 20 25 O 3S Difference (ppbv) -90 -60 -30 0 30 60 90 Latitude (deg) 1000 900 800 700 600 500 400 300 200 100 1 0009008007 006005004 003002 001 00 Pressure (hPa) Figure 7. Zonal mean O3 mixing ratios in the reference EC-Earth simulation (top), the differences compared to the corresponding ERA- Interim simulation (middle), and the contribution from the stratospheric O3 tracer (O3S) to these differences (bottom) for boreal winter (left) and boreal summer (right). We first look at the extratropical upper troposphere?lower stratosphere (250 hPa). Here EC-Earth gives higher O3 con- centrations in the NH and lower concentrations in the SH than the ERA-Interim simulation. At high northern latitudes (60?90? N,), the higher concentrations obtained with EC- Earth are in better agreement with the observational data set. However, EC-Earth underestimates the observational data in boreal spring and summer, which indicates that the down- ward transport in the lower stratosphere may still be too slow. Between 30 and 60? N the higher values obtained with EC-Earth lead to a somewhat stronger overestimation of the observational data. On the other hand, the CMIP5 data set shows even higher concentrations in this region during boreal winter and spring. At high southern latitudes (60?90? S) both simulations underestimate the observational data, but the agreement is worse for EC-Earth. EC-Earth also underesti- mates the observational data between 30 and 60? S, where the ERA-Interim simulation overestimates the observational data, especially in austral spring and summer. In this region the CMIP5 data set gives similar values as obtained with EC- Earth. In the extratropical middle and lower troposphere (500 and 750 hPa, respectively), EC-Earth gives significantly higher concentrations than the ERA-Interim simulation. In the NH, EC-Earth agrees well with both the observational data and the CMIP5 data set in boreal winter. In boreal summer, the www.geosci-model-dev.net/7/2435/2014/ Geosci. Model Dev., 7, 2435?2475, 2014 2454 T. P. C. van Noije et al.: Simulation of chemistry and aerosols with EC-Earth 60-90 o S, 250 hPa JanFebMarApr May Jun Jul AugSep Oct NovDec 0 20 40 60 80 100 120 140 160 180 02 04 060801 0012 014 01 601 80 Ozone Mixing Ratio (ppbv) C MIP 5 D atasetObs . D atasetERA-In te rimE C -E a r t h CMIP5 Dataset Obs. Dataset ERA-Interim EC-Earth 0-30 o S, 250 hPa JanFebMarApr May Jun Jul AugSep Oct NovDec 0 10 20 30 40 50 60 01 02 0304 05060 Ozone Mixing Ratio (ppbv) 0-30 o S, 750 hPa JanFebMarApr May Jun Jul AugSep Oct NovDec 0 10 20 30 40 50 01 02 0304 050 Ozone Mixing Ratio (ppbv) 30-60 o S, 750 hPa JanFebMarApr May Jun Jul AugSep Oct NovDec 0 10 20 30 40 01 02 0304 0 Ozone Mixing Ratio (ppbv) 60-90 o S, 750 hPa JanFebMarApr May Jun Jul AugSep Oct NovDec 0 10 20 30 40 01 02 0304 0 Ozone Mixing Ratio (ppbv) 0-30 o S, 500 hPa JanFebMarApr May Jun Jul AugSep Oct NovDec 0 10 20 30 40 50 60 01 02 0304 05060 Ozone Mixing Ratio (ppbv) 30-60 o S, 500 hPa JanFebMarApr May Jun Jul AugSep Oct NovDec 0 10 20 30 40 50 01 02 0304 050 Ozone Mixing Ratio (ppbv) 60-90 o S, 500 hPa JanFebMarApr May Jun Jul AugSep Oct NovDec 0 10 20 30 40 50 01 02 0304 050 Ozone Mixing Ratio (ppbv) 30-60 o S, 250 hPa JanFebMarApr May Jun Jul AugSep Oct NovDec 0 20 40 60 80 100 120 140 02 04 060801 0012 014 0 Ozone Mixing Ratio (ppbv) Figure 8. Monthly mean O3 mixing ratios at 750, 500, and 250 hPa averaged over different latitude bands in the SH. The results from the reference EC-Earth simulation (solid red lines) and the corresponding ERA-Interim simulation (solid blue lines) are compared against the observational data set (solid black lines) constructed from the Binary Database of Profiles (BDBP). The CMIP5 data set from Cionni et al. (2011) is indicated by the dashed black lines. The contributions from O3S for the EC-Earth and ERA-Interim simulations are shown by the dashed red and blue lines, respectively. concentrations from EC-Earth are significantly higher than in the observational data set. In this season, the concen- trations from the ERA-Interim simulation are either very close to (30?60? N) or slightly lower than the observational estimates (60?90? N). In the SH, EC-Earth shows a much smaller bias relative to the observational data set. At high southern latitudes (60?90? S), the concentrations from EC- Earth are lower than the observational estimates during aus- tral winter and higher during austral summer. EC-Earth is in excellent agreement with the observational data in the lower troposphere between 30 and 60? S. In the tropical upper troposphere (30? S?30? N, 250 hPa), EC-Earth produces lower values than the ERA-Interim simu- lation and is in fairly good agreement with the observational data set. The CMIP5 data set gives significantly lower values in this region. In the tropical middle and lower troposphere, the differ- ences between the EC-Earth and ERA-Interim simulation are relatively small. In the NH tropics (0?30? N), EC-Earth gives somewhat higher concentrations. In the middle troposphere (500 hPa), EC-Earth reproduces the observational data very well during boreal summer and fall, but gives lower values during winter and spring. In any case, EC-Earth is closer to the observational data than both the ERA-Interim sim- ulation and the CMIP5 data set. In the lower troposphere (750 hPa), EC-Earth agrees well with the observational data set in boreal spring and gives slightly higher values in the other seasons. Both simulations are in fairly good agreement with the observational data set. The CMIP5 data set gives significantly lower concentrations in this region. In the SH tropics (0?30? S), both simulations underestimate the obser- vation data, especially in the middle troposphere (500 hPa). Here EC-Earth gives somewhat lower values than the ERA- Interim simulation during austral winter and spring. The CMIP5 data set underestimates the observational data more strongly in the lower troposphere (750 hPa), and also gives somewhat lower values than EC-Earth in the middle tropo- sphere (500 hPa) during austral winter and fall. The results presented in Figs. 8 and 9 can be compared with the evaluation presented by Young et al. (2013), in which present-day tropospheric O3 concentrations from the ACCENT and ACCMIP model ensembles are compared with monthly climatological data sets based on ozonesonde mea- surements as well as satellite retrievals from the Tropo- spheric Emission Spectrometer (TES). In general, our sim- ulations are within the range of concentrations simulated by Geosci. Model Dev., 7, 2435?2475, 2014 www.geosci-model-dev.net/7/2435/2014/ T. P. C. van Noije et al.: Simulation of chemistry and aerosols with EC-Earth 2455 60-90 o N, 250 hPa JanFebMarApr May Jun Jul AugSep Oct NovDec 0 50 100 150 200 250 300 350 400 0501 001 502 002 503003504 00 Ozone Mixing Ratio (ppbv) C MIP 5 D atasetObs . D atasetERA-In te rimE C -E a r t h CMIP5 Dataset Obs. Dataset ERA-Interim EC-Earth 60-90 o N, 500 hPa JanFebMarApr May Jun Jul AugSep Oct NovDec 0 10 20 30 40 50 60 70 80 01 02 0304 050607 080 Ozone Mixing Ratio (ppbv) 30-60 o N, 500 hPa JanFebMarApr May Jun Jul AugSep Oct NovDec 0 10 20 30 40 50 60 70 80 01 02 0304 050607 080 Ozone Mixing Ratio (ppbv) 0-30 o N, 500 hPa JanFebMarApr May Jun Jul AugSep Oct NovDec 0 10 20 30 40 50 60 01 02 0304 05060 Ozone Mixing Ratio (ppbv) 30-60 o N, 250 hPa JanFebMarApr May Jun Jul AugSep Oct NovDec 0 20 40 60 80 100 120 140 160 180 200 02 04 060801 0012 014 01 601 802 00 Ozone Mixing Ratio (ppbv) 0-30 o N, 250 hPa JanFebMarApr May Jun Jul AugSep Oct NovDec 0 10 20 30 40 50 60 70 01 02 0304 050607 0 Ozone Mixing Ratio (ppbv) 30-60 o N, 750 hPa JanFebMarApr May Jun Jul AugSep Oct NovDec 0 10 20 30 40 50 60 70 01 02 0304 050607 0 Ozone Mixing Ratio (ppbv) 60-90 o N, 750 hPa JanFebMarApr May Jun Jul AugSep Oct NovDec 0 10 20 30 40 50 60 01 02 0304 05060 Ozone Mixing Ratio (ppbv) 0-30 o N, 750 hPa JanFebMarApr May Jun Jul AugSep Oct NovDec 0 10 20 30 40 50 01 02 0304 050 Ozone Mixing Ratio (ppbv) Figure 9. Same as Fig. 8, but for the NH. the ACCMIP models. In particular, most ACCMIP models also underestimate the O3 concentrations in the middle and lower troposphere between 0 and 30? S. Likewise they also underestimate the observed seasonal cycle in the upper and middle troposphere between 0 and 30? N. The surface O3 concentrations simulated with EC-Earth and the differences compared to the ERA-Interim simulation are presented in Fig. 10. EC-Earth gives higher surface con- centrations in most of the world, with the exception of some regions located in the tropics and subtropics. In the mid- to high latitudes of the NH, differences up to about 10 ppbv are simulated during the winter season, while even larger differ- ences are found during summer. The simulated surface O3 concentrations have been evalu- ated against in situ surface measurements. The stations used for the evaluation of surface O3 are listed in Table A5. They include stations from the NOAA GMD network and a se- lection of stations included in the World Data Centre for Greenhouse Gases (WDCGG). Data for Mace Head were taken from the European Monitoring and Evaluation Pro- gramme (EMEP). Monthly averages were calculated from the hourly mixing ratio measurements and then averaged over the available years in the simulation period. Figure 11 shows the resulting monthly mixing values for a subset of stations spanning a broad range of latitudes, together with the decadal mean simulation results obtained at the corre- sponding locations. Simulation results are included for the reference EC-Earth simulation and the corresponding ERA- Interim simulation, as well as for the ERA-Interim simula- tion with yearly changes in the emissions from anthropogenic activities and biomass burning (see Table 2). As for CO, the effect of these emission variations on the simulated decadal mean O3 concentrations at the stations used in the evalua- tion is very small, and sometimes barely visible. The sim- ulations with fixed emissions can therefore again be directly compared with the measurements (see Fig. 11 and Table A5). EC-Earth produces higher monthly mean surface concen- trations than the ERA-Interim simulation at all stations, ex- cept at Mauna Loa (Hawaii), Tutuila (American Samoa) and Pyramid on Mount Everest (Nepal). At the Antarctic stations, both simulations underestimate the measurements. Here EC-Earth is closer to the observa- tions than the ERA-Interim simulation, but this is achieved at the expense of the correlation between the measured and simulated monthly concentrations. At Cape Grim (Tasma- nia), the seasonal cycle in both simulations is weaker than in the observations. EC-Earth is in excellent agreement with the observations during the winter months, but overestimates the observations during summer. The ERA-Interim simula- tion, on the other hand, is in good agreement during summer, but underestimates the observations during winter. The ERA-Interim simulation also underestimates the mea- surements at high northern latitudes, especially during win- ter. Here EC-Earth is on average closer to the observations. www.geosci-model-dev.net/7/2435/2014/ Geosci. Model Dev., 7, 2435?2475, 2014 2456 T. P. C. van Noije et al.: Simulation of chemistry and aerosols with EC-Earth -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth, DJF 0 5 10 15 20 25 30 35 40 45 50 55 60 Surface Ozone (ppbv) -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth, JJA 0 5 10 15 20 25 30 35 40 45 50 55 60 Surface Ozone (ppbv) -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth - ERA-Interim, DJF -15 -12.5 -10 -7.5 -5 -2.5 0 2.5 5 7.5 10 12.5 15 Surface Ozone Difference (ppbv) -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth - ERA-Interim, JJA -15 -12.5 -10 -7.5 -5 -2.5 0 2.5 5 7.5 10 12.5 15 Surface Ozone Difference (ppbv) Figure 10. Surface O3 mixing ratios in the reference EC-Earth simulation (top) and the differences compared to the corresponding ERA- Interim simulation (bottom) for boreal winter (left) and boreal summer (right). At Summit (Greenland), EC-Earth is in excellent agreement with the measurements during summer and underestimates the measurements in the other seasons. At Storhofdi (Ice- land), on the other hand, EC-Earth very well reproduces the measured concentrations in winter, but overestimates them in the other seasons. The picture is different at the tropical and subtropical sta- tions, where both simulations show an average positive bias. At Tutuila station, located in the tropics in the SH, the sim- ulations give similar results and systematically overestimate the observations. At Mauna Loa, EC-Earth is in reasonable agreement with the observations during spring and summer and overestimates the observations during fall and winter. Here the difference with the ERA-Interim simulation is rel- atively small compared to the interannual variability in the results. At the other tropical and subtropical stations, EC- Earth shows worse agreement with the observations than the ERA-Interim simulation, depending on the location. EC-Earth also shows an average positive bias at the NH mid-latitude stations. Here the model overestimates the mea- surements especially during summer. With the exception of the high-altitude station Hohenpeissenberg (Germany), the ERA-Interim simulation is closer to the observations at these stations. 4.6 Aerosols In this section the model is evaluated with regard to the sim- ulation of aerosols. Maps of the atmospheric loads of the different aerosol components from the EC-Earth and ERA- Interim simulations are presented in Fig. 12. In Table 6 we compare the corresponding global burdens, lifetimes, and dry and wet deposition rates as well as the emissions of sea salt and mineral dust with results from recent modelling stud- ies, in particular multi-model estimates from AeroCom and ACCMIP. Results on the global budgets of the sulfate pre- cursors DMS, MSA, and SO2 are given in Table A6. Compared to the ERA-Interim simulation, the sulfate load in EC-Earth is on average lower in the tropics and, especially in boreal winter, higher in the extratropics. The decrease in the tropics is mainly caused by a lower chemical production (see Table A6). The increase in the extratropics is the com- bined effect of a higher chemical production and a longer lifetime. The loads of black carbon, organic aerosols, and ni- trate are also higher at high northern latitudes in boreal win- ter. Furthermore, EC-Earth gives higher sea salt loads at high latitudes, especially during local winter and spring. This is mainly due to higher emissions from the oceans (see Ta- ble 6). Since the emission rate calculated in the model de- pends strongly on the 10 m wind speed (Sect. 2.2.9), the Geosci. Model Dev., 7, 2435?2475, 2014 www.geosci-model-dev.net/7/2435/2014/ T. P. C. van Noije et al.: Simulation of chemistry and aerosols with EC-Earth 2457 Cape Grim Station, Tasmania JanFebMarApr May Jun Jul AugSep Oct NovDec 0 10 20 30 40 50 60 70 80 01 02 0304 050607 080 Ozone Mixing Ratio (ppbv) Hohenpeissenberg Station, Germany JanFebMarApr May Jun Jul AugSep Oct NovDec 0 10 20 30 40 50 60 70 80 01 02 0304 050607 080 Ozone Mixing Ratio (ppbv) Tudor Hill Station, Bermuda JanFebMarApr May Jun Jul AugSep Oct NovDec 0 10 20 30 40 50 60 70 80 01 02 0304 050607 080 Ozone Mixing Ratio (ppbv) Tutuila Station, American Samoa JanFebMarApr May Jun Jul AugSep Oct NovDec 0 10 20 30 40 50 60 70 80 01 02 0304 050607 080 Ozone Mixing Ratio (ppbv) Mauna Loa Station, Hawaii JanFebMarApr May Jun Jul AugSep Oct NovDec 0 10 20 30 40 50 60 70 80 01 02 0304 050607 080 Ozone Mixing Ratio (ppbv) South Pole Station JanFebMarApr May Jun Jul AugSep Oct NovDec 0 10 20 30 40 50 60 70 80 01 02 0304 050607 080 Ozone Mixing Ratio (ppbv) Obse rv at i o n sERA-In te rim , v a r. e mi s .ERA-In te rimE C -E a r t h Observations ERA-Interim, var. emis. ERA-Interim EC-Earth Mace Head Station, Ireland JanFebMarApr May Jun Jul AugSep Oct NovDec 0 10 20 30 40 50 60 70 80 01 02 0304 050607 080 Ozone Mixing Ratio (ppbv) Storhofdi Station, Iceland JanFebMarApr May Jun Jul AugSep Oct NovDec 0 10 20 30 40 50 60 70 80 01 02 0304 050607 080 Ozone Mixing Ratio (ppbv) Summit Station, Greenland JanFebMarApr May Jun Jul AugSep Oct NovDec 0 10 20 30 40 50 60 70 80 01 02 0304 050607 080 Ozone Mixing Ratio (ppbv) Figure 11. Comparison of monthly mean surface O3 mixing ratios from the reference EC-Earth simulation (solid red lines) and the two ERA- Interim simulations (solid and dotted blue lines) against in situ measurements at a number of stations included in the NOAA GMD, WDCGG, and/or EMEP databases (solid black lines). The results from the ERA-Interim simulation with interannual variations in the emissions from anthropogenic activities and biomass burning (dotted blue lines) nearly coincide with those from the ERA-Interim simulation where these emissions are fixed to their values for the year 2000 (solid blue lines). The contributions from O3S are shown by the dashed lines at the bottom of each panel (red for EC-Earth, blue for ERA-Interim). emissions at high and mid-latitudes are highest during the winter season. Moreover, small differences in surface winds over the oceans may introduce substantial differences in the emissions. A comparison of the sea salt emissions in both simulations shows that EC-Earth produces higher emissions over large parts of the northern Pacific and the Southern Ocean (not shown). In the tropics, the differences in the aerosol distributions between the two simulations also reflect a shift in the location of the inter-tropical convergence zone (ITCZ). In particular, during boreal winter a southward shift in the aerosol loads can be observed over central Africa and the tropical Atlantic for all components except sea salt. As the mineral-dust and biomass burning emissions are the same in both simulations, this shift in the aerosol distributions is likely caused by dif- ferences in the location of the ITCZ and in the associated transport. The global burdens of the different aerosol components from both simulations are generally on the low side of the ranges obtained in recent model intercomparison studies (see Table 6). On the other hand, their atmospheric lifetimes and the relevant dry and wet deposition rates are well within the multi-model estimates from these studies. This indicates that the emissions of aerosols and/or aerosol precursors are lower in our simulations. As can be verified in Tables 6 and A6, the emissions of sea salt and DMS in our simulations are indeed on the low side of the ranges used in AeroCom and ACCMIP, respectively. Moreover, the volcanic sulfur emissions applied in our model are substantially lower than in the ACCMIP models. The aerosol optical depth (AOD) field from the EC-Earth simulation is quantitatively similar to the result obtained with ERA-Interim (see Fig. 13). The spatial correlation between the multi-annual mean AOD fields from the two simulations is 0.97 and the global mean AOD values differ by only 3 %. EC-Earth gives somewhat higher values at high latitudes, especially during winter and spring. This is primarily due to a higher contribution from sea salt. The higher AOD values simulated by EC-Earth in the Arctic are in somewhat better agreement with ground-based and satellite measurements as well as reanalysis data (see von Hardenberg et al., 2012). In the tropics and at mid-latitudes the AOD differences be- tween the two simulations can be positive or negative, de- pending on the location and the season. During boreal winter www.geosci-model-dev.net/7/2435/2014/ Geosci. Model Dev., 7, 2435?2475, 2014 2458 T. P. C. van Noije et al.: Simulation of chemistry and aerosols with EC-Earth -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth, DJF 0.309 0 0.01 0.02 0.05 0.1 0.2 0.5 1 2 4 6 8 10 Black Carbon Load (mg/m 2 ) -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth, DJF 2.25 0 0.1 0.2 0.5 1 2 5 10 20 40 60 80 100 Organic Aerosol Load (mg/m 2 ) -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth, DJF 0.414 0 0.01 0.02 0.05 0.1 0.2 0.5 1 2 4 68 Nitrate Load (mg/m 2 ) -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth, DJF 13.9 0 0.5 1 2 5 10 15 20 25 30 40 50 Sea Salt Load (mg/m 2 ) -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth, DJF 20.5 0 10 20 50 100 200 300 400 500 600 800 1000 Mineral Dust Load (mg/m 2 ) -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth - ERA-Interim, DJF 0.014 -1 -0.5 -0.2 -0.1 -0.05 0 0.05 0.1 0.2 0.5 1 Black Carbon Load Difference (mg/m 2 ) -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth - ERA-Interim, DJF 0.16 -20 -10 -5 -2 -1 -0.5 0 0.5 1 2 5 10 20 Organic Aerosol Load Difference (mg/m 2 ) -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth - ERA-Interim, DJF 0.218 -2 -1.5 -1 -0.5 -0.2 -0.1 0 0.1 0.2 0.5 1 1.5 2 Nitrate Load Difference (mg/m 2 ) -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth - ERA-Interim, DJF 1.4 -25 -20 -15 -10 -5 -2 -1 0 1 2 5 10 15 20 25 Sea Salt Load Difference (mg/m 2 ) -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth - ERA-Interim, DJF 0.82 -200 -100 -50 -20 -10 0 10 20 50 100 200 Mineral Dust Load Difference (mg/m 2 ) -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth, JJA 0.287 0 0.01 0.02 0.05 0.1 0.2 0.5 1 2 4 6 8 10 Black Carbon Load (mg/m 2 ) -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth, JJA 2.70 0 0.1 0.2 0.5 1 2 5 10 20 40 60 80 100 Organic Aerosol Load (mg/m 2 ) -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth, JJA 0.074 0 0.01 0.02 0.05 0.1 0.2 0.5 1 2 4 68 Nitrate Load (mg/m 2 ) -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth - ERA-Interim, JJA 0.014 -2 -1.5 -1 -0.5 -0.2 -0.1 0 0.1 0.2 0.5 1 1.5 2 Nitrate Load Difference (mg/m 2 ) -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth, JJA 13.2 0 0.5 1 2 5 10 15 20 25 30 40 50 Sea Salt Load (mg/m 2 ) -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth - ERA-Interim, JJA 1.1 -25 -20 -15 -10 -5 -2 -1 0 1 2 5 10 15 20 25 Sea Salt Load Difference (mg/m 2 ) -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth, JJA 24.1 0 10 20 50 100 200 300 400 500 600 800 1000 Mineral Dust Load (mg/m 2 ) -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth - ERA-Interim, JJA -6.1 -200 -100 -50 -20 -10 0 10 20 50 100 200 Mineral Dust Load Difference (mg/m 2 ) -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth - ERA-Interim, JJA -0.021 -1 -0.5 -0.2 -0.1 -0.05 0 0.05 0.1 0.2 0.5 1 Black Carbon Load Difference (mg/m 2 ) -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth - ERA-Interim, JJA -0.022 -20 -10 -5 -2 -1 -0.5 0 0.5 1 2 5 10 20 Organic Aerosol Load Difference (mg/m 2 ) -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth, DJF 2.61 0 0.2 0.5 1 2 4 6 8 10 12 15 20 Sulfate Load (mg/m 2 ) -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth - ERA-Interim, DJF 0.39 -10 -5 -2 -1 -0.5 -0.2 0 0.2 0.5 1 2 5 10 Sulfate Load Difference (mg/m 2 ) -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth, JJA 3.57 0 0.2 0.5 1 2 4 6 8 10 12 15 20 Sulfate Load (mg/m 2 ) -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth - ERA-Interim, JJA -0.11 -10 -5 -2 -1 -0.5 -0.2 0 0.2 0.5 1 2 5 10 Sulfate Load Difference (mg/m 2 ) Figure 12. Total loads of the different aerosol components in the reference EC-Earth simulation and the differences compared to the corre- sponding ERA-Interim simulation for boreal winter (left two columns) and boreal summer (right two columns). The global mean values of the displayed fields are indicated at the top of each panel. Geosci. Model Dev., 7, 2435?2475, 2014 www.geosci-model-dev.net/7/2435/2014/ T. P. C. van Noije et al.: Simulation of chemistry and aerosols with EC-Earth 2459 Table 6. Global budgets, burdens, and lifetimes of the different aerosol components for the reference EC-Earth simulation and the corre- sponding ERA-Interim simulation. Estimates of their contributions to the optical depth at 550 nm are also included. The results are compared with estimates from other studies. EC-Earth ERA-Interim Otherstudies Sulfate Emissions(TgSyear?1) 1.47a Chemicalproduction(TgSyear?1) SO2 +OH 7.80 8.24 S(IV)+H2O2 23.9 24.2 S(IV)+O3 5.42 4.58 Burden(TgS) 0.522 0.498 0.67?0.17d Lifetime(days) 4.93 4.73 5.0?2.0d 4.1?0.7e Drydepositionrate(day?1) 4.68?10?3 4.57?10?3 0.03?0.02e Wetdepositionrate(day?1) 0.198 0.207 0.22?0.05e Opticaldepth 2.13?10?2 2.08?10?2 0.044f Blackcarbon Emissions(Tgyear?1) 7.77 Burden(Tg) 0.145 0.149 0.16?0.07d Lifetime(days) 6.81 6.99 7.4?3.4d 7.1?2.3e Drydepositionrate(day?1) 6.17?10?3 5.65?10?3 0.03?0.02e Wetdepositionrate(day?1) 0.141 0.137 0.12?0.04e Opticaldepth 1.11?10?3 1.15?10?3 0.0085f Organicaerosols Emissions(Tgyear?1) 69.5b Burden(Tg) 1.18 1.16 1.6?0.8g Lifetime(days) 6.18 6.08 5.7?1.6g Drydepositionrate(day?1) 5.23?10?3 4.69?10?3 0.029?0.046g Wetdepositionrate(day?1) 0.157 0.160 0.16?0.04g Opticaldepth 9.28?10?3 9.29?10?3 0.024f Nitrate Burden(TgN) 2.29?10?2 1.27?10?2 0.1?0.0h Opticaldepth 6.82?10?4 3.99?10?4 0.007?0.001h Seasalt Emissions(Pgyear?1) 7.35?0.11c 6.83?0.09c 8.2?8.2i 16.6?33.0e Burden(Tg) 6.81 6.17 7.9?5.5i 7.5?4.1e Lifetime(days) 0.338 0.330 0.48?0.28e Drydepositionrate(day?1) 2.42 2.40 4.3?9.4e Wetdepositionrate(day?1) 0.538 0.630 0.79?0.61e Opticaldepth 2.66?10?2 2.35?10?2 0.055?0.016j Mineraldust Emissions(Pgyear?1) 1.78 1.84?0.90e Burden(Tg) 12.1 13.4 19.2?7.7e Lifetime(days) 2.48 2.75 4.1?1.8e Drydepositionrate(day?1) 0.311 0.287 0.23?0.19e Wetdepositionrate(day?1) 9.20?10?2 7.60?10?2 0.08?0.03e Opticaldepth 1.55?10?2 1.71?10?2 0.043?0.014j a Includes0.12TgSyear?1 fromvolcanoes.b Includes19.1Tgyear?1 representingSOA(seeSect.2.2.5). c Standarddeviationscalculatedfromthesimulatedinterannualvariability. d ACCMIPmulti-modelmeansand standarddeviationsfortheyear2000fromShindelletal.(2013).e AeroComphase-Imulti-modelmeansand standarddeviationsfromTextoretal.(2006). f MACCreanalysis(Benedettietal.,2009)resultsfortheyear2003 asprovidedontheAeroComphase-IIwebinterface(http://aerocom.met.no/cgi-bin/aerocom/surfobs_annualrs.pl; simulationlabelled?ECMWF_FBOV?). g AeroComphase-IImulti-modelmeansandstandarddeviationsfrom Tsigaridisetal.(2014).h Resultsfor1998?2002froma CMIP5simulationwiththeHadley Centreclimatemodel HadGEM2-ESbyBellouinetal.(2011).i AeroComphase-Imulti-modelmeansandstandarddeviationsfrom Textoretal.(2007),basedona selectionofsevenmodelsfromTextoretal.(2006).j MACCreanalysisresultswith uncertaintyestimatesfromBellouinetal.(2013). www.geosci-model-dev.net/7/2435/2014/ Geosci. Model Dev., 7, 2435?2475, 2014 2460 T. P. C. van Noije et al.: Simulation of chemistry and aerosols with EC-Earth -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth - ERA-Interim, DJF 0.0066 -0.2 -0.15 -0.1 -0.05 -0.02 -0.01 0 0.01 0.02 0.05 0.1 0.15 0.2 AOD Difference at 550 nm -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth - ERA-Interim, JJA -0.0018 -0.2 -0.15 -0.1 -0.05 -0.02 -0.01 0 0.01 0.02 0.05 0.1 0.15 0.2 AOD Difference at 550 nm -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth, DJF 0.0716 0 0.01 0.02 0.04 0.06 0.08 0.1 0.15 0.2 0.3 0.4 0.5 0.6 Aerosol Optical Depth at 550 nm -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth, JJA 0.0790 0 0.01 0.02 0.04 0.06 0.08 0.1 0.15 0.2 0.3 0.4 0.5 0.6 Aerosol Optical Depth at 550 nm Figure 13. Aerosol optical depth at 550 nm in the reference EC-Earth simulation (top) and the differences compared to the corresponding ERA-Interim simulation (bottom) for boreal winter (left) and boreal summer (right). The global mean values of the displayed fields are indicated at the top of each panel. a southward shift in the AOD pattern can be observed over central Africa and the tropical Atlantic. This is primarily due to a shift in the contributions from mineral dust and biomass burning (see Fig. A1 in the Appendix), and reflects a shift in the location of the ITCZ. During boreal summer, EC- Earth gives smaller AOD values over large parts of northern Africa and the tropical Atlantic. In the NH this can mainly be attributed to a lower contribution from mineral dust, over the southern equatorial Atlantic to a lower contribution from biomass burning. In most of western Africa and the Sahel, EC-Earth produces lower AOD values than the ERA-Interim simulation in all seasons. EC-Earth also produces somewhat lower AOD values over India and the Arabian Sea from sum- mer to winter, especially during the summer season. This is mainly caused by lower contributions from mineral dust and sulfate (see Fig. A1). We have evaluated the AOD fields from both simulations against remote-sensing data from the Moderate Resolution Imaging Spectroradiometer (MODIS) instrument aboard the Terra and Aqua satellites, part of NASA?s Earth Observing System (EOS). For this analysis, we have used the Level- 3 monthly gridded AOD fields from MODIS collection 5.1, which are provided at 1??1? resolution. We have included the data for the years 2000?2009 and averaged the results from the Terra and Aqua data products. The resulting mean fields were subsequently coarsened to the 3??2? grid of TM5. Both simulations strongly underestimate the AOD values retrieved from MODIS over almost the entire globe (Fig. 14). The mean bias is ?0.083 for EC-Earth and ?0.086 for the ERA-Interim simulation, which is 53 and 54 %, respec- tively, of the retrieved mean value of 0.158. EC-Earth gives a smaller mean bias than the ERA-Interim simulation from boreal autumn to spring, especially in the winter season (see Table A7). There are some land regions where the simulations pro- duce higher values than observed. This is for instance the case over large parts of Australia, which also include desert areas, in all seasons. As it is difficult to accurately retrieve AOD over deserts because of the high reflectivity of the sur- face, biases in these regions can be due to model biases as well as errors in the MODIS retrieval. The simulations also give higher AOD values over the southeastern United States during boreal winter and autumn, over southern parts Cen- tral America during boreal winter, over eastern parts of South America during austral winter and autumn, and over parts of South Africa during austral summer and autumn. We have checked that these biases are not caused by the fact that in the reference EC-Earth simulation and the corresponding ERA-Interim simulation the emissions from anthropogenic Geosci. Model Dev., 7, 2435?2475, 2014 www.geosci-model-dev.net/7/2435/2014/ T. P. C. van Noije et al.: Simulation of chemistry and aerosols with EC-Earth 2461 -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth - MODIS, DJF -0.073 -0.5 -0.2 -0.1 -0.05 -0.02 0 0.02 0.05 0.1 0.2 0.5 AOD Difference at 550 nm -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth - MODIS, JJA -0.087 -0.5 -0.2 -0.1 -0.05 -0.02 0 0.02 0.05 0.1 0.2 0.5 AOD Difference at 550 nm Figure 14. Difference in aerosol optical depth at 550 nm from the reference EC-Earth simulation compared to the MODIS Level-3 product coarsened to the same resolution and averaged over the years 2000?2009 for boreal winter (left) and boreal summer (right). Grid areas where, for all consecutive years, the MODIS data are missing for one or more months during the presented seasons are not included. The mean values of the displayed fields are indicated at the top of each panel. activities and biomass burning were fixed to their values for the year 2000. Biases of similar magnitude are found in the ERA-Interim simulation with emissions varying from year to year. In other parts of the world, the simulated AOD values are generally much lower than the MODIS values. In all seasons, the AOD fields from the simulations cor- relate well with the distributions observed by MODIS (Ta- ble A7). The spatial correlation between the simulated and observed multi-annual mean AOD fields is 0.80 for EC-Earth and 0.79 for ERA-Interim, which means that 65 and 62 %, re- spectively, of the observed spatial variability is captured by the simulations. The observed spatial distribution is slightly better represented by EC-Earth than by the ERA-Interim sim- ulation during boreal winter and autumn, and slightly worse during boreal summer. We have also calculated the temporal correlation between the simulated and observed monthly mean AOD values as a function of geographical location. As we have only in- cluded locations where observations are available for every month of the year, the analysis is restricted to the tropics and mid-latitudes. The resulting seasonal correlation map shows strong spatial variability where regions with high correlations are intermixed with regions with low correlation (Fig. 15, left panel). Moreover, in some regions the observed seasonal cy- cle is better represented by EC-Earth, in other regions by the ERA-Interim simulation (Fig. 15, right panel). For instance, EC-Earth gives higher correlations over the southern equato- rial Atlantic and the southern Indian Ocean, but lower cor- relations over the northern equatorial Atlantic, the Arabian Sea, the Bay of Bengal, and Indonesia. Finally, we compare the contributions from the individual aerosol components to the global mean optical depth in our simulations with estimates from an aerosol reanalysis pro- duced within the MACC project. The MACC reanalysis sys- tem for aerosols is based on the IFS meteorological assimila- tion system with an integrated aerosol module (Morcrette et al., 2009) and uses MODIS retrievals of total AOD at 550 nm to further constrain the aerosol simulation (Benedetti et al., 2009). Because total AOD is assimilated in the reanalysis, it provides a valuable reference data set for evaluating global aerosol models. Compared to the results from the MACC reanalysis, our simulations underestimate the global mean AOD contribu- tions for all components (see Table 6). Both in the reanal- ysis and in our simulations, the components that contribute most to the global mean AOD at 550 nm are sea salt, sulfate, and mineral dust, followed by organic aerosols. Compared to the reanalysis results, the contributions from these compo- nents are underestimated by a factor 2 to 3. It is important to note, however, that the distribution of AOD over the indi- vidual aerosol components in the reanalysis is also subject to model uncertainty. 5 Discussion and conclusions We have integrated the atmospheric chemistry and transport model TM5 into the global climate model EC-Earth. The sys- tem allows for two-way exchange of fields between TM5 and IFS, the atmospheric GCM of EC-Earth. Here we have tested the system in one-way coupled configuration. We have car- ried out a decadal simulation of tropospheric chemistry and aerosols for present-day conditions, and calculated chemi- cal budgets and climatologies of tracer concentrations and aerosol optical depth. We have evaluated the results against corresponding TM5 simulations driven offline by meteoro- logical fields from (1) the ERA-Interim reanalysis and (2) the EC-Earth model itself, as well as against various observa- tional data sets. Differences in transport have been diagnosed from the simulated radon-222 concentrations. Compared to the of- fline simulations, the online-coupled system exhibits more efficient vertical mixing in the troposphere. This is due to www.geosci-model-dev.net/7/2435/2014/ Geosci. Model Dev., 7, 2435?2475, 2014 2462 T. P. C. van Noije et al.: Simulation of chemistry and aerosols with EC-Earth -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth vs. MODIS 0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1 AOD Correlation Coefficient -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth - ERA-Interim -1 -0.8 -0.6 -0.4 -0.2 -0.1 0 0.1 0.2 0.4 0.6 0.8 1 AOD Correlation Coefficient Difference Figure 15. Linear correlation coefficient between the decadal monthly mean aerosol optical depths at 550 nm from the reference EC-Earth simulation and the MODIS Level-3 product coarsened to the same resolution (left), and the difference compared to the corresponding correlation coefficient for the ERA-Interim simulation (right). Grid areas where, for all consecutive years, the MODIS data are missing for one or more months are not included. the different treatment of cumulus convection in the online- coupled system, in which the relevant convective fields are passed from IFS to TM5. In the offline simulations these fields are calculated diagnostically based on a somewhat out- dated parameterization (Tiedtke, 1989). The stronger mixing characteristics seen in the coupled system likely reflect im- provements in the convection scheme made in more recent cycles of IFS (Bechtold et al., 2008; Jung et al., 2010). Compared to the ERA-Interim simulation, the oxidizing capacity in EC-Earth is lower in large parts of the tropi- cal and subtropical troposphere, and higher in the extratrop- ics. The lower oxidizing capacity in the tropics and subtrop- ics is primarily driven by the model?s cold bias in these re- gions, which results in a lower specific humidity. As a con- sequence, the atmospheric lifetime of CH4 is 7 % longer in EC-Earth than in the ERA-Interim simulation: EC-Earth gives a lifetime of 9.4 years, while the ERA-Interim simu- lation gives 8.8 years. Both values are well within the range 9.1?0.9 years, recently estimated by Prather et al. (2012). Differences in vertical mixing and oxidizing capacity also affect the distribution of other chemically reactive gases such as CO and O3. Compared to the ERA-Interim simulation, the total chemical production and destruction of CO are lower in EC-Earth, resulting in very similar total amounts and a 4 % longer lifetime. On the other hand, EC-Earth gives lower CO concentrations in the NH extratropics, due to faster chemical destruction in this region. This leads to a somewhat stronger underestimation of the surface concentrations measured by the NOAA GMD flask sampling network. In both configu- rations, the total chemical production of CO in TM5 is be- low the range of model estimates reported by Shindell et al. (2006b), suggesting that the CBM4 chemistry scheme un- derestimates the production of CO from NMVOCs. The influx of O3 from the stratosphere to the troposphere is 14 % higher in EC-Earth than in the ERA-Interim simula- tion, and is in slightly better agreement with other modelling studies as well as observational estimates. Moreover, the cold bias in EC-Earth tends to slow down the chemical destruc- tion of O3 in the troposphere, resulting in an increase in the net chemical production of O3 in the troposphere. Further- more, enhanced vertical mixing tends to redistribute O3 from higher to lower parts of the troposphere. Overall, the total amount of O3 in the troposphere is 6 % higher in EC-Earth, in better agreement with the ranges reported in the model inter- comparison studies by Stevenson et al. (2006) and Young et al. (2013). The average lifetime of tropospheric O3 increases by 7 % from 23.9 days with ERA-Interim to 25.5 days in EC- Earth. The latter value is higher than the multi-model range reported by Stevenson et al. (2006) and is on the high side of the model results reported by Young et al. (2013). Overall, EC-Earth produces lower concentrations in the upper parts of the tropical and subtropical troposphere and higher concentrations in most of the lower and middle tro- posphere, especially in the extratropics. Similarly, EC-Earth gives higher surface concentrations in most of the world, with the exception of some regions located in the tropics and sub- tropics. This results in a 15 % higher total deposition of O3 compared to the ERA-Interim simulation. The simulated O3 concentrations have been evaluated against a vertically resolved, zonal, and monthly mean data set produced from satellite and ozonesonde observations (Hassler et al., 2009; www.bodeker.com) and against sur- face measurements from various networks. Both simulations show reasonable agreement with the observational data sets and both have their relative strengths and weaknesses de- pending on the location and the season. EC-Earth tends to overestimate the O3 concentrations in the lower troposphere and at the surface in the NH extratropics during boreal sum- mer and fall. Note that this is partly a resolution effect. It is well known that the relatively coarse horizontal res- olutions applied in the current generation of global chem- istry models tends to overestimate the production of O3 in the boundary layer (Wild and Prather, 2006). During bo- real winter and spring, on the other hand, as well as in the Geosci. Model Dev., 7, 2435?2475, 2014 www.geosci-model-dev.net/7/2435/2014/ T. P. C. van Noije et al.: Simulation of chemistry and aerosols with EC-Earth 2463 SH extratropics, the higher surface and lower-tropospheric concentrations produced by EC-Earth are generally in better agreement with the measurements than the results from the ERA-Interim simulation. The aerosol climatologies from both simulations are quan- titatively very similar. EC-Earth gives somewhat higher AOD values at high latitudes especially during winter and spring, mainly due to a higher contribution from sea salt. The global burdens of the various aerosol components are generally on the low side of the ranges obtained in recent model intercom- parison studies like AeroCom and ACCMIP. This is partly caused by lower natural emissions, in particular of sea salt, DMS and volcanic sulfur. However, previous studies indicate that the wet removal of aerosols in TM5 may also be too fast (see Aan de Brugh et al., 2011). A comparison with AOD fields retrieved from MODIS shows that the simulations cap- ture a large part of the spatial variability, but strongly under- estimate the observed values over almost the entire globe. In the system we have developed, the description of atmo- spheric chemistry and aerosols is not integrated into IFS. In- stead, it is taken care of by a separate module, TM5, which is coupled to IFS through OASIS. Previously, a coupled TM5- IFS system using OASIS was developed within the GEMS project (Flemming et al., 2009). However, the data exchange in that system was designed specifically for short-term fore- casts and reanalysis purposes, in which chemical data assim- ilation plays a central role. We also needed to completely redo the technical implementation of the coupling, because the GEMS system made use of an OASIS version that is in- compatible with the version used in EC-Earth. A more recent activity is the development of the Composition-IFS (C-IFS) model within the MACC project. In C-IFS the description of atmospheric chemistry is inte- grated into the IFS model (Flemming et al., 2012). As part of this development, the aerosol scheme of IFS (Morcrette et al., 2009) is also being upgraded and coupled to the gas- phase chemistry. The main advantages of C-IFS compared to the system we have developed are (1) that the description of chemistry and aerosols can be more tightly coupled to the relevant dynamical and physical processes described in IFS, and (2) that there is no external exchange of data. Conversely, the main advantages of our system compared to C-IFS are (1) that the tracer transport in TM5 is locally mass conserv- ing, and (2) that TM5 can be run at a lower resolution than IFS. The latter points are crucial to enable long-term climate integrations, but are less relevant for the short-term forecast and reanalysis simulations which C-IFS has been developed for, and (3) that the TM5 module can be kept more easily up to date with the offline version. The work presented in this study is the first step in the development of EC-Earth into an Earth system model with fully interactive chemistry and aerosols. A number of de- velopments are planned for the near future. First, to im- prove the simulation of aerosol burdens and optical depths, we intend to improve the representation of natural emissions of aerosols and aerosol precursors, and revisit the descrip- tion of the wet removal processes in TM5. At the same time, the calculation of photolysis rates will be updated following Williams et al. (2006, 2012) and coupled to the simulated aerosols. Moreover, the representation of hetero- geneous chemistry will be improved following Huijnen et al. (2014). Another line of work focuses on improving the representation of stratospheric chemistry through simplified schemes, but this is more a long-term project. Meanwhile, the performance and scalability of TM5 has recently been strongly improved, and will be further im- proved in the near future. The new, massively parallel model (named TM5-mp) is currently being implemented into the latest version of EC-Earth (version 3.0). In this system the couplings with the radiation and cloud schemes of IFS will be made, and the exchange period will be reduced from 6 to 3 h or less. A parallel development is the introduction of a carbon cy- cle in EC-Earth, based on the dynamic vegetation model LPJ- GUESS (Smith et al., 2001; Weiss et al., 2014) and the bio- geochemical component of NEMO. As part of these devel- opments, various couplings will be made between TM5 and the terrestrial and marine biosphere. www.geosci-model-dev.net/7/2435/2014/ Geosci. Model Dev., 7, 2435?2475, 2014 2464 T. P. C. van Noije et al.: Simulation of chemistry and aerosols with EC-Earth Appendix A Table A1. Vertical distributions applied to the different emission sources. The emissions from aviation are distributed as provided in the CMIP5 emission data set. Verticaldistributiontype Emissionsector/source Fractionperheightrange(%) 0?30m 30?100m 100?300m 300?600m 600?1000m 1000?2000m Energy Energyproductionanddistribution 0 10 70 20 0 0 Industrial Industrialprocessesandcombustion 10 20 60 10 0 0 Residential Residentialandcommercialcombustion 40 40 20 0 0 0 Waste Wastetreatmentanddisposal 10 20 40 30 0 0 Near-surfacea 80 20 0 0 0 0 Surfaceb 100 0 0 0 0 0 Volcanic VolcanicSO2 0 0 10 30 40 20 0?100m 100?500m 500?1000m 1000?2000m 2000?3000m 3000?6000m Forestfires Tropical(30?S?30?N) 20 20 20 40 0 0 Temperate(30?60?S/N) 20 20 20 40 0 0 High-latitude(60?90?S/N) 10 10 20 20 40 0 a Includessolventproductionandusesmaritimetransport,agriculturalwasteburning,grasslandfires,SOA,andmineraldust.b Includeslandtransport,agriculture,biogenicemissionsfromsoilsandvegetation, oceanicemissions,andradon-222. Table A2. List of stations used for the evaluation of the simulated surface radon-222 concentrations. The mean bias and root mean square errors (RMSE) in the simulated monthly mean concentrations are indicated for the online and offline EC-Earth simulations and the ERA- Interim simulation. Also given are the linear correlation coefficients between the simulated and measured monthly mean concentrations. A diurnal window has been applied to the measurements, except for Cape Grim. The results for the online EC-Earth simulation and the ERA-Interim simulation are separated by a slash; the results for the offline EC-Earth simulation are shown between parentheses. Station Lat. Long. Height Period Window Bias RMSE Correlation (deg) (deg) (m) (years) (hoursLT, inclusive) (Bqm?3) (Bqm?3) coefficient CapeGrim,Tasmania ?40.68 144.69 90 1991?2012 Notapplied 0.11/0.30 0.27/0.33 0.47/0.93 (0.19) (0.28) (0.79) Richmond,Australia ?33.62 150.75 24 2007?2012 14?18 ?0.10/0.33 0.50/0.53 0.81/0.84 (0.07) (0.59) (0.62) MaunaLoa,Hawaii 19.54 ?155.58 4170 2004?2012 8?10 ?0.03/?0.04 0.04/0.04 0.78/0.78 (?0.03) (0.04) (0.78) Gosan,JejuIsland,Korea 33.29 126.16 70 2001?2010 13?17 ?0.97/?0.82 1.07/0.95 0.66/0.59 (?0.96) (1.10) (0.45) SadoIsland,Japan 38.25 138.40 130 2002?2005 11?16 ?0.77/?0.43 0.94/0.73 ?0.70/?0.71 (?0.62) (0.84) (?0.64) Hohenpeissenberg, Germany 47.80 11.02 985 1999?2005 14?18 ?1.30/0.12 1.45/0.83 0.26/0.52 (?0.56) (0.97) (0.13) Geosci. Model Dev., 7, 2435?2475, 2014 www.geosci-model-dev.net/7/2435/2014/ T. P. C. van Noije et al.: Simulation of chemistry and aerosols with EC-Earth 2465 Table A3. Global budgets of oxidized and reduced reactive nitrogen (Tg N year?1) for the reference EC-Earth simulation and the correspond- ing ERA-Interim simulation, compared with the ACCMIP multi-model means and standard deviations for the year 2000 from Lamarque et al. (2013b). The standard deviations indicated for the NOx production by lightning in our simulations are calculated from the interannual variability. EC-Earth ERA-Interim ACCMIP Oxidized nitrogen (NOy) Total NOx emissions 49.6 49.0 49?3 NOx emissions by soils 4.95 NOx production by lightning 6.45?0.06 5.83?0.21 6?2 NOy dry deposition 21.1 20.9 21?7 NOy wet deposition 29.6 28.8 29?5 NOy net chemical production 1.02 0.76 ?1 Reduced nitrogen (NHx) NH3 emissions 48.5 49?2 NH3 dry deposition 21.9 22.3 15?6 NH4 dry deposition 0.0 0.0 5?1 NH3 wet deposition 8.23 8.14 7?4 NH4 wet deposition 18.1 17.8 23?6 NHx net chemical destruction 0.24 0.27 Table A4. List of stations from the NOAA GMD network of flask measurements used for the evaluation of the simulated surface CO mixing ratios. The mean bias and root mean square errors (RMSE) in the simulated monthly mean mixing ratios are indicated for the reference EC-Earth simulation and the corresponding ERA-Interim simulation. Also given are the linear correlation coefficients between the simulated and measured monthly mean concentrations. The results for the EC-Earth and ERA-Interim simulations are separated by a slash. Station Lat. Long. Height Period Bias RMSE Correlation (deg) (deg) (m) (years) (ppbv) (ppbv) coefficient South Pole ?89.98 ?24.80 2810 2000?2009 ?0.2/0.1 2.9/3.7 0.94/0.91 Halley Station, Antarctica ?75.58 ?26.5 30 2000?2009 ?1.2/?0.6 2.4/2.7 0.97/0.94 Cape Grim, Tasmania ?40.68 144.69 94 2000?2009 6.5/6.4 8.8/8.7 0.70/0.67 Tutuila, American Samoa ?14.25 ?170.56 42 2000?2009 ?3.9/?4.3 4.6/4.9 0.90/0.86 Ascension Island ?7.97 ?14.40 85 2000?2009 ?5.2/?3.1 9.3/7.9 0.69/0.83 Ragged Point, Barbados 13.16 ?59.43 15 2000?2009 ?18.3/?18.2 18.6/18.7 0.97/0.96 Mariana Islands, Guam 13.39 144.66 0 2000?2009 ?19.5/?15.9 19.6/16.9 0.99/0.96 Mauna Loa, Hawaii 19.54 ?155.58 3397 2000?2009 ?18.5/?18.4 18.8/18.8 0.98/0.98 Iza?a, Tenerife 28.31 ?16.50 2373 2000?2009 ?25.3/?23.9 25.9/24.6 0.96/0.94 Tudor Hill, Bermuda 32.27 ?64.88 30 2002?2009 ?29.3/?23.2 30.9/24.0 0.97/0.99 Terceira Island, Azores 38.77 ?27.38 19 2000?2009 ?33.9/?27.6 34.5/28.1 0.95/0.96 Mace Head, Ireland 53.33 ?9.90 5 2000?2009 ?30.2/?19.9 31.2/20.7 0.97/0.97 Cold Bay, Alaska 55.21 ?162.72 21 2000?2009 ?36.7/?29.2 39.0/31.5 0.92/0.90 Storhofdi, Iceland 63.40 ?20.29 118 2000?2009 ?34.0/?23.9 35.3/24.9 0.96/0.97 Barrow, Alaska 71.32 ?156.61 11 2000?2009 ?38.1/?28.7 41.0/31.3 0.94/0.96 Ny-?lesund, Spitsbergen 78.91 11.89 474 2000?2009 ?39.0/?28.0 41.0/29.5 0.97/0.98 Alert, Canada 82.45 ?62.51 200 2000?2009 ?38.9/?29.4 41.4/31.5 0.95/0.97 www.geosci-model-dev.net/7/2435/2014/ Geosci. Model Dev., 7, 2435?2475, 2014 2466 T. P. C. van Noije et al.: Simulation of chemistry and aerosols with EC-Earth Table A5. List of stations used for the evaluation of the simulated surface O3 mixing ratios. The mean bias and root mean square errors (RMSE) in the simulated monthly mean mixing ratios are indicated for the reference EC-Earth simulation and the corresponding ERA- Interim simulation. Also given are the linear correlation coefficients between the simulated and measured monthly mean concentrations. The results for the EC-Earth and ERA-Interim simulations are separated by a slash. Station Lat. Long. Height Period Bias RMSE Correlation (deg) (deg) (m) (years) (ppbv) (ppbv) coefficient South Pole ?89.98 ?24.80 2810 2000?2009 ?11.2/?17.1 11.6/17.3 0.70/0.94 Arrival Heights, Antarctica ?77.83 166.20 250 2000?2008 ?6.1/?13.3 8.0/14.1 0.86/0.89 Neumayer, Antarctica ?70.65 ?8.25 42 2000?2009 ?3.3/?10.5 5.6/11.1 0.86/0.97 Syowa, Antarctica ?69.00 39.58 16 2000?2009 ?2.8/?11.1 4.7/11.4 0.91/0.99 Cape Grim, Tasmania ?40.68 144.68 94 2000?2009 3.5/?3.3 5.0/4.9 0.88/0.89 Tutuila, American Samoa ?14.25 ?170.56 42 2000?2009 6.6/5.8 6.7/5.8 0.99/0.99 Ragged Point, Barbados 13.16 ?59.43 15 2006?2009 12.8/8.0 13.1/8.3 0.79/0.91 Cape Verde 16.85 ?24.87 10 2006?2009 11.1/5.9 12.5/7.3 0.31/0.68 Mauna Loa, Hawaii 19.54 ?155.58 3397 2000?2009 2.6/2.7 3.0/3.1 0.95/0.96 Assekrem, Algeria 23.27 5.63 2710 2000?2001, 2003?2009 9.0/5.1 9.5/5.6 0.66/0.78 Mount Everest, Nepal 27.96 86.82 5079 2006?2009 10.3/8.9 12.1/10.5 0.78/0.81 Iza?a, Tenerife 28.30 ?16.50 2367 2000?2009 10.6/2.7 11.6/3.9 0.76/0.83 Tudor Hill, Bermuda 32.27 ?64.88 30 2003?2009 6.2/1.7 7.9/5.8 0.87/0.85 Trinidad Head, California 41.05 ?124.15 107 2002?2009 11.0/2.9 11.9/5.9 0.44/0.38 Jungfraujoch, Switzerland 46.55 7.99 3580 2000?2009 6.9/?1.5 7.7/2.8 0.93/0.94 Payerne, Switzerland 46.82 6.95 490 2000?2009 9.4/1.8 10.1/4.3 40.93/0.93 Zugspitze, Germany 47.42 10.98 2960 2000?2002 7.9/0.1 8.7/3.5 0.90/0.90 Hohenpeissenberg, Germany 47.80 11.02 985 2000?2007 2.8/?10.2 5.5/11.6 0.88/0.91 Mace Head, Ireland 53.33 ?9.90 25 2000?2009 9.3/0.0 10.2/4.1 0.39/0.49 Storhofdi, Iceland 63.40 ?20.29 118 2003?2009 5.5/?6.2 7.2/7.1 0.40/0.69 Barrow, Alaska 71.32 ?156.61 11 2000?2009 2.5/?4.5 8.3/8.0 ?0.26/?0.16 Summit, Greenland 72.58 ?38.48 3216 2000?2009 ?4.0/?13.1 5.2/13.5 0.63/0.68 Geosci. Model Dev., 7, 2435?2475, 2014 www.geosci-model-dev.net/7/2435/2014/ T. P. C. van Noije et al.: Simulation of chemistry and aerosols with EC-Earth 2467 Table A6. Global budgets of DMS, MSA, SO2 and total reactive sulfur together with the global burden and lifetime of SO2 for the reference EC-Earth simulation and the corresponding ERA-Interim simulation. For comparison we have also included ACCMIP multi-model means and standard deviations of emissions and depositions for the year 2000 from Lamarque et al. (2013b). For the gas-phase SO2 and aqueous- phase S(IV) oxidation reactions, which result in the production of SO4, the numbers between parentheses give the separate contributions from 90?30? S, 30? S?30? N, and 30?90? N. EC-Earth ERA-Interim ACCMIP DMS Emissions (Tg S year?1) 19.4?0.2? 19.1?0.3? 23?5 Chemical destruction (Tg S year?1) DMS + OH 14.4 14.5 DMS + NO3 4.93 4.60 MSA Chemical production (Tg S year?1) DMS + OH 1.87 1.79 Wet deposition (Tg S year?1) 1.87 1.79 ?2 SO2 Total emissions (Tg S year?1) 57.2 65?2 Volcanic emissions (Tg S year?1) 4.67 ?12?2 Chemical production (Tg S year?1) DMS + OH 12.6 12.7 DMS + NO3 4.93 4.60 Chemical destruction (Tg S year?1) SO2+ OH 7.80 8.24 (0.43/3.84/3.53) (0.34/4.39/3.52) S(IV) + H2O2 23.9 24.2 (2.75/12.7/8.46) (2.63/13.4/8.11) S(IV) + O3 5.42 4.58 (1.01/2.58/1.83) (0.91/2.02/1.64) Dry deposition (Tg S year?1) 26.1 26.3 Wet deposition (Tg S year?1) 11.5 11.2 Burden (Tg S) 0.317 0.261 Lifetime (days) 1.55 1.28 Total reactive sulfur Emissions (Tg S year?1) 78.1 77.8 89?6 Dry deposition (Tg S year?1) 27.0 27.2 37?10 Wet deposition (Tg S year?1) 51.1 50.7 52?8 ? Standard deviations calculated from the simulated interannual variability. Table A7. Mean biases and linear correlation coefficients between the time averaged AOD fields from the simulations and the MODIS Level-3 product coarsened to the same resolution and averaged over the years 2000?2009. Grid areas where, for all consecutive years, the MODIS data are missing for one or more months during the year or season of interest have not been included in the calculations. The results for the EC-Earth and ERA-Interim simulations are separated by a slash. Season Mean bias Correlation coefficient Observed area (%) Annual ?0.083/?0.086 0.80/0.79 71.8 DJF ?0.073/?0.080 0.76/0.72 82.2 MAM ?0.093/?0.095 0.78/0.78 82.1 JJA ?0.087/?0.085 0.72/0.78 84.1 SON ?0.078/?0.080 0.62/0.60 84.8 www.geosci-model-dev.net/7/2435/2014/ Geosci. Model Dev., 7, 2435?2475, 2014 2468 T. P. C. van Noije et al.: Simulation of chemistry and aerosols with EC-Earth -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth, DJF 0.0011 0 0.01 0.02 0.04 0.06 0.08 0.1 0.15 0.2 0.3 0.4 0.5 0.6 Black Carbon AOD at 550 nm -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth - ERA-Interim, DJF 0.0000 -0.2 -0.15 -0.1 -0.05 -0.02 -0.01 0 0.01 0.02 0.05 0.1 0.15 0.2 Black Carbon AOD Difference at 550 nm -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth, JJA 0.0012 0 0.01 0.02 0.04 0.06 0.08 0.1 0.15 0.2 0.3 0.4 0.5 0.6 Black Carbon AOD at 550 nm -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth - ERA-Interim, JJA -0.0001 -0.2 -0.15 -0.1 -0.05 -0.02 -0.01 0 0.01 0.02 0.05 0.1 0.15 0.2 Black Carbon AOD Difference at 550 nm -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth, DJF 0.0084 0 0.01 0.02 0.04 0.06 0.08 0.1 0.15 0.2 0.3 0.4 0.5 0.6 Organic Aerosol AOD at 550 nm -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth - ERA-Interim, DJF 0.0004 -0.2 -0.15 -0.1 -0.05 -0.02 -0.01 0 0.01 0.02 0.05 0.1 0.15 0.2 Organic Aerosol AOD Difference at 550 nm -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth, JJA 0.0110 0 0.01 0.02 0.04 0.06 0.08 0.1 0.15 0.2 0.3 0.4 0.5 0.6 Organic Aerosol AOD at 550 nm -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth - ERA-Interim, JJA -0.0004 -0.2 -0.15 -0.1 -0.05 -0.02 -0.01 0 0.01 0.02 0.05 0.1 0.15 0.2 Organic Aerosol AOD Difference at 550 nm -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth, DJF 0.0014 0 0.01 0.02 0.04 0.06 0.08 0.1 0.15 0.2 0.3 0.4 0.5 0.6 Nitrate AOD at 550 nm -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth - ERA-Interim, DJF 0.0007 -0.2 -0.15 -0.1 -0.05 -0.02 -0.01 0 0.01 0.02 0.05 0.1 0.15 0.2 Nitrate AOD Difference at 550 nm -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth, JJA 0.0002 0 0.01 0.02 0.04 0.06 0.08 0.1 0.15 0.2 0.3 0.4 0.5 0.6 Nitrate AOD at 550 nm -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth - ERA-Interim, JJA 0.0000 -0.2 -0.15 -0.1 -0.05 -0.02 -0.01 0 0.01 0.02 0.05 0.1 0.15 0.2 Nitrate AOD Difference at 550 nm -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth, DJF 0.0275 0 0.01 0.02 0.04 0.06 0.08 0.1 0.15 0.2 0.3 0.4 0.5 0.6 Sea Salt AOD at 550 nm -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth - ERA-Interim, DJF 0.0031 -0.2 -0.15 -0.1 -0.05 -0.02 -0.01 0 0.01 0.02 0.05 0.1 0.15 0.2 Sea Salt AOD Difference at 550 nm -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth, JJA 0.0266 0 0.01 0.02 0.04 0.06 0.08 0.1 0.15 0.2 0.3 0.4 0.5 0.6 Sea Salt AOD at 550 nm -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth - ERA-Interim, JJA 0.0034 -0.2 -0.15 -0.1 -0.05 -0.02 -0.01 0 0.01 0.02 0.05 0.1 0.15 0.2 Sea Salt AOD Difference at 550 nm -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth, DJF 0.0149 0 0.01 0.02 0.04 0.06 0.08 0.1 0.15 0.2 0.3 0.4 0.5 0.6 Mineral Dust AOD at 550 nm -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth - ERA-Interim, DJF 0.0006 -0.2 -0.15 -0.1 -0.05 -0.02 -0.01 0 0.01 0.02 0.05 0.1 0.15 0.2 Mineral Dust AOD Difference at 550 nm -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth, JJA 0.0147 0 0.01 0.02 0.04 0.06 0.08 0.1 0.15 0.2 0.3 0.4 0.5 0.6 Mineral Dust AOD at 550 nm -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth - ERA-Interim, JJA -0.0038 -0.2 -0.15 -0.1 -0.05 -0.02 -0.01 0 0.01 0.02 0.05 0.1 0.15 0.2 Mineral Dust AOD Difference at 550 nm -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth, DJF 0.0183 0 0.01 0.02 0.04 0.06 0.08 0.1 0.15 0.2 0.3 0.4 0.5 0.6 Sulfate AOD at 550 nm -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth - ERA-Interim, DJF 0.0018 -0.2 -0.15 -0.1 -0.05 -0.02 -0.01 0 0.01 0.02 0.05 0.1 0.15 0.2 Sulfate AOD Difference at 550 nm -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth, JJA 0.0254 0 0.01 0.02 0.04 0.06 0.08 0.1 0.15 0.2 0.3 0.4 0.5 0.6 Sulfate AOD at 550 nm -180 -150 -120 -90 -60 -30 0 30 60 90 120 150 180 -90 -60 -30 0 30 60 90 EC-Earth - ERA-Interim, JJA -0.0009 -0.2 -0.15 -0.1 -0.05 -0.02 -0.01 0 0.01 0.02 0.05 0.1 0.15 0.2 Sulfate AOD Difference at 550 nm Figure A1. Contributions from the different aerosol components to the aerosol optical depth at 550 nm in the reference EC-Earth simulation and the differences compared to the corresponding ERA-Interim simulation for boreal winter (left two columns) and boreal summer (right two columns). The global mean values of the displayed fields are indicated at the top of each panel. Geosci. Model Dev., 7, 2435?2475, 2014 www.geosci-model-dev.net/7/2435/2014/ T. P. C. van Noije et al.: Simulation of chemistry and aerosols with EC-Earth 2469 Acknowledgements. The authors thank Klaus Wyser from the Swedish Meteorological and Hydrological Institute (SMHI) for providing the IFS-NEMO restart fields used to initialize the online EC-Earth simulations and Tido Semmler for providing IFS model-level output from an EC-Earth simulation performed by the Irish National Meteorological Service. 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