ALBERT

Description: 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.

Description: The goal of the Tropospheric Ozone Assessment Report (TOAR) is to provide the research community with an up-to-date scientific assessment of tropospheric ozone, from the surface to the tropopause. While a suite of observations provides significant information on the spatial and temporal distribution of tropospheric ozone, observational gaps make it necessary to use global atmospheric chemistry models to synthesize our understanding of the processes and variables that control tropospheric ozone abundance and its variability. Models facilitate the interpretation of the observations and allow us to make projections of future tropospheric ozone and trace gas distributions for different anthropogenic or natural perturbations. This paper assesses the skill of current-generation global atmospheric chemistry models in simulating the observed present-day tropospheric ozone distribution, variability, and trends. Drawing upon the results of recent international multi-model intercomparisons and using a range of model evaluation techniques, we demonstrate that global chemistry models are broadly skillful in capturing the spatio-temporal variations of tropospheric ozone over the seasonal cycle, for extreme pollution episodes, and changes over interannual to decadal periods. However, models are consistently biased high in the northern hemisphere and biased low in the southern hemisphere, throughout the depth of the troposphere, and are unable to replicate particular metrics that define the longer term trends in tropospheric ozone as derived from some background sites. When the models compare unfavorably against observations, we discuss the potential causes of model biases and propose directions for future developments, including improved evaluations that may be able to better diagnose the root cause of the model-observation disparity. Overall, model results should be approached critically, including determining whether the model performance is acceptable for the problem being addressed, whether biases can be tolerated or corrected, whether the model is appropriately constituted, and whether there is a way to satisfactorily quantify the uncertainty.

Description: Despite the developments in the global modelling of chemistry and of the parameterization of the physical processes, carbon monoxide (CO) concentrations remain underestimated during Northern Hemisphere (NH) winter by most state-of-the-art chemistry transport models. The consequential model bias can in principle originate from either an underestimation of CO sources or an overestimation of its sinks. We address both the role of surface sources and sinks with a series of MOZART (Model for Ozone And Related Tracers) model sensitivity studies for the year 2008 and compare our results to observational data from ground-based stations, satellite observations, and vertical profiles from measurements on passenger aircraft. In our base case simulation using MACCity (Monitoring Atmospheric Composition and Climate project) anthropogenic emissions, the near-surface CO mixing ratios are underestimated in the Northern Hemisphere by more than 20 ppb from December to April, with the largest bias of up to 75 ppb over Europe in January. An increase in global biomass burning or biogenic emissions of CO or volatile organic compounds (VOCs) is not able to reduce the annual course of the model bias and yields concentrations over the Southern Hemisphere which are too high. Raising global annual anthropogenic emissions with a simple scaling factor results in overestimations of surface mixing ratios in most regions all year round. Instead, our results indicate that anthropogenic CO and, possibly, VOC emissions in the MACCity inventory are too low for the industrialized countries only during winter and spring. Reasonable agreement with observations can only be achieved if the CO emissions are adjusted seasonally with regionally varying scaling factors. A part of the model bias could also be eliminated by exchanging the original resistance-type dry deposition scheme with a parameterization for CO uptake by oxidation from soil bacteria and microbes, which reduces the boreal winter dry deposition fluxes. The best match to surface observations, satellite retrievals, and aircraft observations was achieved when the modified dry deposition scheme was combined with increased wintertime road traffic emissions over Europe and North America (factors up to 4.5 and 2, respectively). One reason for the apparent underestimation of emissions may be an exaggerated downward trend in the Representative Concentration Pathway (RCP) 8.5 scenario in these regions between 2000 and 2010, as this scenario was used to extrapolate the MACCity emissions from their base year 2000. This factor is potentially amplified by a lack of knowledge about the seasonality of emissions. A methane lifetime of 9.7 yr for our basic model and 9.8 yr for the optimized simulation agrees well with current estimates of global OH, but we cannot fully exclude a potential effect from errors in the geographical and seasonal distribution of OH concentrations on the modelled CO.

Description: The uncertainties in the global budget of carbon monoxide (CO) are assessed to explain causes for the long-standing issue of Northern Hemispheric wintertime underestimation of CO concentrations in global models. With a series of MOZART sensitivity simulations for the year 2008, the impacts from changing a variety of surface sources and sinks were analyzed. The model results were evaluated with monthly averages of surface station observations from the global CO monitoring network as well as with total columns observed from satellites and with vertical profiles from measurements on passenger aircraft. Our basic simulation using MACCity anthropogenic emissions underestimated Northern Hemispheric near-surface CO concentrations on average by more than 20 ppb from December to April with the largest bias over Europe of up to 75 ppb in January. An increase in global biomass burning or biogenic emissions of CO or volatile organic compounds (VOC) is not able to reduce the annual course of the model bias and yields too high concentrations over the Southern Hemisphere. Raising global annual anthropogenic emissions results in overestimations of surface concentrations in most regions all-year-round. Instead, our results indicate that anthropogenic emissions in the MACCity inventory are too low for the industrialized countries during winter and spring. Thus we found it necessary to adjust emissions seasonally with regionally varying scaling factors. Moreover, exchanging the original resistance-type dry deposition scheme with a parameterization for CO uptake by oxidation from soil bacteria and microbes reduced the boreal winter dry deposition fluxes and could partly correct for the model bias. When combining the modified dry deposition scheme with increased wintertime road traffic emissions over Europe and North America (factors up to 4.5 and 2, respectively) we were able to optimize the match to surface observations and to reduce the model bias significantly with respect to the satellite and aircraft observations. A reason for the apparent underestimation of emissions may be an exaggerated downward trend in the RCP8.5 scenario in these regions between 2000 and 2010, as this scenario was used to extrapolate the MACCity emissions from their base year 2000. This factor is potentially amplified by a lack of knowledge about the seasonality of emissions. A methane lifetime of 9.7 yr for our basic model and 9.8 yr for the optimized simulation agrees well with current estimates of global OH, but we cannot exclude a potential effect from errors in the geographical and seasonal distribution of OH concentrations. Finally, underestimated emissions from anthropogenic VOCs can also account for a small part of the missing CO concentrations.

Description: Daily global analyses and 5 day forecasts are generated in the context of the European Monitoring Atmospheric Composition and Climate (MACC) project using an extended version of the Integrated Forecasting System (IFS) of the European Centre for Medium-Range Weather Forecasts (ECMWF). IFS now includes modules for chemistry, deposition and emission of reactive gases, aerosols, and greenhouse gases, and the 4-dimensional variational data assimilation scheme makes use of multiple satellite observations of atmospheric composition in addition to meteorological observations. This paper describes the data assimilation setup of the new Composition-IFS (C-IFS) with respect to reactive gases and validates analysis fields of ozone (O3), carbon monoxide (CO), and nitrogen dioxide (NO2) for the year 2008 against independent observations and a control run without data assimilation. The largest improvement in CO by assimilation of MOPITT CO columns is seen in the lower troposphere of the Northern Hemisphere (NH) Extratropics during winter, and during the South African biomass burning season. The assimilation of several O3 total column and stratospheric profile retrievals greatly improves the total column, stratospheric and upper tropospheric O3 analysis fields relative to the control run. The impact on lower tropospheric ozone, which comes from the residual of the total column and stratospheric profile O3 data, is smaller, but nevertheless there is some improvement particularly in the NH during winter and spring. The impact of the assimilation of OMI tropospheric NO2 columns is small because of the short lifetime of NO2, suggesting that NO2 observations would be better used to adjust emissions instead of initial conditions. The results further indicate that the quality of the tropospheric analyses and of the stratospheric ozone analysis obtained with the C-IFS system has improved compared to the previous "coupled" model system of MACC.

Description: A representation of atmospheric chemistry has been included in the Integrated Forecasting System (IFS) of the European Centre for Medium-range Weather Forecasts (ECMWF). The new chemistry modules complement the aerosol modules of the IFS for atmospheric composition, which is named C-IFS. C-IFS for chemistry supersedes a coupled system, in which the Chemical Transport Model (CTM) Model for OZone and Related chemical Tracers 3 was two-way coupled to the IFS (IFS-MOZART). This paper contains a description of the new on-line implementation, an evaluation with observations and a comparison of the performance of C-IFS with MOZART and with a re-analysis of atmospheric composition produced by IFS-MOZART within the Monitoring Atmospheric Composition and Climate (MACC) project. The chemical mechanism of C-IFS is an extended version of the Carbon Bond 2005 (CB05) chemical mechanism as implemented in the CTM Transport Model 5 (TM5). CB05 describes tropospheric chemistry with 54 species and 126 reactions. Wet deposition and lightning nitrogen monoxide (NO) emissions are modelled in C-IFS using the detailed input of the IFS physics package. A one-year simulation by C-IFS, MOZART and the MACC re-analysis is evaluated against ozonesondes, carbon monoxide (CO) aircraft profiles, European surface observations of ozone (O3), CO, sulphur dioxide (SO2) and nitrogen dioxide (NO2) as well as satellite retrievals of CO, tropospheric NO2 and formaldehyde. Anthropogenic emissions from the MACC/CityZen (MACCity) inventory and biomass burning emissions from the Global Fire Assimilation System (GFAS) data set were used in the simulations by both C-IFS and MOZART. C-IFS (CB05) showed an improved performance with respect to MOZART for CO, upper tropospheric O3, winter time SO2 and was of a similar accuracy for other evaluated species. C-IFS (CB05) is about ten times more computationally efficient than IFS-MOZART.

Description: The European MACC (Monitoring Atmospheric Composition and Climate) project is preparing the operational Copernicus Atmosphere Monitoring Service (CAMS), one of the services of the European Copernicus Programme on Earth observation and environmental services. MACC uses data assimilation to combine in situ and remote sensing observations with global and regional models of atmospheric reactive gases, aerosols, and greenhouse gases, and is based on the Integrated Forecasting System of the European Centre for Medium-Range Weather Forecasts (ECMWF). The global component of the MACC service has a dedicated validation activity to document the quality of the atmospheric composition products. In this paper we discuss the approach to validation that has been developed over the past 3 years. Topics discussed are the validation requirements, the operational aspects, the measurement data sets used, the structure of the validation reports, the models and assimilation systems validated, the procedure to introduce new upgrades, and the scoring methods. One specific target of the MACC system concerns forecasting special events with high-pollution concentrations. Such events receive extra attention in the validation process. Finally, a summary is provided of the results from the validation of the latest set of daily global analysis and forecast products from the MACC system reported in November 2014.

Description: A representation of atmospheric chemistry has been included in the Integrated Forecasting System (IFS) of the European Centre for Medium-Range Weather Forecasts (ECMWF). The new chemistry modules complement the aerosol modules of the IFS for atmospheric composition, which is named C-IFS. C-IFS for chemistry supersedes a coupled system in which chemical transport model (CTM) Model for OZone and Related chemical Tracers 3 was two-way coupled to the IFS (IFS-MOZART). This paper contains a description of the new on-line implementation, an evaluation with observations and a comparison of the performance of C-IFS with MOZART and with a re-analysis of atmospheric composition produced by IFS-MOZART within the Monitoring Atmospheric Composition and Climate (MACC) project. The chemical mechanism of C-IFS is an extended version of the Carbon Bond 2005 (CB05) chemical mechanism as implemented in CTM Transport Model 5 (TM5). CB05 describes tropospheric chemistry with 54 species and 126 reactions. Wet deposition and lightning nitrogen monoxide (NO) emissions are modelled in C-IFS using the detailed input of the IFS physics package. A 1 year simulation by C-IFS, MOZART and the MACC re-analysis is evaluated against ozonesondes, carbon monoxide (CO) aircraft profiles, European surface observations of ozone (O3), CO, sulfur dioxide (SO2) and nitrogen dioxide (NO2) as well as satellite retrievals of CO, tropospheric NO2 and formaldehyde. Anthropogenic emissions from the MACC/CityZen (MACCity) inventory and biomass burning emissions from the Global Fire Assimilation System (GFAS) data set were used in the simulations by both C-IFS and MOZART. C-IFS (CB05) showed an improved performance with respect to MOZART for CO, upper tropospheric O3, and wintertime SO2, and was of a similar accuracy for other evaluated species. C-IFS (CB05) is about 10 times more computationally efficient than IFS-MOZART.

Description: The European MACC (Monitoring Atmospheric Composition and Climate) project is preparing the operational Copernicus Atmosphere Monitoring Service (CAMS), one of the services of the European Copernicus Programme on Earth observation and environmental services. MACC uses data assimilation to combine in-situ and remote sensing observations with global and regional models of atmospheric reactive gases, aerosols and greenhouse gases, and is based on the Integrated Forecast System of the ECMWF. The global component of the MACC service has a dedicated validation activity to document the quality of the atmospheric composition products. In this paper we discuss the approach to validation that has been developed over the past three years. Topics discussed are the validation requirements, the operational aspects, the measurement data sets used, the structure of the validation reports, the models and assimilation systems validated, the procedure to introduce new upgrades, and the scoring methods. One specific target of the MACC system concerns forecasting special events with high pollution concentrations. Such events receive extra attention in the validation process. Finally, a summary is provided of the results from the validation of the latest set of daily global analysis and forecast products from the MACC system reported in November 2014.