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: We examine the response of Arctic gas and aerosol concentrations to perturbations in pollutant emissions from Europe, East and South Asia, and North America using results from a coordinated model intercomparison. These sensitivities to regional emissions (mixing ratio change per unit emission) vary widely across models and species. Intermodel differences are systematic, however, so that the relative importance of different regions is robust. North America contributes the most to Arctic ozone pollution. For aerosols and CO, European emissions dominate at the Arctic surface but Asian emissions become progressively more important with altitude, and are dominant in the upper troposphere. Sensitivities show strong seasonality: surface sensitivities typically maximize during boreal winter for European and during spring for East Asian and North American emissions. Mid-tropospheric sensitivities, however, nearly always maximize during spring or summer for all regions. Deposition of black carbon (BC) onto Greenland is most sensitive to North American emissions. North America and Europe each contribute ~40% of total BC deposition to Greenland, with ~20% from East Asia. Elsewhere in the Arctic, both sensitivity and total BC deposition are dominated by European emissions. Model diversity for aerosols is especially large, resulting primarily from differences in aerosol physics and removal. Comparison of aerosols with observations indicates problems in either the models or interpretation of the measurements. For gas phase pollutants such as CO and O3, which are relatively well-simulated, the processes contributing most to uncertainties depend on the source region. Uncertainties in the Arctic surface CO response to emissions perturbations are dominated by emissions for East Asian sources, while uncertainties in transport, emissions, and oxidation are comparable for European and North American sources. At higher levels, model-to-model variations in transport and oxidation are most important. Differences in photochemistry appear to play the largest role in the intermodel variations in Arctic ozone sensitivity.

Description: Within ACCENT, a European Network of Excellence, eighteen atmospheric models from the U.S., Europe, and Japan calculated present (2000) and future (2030) concentrations of ozone at the Earth's surface with hourly temporal resolution. Comparison of model results with surface ozone measurements in 14 world regions indicates that levels and seasonality of surface ozone in North America and Europe are characterized well by global models, with annual average biases typically within 5–10 nmol/mol. However, comparison with rather sparse observations over some regions suggest that most models overestimate annual ozone by 15–20 nmol/mol in some locations. Two scenarios from the International Institute for Applied Systems Analysis (IIASA) and one from the Intergovernmental Panel on Climate Change Special Report on Emissions Scenarios (IPCC SRES) have been implemented in the models. This study focuses on changes in near-surface ozone and their effects on human health and vegetation. Different indices and air quality standards are used to characterise air quality. We show that often the calculated changes in the different indices are closely inter-related. Indices using lower thresholds are more consistent between the models, and are recommended for global model analysis. Our analysis indicates that currently about two-thirds of the regions considered do not meet health air quality standards, whereas only 2–4 regions remain below the threshold. Calculated air quality exceedances show moderate deterioration by 2030 if current emissions legislation is followed and slight improvements if current emissions reduction technology is used optimally. For the "business as usual" scenario severe air quality problems are predicted. We show that model simulations of air quality indices are particularly sensitive to how well ozone is represented, and improved accuracy is needed for future projections. Additional measurements are needed to allow a more quantitative assessment of the risks to human health and vegetation from changing levels of surface ozone.

Description: The transport of tracers in the general circulation model ECHAM5 is analysed using 9 independent idealized tracers with constant lifetimes released in different altitude regions of the atmosphere. The source regions were split into the tropics, Northern and Southern Hemisphere. The dependency of tracer transport on model resolution is tested in the resolutions T21L19, T42L19, T42L31, T63L31 and T106L31, by employing tracers with a globally uniform lifetime of 5 months. Each of the experiments uses prescribed sea surface temperatures and sea ice fields of the 1990s. The influence of meteorology and tracer lifetimes were tested by performing additional experiments in the T63L31 resolution, by nudging ECHAM5 towards the European Centre for Medium Range Weather Forecast 40 years re-analysis data (ERA40), and by using tracer lifetimes of 0.5 and 50 months, respectively. The transport of tracers is faster in the finer resolution models and is mostly dependent on the number of vertical levels. We found a decrease in the inter-hemispheric transport of tracers with source region at the surface or the tropopause in the coarse resolution models due to increasing recirculation within the source region and vertical mixing. However, a coarse model resolution leads to enhanced inter-hemispheric transport in the stratosphere. The use of ERA40 data only slightly affects the inter-hemispheric transport of surface and tropopause tracers, whereas it increases the inter-hemispheric and vertical transport in the stratosphere by up to 100% and by a factor of 2.5, respectively. The inter-hemispheric transport time was deduced from simulations with tracers of infinite lifetime and source regions at the surface in the Northern and Southern Hemisphere. Again, the transport was found to be faster for models with higher vertical resolution. We find inter-hemispheric transport times of about 7 to 9 months which are lower than the values reported in the literature, based for example on 85Kr observations.

Description: An ozone climatology based on ozone soundings for the last 15 years has been constructed for model evaluation and comparisons to other observations. Vertical ozone profiles for 41 stations around the globe have been compiled and averaged for the years 1980–1994 and 1995–2009. The climatology provides information about the median and the width of the ozone probability distribution function, as well as interannual variability of ozone between 1995 and 2009, in pressure and tropopause-referenced altitudes. In addition to single stations, regional aggregates are presented, combining stations with similar ozone characteristics. The Hellinger distance is introduced as a new diagnostic to compare the variability of ozone distributions within each region and used for model evaluation purposes. This measure compares not only the mean, but also the shape of distributions. The representativeness of regional aggregates is discussed using independent observations from surface stations and MOZAIC aircraft data. Ozone from all of these data sets show an excellent agreement within the range of the interannual variability, especially if a sufficient number of measurements are available, as is the case for West Europe. Within the climatology, a significant longitudinal variability of ozone in the troposphere and lower stratosphere in the northern mid- and high latitudes is found. The climatology is used to evaluate results from two model intercomparison activities, HTAP for the troposphere and CCMVal2 for the tropopause region and the stratosphere. HTAP ozone is in good agreement with observations in the troposphere within their range of uncertainty, but ozone peaks too early in the Northern Hemisphere spring. The strong gradients of ozone around the tropopause are less well captured by many models. Lower stratospheric ozone is overestimated for all regions by the multi-model mean of CCMVal2 models. Individual models also show major shortcomings in reproducing the shape of ozone probability distribution functions in various regions and different altitudes, which might have significant implications for the radiative budgets in those models.

Description: Understanding historical trends of trace gas and aerosol distributions in the troposphere is essential to evaluate the efficiency of existing strategies to reduce air pollution and to design more efficient future air quality and climate policies. We performed coupled photochemistry and aerosol microphysics simulations for the period 1980–2005 using the aerosol-chemistry-climate model ECHAM5-HAMMOZ, to assess our understanding of long-term changes and inter-annual variability of the chemical composition of the troposphere, and in particular of ozone and sulfate concentrations, for which long-term surface observations are available. In order to separate the impact of the anthropogenic emissions and natural variability on atmospheric chemistry, we compare two model experiments, driven by the same ECMWF re-analysis data, but with varying and constant anthropogenic emissions, respectively. Our model analysis indicates an increase of ca. 1 ppbv (0.055 ± 0.002 ppbv yr−1) in global average surface O3 concentrations due to anthropogenic emissions, but this trend is largely masked by the larger O3 anomalies due to the variability of meteorology and natural emissions. The changes in meteorology (not including stratospheric variations) and natural emissions account for the 75 % of the total variability of global average surface O3 concentrations. Regionally, annual mean surface O3 concentrations increased by 1.3 and 1.6 ppbv over Europe and North America, respectively, despite the large anthropogenic emission reductions between 1980 and 2005. A comparison of winter and summer O3 trends with measurements shows a qualitative agreement, except in North America, where our model erroneously computed a positive trend. Simulated O3 increases of more than 4 ppbv in East Asia and 5 ppbv in South Asia can not be corroborated with long-term observations. Global average sulfate surface concentrations are largely controlled by anthropogenic emissions. Globally natural emissions are an important driver determining AOD variations. Regionally, AOD decreased by 28 % over Europe, while it increased by 19 % and 26 % in East and South Asia. The global radiative perturbation calculated in our model for the period 1980–2005 was rather small (0.05 W m−2 for O3 and 0.02 W m−2 for total aerosol direct effect), but larger perturbations ranging from −0.54 to 1.26 W m−2 are estimated in those regions where anthropogenic emissions largely varied.

Description: The 2008 Antarctic ozone hole was one of the largest and most long-lived in recent years. Predictions of the ozone hole were made in near-real time (NRT) and hindcast mode with the Integrated Forecast System (IFS) of the European Centre for Medium-Range Weather Forecasts (ECMWF). The forecasts were carried out both with and without assimilation of satellite observations from multiple instruments to provide more realistic initial conditions. Three different chemistry schemes were applied for the description of stratospheric ozone chemistry: (i) a linearization of the ozone chemistry, (ii) the stratospheric chemical mechanism of the Model of Ozone and Related Chemical Tracers, version 3, (MOZART-3) and (iii) the relaxation to climatology as implemented in the Transport Model, version 5, (TM5). The IFS uses the latter two schemes by means of a two-way coupled system. Without assimilation, the forecasts showed model-specific shortcomings in predicting start time, extent and duration of the ozone hole. The assimilation of satellite observations from the Microwave Limb Sounder (MLS), the Ozone Monitoring Instrument (OMI), the Solar Backscattering Ultraviolet radiometer (SBUV-2) and the SCanning Imaging Absorption spectroMeter for Atmospheric CartograpHY (SCIAMACHY) led to a significant improvement of the forecasts when compared with total columns and vertical profiles from ozone sondes. The combined assimilation of observations from multiple instruments helped to overcome limitations of the ultraviolet (UV) sensors at low solar elevation over Antarctica. The assimilation of data from MLS was crucial to obtain a good agreement with the observed ozone profiles both in the polar stratosphere and troposphere. The ozone analyses by the three model configurations were very similar despite the different underlying chemistry schemes. Using ozone analyses as initial conditions had a very beneficial but variable effect on the predictability of the ozone hole over 15 days. The initialized forecasts with the MOZART-3 chemistry produced the best predictions of the increasing ozone hole whereas the linear scheme showed the best results during the ozonehole closure.