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Although quantitative isotope data from speleothems has been used to evaluate isotope-enabled model simulations, currently no consensus exists regarding the most appropriate methodology through which to achieve this. A number of modelling groups will be running isotope-enabled palaeoclimate simulations in the framework of the Coupled Model Intercomparison Project Phase 6, so it is timely to evaluate different approaches to using the speleothem data for data-model comparisons. Here, we illustrate this using 456 globally distributed speleothem delta O-18 records from an updated version of the Speleothem Isotopes Synthesis and Analysis (SISAL) database and palaeoclimate simulations generated using the ECHAM5-wiso isotope-enabled atmospheric circulation model. We show that the SISAL records reproduce the first-order spatial patterns of isotopic variability in the modern day, strongly supporting the application of this dataset for evaluating model-derived isotope variability into the past. However, the discontinuous nature of many speleothem records complicates the process of procuring large numbers of records if data-model comparisons are made using the traditional approach of comparing anomalies between a control period and a given palaeoclimate experiment. To circumvent this issue, we illustrate techniques through which the absolute isotope values during any time period could be used for model evaluation. Specifically, we show that speleothem isotope records allow an assessment of a model's ability to simulate spatial isotopic trends. Our analyses provide a protocol for using speleothem isotope data for model evaluation, including screening the observations to take into account the impact of speleothem mineralogy on delta O-18 values, the optimum period for the modern observational baseline and the selection of an appropriate time window for creating means of the isotope data for palaeo-time-slices. European Geosciences Union - W2017/413; Irish Centre for Research in Applied Geosciences (iCRAG); European Association of Geochemistry (Early Career Ambassadors program 2017); Quaternary Research Association UK; Navarino Environmental Observatory, Stockholm University; University College Dublin, Savillex (UK) - SF1428; Ibn Zohr University, Morocco; University of Reading; European Research Council - 694481; Natural Environment Research Council (JPI-Belmont project "PAleao-Constraints on Monsoon Evolution and Dynamics (PACMEDY)"); Geological Survey Ireland - 2017-SC-056; Royal Irish Academy; Deutsche Forschungsgemeinschaft - RE3994/2-1; Past Global Changes (PAGES) programme; info:eu-repo/semantics/publishedVersion

International audience; This study presents the version of the LMDZ global atmospheric model used as the atmospheric component of the Institut Pierre Simon Laplace coupled model (IPSL-CM6A-LR) to contribute to the 6th phase of the international Coupled Model Intercomparison Project (CMIP6). This LMDZ6A version includes original convective parameterizations that define the LMDZ "New Physics": a mass flux parameterization of the organized structures of the convective boundary layer, the "thermal plume model," and a parameterization of the cold pools created by reevaporation of convective rainfall. The vertical velocity associated with thermal plumes and gust fronts of cold pools are used to control the triggering and intensity of deep convection. Because of several shortcomings, the early version 5B of this New Physics was worse than the previous "Standard Physics" version 5A regarding several classical climate metrics. To overcome these deficiencies, version 6A includes new developments: a stochastic triggering of deep convection, a modification of the thermal plume model that allows the representation of stratocumulus and cumulus clouds in a unified framework, an improved parameterization of very stable boundary layers, and the modification of the gravity waves scheme targeting the quasi-biennal oscillation in the stratosphere. These improvements to the physical content and a more well-defined tuning strategy led to major improvements in the LMDZ6A version model climatology. Beyond the presentation of this particular model version and documentation of its climatology, the present paper underlines possible methodological pathways toward model improvement that can be shared across modeling groups. Plain Language Summary The improvement of global numerical models is essential for the anticipation of future climate changes. We present significant advances in the physical content of a particular atmospheric model which contributes to the simulations of the Coupled Model Intercomparison project CMIP that feed reports from the IPCC. We document in particular the improvements of the representation through "parameterizations" of convective and cloudy processes. The article emphasizes the importance of strengthening the formalization of the methodology of development and tuning of models, so that new physical ideas can be translated into effective improvement of the climate representation.

We present WASP-43b climate simulations with deep wind jets (down to 700 bar) that are linked to retrograde (westward) flow at the equatorial day side for p < 0.1 bar. Retrograde flow inhibits efficient eastward heat transport and naturally explains the small hotspot shift and large day-night-side gradient of WASP-43b (Porb = Prot = 0.8135 d) observed with Spitzer. We find that deep wind jets are mainly associated with very fast rotations (Prot = Porb ≤ 1.5 d) which correspond to the Rhines length smaller than 2 planetary radii. We also diagnose wave activity that likely gives rise to deviations from superrotation. Further, we show that we can achieve full steady state in our climate simulations by imposing a deep forcing regime for p > 10 bar: convergence time-scale τconv = 106–108 s to a common adiabat, as well as linear drag at depth (p ≥ 200 bar), which mimics to first-order magnetic drag. Lower boundary stability and the deep forcing assumptions were also tested with climate simulations for HD 209458b (Porb = Prot = 3.5 d). HD 209458b simulations always show shallow wind jets (never deeper than 100 bar) and unperturbed superrotation. If we impose a fast rotation (Porb = Prot = 0.8135 d), also the HD 209458b-like simulation shows equatorial retrograde flow at the day side. We conclude that the placement of the lower boundary at p = 200 bar is justified for slow rotators like HD 209458b, but we suggest that it has to be placed deeper for fast-rotating, dense hot Jupiters (Porb ≤ 1.5 d) like WASP-43b. Our study highlights that the deep atmosphere may have a strong influence on the observable atmospheric flow in some hot Jupiters.

Polychlorinated biphenyls (PCBs) can be used as chemical sentinels for the assessment of anthropogenic influences on Arctic environmental change. We present an overview of studies on PCBs in the Arctic and combine these with the findings from ArcRisk—a major European Union-funded project aimed at examining the effects of climate change on the transport of contaminants to and their behaviour of in the Arctic—to provide a case study on the behaviour and impact of PCBs over time in the Arctic. PCBs in the Arctic have shown declining trends in the environment over the last few decades. Atmospheric long-range transport from secondary and primary sources is the major input of PCBs to the Arctic region. Modelling of the atmospheric PCB composition and behaviour showed some increases in environmental concentrations in a warmer Arctic, but the general decline in PCB levels is still the most prominent feature. ‘Within-Arctic’ processing of PCBs will be affected by climate change-related processes such as changing wet deposition. These in turn will influence biological exposure and uptake of PCBs. The pan-Arctic rivers draining large Arctic/sub-Arctic catchments provide a significant source of PCBs to the Arctic Ocean, although changes in hydrology/sediment transport combined with a changing marine environment remain areas of uncertainty with regard to PCB fate. Indirect effects of climate change on human exposure, such as a changing diet will influence and possibly reduce PCB exposure for indigenous peoples. Body burdens of PCBs have declined since the 1980s and are predicted to decline further., Environmental Science and Pollution Research, ISSN:0944-1344, ISSN:1614-7499

The Coupled Model Intercomparison Project (CMIP) is now moving into its sixth phase and aims at a more routine evaluation of the models as soon as the model output is published to the Earth System Grid Federation (ESGF). To meet this goal the Earth System Model Evaluation Tool (ESMValTool), a community diagnostics and performance metrics tool for the systematic evaluation of Earth system models (ESMs) in CMIP, has been developed and a first version (1.0) released as open source software in 2015. Here, an enhanced version of the ESMValTool is presented that exploits a subset of Essential Climate Variables (ECVs) from the European Space Agency's Climate Change Initiative (ESA CCI) Phase 2 and this version is used to demonstrate the value of the data for model evaluation. This subset includes consistent, long-term time series of ECVs obtained from harmonized, reprocessed products from different satellite instruments for sea surface temperature, sea ice, cloud, soil moisture, land cover, aerosol, ozone, and greenhouse gases. The ESA CCI data allow 'extending the calculation of performance metrics as summary statistics for some variables and add an important alternative data set in other cases where observations are already available. The provision of uncertainty estimates on a per grid basis for the ESA CCI data sets is used in a new extended version of the Taylor diagram and provides important additional information for a more objective evaluation of the models. In our analysis we place a specific focus on the comparability of model and satellite data both in time and space. The ESA CCI data are well suited for an evaluation of results from global climate models across ESM compartments as well as an analysis of long-term trends, variability and change in the context of a changing climate. The enhanced version of the ESMValTool is released as open source software and ready to support routine model evaluation in CMIP6 and at individual modeling centers. (C) 2017 Elsevier Inc. All rights reserved.

Aerosol effects on low warm clouds over the Yangtze River Delta (YRD, eastern China) are examined using co-located MODIS, CALIOP and CloudSat observations. By taking the vertical locations of aerosol and cloud layers into account, we use simultaneously observed aerosol and cloud data to investigate relationships between cloud properties and the amount of aerosol particles (using aerosol optical depth, AOD, as a proxy). Also, we investigate the impact of aerosol types on the variation of cloud properties with AOD. Finally, we explore how meteorological conditions affect these relationships using ERA-Interim reanalysis data. This study shows that the relation between cloud properties and AOD depends on the aerosol abundance, with a different behaviour for low and high AOD (i.e. AOD 0.35). This applies to cloud droplet effective radius (CDR) and cloud fraction (CF), but not to cloud optical thickness (COT) and cloud top pressure (CTP). COT is found to decrease when AOD increases, which may be due to radiative effects and retrieval artefacts caused by absorbing aerosol. Conversely, CTP tends to increase with elevated AOD, indicating that the aerosol is not always prone to expand the vertical extension. It also shows that the COT–CDR and CWP (cloud liquid water path)–CDR relationships are not unique, but affected by atmospheric aerosol loading. Furthermore, separation of cases with either polluted dust or smoke aerosol shows that aerosol–cloud interaction (ACI) is stronger for clouds mixed with smoke aerosol than for clouds mixed with dust, which is ascribed to the higher absorption efficiency of smoke than dust. The variation of cloud properties with AOD is analysed for various relative humidity and boundary layer thermodynamic and dynamic conditions, showing that high relative humidity favours larger cloud droplet particles and increases cloud formation, irrespective of vertical or horizontal level. Stable atmospheric conditions enhance cloud cover horizontally. However, unstable atmospheric conditions favour thicker and higher clouds. Dynamically, upward motion of air parcels can also facilitate the formation of thicker and higher clouds. Overall, the present study provides an understanding of the impact of aerosols on cloud properties over the YRD. In addition to the amount of aerosol particles (or AOD), evidence is provided that aerosol types and ambient environmental conditions need to be considered to understand the observed relationships between cloud properties and AOD.

This paper presents a comprehensive description and benchmark evaluation of the tropospheric gas-phase chemistry component of the Multiscale Online Nonhydrostatic AtmospheRe CHemistry model (NMMB-MONARCH), formerly known as NMMB/BSC-CTM, that can be run on both regional and global domains. Here, we provide an extensive evaluation of a global annual cycle simulation using a variety of background surface stations (EMEP, WDCGG and CASTNET), ozonesondes (WOUDC, CMD and SHADOZ), aircraft data (MOZAIC and several campaigns), and satellite observations (SCIAMACHY and MOPITT). We also include an extensive discussion of our results in comparison to other state-of-the-art models. We note that in this study, we omitted aerosol processes and some natural emissions (lightning and volcano emissions). The model shows a realistic oxidative capacity across the globe. The seasonal cycle for CO is fairly well represented at different locations (correlations around 0.3–0.7 in surface concentrations), although concentrations are underestimated in spring and winter in the Northern Hemisphere, and are overestimated throughout the year at 800 and 500 hPa in the Southern Hemisphere. Nitrogen species are well represented in almost all locations, particularly NO2 in Europe (root mean square error – RMSE – below 5 ppb). The modeled vertical distributions of NOx and HNO3 are in excellent agreement with the observed values and the spatial and seasonal trends of tropospheric NO2 columns correspond well to observations from SCIAMACHY, capturing the highly polluted areas and the biomass burning cycle throughout the year. Over Asia, the model underestimates NOx from March to August, probably due to an underestimation of NOx emissions in the region. Overall, the comparison of the modeled CO and NO2 with MOPITT and SCIAMACHY observations emphasizes the need for more accurate emission rates from anthropogenic and biomass burning sources (i.e., specification of temporal variability). The resulting ozone (O3) burden (348 Tg) lies within the range of other state-of-the-art global atmospheric chemistry models. The model generally captures the spatial and seasonal trends of background surface O3 and its vertical distribution. However, the model tends to overestimate O3 throughout the troposphere in several stations. This may be attributed to an overestimation of CO concentration over the Southern Hemisphere leading to an excessive production of O3 or to the lack of specific chemistry (e.g., halogen chemistry, aerosol chemistry). Overall, O3 correlations range between 0.6 and 0.8 for daily mean values. The overall performance of the NMMB-MONARCH is comparable to that of other state-of-the-art global chemistry models. The authors wish to thank WOUDC, GAW, EMEP, WDCGG, CASTNET-EPA, NADP and EANET for the provision of measurement stations. The authors acknowledge for the strong support of the European Commission, Airbus, and the Airlines (Lufthansa, Austrian, Air France) who carry free of charge the MOZAIC equipment and perform the maintenance since 1994. MOZAIC is presently funded by INSU-CNRS (France), Meteo-France, and Forschungszentrum (FZJ, Julich, Germany). The MOZAIC database is supported by ETHER (CNES and INSU-CNRS). Also, thanks go to the free use of the MOPITTCO data obtained from the NASA Langley Research Center Atmospheric Science Data Center. SCIAMACHY radiances have been provided by ESA. We also thank Beatriz Monge-Sanz for providing the COPCAT coefficients. This work is funded by grants CGL2013-46736-R, Supercomputación and e-ciencia Project (CSD2007-0050) from the Consolider-Ingenio 2010 program of the Spanish Ministry of Economy and Competitiveness. Further support was provided by the SEV-2011-00067 grant of the Severo Ochoa Program, awarded by the Spanish Government. Andreas Hilboll received funding from the Earth System Science Research School (ESSReS), an initiative of the Helmholtz Association of German research centres (HGF) at the Alfred Wegener Institute for Polar and Marine Research. Carlos Pérez García-Pando acknowledges long-term support from the AXA Research Fund. The authors thankfully acknowledge the computer resources at MareNostrum and the technical support provided by Barcelona Supercomputing Center (RES-AECT-2015-1-0007). Comments from two anonymous reviewers are gratefully acknowledge.

A multi-layer ozone (O3) dry deposition model has been implemented into SOSAA (a model to Simulate the concentrations of Organic vapours, Sulphuric Acid and Aerosols) to improve the representation of O3 within and above the forest canopy in the planetary boundary layer where O3 is a key oxidant agent of biogenic volatile organic compounds (BVOCs) and thus affecting organic aerosol processes. We aim to predict the O3 uptake by a boreal forest canopy under varying environmental conditions and analyse the influence of different factors on total O3 uptake by the canopy as well as the vertical distribution of deposition sinks inside the canopy. We evaluated the newly implemented canopy deposition model by an extensive comparison of simulated and observed O3 fluxes and concentration profiles within and above the boreal forest canopy at SMEAR II (the Station to Measure Ecosystem-Atmosphere Relation II) in Hyytiälä, Finland, in August, 2010. The first half of August showed extremely warm and dry conditions which were probably representative for summer conditions prevailing at this site in future. The simulated O3 turbulent fluxes at the canopy top and the O3 concentration profiles inside the canopy agreed well with the measurement, which indicated that the turbulent transport and the O3 dry deposition onto the canopy and soil surface appeared to be properly represented in the model. In this model, the fraction of wet surface on vegetation leaves was parameterised according to the ambient relative humidity (RH). Model results showed that when RH was larger than 70 % the O3 uptake onto wet skin contributed 48.6 % to the total deposition during nighttime and 22.0 % during daytime. In addition, most of the O3 deposition occurred below 0.8 hc (canopy height) at this site. The contribution of sub-canopy deposition below 4.2 m was modelled to be about 40 % of the total O3 deposition during daytime which was similar to previous studies. Whereas for nighttime, the simulated sub-canopy deposition contributed 40–65 % to the total O3 deposition which was about two times as that in previous studies (25–30 %). The overall contribution of soil uptake was estimated as 36.5 %. These results indicated the importance of non-stomatal O3 uptake processes, especially the uptake on wet skin and soil surface. Furthermore, a qualitative evaluation of the chemical removal time scales indicated that the chemical removal rate within canopy was about 5 % of the total deposition flux at daytime and 16 % at nighttime under current knowledge of air chemistry. The evaluation of the O3 deposition processes provides improved understanding about the mechanisms involved in the removal of O3 for this boreal forest site which are also relevant to the removal of other reactive compounds such as the BVOCs and their oxidation products, which will be focus of a follow-up study.

Aerosol-cloud interactions are the largest source of uncertainty in the radiative forcing of the global climate. A phenomenon not included in the estimates of the total net forcing is the potential increase in upper tropospheric humidity (UTH) by anthropogenic aerosols via changes in the microphysics of deep convection. Using remote sensing data over the ocean east of China in summer, we show that increased aerosol loads are associated with an UTH increase of 2.2 ± 1.5 in units of relative humidity. We show that humidification of aerosols or other meteorological covariation is very unlikely to be the cause for this result indicating relevance for the global climate. In tropical moist air such an UTH increase leads to a regional radiative effect of 0.5 ± 0.4 W m−2. We conclude that the effect of aerosols on UTH should be included in future studies of anthropogenic climate change and climate sensitivity.

Two hundred fifty-two transient drops in atmospheric pressure, likely caused by passing convective vortices, were detected by the Rover Environmental Monitoring Station instrument during the first Martian year of the Mars Science Laboratory (MSL) landed mission. These events resembled the vortex signatures detected by the previous Mars landers Pathfinder and Phoenix; however, the MSL observations contained fewer pressure drops greater than 1.5 Pa and none greater than 3.0 Pa. Apparently, these vortices were generally not lifting dust as only one probable dust devil has been observed visually by MSL. The obvious explanation for this is the smaller number of strong vortices with large central pressure drops since according to Arvidson et al. [2014] ample dust seems to be present on the surface. The annual variation in the number of detected convective vortices followed approximately the variation in Dust Devil Activity (DDA) predicted by the MarsWRF numerical climate model. This result does not prove, however, that the amount of dust lifted by dust devils would depend linearly on DDA, as is assumed in several numerical models of the Martian atmosphere, since dust devils are only the most intense fraction of all convective vortices on Mars, and the amount of dust that can be lifted by a dust devil depends on its central pressure drop. Sol-to-sol variations in the number of vortices were usually small. However, on 1 Martian solar day a sudden increase in vortex activity, related to a dust storm front, was detected.

The aim of this paper is to assess the impacts of projected climate change on a Mediterranean catchment, and to analyze the effects of a suite of representative land use practices as an adaptation tool to reduce climate change-driven erosion and hydrologic extremes. Relevant climatic variables from the ERA-Interim global atmospheric reanalysis of the European Centre for Medium-Range Weather Forecasts (ECMWF) were downscaled for the study area, and perturbed with the anomalies of 23 global circulation models for three emission scenarios (B1, A1B and A2). Both a projected daily rainfall time series for the period 2010-2100, and a single precipitation event with a one-hundred year return period were used to assess the impact of climate change. The downscaled data were fed into a distributed hydro-sedimentary model (TETIS) with five land use configurations representative of future demographic tendencies, geographical characteristics and land management policies (e.g. European Union CAP). The projected changes showed a general decrease in runoff and sediment production by the end of the century regardless of land use configuration. Sediment production showed a positive relationship with an increase in agricultural land and a decrease in natural land under present day agricultural management. According to our simulations, some conservation practices in agriculture can effectively reduce net erosion while maintaining agricultural production. As such, they can play a critical role as an adaptation tool to reduce climate change impacts in the 21st century., This study was funded by the Spanish Ministry of Economy and Competitiveness through the research projects CLARIES (ref. CGL2011-29176) and PALEOMED (CGL2014-58127-C3-1-R).

The ALADIN System is a numerical weather prediction system (NWP) developed by the international ALADIN consortium for operational weather forecasting and research purposes. It is based on a code that is shared with the global model IFS of the ECMWF and the ARPEGE model of Météo-France. Today, this system can be used to provide a multitude of high-resolution limited-area model (LAM) configurations. A few configurations are thoroughly validated and prepared to be used for the operational weather forecasting in the 16 Partner Institutes of this consortium. These configurations are called the ALADIN Canonical Model Configurations (CMCs). There are currently three CMCs: the ALADIN baseline-CMC, the AROME CMC and the ALARO CMC. Other configurations are possible for research, such as process studies and climate simulations. The purpose of this paper is (i) to define the ALADIN System in relation to the global counterparts IFS and ARPEGE, (ii) to explain the notion of the CMCs and to document their most recent versions, and (iii) to illustrate the process of the validation and the porting of these configurations to the operational forecast suites of the Partner Institutes of the ALADIN consortium. This paper is restricted to the forecast model only; data assimilation techniques and postprocessing techniques are part of the ALADIN System but they are not discussed here.

The impacts of representing cloud microphysical processes in a stochastic subcolumn framework are investigated, with emphasis on estimating the aerosol indirect effect. It is shown that subgrid treatment of cloud activation and autoconversion of cloud water to rain reduce the impact of anthropogenic aerosols on cloud properties and thus reduce the global mean aerosol indirect effect by 19%, from −1.59 to −1.28 W m−2. This difference is partly related to differences in the model basic state; in particular, the liquid water path (LWP) is smaller and the shortwave cloud radiative forcing weaker when autoconversion is computed separately for each subcolumn. However, when the model is retuned so that the differences in the basic state LWP and radiation balance are largely eliminated, the global-mean aerosol indirect effect is still 14% smaller (i.e. −1.37 W m−2) than for the model version without subgrid treatment of cloud activation and autoconversion. The results show the importance of considering subgrid variability in the treatment of autoconversion. Representation of several processes in a self-consistent subgrid framework is emphasized. This paper provides evidence that omitting subgrid variability in cloud microphysics contributes to the apparently chronic overestimation of the aerosol indirect effect by climate models, as compared to satellite-based estimates.

Much of the uncertainty in estimates of the anthropogenic forcing of climate change comes from uncertainties in the instantaneous effect of aerosols on cloud albedo, known as the Twomey effect or the radiative forcing from aerosol–cloud interactions (RFaci), a component of the total or effective radiative forcing. Because aerosols serving as cloud condensation nuclei can have a strong influence on the cloud droplet number concentration (Nd), previous studies have used the sensitivity of the Nd to aerosol properties as a constraint on the strength of the RFaci. However, recent studies have suggested that relationships between aerosol and cloud properties in the present-day climate may not be suitable for determining the sensitivity of the Nd to anthropogenic aerosol perturbations. Using an ensemble of global aerosol–climate models, this study demonstrates how joint histograms between Nd and aerosol properties can account for many of the issues raised by previous studies. It shows that if the anthropogenic contribution to the aerosol is known, the RFaci can be diagnosed to within 20% of its actual value. The accuracy of different aerosol proxies for diagnosing the RFaci is investigated, confirming that using the aerosol optical depth significantly underestimates the strength of the aerosol–cloud interactions in satellite data.

A multilayer gas dry deposition model has been developed and implemented into a one-dimensional chemical transport model SOSAA (model to Simulate the concentrations of Organic vapours, Sulphuric Acid and Aerosols) to calculate the dry deposition velocities for all the gas species included in the chemistry scheme. The new model was used to analyse in-canopy sources and sinks, including gas emissions, chemical production and loss, dry deposition, and turbulent transport of 12 featured biogenic volatile organic compounds (BVOCs) or groups of BVOCs (e.g. monoterpenes, isoprene+2-methyl-3-buten-2-ol (MBO), sesquiterpenes, and oxidation products of mono- and sesquiterpenes) in July 2010 at the boreal forest site SMEAR II (Station for Measuring Ecosystem–Atmosphere Relations). According to the significance of modelled monthly-averaged individual source and sink terms inside the canopy, the selected BVOCs were classified into five categories: 1. Most of emitted gases are transported out of the canopy (monoterpenes, isoprene + MBO). 2. Chemical reactions remove a significant portion of emitted gases (sesquiterpenes). 3. Bidirectional fluxes occur since both emission and dry deposition are crucial for the in-canopy concentration tendency (acetaldehyde, methanol, acetone, formaldehyde). 4. Gases removed by deposition inside the canopy are compensated for by the gases transported from above the canopy (acetol, pinic acid, β-caryophyllene's oxidation product BCSOZOH). 5. The chemical production is comparable to the sink by deposition (isoprene's oxidation products ISOP34OOH and ISOP34NO3). Most of the simulated sources and sinks were located above about 0.2 hc (canopy height) for oxidation products and above about 0.4 hc for emitted species except formaldehyde. In addition, soil deposition (including deposition onto understorey vegetation) contributed 11–61 % to the overall in-canopy deposition. The emission sources peaked at about 0.8–0.9 hc, which was higher than 0.6 hc where the maximum of dry deposition onto overstorey vegetation was located. This study provided a method to enable the quantification of the exchange between atmosphere and biosphere for numerous BVOCs, which could be applied in large-scale models in future. With this more explicit canopy exchange modelling system, this study analysed both the temporal and spatial variations in individual in-canopy sources and sinks, as well as their combined effects on driving BVOC exchange. In this study 12 featured BVOCs or BVOC groups were analysed. Other compounds could also be investigated similarly by being classified into these five categories.

To quantify changes in air pollution over Europe at the 2050 horizon, we designed a comprehensive modelling system that captures the external factors considered to be most relevant, and that relies on up-to-date and consistent sets of air pollution and climate policy scenarios. Global and regional climate as well as global chemistry simulations are based on the recent representative concentration pathways (RCP) produced for the Fifth Assessment Report (AR5) of the IPCC (Intergovernmental Panel on Climate Change) whereas regional air quality modelling is based on the updated emissions scenarios produced in the framework of the Global Energy Assessment. We explored two diverse scenarios: a reference scenario where climate policies are absent and a mitigation scenario which limits global temperature rise to within 2 °C by the end of this century. This first assessment of projected air quality and climate at the regional scale based on CMIP5 (5th Coupled Model Intercomparison Project) climate simulations is in line with the existing literature using CMIP3. The discrepancy between air quality simulations obtained with a climate model or with meteorological reanalyses is pointed out. Sensitivity simulations show that the main factor driving future air quality projections is air pollutant emissions, rather than climate change or intercontinental transport of pollution. Whereas the well documented "climate penalty" that weights upon ozone (increase of ozone pollution with global warming) over Europe is confirmed, other features appear less robust compared to the literature, such as the impact of climate on PM2.5. The quantitative disentangling of external factors shows that, while several published studies focused on the climate penalty bearing upon ozone, the contribution of the global ozone burden is somewhat overlooked in the literature.

The shallow overturning circulation of the oceans transports heat from the tropics to the mid-latitudes. This overturning also influences the uptake and storage of anthropogenic carbon (Cant). We demonstrate this by quantifying the relative importance of ocean thermodynamics, circulation and biogeochemistry in a global biochemistry and circulation model. Almost 2/3 of the Cant ocean uptake enters via gas exchange in waters that are lighter than the base of the ventilated thermocline. However, almost 2/3 of the excess Cant is stored below the thermocline. Our analysis shows that subtropical waters are a dominant component in the formation of subpolar waters and that these water masses essentially form a common Cant reservoir. This new method developed and presented here is intrinsically Lagrangian, as it by construction only considers the velocity or transport of waters across isopycnals. More generally, our approach provides an integral framework for linking ocean thermodynamics with biogeochemistry.

International audience; The isotopic compositions of oxygen and hydrogen in ice cores are invaluable tools for the reconstruction of past climate variations. Used alone, they give insights into the variations of the local temperature, whereas taken together they can provide information on the climatic conditions at the point of origin of the moisture. However, recent analyses of snow from shallow pits indicate that the climatic signal can become erased in very low accumulation regions, due to local processes of snow reworking. The signal-to-noise ratio decreases and the climatic signal can then only be retrieved using stacks of several snow pits. Obviously, the signal is not completely lost at this stage, otherwise it would be impossible to extract valuable climate information from ice cores as has been done, for instance, for the last glaciation. To better understand how the climatic signal is passed from the precipitation to the snow, we present here results from varied snow samples from East Antarctica. First, we look at the relationship between isotopes and temperature from a geographical point of view, using results from three traverses across Antarctica, to see how the relationship is built up through the distillation process. We also take advantage of these measures to see how second-order parameters (d-excess and 17 O-excess) are related to δ 18 O and how they are controlled. d-excess increases in the interior of the continent (i.e., when δ 18 O decreases), due to the distillation process, whereas 17 O-excess decreases in remote areas, due to kinetic fractionation at low temperature. In both cases, these changes are associated with the loss of original information regarding the source. Then, we look at the same relationships in precipitation samples collected over 1 year at Dome C and Vos-tok, as well as in surface snow at Dome C. We note that the slope of the δ 18 O vs. temperature (T) relationship decreases in these samples compared to those from the traverses, and thus caution is advocated when using spatial slopes for past Published by Copernicus Publications on behalf of the European Geosciences Union. 838 A. Touzeau et al.: Acquisition of isotopic composition for surface snow in East Antarctica climate reconstruction. The second-order parameters behave in the same way in the precipitation as in the surface snow from traverses, indicating that similar processes are active and that their interpretation in terms of source climatic parameters is strongly complicated by local temperature effects in East Antarctica. Finally we check if the same relationships between δ 18 O and second-order parameters are also found in the snow from four snow pits. While the d-excess remains opposed to δ 18 O in most snow pits, the 17 O-excess is no longer positively correlated to δ 18 O and even shows anti-correlation to δ 18 O at Vostok. This may be due to a strato-spheric influence at this site and/or to post-deposition processes .

Desert dust plays an important role in the climate system through its impact on Earth¿s radiative budget and its role in the biogeochemical cycle as a source of iron in highnutrient- low-chlorophyll regions. A large degree of diversity exists between the many global models that simulate the dust cycle to estimate its impact on climate. We present the results of a broad intercomparison of a total of 15 global aerosol models within the AeroCom project. Each model is compared to observations focusing on variables responsible for the uncertainties in estimating the direct radiative effect and the dust impact on the biogeochemical cycle, i.e., aerosol optical depth (AOD) and dust deposi10 tion. Additional comparisons to Angstro¨m Exponent (AE), coarse mode AOD and dust surface concentration are included to extend the assessment of model performance. These datasets form a benchmark data set which is proposed for model inspection and future dust model developments. In general, models perform better in simulating climatology of vertically averaged integrated parameters (AOD and AE) in dusty sites 15 than they do with total deposition and surface concentration. Almost all models overestimate deposition fluxes over Europe, the Indian Ocean, the Atlantic Ocean and ice core data. Differences among the models arise when simulating deposition at remote sites with low fluxes over the Pacific and the Southern Atlantic Ocean. This study also highlights important differences in models ability to reproduce the deposition flux over Antarctica. The cause of this discrepancy could not be identified but different dust regimes at each site and issues with data quality should be considered. Models generally simulate better surface concentration at stations downwind of the main sources than at remote ones. Likewise, they simulate better surface concentration at stations affected by Saharan dust than at stations affected by Asian dust. Most models simulate the gradient in AOD and AE between the different dusty regions, however the seasonality and magnitude of both variables is better simulated at African stations than Middle East ones. The models also reproduce the dust transport across the Atlantic in terms of both AOD and AE; they simulate the offshore transport of West Africa throughout the year and limit the transport across the Atlantic to the summer months, yet overestimating the AOD and transporting too fine particles. However, most of the models do not reproduce the southward displacement of the dust cloud during the winter responsible of the transport of dust into South America. Based on the dependency of AOD on aerosol 5 burden and size distribution we use model data bias with respect to AOD and AE and infer on the over/under estimation of the dust emissions. According to this we suggest the emissions in the Sahara be between 792 and 2271 Tg/yr and the one in the Middle East between 376 and 526 Tg/yr., JRC.DDG.H.2-Climate change and air quality

Simulations of a regional (approx. 50 km resolution) circulation model REMOiso with embedded stable water isotope module covering the period 1958-2001 are compared with the two instrumental climate and four isotope series (d18O) from western Svalbard. We examine the data from ice cores drilled on Svalbard ice caps in 1997 (Lomonosovfonna, 1250 m asl) and 2005 (Holtedahlfonna, 1150 m asl) and the GNIP series from Ny-angstrom lesund and Isfjord Radio. The surface air temperature (SAT) and precipitation data from Longyearbyen and Ny-angstrom lesund are used to assess the skill of the model in reproducing the local climate. The model successfully captures the climate variations on the daily to multidecadal times scales although it tends to systematically underestimate the winter SAT. Analysis suggests that REMOiso performs better at simulating isotope compositions of precipitation in the winter than summer. The simulated and measured Holtedahlfonna d18O series agree reasonably well, whereas no significant correlation has been observed between the modelled and measured Lomonosovfonna ice core isotopic series. It is shown that sporadic nature as well as variability in the amount inherent in precipitation process potentially limits the accuracy of the past SAT reconstruction from the ice core data. This effect in the study area is, however, diminished by the role of other factors controlling d18O in precipitation, most likely sea ice extent, which is directly related with the SAT anomalies. Copyright (C) 2011 John Wiley & Sons, Ltd.

This paper presents an evaluation of a new linear parameterization valid for the troposphere and the stratosphere, based on a first order approximation of the carbon monoxide (CO) continuity equation. This linear scheme (hereinafter noted LINCO) has been implemented in the 3-D Chemical Transport Model (CTM) MOCAGE of Météo-France. On the one hand, a one and a half years of LINCO simulation has been compared to output obtained from a detailed chemical scheme output. In spite of small differences, the seasonal and global CO distributions obtained by both schemes present similar general characteristics. The mean differences between both schemes remain small within about ±25 ppbv (part per billion by volume) in the troposphere and ±15 ppbv in the stratosphere. On the other hand, LINCO has been compared to diverse observations from satellite instruments covering the troposphere (Measurements Of Pollution In The Troposphere: MOPITT) and the stratosphere (Microwave Limb Sounder: MLS) and also from aircraft (Measurements of ozone and water vapour by Airbus in-service aircraft: MOZAIC programme) mostly flying in the upper troposphere and lower stratosphere. A good agreement is generally found in the troposphere and the lower stratosphere. In the troposphere, the LINCO seasonal variations as well as the vertical and horizontal distributions are quite close to MOPITT CO observations. However, a bias of ~−40 ppbv is observed at 700 hPa between LINCO and MOPITT which is probably caused by too low emission values. In the stratosphere, MLS and LINCO present similar large-scale patterns, except over the poles where the CO concentration is underestimated by the model. We suggest that the underestimation of CO at polar latitudes is not related to the linear scheme but is induced by a too rapid transport by the meridional circulation. In the UTLS (Upper Troposphere Lower Stratosphere), LINCO tends to slightly overestimate the MOZAIC aircraft observations, with general small biases less than 2%. LINCO is a simple parameterization compared to a detailed chemical scheme, allowing very fast calculations and thus making possible long reanalyses of MOPITT CO data. The computational cost just corresponds to the transport of an additional passive tracer. For this, we used a variational 3-D-FGAT (First Guess at Appropriate Time) method in conjunction with MOCAGE for a long run of one and a half years. The data assimilation greatly improves the vertical CO distribution in the troposphere from 700 to 350 hPa compared to independent MOZAIC profiles. At 146 hPa, the assimilated CO 2-D distribution is improved compared to MLS observations by reducing the bias up to a factor of 2 in the tropics. At extratropical latitudes, the assimilated fields tend to underestimate the CO concentrations resulting from an excessive equator to pole circulation. This study confirms that the linear scheme is able to simulate reasonably well the CO distribution in the troposphere and in the lower stratosphere. Therefore, the low computing cost of the linear scheme opens new perspectives to make free runs and CO data assimilation runs at high resolution and over periods of several years.

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Dutay, J. -C. Lacan, F. Jeandel, C. Lacan, Francois/B-8032-2009 38 COPERNICUS GESELLSCHAFT MBH GOTTINGEN BIOGEOSCIENCES; The decoupled behaviour observed between Nd isotopic composition (Nd IC, also referred as epsilon(Nd)) and Nd concentration cycles has led to the notion of a 'Nd paradox'. While epsilon(Nd) behaves in a quasi-conservative way in the open ocean, leading to its broad use as a water-mass tracer, Nd concentration displays vertical profiles that increase with depth, together with a deep-water enrichment along the global thermohaline circulation. This non-conservative behaviour is typical of nutrients affected by scavenging in surface waters and remineralisation at depth. In addition, recent studies suggest the only way to reconcile both concentration and Nd IC oceanic budgets, is to invoke a 'Boundary Exchange' process (BE, defined as the co-occurrence of transfer of elements from the margin to the sea with removal of elements from the sea by Boundary Scavenging) as a source-sink term. However, these studies do not simulate the input/output fluxes of Nd to the ocean, and therefore prevents from crucial information that limits our understanding of Nd decoupling. To investigate this paradox on a global scale, this study uses for the first time a fully prognostic coupled dynamical/biogeochemical model with an explicit representation of Nd sources and sinks to simulate the Nd oceanic cycle. Sources considered include dissolved river fluxes, atmospheric dusts and margin sediment re-dissolution. Sinks are scavenging by settling particles. This model simulates the global features of the Nd oceanic cycle well, and produces a realistic distribution of Nd concentration (correct order of magnitude, increase with depth and along the conveyor belt, 65% of the simulated values fit in the +/- 10 pmol/kg envelop when compared to the data) and isotopic composition (inter-basin gradient, characterization of the main water-masses, more than 70% of the simulated values fit in the +/- 3 epsilon(Nd) envelop when compared to the data), though a slight overestimation of Nd concentrations in the deep Pacific Ocean may reveal an underestimation of the particle fields by the biogeochemical model. Our results indicate 1) vertical cycling (scavenging/remineralisation) is absolutely necessary to simulate both concentration and epsilon(Nd), and 2) BE is the dominant Nd source to the ocean. The estimated BE flux (1.1x10(10) g(Nd)/yr) is much higher than both dissolved river discharge (2.6x10(8) g(Nd)/yr) and atmospheric inputs (1.0x10(8) g(Nd)/yr) that both play negligible role in the water column but are necessary to reconcile Nd IC in surface and subsurface waters. This leads to a new calculated residence time of 360 yrs for Nd in the ocean. The BE flux requires the dissolution of 3 to 5% of the annual flux of continental weathering deposited via the solid river discharge to the continental margin.

A new field of study, "decadal prediction," is emerging in climate science. Decadal prediction lies between seasonal/interannual forecasting and longer-term climate change projections, and focuses on time-evolving regional climate conditions over the next 10-30 yr. Numerous assessments of climate information user needs have identified this time scale as being important to infrastructure planners, water resource managers, and many others. It is central to the information portfolio required to adapt effectively to and through climatic changes. At least three factors influence time-evolving regional climate at the decadal time scale: 1) climate change commitment (further warming as the coupled climate system comes into adjustment with increases of greenhouse gases that have already occurred), 2) external forcing, particularly from future increases of greenhouse gases and recovery of the ozone hole, and 3) internally generated variability. Some decadal prediction skill has been demonstrated to arise from the first two of these factors, and there is evidence that initialized coupled climate models can capture mechanisms of internally generated decadal climate variations, thus increasing predictive skill globally and particularly regionally. Several methods have been proposed for initializing global coupled climate models for decadal predictions, all of which involve global time-evolving threedimensional ocean data, including temperature and salinity. An experimental framework to address decadal predictability/prediction is described in this paper and has been incorporated into the coordinated Coupled Model Intercomparison Model, phase 5 (CMIP5) experiments, some of which will be assessed for the IPCC Fifth Assessment Report (AR5). These experiments will likely guide work in this emerging field over the next 5 yr.

Over the last decade, global-scale data sets of atmospheric water vapor isotopologues (HDO) have become available from different remote sensing instruments. Due to the observational geometry and the spectral ranges that are used, few satellites sample water isotopologues in the lower troposphere, where the bulk of hydrological processes within the atmosphere take place. Here, we compare three satellite HDO data sets, two from the Tropospheric Emission Spectrometer (TES retrieval version 4 and 5) and one from SCIAMACHY (SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY), with results from the atmospheric global circulation model ECHAM4 (European Centre HAMburg 4). We examine a list of known isotopologue effects to qualitatively benchmark the various observational data sets. TES version 5 (TESV5), TES version 4 (TESV4), SCIAMACHY, ECHAM, and ECHAM convolved with averaging kernels of TES version 5 (ECHAMAK5) successfully reproduced a number of established isotopologue effects such as the latitude effect, the amount effect, and the continental effect. The improvement of TESV5 over TESV4 is confirmed by the steeper latitudinal gradient at higher latitudes in agreement with SCIAMACHY. Also the representation of other features of the water isotopologue cycle, such as the seasonally varying signal in the tropics due to the movement of the Intertropical Convergence Zone (ITCZ), is improved in TESV5 and SCIAMACHY compared to TESV4. A known humidity bias due to the cross correlation of H2O and HDO measurements, which is of particular importance for instruments with low sensitivity close to the surface, was analyzed by applying either a humidity bias correction or a suitable a posteriori analysis. We suggest that the qualitative and quantitative tests carried out in this study could become benchmark tests for evaluation of future satellite isotopologue data sets.

Representation of atmospheric transport is a major source of error in the estimation of greenhouse gas sources and sinks by inverse modelling. Here we assess the impact on trace gas mole fractions of the new physical parameterizations recently implemented in the atmospheric global climate model LMDz to improve vertical diffusion, mesoscale mixing by thermal plumes in the planetary boundary layer (PBL), and deep convection in the troposphere. At the same time, the horizontal and vertical resolution of the model used in the inverse system has been increased. The aim of this paper is to evaluate the impact of these developments on the representation of trace gas transport and chemistry, and to anticipate the implications for inversions of greenhouse gas emissions using such an updated model. Comparison of a one-dimensional version of LMDz with large eddy simulations shows that the thermal scheme simulates shallow convective tracer transport in the PBL over land very efficiently, and much better than previous versions of the model. This result is confirmed in three-dimensional simulations, by a much improved reproduction of the radon-222 diurnal cycle. However, the enhanced dynamics of tracer concentrations induces a stronger sensitivity of the new LMDz configuration to external meteorological forcings. At larger scales, the inter-hemispheric exchange is slightly slower when using the new version of the model, bringing them closer to observations. The increase in the vertical resolution (from 19 to 39 layers) significantly improves the representation of stratosphere/troposphere exchange. Furthermore, changes in atmospheric thermodynamic variables, such as temperature, due to changes in the PBL mixing modify chemical reaction rates, which perturb chemical equilibriums of reactive trace gases. One implication of LMDz model developments for future inversions of greenhouse gas emissions is the ability of the updated system to assimilate a larger amount of highfrequency data sampled at high-variability stations. Others implications are discussed at the end of the paper., JRC.H.2-Air and Climate

Many of the next generation of global climate models will include aerosol schemes which explicitly simulate the microphysical processes that determine the particle size distribution. These models enable aerosol optical properties and cloud condensation nuclei (CCN) concentrations to be determined by fundamental aerosol processes, which should lead to a more physically based simulation of aerosol direct and indirect radiative forcings. This study examines the global variation in particle size distribution simulated by 12 global aerosol microphysics models to quantify model diversity and to identify any common biases against observations. Evaluation against size distribution measurements from a new European network of aerosol supersites shows that the mean model agrees quite well with the observations at many sites on the annual mean, but there are some seasonal biases common to many sites. In particular, at many of these European sites, the accumulation mode number concentration is biased low during winter and Aitken mode concentrations tend to be overestimated in winter and underestimated in summer. At high northern latitudes, the models strongly underpredict Aitken and accumulation particle concentrations compared to the measurements, consistent with previous studies that have highlighted the poor performance of global aerosol models in the Arctic. In the marine boundary layer, the models capture the observed meridional variation in the size distribution, which is dominated by the Aitken mode at high latitudes, with an increasing concentration of accumulation particles with decreasing latitude. Considering vertical profiles, the models reproduce the observed peak in total particle concentrations in the upper troposphere due to new particle formation, although modelled peak concentrations tend to be biased high over Europe. Overall, the multi-model-mean data set simulates the global variation of the particle size distribution with a good degree of skill, suggesting that most of the individual global aerosol microphysics models are performing well, although the large model diversity indicates that some models are in poor agreement with the observations. Further work is required to better constrain size-resolved primary and secondary particle number sources, and an improved understanding of nucleation and growth (e.g. the role of nitrate and secondary organics) will improve the fidelity of simulated particle size distributions.

Tropospheric trace gas and aerosol pollutants have adverse effects on health, environment and climate. In order to quantify and mitigate such effects, a wide range of processes leading to the formation and transport of pollutants must be considered, understood and represented in numerical models. Regional scale pollution episodes result from the combination of several factors: high emissions (from anthropogenic or natural sources), stagnant meteorological conditions, kinetics and efficiency of the chemistry and the deposition. All these processes are highly variable in time and space, and their relative contribution to the pollutants budgets can be quantified with chemistry-transport models. The CHIMERE chemistry-transport model is dedicated to regional atmospheric pollution event studies. Since it has now reached a certain level a maturity, the new stable version, CHIMERE 2013, is described to provide a reference model paper. The successive developments of the model are reviewed on the basis of published investigations that are referenced in order to discuss the scientific choices and to provide an overview of the main results.

This paper evaluates the current status of global modeling of the organic aerosol (OA) in the troposphere and analyzes the differences between models as well as between models and observations. Thirty-one global chemistry transport models (CTMs) and general circulation models (GCMs) have participated in this intercomparison, in the framework of AeroCom phase II. The simulation of OA varies greatly between models in terms of the magnitude of primary emissions, secondary OA (SOA) formation, the number of OA species used (2 to 62), the complexity of OA parameterizations (gas-particle partitioning, chemical aging, multiphase chemistry, aerosol microphysics), and the OA physical, chemical and optical properties. The diversity of the global OA simulation results has increased since earlier AeroCom experiments, mainly due to the increasing complexity of the SOA parameterization in models, and the implementation of new, highly uncertain, OA sources. Diversity of over one order of magnitude exists in the modeled vertical distribution of OA concentrations that deserves a dedicated future study. Furthermore, although the OA / OC ratio depends on OA sources and atmospheric processing, and is important for model evaluation against OA and OC observations, it is resolved only by a few global models. The median global primary OA (POA) source strength is 56 Tg a−1 (range 34–144 Tg a−1) and the median SOA source strength (natural and anthropogenic) is 19 Tg a−1 (range 13–121 Tg a−1). Among the models that take into account the semi-volatile SOA nature, the median source is calculated to be 51 Tg a−1 (range 16–121 Tg a−1), much larger than the median value of the models that calculate SOA in a more simplistic way (19 Tg a−1; range 13–20 Tg a−1, with one model at 37 Tg a−1). The median atmospheric burden of OA is 1.4 Tg (24 models in the range of 0.6–2.0 Tg and 4 between 2.0 and 3.8 Tg), with a median OA lifetime of 5.4 days (range 3.8–9.6 days). In models that reported both OA and sulfate burdens, the median value of the OA/sulfate burden ratio is calculated to be 0.77; 13 models calculate a ratio lower than 1, and 9 models higher than 1. For 26 models that reported OA deposition fluxes, the median wet removal is 70 Tg a−1 (range 28–209 Tg a−1), which is on average 85% of the total OA deposition. Fine aerosol organic carbon (OC) and OA observations from continuous monitoring networks and individual field campaigns have been used for model evaluation. At urban locations, the model–observation comparison indicates missing knowledge on anthropogenic OA sources, both strength and seasonality. The combined model–measurements analysis suggests the existence of increased OA levels during summer due to biogenic SOA formation over large areas of the USA that can be of the same order of magnitude as the POA, even at urban locations, and contribute to the measured urban seasonal pattern. Global models are able to simulate the high secondary character of OA observed in the atmosphere as a result of SOA formation and POA aging, although the amount of OA present in the atmosphere remains largely underestimated, with a mean normalized bias (MNB) equal to −0.62 (−0.51) based on the comparison against OC (OA) urban data of all models at the surface, −0.15 (+0.51) when compared with remote measurements, and −0.30 for marine locations with OC data. The mean temporal correlations across all stations are low when compared with OC (OA) measurements: 0.47 (0.52) for urban stations, 0.39 (0.37) for remote stations, and 0.25 for marine stations with OC data. The combination of high (negative) MNB and higher correlation at urban stations when compared with the low MNB and lower correlation at remote sites suggests that knowledge about the processes that govern aerosol processing, transport and removal, on top of their sources, is important at the remote stations. There is no clear change in model skill with increasing model complexity with regard to OC or OA mass concentration. However, the complexity is needed in models in order to distinguish between anthropogenic and natural OA as needed for climate mitigation, and to calculate the impact of OA on climate accurately.

A sulfur cycle model is coupled to a global chemistry-climate model. The simulated surface sulfate concentrations are generally within a factor of 2 of observed concentrations, and display a realistic seasonality for most background locations. However, the model tends to underestimate sulfate and overestimate surface SO 2 at relatively polluted locations. A possible explanation for this is that additional oxidation reactions not considered in the model, may be important. Calculated tropospheric sulfate column abundances exceed those of previous studies, which is predominantly associated with a less efficient nucleation scavenging in wet convective updrafts. Through the simultaneous calculation of the sulfur cycle and tropospheric photochemistry, simulated H 2 O 2 and SO 2 concentrations are strongly linked, especially in polluted areas. The coupled model simulates a stronger oxidant limitation and, consequently, a smaller contribution to sulfate formation by H 2 O 2 oxidation of SO 2 when compared to sulfur cycle models that use monthly averaged oxidant distributions as input. In the polluted NH, the differences in calculated sulfate columns are largest in winter and relatively small in summer. Therefore, the coupling between the sulfur cycle and the oxidant chemistry is expected to have a minor impact on the calculation of the indirect and direct radiative forcing by sulfate. An empirical relation between sulfate concentration and cloud drop number concentration, derived from cloud measurements at Grean Dun Fell (UK), is applied to the simulated cloud and sulfate fields to derive distributions of effective could drop radii. Additionally, a relation between wind speed and cloud drop number concentration is applied over marine regions to account for the effect of seasalt aerosol on cloud formation when sulfate concentrations are relatively low. Calculated droplet radii are systematically underestimated by about 10–20% in the NH compared to satellite derived values, but they agree relatively well in the SH. DOI: 10.1034/j.1600-0889.1998.t01-2-00002.x

The characteristics of the mid-Pliocene warm period (mPWP: 3.264–3.025 Ma BP) have been examined using geological proxies and climate models. While there is agreement between models and data, details of regional climate differ. Uncertainties in prescribed forcings and in proxy data limit the utility of the interval to understand the dynamics of a warmer than present climate or evaluate models. This uncertainty comes, in part, from the reconstruction of a time slab rather than a time slice , where forcings required by climate models can be more adequately constrained. Here, we describe the rationale and approach for identifying a time slice(s) for Pliocene environmental reconstruction. A time slice centred on 3.205 Ma BP (3.204–3.207 Ma BP) has been identified as a priority for investigation. It is a warm interval characterized by a negative benthic oxygen isotope excursion (0.21–0.23‰) centred on marine isotope stage KM5c (KM5.3). It occurred during a period of orbital forcing that was very similar to present day. Climate model simulations indicate that proxy temperature estimates are unlikely to be significantly affected by orbital forcing for at least a precession cycle centred on the time slice, with the North Atlantic potentially being an important exception.

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−1, 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.

International audience; A modelling experiment has been conceived to assess the impact of transport model errors on methane emissions estimated in an atmospheric inversion system. Synthetic methane observations, obtained from 10 different model outputs from the international TransCom-CH 4 model inter-comparison exercise, are combined with a prior scenario of methane emissions and sinks, and integrated into the three-component PYVAR-LMDZ-SACS (PYthon VARiational-Laboratoire de Météorologie Dy-namique model with Zooming capability-Simplified Atmospheric Chemistry System) inversion system to produce 10 different methane emission estimates at the global scale for the year 2005. The same methane sinks, emissions and initial conditions have been applied to produce the 10 synthetic observation datasets. The same inversion setup (statistical errors, prior emissions, inverse procedure) is then applied to derive flux estimates by inverse modelling. Consequently, only differences in the modelling of atmospheric transport may cause differences in the estimated fluxes. In our framework, we show that transport model errors lead to a discrepancy of 27 Tg yr −1 at the global scale, representing 5 % of total methane emissions. At continental and annual scales, transport model errors are proportionally larger than at the global scale, with errors ranging from 36 Tg yr −1 in North America to 7 Tg yr −1 in Boreal Eurasia (from 23 to 48 %, respectively). At the model grid-scale, the spread of inverse estimates can reach 150 % of the prior flux. Therefore, transport model errors contribute significantly to overall uncertainties in emission estimates by inverse modelling , especially when small spatial scales are examined. Sensitivity tests have been carried out to estimate the impact of the measurement network and the advantage of higher horizontal resolution in transport models. The large differences found between methane flux estimates inferred in these different configurations highly question the consistency of transport model errors in current inverse systems. Future inversions should include more accurately prescribed observation covariances matrices in order to limit Published by Copernicus Publications on behalf of the European Geosciences Union. 9918 R. Locatelli et al.: Transport model errors in methane inversions the impact of transport model errors on estimated methane fluxes.

A modified cumulus convection parametrisation scheme is presented. This scheme computes the mass of air transported upward in a cumulus cell using conservation of moisture and a detailed distribution of convective precipitation provided by a reanalysis dataset. The representation of vertical transport within the scheme includes entrainment and detrainment processes in convective updrafts and downdrafts. Output from the proposed parametrisation scheme is employed in the National Institute for Environmental Studies (NIES) global chemical transport model driven by JRA-25/JCDAS reanalysis. The simulated convective precipitation rate and mass fluxes are compared with observations and reanalysis data. A simulation of the short-lived tracer 222Rn is used to further evaluate the performance of the cumulus convection scheme. Simulated distributions of 222Rn are evaluated against observations at the surface and in the free troposphere, and compared with output from models that participated in the TransCom-CH4 Transport Model Intercomparison. From this comparison, we demonstrate that the proposed convective scheme in general is consistent with observed and modeled results.

The Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) consists of a series of time slice experiments targeting the long-term changes in atmospheric composition between 1850 and 2100, with the goal of documenting composition changes and the associated radiative forcing. In this overview paper, we introduce the ACCMIP activity, the various simulations performed (with a requested set of 14) and the associated model output. The 16 ACCMIP models have a wide range of horizontal and vertical resolutions, vertical extent, chemistry schemes and interaction with radiation and clouds. While anthropogenic and biomass burning emissions were specified for all time slices in the ACCMIP protocol, it is found that the natural emissions are responsible for a significant range across models, mostly in the case of ozone precursors. The analysis of selected present-day climate diagnostics (precipitation, temperature, specific humidity and zonal wind) reveals biases consistent with state-of-the-art climate models. The model-to-model comparison of changes in temperature, specific humidity and zonal wind between 1850 and 2000 and between 2000 and 2100 indicates mostly consistent results. However, models that are clear outliers are different enough from the other models to significantly affect their simulation of atmospheric chemistry.

REMO-HAM is a new regional aerosol-climate model. It is based on the REMO regional climate model and includes most of the major aerosol processes. The structure for aerosol is similar to the global aerosol-climate model ECHAM5-HAM, for example the aerosol module HAM is coupled with a two-moment stratiform cloud scheme. On the other hand, REMO-HAM does not include an online coupled aerosol-radiation nor a secondary organic aerosol module. In this work, we evaluate the model and compare the results against ECHAM5-HAM and measurements. Four different measurement sites were chosen for the comparison of total number concentrations, size distributions and gas phase sulfur dioxide concentrations: Hyytiälä in Finland, Melpitz in Germany, Mace Head in Ireland and Jungfraujoch in Switzerland. REMO-HAM is run with two different resolutions: 50 × 50 km2 and 10 × 10 km2. Based on our simulations, REMO-HAM is in reasonable agreement with the measured values. The differences in the total number concentrations between REMO-HAM and ECHAM5-HAM can be mainly explained by the difference in the nucleation mode. Since we did not use activation nor kinetic nucleation for the boundary layer, the total number concentrations are somewhat underestimated. From the meteorological point of view, REMO-HAM represents the precipitation fields and 2 m temperature profile very well compared to measurement. Overall, we show that REMO-HAM is a functional aerosol-climate model, which will be used in further studies.

A global chemistry-climate model LMDz_INCA is used to investigate the contribution of African and Asian emissions to tropospheric ozone over Central and West Africa during the summer monsoon. The model results show that ozone in this region is most sensitive to lightning NOx and to Central African biomass burning emissions. However, other emission categories also contribute significantly to regional ozone. The maximum ozone changes due to lightning NOx occur in the upper troposphere between 400 hPa and 200 hPa over West Africa and downwind over the Atlantic Ocean. Biomass burning emissions mainly influence ozone in the lower and middle troposphere over Central Africa, and downwind due to westward transport. Biogenic emissions of volatile organic compounds, which can be uplifted from the lower troposphere to higher altitudes by the deep convection that occurs over West Africa during the monsoon season, lead to maximum ozone changes in the lower stratosphere region. Soil NOx emissions over the Sahel region make a significant contribution to ozone in the lower troposphere. In addition, convective uplift of these emissions and subsequent ozone production are also an important source of ozone in the upper troposphere over West Africa. Concerning African anthropogenic emissions, they only make a small contribution to ozone compared to the other emission categories. The model results indicate that most ozone changes due to African emissions occur downwind, especially over the Atlantic Ocean, far from the emission regions. The import of Asian emissions also makes a considerable contribution to ozone concentrations above 150 hPa and has to be taken into account in studies of the ozone budget over Africa. Using IPCC AR5 (Intergovernmental Panel on Climate Change; Fifth Assessment Report) estimates of anthropogenic emissions for 2030 over Africa and Asia, model calculations show larger changes in ozone over Africa due to growth in Asian emissions compared to African emissions over the next 20 yr.

Subfossil pollen and plant macrofossil data derived from C-14-dated sediment profiles can provide quantitative information on glacial and interglacial climates. The data allow climate variables related to growing-season warmth, winter cold, and plant-available moisture to be reconstructed. Continental-scale reconstructions have been made for the mid-Holocene (MH, around 6 ka) and Last Glacial Maximum (LGM, around 21 ka), allowing comparison with palaeoclimate simulations currently being carried out as part of the fifth Assessment Report (AR5) of the Intergovernmental Panel on Climate Change. The synthesis of the available MH and LGM climate reconstructions and their uncertainties, obtained using modern-analogue, regression and model-inversion techniques, is presented for four temperature variables and two moisture variables. Reconstructions of the same variables based on surface-pollen assemblages are shown to be accurate and unbiased. Reconstructed LGM and MH climate anomaly patterns are coherent, consistent between variables, and robust with respect to the choice of technique. They support a conceptual model of the controls of Late Quaternary climate change whereby the first-order effects of orbital variations and greenhouse forcing on the seasonal cycle of temperature are predictably modified by responses of the atmospheric circulation and surface energy balance. UK Natural Environment Research Council; International Quaternary Association (INQUA) [0801]; QUEST (Quantifying Uncertainties in the Earth System) programme; US National Science Foundation; Natural Sciences and Engineering Research Council of Canada (NSERC); Canadian Foundation for Climate and Atmospheric Sciences (CFCAS); Natural Environment Research Council [quest010001, NE/F014600/1] info:eu-repo/semantics/publishedVersion

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Prof. S.-I. An is also acknowledged for fruitful discussions. The investigation was funded by RFBR (Russian foundation for basic researches) grants No. 08-05-00243 and international grant No. 0805-92550 CNRS-RFBR. 2 VERSITA WARSAW CENT EUR J GEOSCI; The intraseasonal tropical variability (ITV) patterns in the tropical troposphere are documented using double space-time Fourier analysis. Madden and Julian oscillations (MJO) as well as equatorial coupled waves (Kelvin and Rossby) are investigated based on the NCEP/NCAR Reanalysis data for the 1977-2006 period and the outputs of an intermediate ocean-atmosphere coupled model named LODCA-OTCM. A strong seasonal dependence of the ITV/ENSO relationship is evidenced. The leading relationship for equatorial Rossby waves (with the correlation of the same order than for the MJO) is documented; namely, it is shown that intensification of Rossby waves in the central Pacific during boreal summer precedes by half a year the peak of El Nino. The fact that MJO activity in spring-summer is associated to the strength of subsequent El Nino is confirmed. It is shown that LODCA-QTCM is capable of simulating the convectively coupled equatorial waves in outgoing long wave radiation and zonal wind at 850 hPa fields with skill comparable to other Coupled General Circulation Models. The ITV/ENSO relationship is modulated at low frequency. In particular the periods of low ENSO amplitude are associated with weaker MJO activity and a cancellation of MJO at the ENSO development phase. In opposition, during the decaying phase, MJO signal is strong. The periods of strong ENSO activity are associated with a marked coupling between MJO, Kelvin and equatorially Rossby waves and ENSO; the precursor signal of MJO (Rossby waves) in the western (central) Pacific is obvious. The results provide material for the observed change in ENSO characteristics in recent years and question whether the characteristics of the ITV/ENSO relationship may be sensitive to the observed warming in the central tropical Pacific.

We present a comprehensive description and benchmark evaluation of the tropospheric chemistry version of the global chemistry transport model TM5 (Tracer Model 5, version TM5-chem-v3.0). A full description is given concerning the photochemical mechanism, the interaction with aerosol, the treatment of the stratosphere, the wet and dry deposition parameterizations, and the applied emissions. We evaluate the model against a suite of ground-based, satellite, and aircraft measurements of components critical for understanding global photochemistry for the year 2006. The model exhibits a realistic oxidative capacity at a global scale. The methane lifetime is 8.9 years with an associated lifetime of methyl chloroform of 5.86 years, which is similar to that derived using an optimized hydroxyl radical field. The model reproduces the spatial and seasonal variation in background surface ozone concentrations and tropospheric ozone profiles from the World Ozone and Ultraviolet Radiation Data Centre to within 10 ppbv, but at several tropical stations the model tends to underestimate ozone in the free troposphere. The presented model results benchmark the TM5 tropospheric chemistry version, which is currently in use in several international cooperation activities, and upon which future model improvements will take place. The seasonal cycle in observed carbon monoxide (CO) is well simulated at different regions across the globe. In the Northern Hemisphere CO concentrations are underestimated by about 20 ppbv in spring and 10 ppbv in summer, which is related to missing chemistry and underestimated emissions from higher hydrocarbons, as well as to uncertainties in the seasonal variation of CO emissions. The model also captures the spatial and seasonal variation in formaldehyde tropospheric columns as observed by SCIAMACHY. Positive model biases over the Amazon and eastern United States point to uncertainties in the isoprene emissions as well as its chemical breakdown. Simulated tropospheric nitrogen dioxide columns correspond well to observations from the Ozone Monitoring Instrument in terms of its seasonal and spatial variability (with a global spatial correlation coefficient of 0.89), but TM5 fields are lower by 25¿ 40%. This is consistent with earlier studies pointing to a high bias of 0¿30% in the OMI retrievals, but uncertainties in the emission inventories have probably also contributed 25 to the discrepancy. TM5 tropospheric nitrogen dioxide profiles are in good agreement (within 0.1 ppbv) with in situ aircraft observations from the INTEX-B campaign over (the Gulf of) Mexico., JRC.DDG.H.2-Climate change

Changes in marine net primary productivity (PP) and export of particulate organic carbon (EP) are projected over the 21st century with four global coupled carbon cycle-climate models. These include representations of marine ecosystems and the carbon cycle of different structure and complexity. All four models show a decrease in global mean PP and EP between 2 and 20% by 2100 relative to preindustrial conditions, for the SRES A2 emission scenario. Two different regimes for productivity changes are consistently identified in all models. The first chain of mechanisms is dominant in the low- and mid-latitude ocean and in the North Atlantic: reduced input of macro-nutrients into the euphotic zone related to enhanced stratification, reduced mixed layer depth, and slowed circulation causes a decrease in macro-nutrient concentrations and in PP and EP. The second regime is projected for parts of the Southern Ocean: an alleviation of light and/or temperature limitation leads to an increase in PP and EP as productivity is fueled by a sustained nutrient input. A region of disagreement among the models is the Arctic, where three models project an increase in PP while one model projects a decrease. Projected changes in seasonal and interannual variability are modest in most regions. Regional model skill metrics are proposed to generate multi-model mean fields that show an improved skill in representing observation-based estimates compared to a simple multi-model average. Model results are compared to recent productivity projections with three different algorithms, usually applied to infer net primary production from satellite observations.

The effects of unified aerosol sources on global aerosol fields simulated by different models are examined in this paper. We compare results from two AeroCom experiments, one with different (ExpA) and one with unified emissions, injection heights, and particle sizes at the source (ExpB). Surprisingly, harmonization of aerosol sources has only a small impact on the simulated inter-model diversity of the global aerosol burden, and consequently global optical properties, as the results are largely controlled by model-specific transport, removal, chemistry (leading to the formation of secondary aerosols) and parameterizations of aerosol microphysics (e.g., the split between deposition pathways) and to a lesser extent by the spatial and temporal distributions of the (precursor) emissions. The burdens of black carbon and especially sea salt become more coherent in ExpB only, because the large ExpA diversities for these two species were caused by a few outliers. The experiment also showed that despite prescribing emission fluxes and size distributions, ambiguities in the implementation in individual models can lead to substantial differences. These results indicate the need for a better understanding of aerosol life cycles at process level (including spatial dispersal and interaction with meteorological parameters) in order to obtain more reliable results from global aerosol simulations. This is particularly important as such model results are used to assess the consequences of specific air pollution abatement strategies.

We show how a general formulation of the Fluctuation-Response Relation is able to describe in detail the connection between response properties to external perturbations and spontaneous fluctuations in systems with fast and slow variables. The method is tested by using the 360-variable Lorenz-96 model, where slow and fast variables are coupled to one another with reciprocal feedback, and a simplified low dimensional system. In the Fluctuation-Response context, the influence of the fast dynamics on the slow dynamics relies in a non trivial behavior of a suitable quadratic response function. This has important consequences for the modeling of the slow dynamics in terms of a Langevin equation: beyond a certain intrinsic time interval even the optimal model can give just statistical prediction., 40 pages

This work was carried out to understand the mechanisms leading to lofting and large-scale advection of aerosols over the Indian Ocean region due to interaction of the sea breeze with the northeast monsoon winds along the west coast of India. European Centre for Medium-Range Weather Forecasts (ECMWF) wind fields for the months of February and March 1999 were analyzed at various times of day. Intense sea breeze activity was observed at 1200 UT (1730 local time) along the west coast of India with average intensity larger in March than in February. The sea breeze was seen to extend inland deeper in March than in February. Lofting of air observed as high as 800 hPa (approximately 2 km above sea level) could lead to entrainment of aerosols into the free troposphere and long-range transport. Upward motion of air was observed everywhere along the west coast of India (from 8 degrees to 20 degrees N), on average higher in March than in February, because of convergence between the sea breeze and the synoptic-scale flow. A region of intense lofting of air and well-defined convergence was observed along the coast of the Karnataka region (12 degrees-16 degrees N). A simulation with a general circulation model nudged with ECMWF data indicated that the intrusion of marine air masses with low concentrations of organic matter is seen as deep as 64 km inland in the evening (1500 UT). Intrusion of the sea-salt plume is seen to a maximum distance of around 200 km from 1500 until 2300 UT. A well-developed lofted layer of aerosols as high as 3 km was also simulated during sea breeze activity along the west coast of India. The general circulation model simulation shows a clear diurnal evolution of the vertical profile of the aerosol extinction coefficient at Goa but fails to reproduce several features of the lidar observations, for example, the marked diurnal variability of the upper layers between 1 and 3 km. However, the model simulates a diurnal cycle at the surface (0-0.7 km) that is not apparent in lidar measurements. The model simulates long-range transport and captures the lofted plume downwind of the west coast of India. However, there was a 1-2 day delay in the model transport of lofted aerosols at higher layers to Hulule, 700 km downwind of India, when compared to lidar observations.

Global tropospheric ozone distributions, budgets, and radiative forcings from an ensemble of 26 state-of-the-art atmospheric chemistry models have been intercompared and synthesized as part of a wider study into both the air quality and climate roles of ozone. Results from three 2030 emissions scenarios, broadly representing "optimistic," "likely," and "pessimistic" options, are compared to a base year 2000 simulation. This base case realistically represents the current global distribution of tropospheric ozone. A further set of simulations considers the influence of climate change over the same time period by forcing the central emissions scenario with a surface warming of around 0.7K. The use of a large multimodel ensemble allows us to identify key areas of uncertainty and improves the robustness of the results. Ensemble mean changes in tropospheric ozone burden between 2000 and 2030 for the 3 scenarios range from a 5% decrease, through a 6% increase, to a 15% increase. The intermodel uncertainty (±1 standard deviation) associated with these values is about ±25%. Model outliers have no significant influence on the ensemble mean results. Combining ozone and methane changes, the three scenarios produce radiative forcings of -50, 180, and 300 mW m-2, compared to a CO2 forcing over the same time period of 800-1100 mW m-2. These values indicate the importance of air pollution emissions in short- to medium-term climate forcing and the potential for stringent/lax control measures to improve/worsen future climate forcing. The model sensitivity of ozone to imposed climate change varies between models but modulates zonal mean mixing ratios by ±5 ppbv via a variety of feedback mechanisms, in particular those involving water vapor and stratosphere-troposphere exchange. This level of climate change also reduces the methane lifetime by around 4%. The ensemble mean year 2000 tropospheric ozone budget indicates chemical production, chemical destruction, dry deposition and stratospheric input fluxes of 5100, 4650, 1000 and 550 Tg(O3) yr-1, respectively. These values are significantly different to the mean budget documented by the Intergovernmental Panel on Climate Change (IPCC) Third Assessment Report (TAR). The mean ozone burden (340 Tg(O3)) is 10% larger than the IPCC TAR estimate, while the mean ozone lifetime (22 days) is 10% shorter. Results from individual models show a correlation between ozone burden and lifetime, and each model's ozone burden and lifetime respond in similar ways across the emissions scenarios. The response to climate change is much less consistent. Models show more variability in the tropics compared to midlatitudes. Some of the most uncertain areas of the models include treatments of deep tropical convection, including lightning NOx production; isoprene emissions from vegetation and isoprene's degradation chemistry; stratosphere-troposphere exchange; biomass burning; and water vapor concentrations. Copyright 2006 by the American Geophysical Union.

International audience; The distribution of the fossil fuel component in atmospheric CO$_2$ cannot be measured directly at a cheap cost. Could anthropogenic tracers with source patterns similar to fossil fuel CO$_2$ then be used for that purpose? Here we present and evaluate a methodology using surrogate tracers, CO, SF$_6$, and C$_2$Cl$_4$, to deduce fossil fuel CO$_2$. A three-dimensional atmospheric chemistry transport model is used to simulate the relationship between each tracer and fossil fuel CO$_2$. In summertime the regression slopes between fossil fuel CO$_2$ and surrogate tracers show large spatial variations for chemically active tracers ( CO and C$_2$Cl$_4$), although C$_2$Cl$_4$ presents less scatter than CO. At two tall tower sites in the United States ( WLEF, Wisconsin, and WITN, North Carolina), we found that in summertime the C$_2$Cl$_4$ (CO) versus fossil CO$_2$ slope is on average up to 15% ( 25%) higher than in winter. We show that for C$_2$Cl$_4$ this seasonal variation is due to OH oxidation. For CO the seasonal variation is due to both chemistry and mixing with nonanthropogenic CO sources. In wintertime the three surrogate tracers SF$_6$, C$_2$Cl$_4$, and CO are about equally as good indicators of the presence of fossil CO$_2$. However, our model strongly underestimates the variability of SF$_6$ at both towers, probably because of unaccounted for emissions. Hence poor knowledge of emission distribution hampers the use of SF$_6$ as a surrogate tracer. From a practical point of view we recommend the use of C$_2$Cl$_4$ as a proxy of fossil CO$_2$. We also recommend the use of tracers to separate fossil CO$_2$. Despite the fact that the uncertainty on the regression slope is on the order of 30%, the tracer approach is likely to have less bias than when letting one model with one inventory emission map calculate the fossil CO$_2$ distribution.

We analyze present-day and future carbon monoxide (CO) simulations in 26 state-of-the-art atmospheric chemistry models run to study future air quality and climate change. In comparison with near-global satellite observations from the MOPITT instrument and local surface measurements, the models show large underestimates of Northern Hemisphere (NH) extratropical CO, while typically performing reasonably well elsewhere. The results suggest that year-round emissions, probably from fossil fuel burning in east Asia and seasonal biomass burning emissions in south-central Africa, are greatly underestimated in current inventories such as IIASA and EDGAR3.2. Variability among models is large, likely resulting primarily from intermodel differences in representations and emissions of nonmethane volatile organic compounds (NMVOCs) and in hydrologic cycles, which affect OH and soluble hydrocarbon intermediates. Global mean projections of the 2030 CO response to emissions changes are quite robust. Global mean midtropospheric (500 hPa) CO increases by 12.6 +/- 3.5 ppbv (16%) for the high-emissions (A2) scenario, by 1.7 +/- 1.8 ppbv (2%) for the midrange (CLE) scenario, and decreases by 8.1 +/- 2.3 ppbv (11%) for the low-emissions (MFR) scenario. Projected 2030 climate changes decrease global 500 hPa CO by 1.4 +/- 1.4 ppbv. Local changes can be much larger. In response to climate change, substantial effects are seen in the tropics, but intermodel variability is quite large. The regional CO responses to emissions changes are robust across models, however. These range from decreases of 10-20 ppbv over much of the industrialized NH for the CLE scenario to CO increases worldwide and year-round under A2, with the largest changes over central Africa (20-30 ppbv), southern Brazil (20-35 ppbv) and south and east Asia (30-70 ppbv). The trajectory of future emissions thus has the potential to profoundly affect air quality over most of the world's populated areas.

International audience Properly handling satellite data to constrain the inversion of CO2 sources and sinks at the Earth surface is a challenge motivated by the limitations of the current surface observation network. In this paper we present a Bayesian inference scheme to tackle this issue. It is based on the same theoretical principles as most inversions of the flask network but uses a variational formulation rather than a pure matrix-based one in order to cope with the large amount of satellite data. The minimization algorithm iteratively computes the optimum solution to the inference problem as well as an estimation of its error characteristics and some quantitative measures of the observation information content. A global climate model, guided by analyzed winds, provides information about the atmospheric transport to the inversion scheme. A surface flux climatology regularizes the inference problem. This new system has been applied to 1 year's worth of retrievals of vertically integrated CO2 concentrations from the Television Infrared Observation Satellite Operational Vertical Sounder (TOVS). Consistent with a recent study that identified regional biases in the TOVS retrievals, the inferred fluxes are not useful for biogeochemical analyses. In addition to the detrimental impact of these biases, we find a sensitivity of the results to the formulation of the prior uncertainty and to the accuracy of the transport model. Notwithstanding these difficulties, four-dimensional inversion schemes of the type presented here could form the basis of multisensor data assimilation systems for the estimation of the surface fluxes of key atmospheric compounds.

Spatial and temporal variations of atmospheric CO2 concentrations contain information about surface sources and sinks, which can be quantitatively interpreted through tracer transport inversion. Previous CO2 inversion calculations obtained differing results due to different data, methods and transport models used. To isolate the sources of uncertainty, we have conducted a set of annual mean inversion experiments in which 17 different transport models or model variants were used to calculate regional carbon sources and sinks from the same data with a standardized method. Simulated transport is a significant source of uncertainty in these calculations, particularly in the response to prescribed “background” fluxes due to fossil fuel combustion, a balanced terrestrial biosphere, and air–sea gas exchange. Individual model-estimated fluxes are often a direct reflection of their response to these background fluxes. Models that generate strong surface maxima near background exchange locations tend to require larger uptake near those locations. Models with weak surface maxima tend to have less uptake in those same regions but may infer small sources downwind. In some cases, individual model flux estimates cannot be analyzed through simple relationships to background flux responses but are likely due to local transport differences or particular responses at individual CO2 observing locations. The response to the background biosphere exchange generates the greatest variation in the estimated fluxes, particularly over land in the Northern Hemisphere. More observational data in the tropical regions may help in both lowering the uncertain tropical land flux uncertainties and constraining the northern land estimates because of compensation between these two broad regions in the inversion. More optimistically, examination of the model-mean retrieved fluxes indicates a general insensitivity to the prior fluxes and the prior flux uncertainties. Less uptake in the Southern Ocean than implied by oceanographic observations, and an evenly distributed northern land sink, remain in spite of changes in this aspect of the inversion setup.]DOI: 10.1034/j.1600-0889.2003.00049.x

Measurements made during the Indian Ocean Experiment (INDOEX) in 1998, indicate likely regional atmospheric effects of sulphate aerosol over India including the potential for cloud processing of SO 2 to sulphate. Sulphate aerosol production in clouds was examined for cloud characteristics and pollutant concentrations typical of the Indian region, to assess the contribution of different mechanisms to sulphate formation. A simple model was formulated incorporating gas-liquid equilibria, gas-phase mass transfer, SO 2 oxidation in the gas phase by OH· radicals and in the aqueous phase by H 2 O 2 , O 3 and O 2 catalysed by Fe 3+ and Mn 2+ in a cloud with uniformly sized drops. Sulphate formation was simulated in St/Sc, Cu and Cb clouds using an initial pH of 6.5, likely to occur in this region, for cloud drop diameters of 10, 50 and 100 μm. The clouds were assumed to have nucleated on ammonium sulphate aerosols and contained reported background concentrations of these ions in clean rainwater over the Indian ocean. The simulations produced final cloud pHs of 4.5–5 and final sulphate concentrations of 25–90 μM, in agreement with the range of reported preliminary measurements. An examination of mass transfer effects showed that the characteristic diffusion times of H 2 O 2 and SO 2 were lower by a factor of 10 or more than the respective reaction times, indicating that mass transfer effects would not limit the rate of S VI formation under likely atmospheric conditions. Sulphate formation in St/Sc clouds was shown to likely be SO 2 limited in July and H 2 O 2 limited in January. In all cases, the gas phase reaction and the O 2 reaction catalysed by Mn 2+ and Fe 3+ contributed less than 1% to the S VI produced. In St/Sc and Cu clouds, 85–96% of the S VI was from the H 2 O 2 reaction. In Cb clouds about 60–75% of the S VI was from the H 2 O 2 reaction and 25–41% from the O 3 reaction. In Cb clouds, the short residence and the persistence of alkaline conditions in the earlier part of the cloud cycle, enhance the contribution of the O 3 reaction to the greatest extent. If alkaline conditions were to persist throughout the cloud cycle (from cation chemistry not simulated in this model), the contribution of the O 3 reaction to S VI could be further enhanced. DOI: 10.1034/j.1600-0889.2001.01015.x

Large variations in the composition, structure, and function of Arctic ecosystems are determined by climatic gradients, especially of growing-season warmth, soil moisture, and snow cover. A unified circumpolar classification recognizing five types of tundra was developed. The geographic distributions of vegetation types north of 55°N, including the position of the forest limit and the distributions of the tundra types, could be predicted from climatology using a small set of plant functional types embedded in the biogeochemistry-biogeography model BIOME4. Several palaeoclimate simulations for the last glacial maximum (LGM) and mid-Holocene were used to explore the possibility of simulating past vegetation patterns, which are independently known based on pollen data. The broad outlines of observed changes in vegetation were captured. LGM simulations showed the major reduction of forest, the great extension of graminoid and forb tundra, and the restriction of low- and high-shrub tundra (although not all models produced sufficiently dry conditions to mimic the full observed change). Mid-Holocene simulations reproduced the contrast between northward forest extension in western and central Siberia and stability of the forest limit in Beringia. Projection of the effect of a continued exponential increase in atmospheric CO2 concentration, based on a transient ocean-atmosphere simulation including sulfate aerosol effects, suggests a potential for larger changes in Arctic ecosystems during the 21st century than have occurred between mid-Holocene and present. Simulated physiological effects of the CO2 increase (to > 700 ppm) at high latitudes were slight compared with the effects of the change in climate.