A new version of the general circulation model CNRM-CM has been developed jointly by CNRM-GAME (Centre National de Recherches Météorologiques—Groupe d’études de l’Atmosphère Météorologique) and ...Cerfacs (Centre Européen de Recherche et de Formation Avancée) in order to contribute to phase 5 of the Coupled Model Intercomparison Project (CMIP5). The purpose of the study is to describe its main features and to provide a preliminary assessment of its mean climatology. CNRM-CM5.1 includes the atmospheric model ARPEGE-Climat (v5.2), the ocean model NEMO (v3.2), the land surface scheme ISBA and the sea ice model GELATO (v5) coupled through the OASIS (v3) system. The main improvements since CMIP3 are the following. Horizontal resolution has been increased both in the atmosphere (from 2.8° to 1.4°) and in the ocean (from 2° to 1°). The dynamical core of the atmospheric component has been revised. A new radiation scheme has been introduced and the treatments of tropospheric and stratospheric aerosols have been improved. Particular care has been devoted to ensure mass/water conservation in the atmospheric component. The land surface scheme ISBA has been externalised from the atmospheric model through the SURFEX platform and includes new developments such as a parameterization of sub-grid hydrology, a new freezing scheme and a new bulk parameterisation for ocean surface fluxes. The ocean model is based on the state-of-the-art version of NEMO, which has greatly progressed since the OPA8.0 version used in the CMIP3 version of CNRM-CM. Finally, the coupling between the different components through OASIS has also received a particular attention to avoid energy loss and spurious drifts. These developments generally lead to a more realistic representation of the mean recent climate and to a reduction of drifts in a preindustrial integration. The large-scale dynamics is generally improved both in the atmosphere and in the ocean, and the bias in mean surface temperature is clearly reduced. However, some flaws remain such as significant precipitation and radiative biases in many regions, or a pronounced drift in three dimensional salinity.
The Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) examined the short-lived drivers of climate change in current climate models. Here we evaluate the 10 ACCMIP models that ...included aerosols, 8 of which also participated in the Coupled Model Intercomparison Project phase 5 (CMIP5). The models reproduce present-day total aerosol optical depth (AOD) relatively well, though many are biased low. Contributions from individual aerosol components are quite different, however, and most models underestimate east Asian AOD. The models capture most 1980–2000 AOD trends well, but underpredict increases over the Yellow/Eastern Sea. They strongly underestimate absorbing AOD in many regions. We examine both the direct radiative forcing (RF) and the forcing including rapid adjustments (effective radiative forcing; ERF, including direct and indirect effects). The models' all-sky 1850 to 2000 global mean annual average total aerosol RF is (mean; range) −0.26 W m−2; −0.06 to −0.49 W m−2. Screening based on model skill in capturing observed AOD yields a best estimate of −0.42 W m−2; −0.33 to −0.50 W m−2, including adjustment for missing aerosol components in some models. Many ACCMIP and CMIP5 models appear to produce substantially smaller aerosol RF than this best estimate. Climate feedbacks contribute substantially (35 to −58%) to modeled historical aerosol RF. The 1850 to 2000 aerosol ERF is −1.17 W m−2; −0.71 to −1.44 W m−2. Thus adjustments, including clouds, typically cause greater forcing than direct RF. Despite this, the multi-model spread relative to the mean is typically the same for ERF as it is for RF, or even smaller, over areas with substantial forcing. The largest 1850 to 2000 negative aerosol RF and ERF values are over and near Europe, south and east Asia and North America. ERF, however, is positive over the Sahara, the Karakoram, high Southern latitudes and especially the Arctic. Global aerosol RF peaks in most models around 1980, declining thereafter with only weak sensitivity to the Representative Concentration Pathway (RCP). One model, however, projects approximately stable RF levels, while two show increasingly negative RF due to nitrate (not included in most models). Aerosol ERF, in contrast, becomes more negative during 1980 to 2000. During this period, increased Asian emissions appear to have a larger impact on aerosol ERF than European and North American decreases due to their being upwind of the large, relatively pristine Pacific Ocean. There is no clear relationship between historical aerosol ERF and climate sensitivity in the CMIP5 subset of ACCMIP models. In the ACCMIP/CMIP5 models, historical aerosol ERF of about −0.8 to −1.5 W m−2 is most consistent with observed historical warming. Aerosol ERF masks a large portion of greenhouse forcing during the late 20th and early 21st century at the global scale. Regionally, aerosol ERF is so large that net forcing is negative over most industrialized and biomass burning regions through 1980, but remains strongly negative only over east and southeast Asia by 2000. Net forcing is strongly positive by 1980 over most deserts, the Arctic, Australia, and most tropical oceans. Both the magnitude of and area covered by positive forcing expand steadily thereafter.
Ozone (O3) from 17 atmospheric chemistry models taking part in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) has been used to calculate tropospheric ozone radiative ...forcings (RFs). All models applied a common set of anthropogenic emissions, which are better constrained for the present-day than the past. Future anthropogenic emissions follow the four Representative Concentration Pathway (RCP) scenarios, which define a relatively narrow range of possible air pollution emissions. We calculate a value for the pre-industrial (1750) to present-day (2010) tropospheric ozone RF of 410 mW m−2. The model range of pre-industrial to present-day changes in O3 produces a spread (±1 standard deviation) in RFs of ±17%. Three different radiation schemes were used – we find differences in RFs between schemes (for the same ozone fields) of ±10%. Applying two different tropopause definitions gives differences in RFs of ±3%. Given additional (unquantified) uncertainties associated with emissions, climate-chemistry interactions and land-use change, we estimate an overall uncertainty of ±30% for the tropospheric ozone RF. Experiments carried out by a subset of six models attribute tropospheric ozone RF to increased emissions of methane (44±12%), nitrogen oxides (31 ± 9%), carbon monoxide (15 ± 3%) and non-methane volatile organic compounds (9 ± 2%); earlier studies attributed more of the tropospheric ozone RF to methane and less to nitrogen oxides. Normalising RFs to changes in tropospheric column ozone, we find a global mean normalised RF of 42 mW m−2 DU−1, a value similar to previous work. Using normalised RFs and future tropospheric column ozone projections we calculate future tropospheric ozone RFs (mW m−2; relative to 1750) for the four future scenarios (RCP2.6, RCP4.5, RCP6.0 and RCP8.5) of 350, 420, 370 and 460 (in 2030), and 200, 300, 280 and 600 (in 2100). Models show some coherent responses of ozone to climate change: decreases in the tropical lower troposphere, associated with increases in water vapour; and increases in the sub-tropical to mid-latitude upper troposphere, associated with increases in lightning and stratosphere-to-troposphere transport. Climate change has relatively small impacts on global mean tropospheric ozone RF.
We have analysed time-slice simulations from 17 global models, participating in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP), to explore changes in present-day (2000) ...hydroxyl radical (OH) concentration and methane (CH4) lifetime relative to preindustrial times (1850) and to 1980. A comparison of modeled and observation-derived methane and methyl chloroform lifetimes suggests that the present-day global multi-model mean OH concentration is overestimated by 5 to 10% but is within the range of uncertainties. The models consistently simulate higher OH concentrations in the Northern Hemisphere (NH) compared with the Southern Hemisphere (SH) for the present-day (2000; inter-hemispheric ratios of 1.13 to 1.42), in contrast to observation-based approaches which generally indicate higher OH in the SH although uncertainties are large. Evaluation of simulated carbon monoxide (CO) concentrations, the primary sink for OH, against ground-based and satellite observations suggests low biases in the NH that may contribute to the high north–south OH asymmetry in the models. The models vary widely in their regional distribution of present-day OH concentrations (up to 34%). Despite large regional changes, the multi-model global mean (mass-weighted) OH concentration changes little over the past 150 yr, due to concurrent increases in factors that enhance OH (humidity, tropospheric ozone, nitrogen oxide (NOx) emissions, and UV radiation due to decreases in stratospheric ozone), compensated by increases in OH sinks (methane abundance, carbon monoxide and non-methane volatile organic carbon (NMVOC) emissions). The large inter-model diversity in the sign and magnitude of preindustrial to present-day OH changes (ranging from a decrease of 12.7% to an increase of 14.6%) indicate that uncertainty remains in our understanding of the long-term trends in OH and methane lifetime. We show that this diversity is largely explained by the different ratio of the change in global mean tropospheric CO and NOx burdens (Delta CO/Delta NOx, approximately represents changes in OH sinks versus changes in OH sources) in the models, pointing to a need for better constraints on natural precursor emissions and on the chemical mechanisms in the current generation of chemistry-climate models. For the 1980 to 2000 period, we find that climate warming and a slight increase in mean OH (3.5 +/- 2.2%) leads to a 4.3 +/- 1.9% decrease in the methane lifetime. Analysing sensitivity simulations performed by 10 models, we find that preindustrial to present-day climate change decreased the methane lifetime by about four months, representing a negative feedback on the climate system. Further, we analysed attribution experiments performed by a subset of models relative to 2000 conditions with only one precursor at a time set to 1860 levels. We find that global mean OH increased by 46.4 +/- 12.2% in response to preindustrial to present-day anthropogenic NOx emission increases, and decreased by 17.3 +/-2.3%, 7.6 +/- 1.5%, and 3.1 +/- 3.0% due to methane burden, and anthropogenic CO, and NMVOC emissions increases, respectively.
National and European legislation over the past 20 yr, and the modernisation or removal of industrial sources, have significantly reduced European ozone precursor emissions. This study quantifies ...observed and modelled European ozone annual and seasonal linear trends from 158 harmonised rural background monitoring stations over a constant time period of a decade (1996–2005). Mean ozone concentrations are investigated, in addition to the ozone 5th percentiles as a measure of the baseline or background conditions, and the 95th percentiles that are representative of the peak concentration levels. This study aims to characterise and quantify surface European ozone concentrations and trends and assess the impact of the changing anthropogenic emission tracers on the observed and modelled trends. Significant (p<0.1) positive annual trends in ozone mean, 5th and 95th percentiles are observed at 54 %, 52 % and 45 % of sites respectively (85 sites, 82 sites and 71 sites). Spatially, sites in central and north-western Europe tend to display positive annual ozone trends in mean, 5th and 95th percentiles. Significant negative annual trends in ozone mean 5th and 95th percentiles are observed at 11 %, 12 % and 12 % of sites respectively (18 sites, 19 sites and 19 sites) which tend to be located in the eastern and south-western extremities of Europe. European-averaged annual trends have been calculated from the 158 sites in this study. Overall there is a net positive annual trend in observed ozone mean (0.16±0.02 ppbv yr−1 (2σ error)), 5th (0.13±0.02 ppbv yr−1) and 95th (0.16±0.03 ppbv yr−1) percentiles, representative of positive trends in mean, baseline and peak ozone. Assessing the sensitivity of the derived overall trends to the constituent years shows that the European heatwave year of 2003 has significant positive influence and 1998 the converse effect; demonstrating the masking effect of inter-annual variability on decadal based ozone trends. The European scale 3-D CTM CHIMERE was used to simulate hourly O3 concentrations for the period 1996–2005. Comparisons between the 158 observed ozone trends to those equivalent sites extracted from regional simulations by CHIMERE better match the observed increasing annual ozone (predominantly in central and north-western Europe) for 5th percentiles, than for mean or 95th ozone percentiles. The European-averaged annual ozone trend in CHIMERE 5th percentiles (0.13±0.01 ppbv yr−1) matches the corresponding observed trend extremely well, but displays a negative trend for the 95th percentile (−0.03±0.02 ppbv yr−1) where a positive ozone trend is observed. Inspection of the EU-averaged monthly means of ozone shows that the CHIMERE model is overestimating the summer month O3 levels. In comparison to trends in EMEP emissions inventories, with the exception of Austria-Hungary, we do not find that anthropogenic NOx and VOC reductions have a substantial effect on observed annual mean O3 trends in the rest of Europe. On a ten year time-scale presented in this study, O3 trends related to anthropogenic NOx and VOC reductions are being masked as a result of a number of factors including meteorological variability, changes in background ozone and shifts in source patterns.
Results from simulations performed for the Atmospheric Chemistry and Climate Modeling Intercomparison Project (ACCMIP) are analysed to examine how OH and methane lifetime may change from present day ...to the future, under different climate and emissions scenarios. Present day (2000) mean tropospheric chemical lifetime derived from the ACCMIP multi-model mean is 9.8+/-1.6 yr (9.3+/-0.9 yr when only including selected models), lower than a recent observationally-based estimate, but with a similar range to previous multi-model estimates. Future model projections are based on the four Representative Concentration Pathways (RCPs), and the results also exhibit a large range. Decreases in global methane lifetime of 4.5 +/- 9.1% are simulated for the scenario with lowest radiative forcing by 2100 (RCP 2.6), while increases of 8.5+/-10.4% are simulated for the scenario with highest radiative forcing (RCP 8.5). In this scenario, the key driver of the evolution of OH and methane lifetime is methane itself, since its concentration more than doubles by 2100 and it consumes much of the OH that exists in the troposphere. Stratospheric ozone recovery, which drives tropospheric OH decreases through photolysis modifications, also plays a partial role. In the other scenarios, where methane changes are less drastic, the interplay between various competing drivers leads to smaller and more diverse OH and methane lifetime responses, which are difficult to attribute. For all scenarios, regional OH changes are even more variable, with the most robust feature being the large decreases over the remote oceans in RCP8.5. Through a regression analysis, we suggest that differences in emissions of non-methane volatile organic compounds and in the simulation of photolysis rates may be the main factors causing the differences in simulated present day OH and methane lifetime. Diversity in predicted changes between present day and future OH was found to be associated more strongly with differences in modelled temperature and stratospheric ozone changes. Finally, through perturbation experiments we calculated an OH feedback factor (F) of 1.24 from present day conditions (1.50 from 2100 RCP8.5 conditions) and a climate feedback on methane lifetime of 0.33+-0.13 yr/K, on average. Models that did not include interactive stratospheric ozone effects on photolysis showed a stronger sensitivity to climate, as they did not account for negative effects of climate-driven stratospheric ozone recovery on tropospheric OH, which would have partly offset the overall OH/methane lifetime response to climate change.
Organic compounds emitted in the atmosphere are oxidized in complex reaction sequences that produce a myriad of intermediates. Although the cumulative importance of these organic intermediates is ...widely acknowledged, there is still a critical lack of information concerning the detailed composition of the highly functionalized secondary organics in the gas and condensed phases. The evaluation of their impacts on pollution episodes, climate, and the tropospheric oxidizing capacity requires modelling tools that track the identity and reactivity of organic carbon in the various phases down to the ultimate oxidation products, CO and CO2. However, a fully detailed representation of the atmospheric transformations of organic compounds involves a very large number of intermediate species, far in excess of the number that can be reasonably written manually. This paper describes (1) the development of a data processing tool to generate the explicit gas-phase oxidation schemes of acyclic hydrocarbons and their oxidation products under tropospheric conditions and (2) the protocol used to select the reaction products and the rate constants. Results are presented using the fully explicit oxidation schemes generated for two test species: n-heptane and isoprene. Comparisons with well-established mechanisms were performed to evaluate these generated schemes. Some preliminary results describing the gradual change of organic carbon during the oxidation of a given parent compound are presented.
We use 23 atmospheric chemistry transport models to calculate current and future (2030) deposition of reactive nitrogen (NOy, NHx) and sulfate (SOx) to land and ocean surfaces. The models are driven ...by three emission scenarios: (1) current air quality legislation (CLE); (2) an optimistic case of the maximum emissions reductions currently technologically feasible (MFR); and (3) the contrasting pessimistic IPCC SRES A2 scenario. An extensive evaluation of the present‐day deposition using nearly all information on wet deposition available worldwide shows a good agreement with observations in Europe and North America, where 60–70% of the model‐calculated wet deposition rates agree to within ±50% with quality‐controlled measurements. Models systematically overestimate NHx deposition in South Asia, and underestimate NOy deposition in East Asia. We show that there are substantial differences among models for the removal mechanisms of NOy, NHx, and SOx, leading to ±1 σ variance in total deposition fluxes of about 30% in the anthropogenic emissions regions, and up to a factor of 2 outside. In all cases the mean model constructed from the ensemble calculations is among the best when comparing to measurements. Currently, 36–51% of all NOy, NHx, and SOx is deposited over the ocean, and 50–80% of the fraction of deposition on land falls on natural (nonagricultural) vegetation. Currently, 11% of the world's natural vegetation receives nitrogen deposition in excess of the “critical load” threshold of 1000 mg(N) m−2 yr−1. The regions most affected are the United States (20% of vegetation), western Europe (30%), eastern Europe (80%), South Asia (60%), East Asia (40%), southeast Asia (30%), and Japan (50%). Future deposition fluxes are mainly driven by changes in emissions, and less importantly by changes in atmospheric chemistry and climate. The global fraction of vegetation exposed to nitrogen loads in excess of 1000 mg(N) m−2 yr−1 increases globally to 17% for CLE and 25% for A2. In MFR, the reductions in NOy are offset by further increases for NHx deposition. The regions most affected by exceedingly high nitrogen loads for CLE and A2 are Europe and Asia, but also parts of Africa.
The recent increase of atmospheric methane is investigated by using two atmospheric inversions to quantify the distribution of sources and sinks for the 2006-2008 period, and a process-based model of ...methane emissions by natural wetland ecosystems. Methane emissions derived from the two inversions are consistent at a global scale: emissions are decreased in 2006 (-7 Tg) and increased in 2007 (+21 Tg) and 2008 (+18 Tg), as compared to the 1999-2006 period. The agreement on the latitudinal partition of the flux anomalies for the two inversions is fair in 2006, good in 2007, and not good in 2008. In 2007, a positive anomaly of tropical emissions is found to be the main contributor to the global emission anomalies (~60-80%) for both inversions, with a dominant share attributed to natural wetlands (~2/3), and a significant contribution from high latitudes (~25%). The wetland ecosystem model produces smaller and more balanced positive emission anomalies between the tropics and the high latitudes for 2006, 2007 and 2008, mainly due to precipitation changes during these years. At a global scale, the agreement between the ecosystem model and the inversions is good in 2008 but not satisfying in 2006 and 2007. Tropical South America and Boreal Eurasia appear to be major contributors to variations in methane emissions consistently in the inversions and the ecosystem model. Finally, changes in OH radicals during 2006-2008 are found to be less than 1% in inversions, with only a small impact on the inferred methane emissions.
Understanding the surface O3 response over a “receptor” region to emission changes over a foreign “source” region is key to evaluating the potential gains from an international approach to abate ...ozone (O3) pollution. We apply an ensemble of 21 global and hemispheric chemical transport models to estimate the spatial average surface O3 response over east Asia (EA), Europe (EU), North America (NA), and south Asia (SA) to 20% decreases in anthropogenic emissions of the O3 precursors, NOx, NMVOC, and CO (individually and combined), from each of these regions. We find that the ensemble mean surface O3 concentrations in the base case (year 2001) simulation matches available observations throughout the year over EU but overestimates them by >10 ppb during summer and early fall over the eastern United States and Japan. The sum of the O3 responses to NOx, CO, and NMVOC decreases separately is approximately equal to that from a simultaneous reduction of all precursors. We define a continental‐scale “import sensitivity” as the ratio of the O3 response to the 20% reductions in foreign versus “domestic” (i.e., over the source region itself) emissions. For example, the combined reduction of emissions from the three foreign regions produces an ensemble spatial mean decrease of 0.6 ppb over EU (0.4 ppb from NA), less than the 0.8 ppb from the reduction of EU emissions, leading to an import sensitivity ratio of 0.7. The ensemble mean surface O3 response to foreign emissions is largest in spring and late fall (0.7–0.9 ppb decrease in all regions from the combined precursor reductions in the three foreign regions), with import sensitivities ranging from 0.5 to 1.1 (responses to domestic emission reductions are 0.8–1.6 ppb). High O3 values are much more sensitive to domestic emissions than to foreign emissions, as indicated by lower import sensitivities of 0.2 to 0.3 during July in EA, EU, and NA when O3 levels are typically highest and by the weaker relative response of annual incidences of daily maximum 8‐h average O3 above 60 ppb to emission reductions in a foreign region (<10–20% of that to domestic) as compared to the annual mean response (up to 50% of that to domestic). Applying the ensemble annual mean results to changes in anthropogenic emissions from 1996 to 2002, we estimate a Northern Hemispheric increase in background surface O3 of about 0.1 ppb a−1, at the low end of the 0.1–0.5 ppb a−1 derived from observations. From an additional simulation in which global atmospheric methane was reduced, we infer that 20% reductions in anthropogenic methane emissions from a foreign source region would yield an O3 response in a receptor region that roughly equals that produced by combined 20% reductions of anthropogenic NOx, NMVOC, and CO emissions from the foreign source region.
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