Laboratoire d'Aérologie

Abstract. We present and discuss a new dataset of gridded emissions covering the historical period (1850–2000) in decadal increments at a horizontal resolution of 0.5° in latitude and longitude. The primary purpose of this inventory is to provide consistent gridded emissions of reactive gases and aerosols for use in chemistry model simulations needed by climate models for the Climate Model Intercomparison Program #5 (CMIP5) in support of the Intergovernmental Panel on Climate Change (IPCC) Fifth Assessment report (AR5). Our best estimate for the year 2000 inventory represents a combination of existing regional and global inventories to capture the best information available at this point; 40 regions and 12 sectors are used to combine the various sources. The historical reconstruction of each emitted compound, for each region and sector, is then forced to agree with our 2000 estimate, ensuring continuity between past and 2000 emissions. Simulations from two chemistry-climate models are used to test the ability of the emission dataset described here to capture long-term changes in atmospheric ozone, carbon monoxide and aerosol distributions. The simulated long-term change in the Northern mid-latitudes surface and mid-troposphere ozone is not quite as rapid as observed. However, stations outside this latitude band show much better agreement in both present-day and long-term trend. The model simulations indicate that the concentration of carbon monoxide is underestimated at the Mace Head station; however, the long-term trend over the limited observational period seems to be reasonably well captured. The simulated sulfate and black carbon deposition over Greenland is in very good agreement with the ice-core observations spanning the simulation period. Finally, aerosol optical depth and additional aerosol diagnostics are shown to be in good agreement with previously published estimates and observations.

Abstract. Ozone holds a certain fascination in atmospheric science. It is ubiquitous in the atmosphere, central to tropospheric oxidation chemistry, yet harmful to human and ecosystem health as well as being an important greenhouse gas. It is not emitted into the atmosphere but is a byproduct of the very oxidation chemistry it largely initiates. Much effort is focused on the reduction of surface levels of ozone owing to its health and vegetation impacts, but recent efforts to achieve reductions in exposure at a country scale have proved difficult to achieve owing to increases in background ozone at the zonal hemispheric scale. There is also a growing realisation that the role of ozone as a short-lived climate pollutant could be important in integrated air quality climate change mitigation. This review examines current understanding of the processes regulating tropospheric ozone at global to local scales from both measurements and models. It takes the view that knowledge across the scales is important for dealing with air quality and climate change in a synergistic manner. The review shows that there remain a number of clear challenges for ozone such as explaining surface trends, incorporating new chemical understanding, ozone–climate coupling, and a better assessment of impacts. There is a clear and present need to treat ozone across the range of scales, a transboundary issue, but with an emphasis on the hemispheric scales. New observational opportunities are offered both by satellites and small sensors that bridge the scales.

We use 23 atmospheric chemistry transport models to calculate current and future (2030) deposition of reactive nitrogen (NO y , NH x ) and sulfate (SO x ) to land and ocean surfaces. The models are driven by three emission scenarios: (1) current air quality legislation (CLE); (2) an optimistic case of the maximum emissions reductions currently technologically feasible (MFR); and (3) the contrasting pessimistic IPCC SRES A2 scenario. An extensive evaluation of the present‐day deposition using nearly all information on wet deposition available worldwide shows a good agreement with observations in Europe and North America, where 60–70% of the model‐calculated wet deposition rates agree to within ±50% with quality‐controlled measurements. Models systematically overestimate NH x deposition in South Asia, and underestimate NO y deposition in East Asia. We show that there are substantial differences among models for the removal mechanisms of NO y , NH x , and SO x , leading to ±1 σ variance in total deposition fluxes of about 30% in the anthropogenic emissions regions, and up to a factor of 2 outside. In all cases the mean model constructed from the ensemble calculations is among the best when comparing to measurements. Currently, 36–51% of all NO y , NH x , and SO x is deposited over the ocean, and 50–80% of the fraction of deposition on land falls on natural (nonagricultural) vegetation. Currently, 11% of the world's natural vegetation receives nitrogen deposition in excess of the “critical load” threshold of 1000 mg(N) m −2 yr −1 . The regions most affected are the United States (20% of vegetation), western Europe (30%), eastern Europe (80%), South Asia (60%), East Asia (40%), southeast Asia (30%), and Japan (50%). Future deposition fluxes are mainly driven by changes in emissions, and less importantly by changes in atmospheric chemistry and climate. The global fraction of vegetation exposed to nitrogen loads in excess of 1000 mg(N) m −2 yr −1 increases globally to 17% for CLE and 25% for A2. In MFR, the reductions in NO y are offset by further increases for NH x deposition. The regions most affected by exceedingly high nitrogen loads for CLE and A2 are Europe and Asia, but also parts of Africa.

Regional climate models are important research tools available to scientists around the world, including in economically developing nations (EDNs). The Earth Systems Physics (ESP) group of the Abdus Salam International Centre for Theoretical Physics (ICTP) maintains and distributes a state-of-the-science regional climate model called the ICTP Regional Climate Model version 3 (RegCM3), which is currently being used by a large research community for a diverse range of climate-related studies. The RegCM3 is the central, but not only, tool of the ICTP-maintained Regional Climate Research Network (RegCNET) aimed at creating south–south and north–south scientific interactions on the topic of climate and associated impacts research and modeling. In this paper, RegCNET, RegCM3, and illustrative results from RegCM3 benchmark simulations applied over south Asia, Africa, and South America are presented. It is shown that RegCM3 performs reasonably well over these regions and is therefore useful for climate studies in EDNs.

A global assessment of precipitation chemistry and deposition has been carried out under the direction of the World Meteorological Organization (WMO) Global Atmosphere Watch (GAW) Scientific Advisory Group for Precipitation Chemistry (SAG-PC). The assessment addressed three questions: (1) what do measurements and model estimates of precipitation chemistry and wet, dry and total deposition of sulfur, nitrogen, sea salt, base cations, organic acids, acidity, and phosphorus show globally and regionally? (2) has the wet deposition of major ions changed since 2000 (and, where information and data are available, since 1990) and (3) what are the major gaps and uncertainties in our knowledge? To that end, regionally-representative measurements for two 3-year-averaging periods, 2000–2002 and 2005–2007, were compiled worldwide. Data from the 2000–2002 averaging period were combined with 2001 ensemble-mean modeling results from 21 global chemical transport models produced in Phase 1 of the Coordinated Model Studies Activities of the Task Force on Hemispheric Transport of Air Pollution (TF HTAP). The measurement data and modeling results were used to generate global and regional maps of major ion concentrations in precipitation and deposition. A major product of the assessment is a database of quality assured ion concentration and wet deposition data gathered from regional and national monitoring networks. The database is available for download from the World Data Centre for Precipitation Chemistry (http://wdcpc.org/). The assessment concludes that global concentrations and deposition of sulfur and nitrogen are reasonably well characterized with levels generally highest near emission sources and more than an order of magnitude lower in areas largely free of anthropogenic influences. In many parts of the world, wet deposition of reduced nitrogen exceeds that of oxidized nitrogen and is increasing. Sulfur and nitrogen concentrations and deposition in North America and Europe have declined significantly in line with emission reduction policies. Major regions of the world, including South America, the more remote areas of North America, much of Asia, Africa, Oceania, polar regions, and all of the oceans, are inadequately sampled for all of the major ions in wet and dry deposition, and particularly so for phosphorus, organic forms of nitrogen, and weak acids including carbonates and organic acids. Measurement-based inferential estimates of dry deposition are limited to sulfur and some nitrogen in only a few regions of the world and methods are highly uncertain. The assessment concludes with recommendations to address major gaps and uncertainties in global ion concentration and deposition measurements.

The impact of drops impinging one by one on a solid surface is studied experimentally and theoretically. The impact process is observed by means of a charge-coupled-device camera, its pictures processed by computer. Low-velocity impact results in spreading and in propagation of capillary waves, whereas at higher velocities splashing (i.e. the emergence of a cloud of small secondary droplets, absent in the former case) sets in. Capillary waves are studied in some detail in separate experiments. The dynamics of the extension of liquid lamellae produced by an impact in the case of splashing is recorded. The secondary-droplet size distributions and the total volume of these droplets are measured, and the splashing threshold is found as a function of the impact parameters. The pattern of the capillary waves is predicted to be self-similar. The calculated wave profile agrees well with the experimental data. It is shown theoretically that the splashing threshold corresponds to the onset of a velocity discontinuity propagating over the liquid layer on the wall. This discontinuity shows several aspects of a shock. In an incompressible liquid such a discontinuity can only exist in the presence of a sink at its front. The latter results in the emergence of a circular crown-like sheet virtually normal to the wall and propagating with the discontinuity. It is predicted theoretically and recorded in the experiment. The crown is unstable owing to the formation of cusps at the free rim at its top edge, which results in the splashing effect. The onset velocity of splashing and the rate of propagation of the kinematic discontinuity are calculated and the theoretical results agree fairly well with the experimental data. The structure of the discontinuity is shown to match the outer solution.

Abstract. The Meso-NH Atmospheric Simulation System is a joint effort of the Centre National de Recherches Météorologiques and Laboratoire d'Aérologie. It comprises several elements; a numerical model able to simulate the atmospheric motions, ranging from the large meso-alpha scale down to the micro-scale, with a comprehensive physical package, a flexible file manager, an ensemble of facilities to prepare initial states, either idealized or interpolated from meteorological analyses or forecasts, a flexible post-processing and graphical facility to visualize the results, and an ensemble of interactive procedures to control these functions. Some of the distinctive features of this ensemble are the following: the model is currently based on the Lipps and Hemler form of the anelastic system, but may evolve towards a more accurate form of the equations system. In the future, it will allow for simultaneous simulation of several scales of motion, by the so-called "interactive grid-nesting technique". It allows for the in-line computation and accumulation of various terms of the budget of several quantities. It allows for the transport and diffusion of passive scalars, to be coupled with a chemical module. It uses the relatively new Fortran 90 compiler. It is tailored to be easily implemented on any UNIX machine. Meso-NH is designed as a research tool for small and meso-scale atmospheric processes. It is freely accessible to the research community, and we have tried to make it as "user-friendly" as possible, and as general as possible, although these two goals sometimes appear contradictory. The present paper presents a general description of the adiabatic formulation and some of the basic validation simulations. A list of the currently available physical parametrizations and initialization methods is also given. A more precise description of these aspects will be provided in a further paper.

Abstract Tropospheric ozone plays a major role in Earth’s atmospheric chemistry processes and also acts as an air pollutant and greenhouse gas. Due to its short lifetime, and dependence on sunlight and precursor emissions from natural and anthropogenic sources, tropospheric ozone’s abundance is highly variable in space and time on seasonal, interannual and decadal time-scales. Recent, and sometimes rapid, changes in observed ozone mixing ratios and ozone precursor emissions inspired us to produce this up-to-date overview of tropospheric ozone’s global distribution and trends. Much of the text is a synthesis of in situ and remotely sensed ozone observations reported in the peer-reviewed literature, but we also include some new and extended analyses using well-known and referenced datasets to draw connections between ozone trends and distributions in different regions of the world. In addition, we provide a brief evaluation of the accuracy of rural or remote surface ozone trends calculated by three state-of-the-science chemistry-climate models, the tools used by scientists to fill the gaps in our knowledge of global tropospheric ozone distribution and trends.

The Tropospheric Ozone Assessment Report (TOAR) is an activity of the International Global Atmospheric Chemistry Project. This paper is a component of the report, focusing on the present-day distribution and trends of tropospheric ozone relevant to climate and global atmospheric chemistry model evaluation. Utilizing the TOAR surface ozone database, several figures present the global distribution and trends of daytime average ozone at 2702 non-urban monitoring sites, highlighting the regions and seasons of the world with the greatest ozone levels. Similarly, ozonesonde and commercial aircraft observations reveal ozone’s distribution throughout the depth of the free troposphere. Long-term surface observations are limited in their global spatial coverage, but data from remote locations indicate that ozone in the 21st century is greater than during the 1970s and 1980s. While some remote sites and many sites in the heavily polluted regions of East Asia show ozone increases since 2000, many others show decreases and there is no clear global pattern for surface ozone changes since 2000. Two new satellite products provide detailed views of ozone in the lower troposphere across East Asia and Europe, revealing the full spatial extent of the spring and summer ozone enhancements across eastern China that cannot be assessed from limited surface observations. Sufficient data are now available (ozonesondes, satellite, aircraft) across the tropics from South America eastwards to the western Pacific Ocean, to indicate a likely tropospheric column ozone increase since the 1990s. The 2014–2016 mean tropospheric ozone burden (TOB) between 60°N–60°S from five satellite products is 300 Tg ± 4%. While this agreement is excellent, the products differ in their quantification of TOB trends and further work is required to reconcile the differences. Satellites can now estimate ozone’s global long-wave radiative effect, but evaluation is difficult due to limited in situ observations where the radiative effect is greatest.

While most land models developed for use with climate models represent vegetation as discrete biomes, this is, at least for mixed life‐form biomes, inconsistent with the leaf‐level and whole‐plant physiological parameterizations needed to couple these biogeophysical models with biogeochemical and ecosystem dynamics models. In this paper, we present simulations with the National Center for Atmospheric Research land surface model (NCAR LSM) that examined the effect of representing vegetation as patches of plant functional types (PFTs) that coexist within a model grid cell. This approach is consistent with ecological theory and models and allows for unified treatment of vegetation in climate and ecosystem models. In the standard NCAR LSM the PFT composition and leaf area for each grid cell are obtained by classifying grid cells as 1 of 28 possible biomes. Here, we develop a data set from 1‐km satellite data that provides each model grid cell a unique PFT composition and leaf area for each PFT. Global simulations at 3° × 3° spatial resolution showed that ground temperature, ground evaporation, and northern high‐latitude winter albedo exhibited direct responses to these landscape changes, which led to indirect effects such as in soil moisture and sensible and latent heat fluxes. Additional simulations at 2° × 2° and 1° × 1° spatial resolution showed that low‐resolution simulations masked landscape heterogeneity in both approaches but the satellite‐based, continuous representation of vegetation reduced model sensitivity to resolution. It is argued that the use of spatially continuous distributions of coexisting PFTs is a necessary step to link climate and ecosystem models.

Abstract A bulk mass‐flux convection parametrization for deep and shallow convection is presented that includes an efficient and straightforward treatment of numerics, moist thermodynamics and convective downdraughts. The scheme is evaluated in a single‐column model context for a tropical deep‐convective period and a trade‐wind cumulus case. Preliminary applications in a global numerical weather‐prediction model and a mesoscale model are also discussed. The results suggest that the present scheme provides reasonable solutions in terms of predicted rainfall, and tropical temperature and moisture structures. The application of the scheme to various scales is supported by the use of a convective available potential energy convective closure that assures a smooth interaction with the large‐scale environment and efficiently suppresses conditional instability of the second kind‐like spin‐up processes on the grid‐scale. Finally, the theoretical and practical limits of the present approach are discussed together with possible future developments.

Abstract. An eight-year long reanalysis of atmospheric composition data covering the period 2003–2010 was constructed as part of the FP7-funded Monitoring Atmospheric Composition and Climate project by assimilating satellite data into a global model and data assimilation system. This reanalysis provides fields of chemically reactive gases, namely carbon monoxide, ozone, nitrogen oxides, and formaldehyde, as well as aerosols and greenhouse gases globally at a horizontal resolution of about 80 km for both the troposphere and the stratosphere. This paper describes the assimilation system for the reactive gases and presents validation results for the reactive gas analysis fields to document the data set and to give a first indication of its quality. Tropospheric CO values from the MACC reanalysis are on average 10–20% lower than routine observations from commercial aircrafts over airports through most of the troposphere, and have larger negative biases in the boundary layer at urban sites affected by air pollution, possibly due to an underestimation of CO or precursor emissions. Stratospheric ozone fields from the MACC reanalysis agree with ozonesondes and ACE-FTS data to within ±10% in most seasons and regions. In the troposphere the reanalysis shows biases of −5% to +10% with respect to ozonesondes and aircraft data in the extratropics, but has larger negative biases in the tropics. Area-averaged total column ozone agrees with ozone fields from a multi-sensor reanalysis data set to within a few percent. NO2 fields from the reanalysis show the right seasonality over polluted urban areas of the NH and over tropical biomass burning areas, but underestimate wintertime NO2 maxima over anthropogenic pollution regions and overestimate NO2 in northern and southern Africa during the tropical biomass burning seasons. Tropospheric HCHO is well simulated in the MACC reanalysis even though no satellite data are assimilated. It shows good agreement with independent SCIAMACHY retrievals over regions dominated by biogenic emissions with some anthropogenic input, such as the eastern US and China, and also over African regions influenced by biogenic sources and biomass burning.

Measurements of Pollution in the Troposphere (MOPITT) is a new remote sensing instrument aboard the Earth Observing System (EOS) “Terra” satellite which exploits gas correlation radiometry principles to quantify tropospheric concentrations of carbon monoxide (CO) and methane (CH 4 ). The MOPITT CO retrieval algorithm employs a nonlinear optimal estimation method to iteratively solve for the CO profile which is statistically most consistent with both the satellite‐measured radiances and a priori information. The algorithm's theoretical basis is described in terms of the observed radiances and their weighting functions, the a priori information, and the retrieval averaging kernels. Examples of actual CO retrievals over scenes with contrasting pollution conditions are demonstrated, and interpreted in the context of the retrieval averaging kernels and a priori.

The emissions of carbon dioxide (CO 2 ) and methane (CH 4 ) from the Petit Saut hydroelectric reservoir (Sinnamary River, French Guiana) to the atmosphere were quantified for 10 years since impounding in 1994. Diffusive emissions from the reservoir surface were computed from direct flux measurements in 1994, 1995, and 2003 and from surface concentrations monitoring. Bubbling emissions, which occur only at water depths lower than 10 m, were interpolated from funnel measurements in 1994, 1997, and 2003. Degassing at the outlet of the dam downstream of the turbines was calculated from the difference in gas concentrations upstream and downstream of the dam and the turbined discharge. Diffusive emissions from the Sinnamary tidal river and estuary were quantified from direct flux measurements in 2003 and concentrations monitoring. Total carbon emissions were 0.37 ± 0.01 Mt yr −1 C (CO 2 emissions, 0.30 ± 0.02; CH 4 emissions, 0.07 ± 0.01) the first 3 years after impounding (1994–1996) and then decreased to 0.12 ± 0.01 Mt yr −1 C (CO 2 , 0.10 ± 0.01; CH 4 , 0.016 ± 0.006) since 2000. On average over the 10 years, 61% of the CO 2 emissions occurred by diffusion from the reservoir surface, 31% from the estuary, 7% by degassing at the outlet of the dam, and a negligible fraction by bubbling. CH 4 diffusion and bubbling from the reservoir surface were predominant (40% and 44%, respectively) only the first year after impounding. Since 1995, degassing at an aerating weir downstream of the turbines has become the major pathway for CH 4 emissions, reaching 70% of the total CH 4 flux. In 2003, river carbon inputs were balanced by carbon outputs to the ocean and were about 3 times lower than the atmospheric flux, which suggests that 10 years after impounding, the flooded terrestrial carbon is still the predominant contributor to the gaseous emissions. In 10 years, about 22% of the 10 Mt C flooded was lost to the atmosphere. Our results confirm the significance of greenhouse gas emissions from tropical reservoir but stress the importance of: (1) considering all the gas pathways upstream and downstream of the dams and (2) taking into account the reservoir age when upscaling emissions rates at the global scale.

Abstract A new diagnostic convective closure, which is dependent on convective available potential energy (CAPE), is derived under the quasi-equilibrium assumption for the free troposphere subject to boundary layer forcing. The closure involves a convective adjustment time scale for the free troposphere and a coupling coefficient between the free troposphere and the boundary layer based on different time scales over land and ocean. Earlier studies with the ECMWF Integrated Forecasting System (IFS) have already demonstrated the model’s ability to realistically represent tropical convectively coupled waves and synoptic variability with use of the “standard” CAPE closure, given realistic entrainment rates. A comparison of low-resolution seasonal integrations and high-resolution short-range forecasts against complementary satellite and radar data shows that with the extended CAPE closure it is also possible, independent of model resolution and time step, to realistically represent nonequilibrium convection such as the diurnal cycle of convection and the convection tied to advective boundary layers, although representing the late night convection over land remains a challenge. A more in-depth regional analysis of the diurnal cycle and the closure is provided for the continental United States and particularly Africa, including comparison with data from satellites and a cloud-resolving model (CRM). Consequences for global numerical weather prediction (NWP) are not only a better phase representation of convection, but also better forecasts of its spatial distribution and local intensity.

The HMG-box transcription factor Sox9 is expressed in the intestinal epithelium, specifically, in stem/progenitor cells and in Paneth cells. Sox9 expression requires an active beta-catenin-Tcf complex, the transcriptional effector of the Wnt pathway. This pathway is critical for numerous aspects of the intestinal epithelium physiopathology, but processes that specify the cell response to such multipotential signals still remain to be identified. We inactivated the Sox9 gene in the intestinal epithelium to analyze its physiological function. Sox9 inactivation affected differentiation throughout the intestinal epithelium, with a disappearance of Paneth cells and a decrease of the goblet cell lineage. Additionally, the morphology of the colon epithelium was severely altered. We detected general hyperplasia and local crypt dysplasia in the intestine, and Wnt pathway target genes were up-regulated. These results highlight the central position of Sox9 as both a transcriptional target and a regulator of the Wnt pathway in the regulation of intestinal epithelium homeostasis.

Abiotic release of nitrous acid (HONO) in equilibrium with soil nitrite (NO2(-)) was suggested as an important contributor to the missing source of atmospheric HONO and hydroxyl radicals (OH). The role of total soil-derived HONO in the biogeochemical and atmospheric nitrogen cycles, however, has remained unknown. In laboratory experiments, we found that for nonacidic soils from arid and arable areas, reactive nitrogen emitted as HONO is comparable with emissions of nitric oxide (NO). We show that ammonia-oxidizing bacteria can directly release HONO in quantities larger than expected from the acid-base and Henry's law equilibria of the aqueous phase in soil. This component of the nitrogen cycle constitutes an additional loss term for fixed nitrogen in soils and a source for reactive nitrogen in the atmosphere.

The optical spectrograph and infrared imager system (OSIRIS) on board the Odin spacecraft is designed to retrieve altitude profiles of terrestrial atmospheric minor species by observing limb-radiance profiles. The grating optical spectrograph (OS) obtains spectra of scattered sunlight over the range 280–800 nm with a spectral resolution of approximately 1 nm. The Odin spacecraft performs a repetitive vertical limb scan to sweep the OS 1 km vertical field of view over selected altitude ranges from approximately 10 to 100 km. The terrestrial absorption features that are superimposed on the scattered solar spectrum are monitored to derive the minor species altitude profiles. The spectrograph also detects the airglow, which can be used to study the mesosphere and lower thermosphere. The other part of OSIRIS is a three-channel infrared imager (IRI) that uses linear array detectors to image the vertical limb radiance over an altitude range of approximately 100 km. The IRI observes both scattered sunlight and the airglow emissions from the oxygen infrared atmospheric band at 1.27 µm and the OH (3-1) Meinel band at 1.53 µm. A tomographic inversion technique is used with a series of these vertical images to derive the two-dimensional distribution of the emissions within the orbit plane. PACS Nos.: 07.05.Pj, 07.60.Dq, 07.60.Rd, 07.87, 94.10.Dy, 94.10.Fa, 94.10.Gb, 94.10.Rk

In order to drive atmospheric models performing forecasts and analyses of air quality and atmospheric composition, an accurate quantification of surface emissions from anthropogenic and natural sources is required. As part of the European Copernicus Atmosphere Service (CAMS), diverse emission datasets have been developed. Global and regional European anthropogenic emissions for several sectors for a large number of atmospheric compounds have been developed. In addition, detailed emissions from ships based on ship identification systems have been developed. Different datasets providing natural emissions are being processed, such as the emissions of biogenic volatile organic compounds from vegetation, nitrogen compounds emissions from soils, emissions from the oceans and emissions from volcanoes. Methodologies for evaluating the emissions and their consistency at different scales are being generated. Temporal profiles at different scales are also being developed.All the emissions developed in CAMS are available from the ECCAD (Emissions of atmospheric Compounds and Compilation of Ancillary Data (eccad.aeris-data.fr) database.

Abstract. 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 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 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. 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.