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.

Changes in baseline (here understood as representative of continental to hemispheric scales) tropospheric O₃ concentrations that have occurred at northern mid-latitudes over the past six decades are quantified from available measurement records with the goal of providing benchmarks to which retrospective model calculations of the global O₃ distribution can be compared. Eleven data sets (ten ground-based and one airborne) including six European (beginning in the 1950's and before), three North American (beginning in 1984) and two Asian (beginning in 1991) are analyzed. When the full time periods of the data records are considered a consistent picture emerges; O₃ has increased at all sites in all seasons at approximately 1% yr^−1 relative to the site's 2000 yr mixing ratio in each season. For perspective, this rate of increase sustained from 1950 to 2000 corresponds to an approximate doubling. There is little if any evidence for statistically significant differences in average rates of increase among the sites, regardless of varying length of data records. At most sites (most definitively at the European sites) the rate of increase has slowed over the last decade (possibly longer), to the extent that at present O₃ is decreasing at some sites in some seasons, particularly in summer. The average rate of increase before 2000 shows significant seasonal differences (1.08 ± 0.09, 0.89 ± 0.10, 0.85 ± 0.11 and 1.21 ± 0.12% yr^−1 in spring, summer, autumn and winter, respectively, over North America and Europe)

[1] We used laser-induced fluorescence to measure the concentrations of OH and HO 2 radicals in central Tokyo during two intensive campaigns (IMPACT IVand IMPACT L) in January-February and July-August 2004. The estimated detection limit for the 10-min data was 1.3 Â 10 5 cm À3 for the nighttime and 5.2 Â 10 5 cm À3 for the daytime. The median values of the daytime peak concentrations of HO 2 were 1.1 and 5.7 pptv for the winter and summer periods, respectively, while the values for OH were 1.5 Â 10 6 and 6.3 Â 10 6 cm À3 . High HO 2 mixing ratios (>50 pptv) were observed on a day in summer when O 3 mixing ratios exceeded 100 ppbv. The average nighttime concentrations of HO 2 were 0.7 and 2.6 pptv for the winter and summer periods, respectively, while the values for OH were 1.8 Â 10 5 and 3.7 Â 10 5 cm À3 . A photochemical box model constrained by ancillary observations was able to reproduce daytime OH concentrations reasonably well for both periods, although daytime HO 2 concentrations were underestimated in winter and overestimated in summer. Increasing the wintertime hydrocarbon concentrations in the model led to an increase in daytime HO 2 concentrations, thereby showing better agreement with observations; however, the model continued to underestimate HO 2 concentrations at high NO mixing ratios. This underestimate was most pronounced in the mornings of both periods and during the daytime in winter. We studied processes that are capable of explaining this discrepancy, including unknown reactions of HNO 4 or an unidentified HO x source that is linearly scalable to the NO mixing ratio. The important processes in terms of producing radicals were the olefin + O 3 reactions in the nighttime of both periods and during the daytime in winter, the photolysis of carbonyls in the daytime for both periods, and the photolysis of HONO during the daytime in winter (using measured HONO concentrations) and during mornings in summer (using estimated HONO concentrations).

Two recent papers have quantified long-term ozone (O 3 ) changes observed at northern midlatitude sites that are believed to represent baseline (here understood as representative of continental to hemispheric scales) conditions. Three chemistry-climate models (NCAR CAM-chem, GFDL-CM3, and GISS-E2-R) have calculated retrospective tropospheric O 3 concentrations as part of the Atmospheric Chemistry and Climate Model Intercomparison Project and Coupled Model Intercomparison Project Phase 5 model intercomparisons. We present an approach for quantitative comparisons of model results with measurements for seasonally averaged O 3 concentrations. There is considerable qualitative agreement between the measurements and the models, but there are also substantial and consistent quantitative disagreements. Most notably, models (1) overestimate absolute O 3 mixing ratios, on average by~5 to 17 ppbv in the year 2000, (2) capture only~50% of O 3 changes observed over the past five to six decades, and little of observed seasonal differences, and (3) capture~25 to 45% of the rate of change of the long-term changes. These disagreements are significant enough to indicate that only limited confidence can be placed on estimates of present-day radiative forcing of tropospheric O 3 derived from modeled historic concentration changes and on predicted future O 3 concentrations. Evidently our understanding of tropospheric O 3 , or the incorporation of chemistry and transport processes into current chemical climate models, is incomplete. Modeled O 3 trends approximately parallel estimated trends in anthropogenic emissions of NO x , an important O 3 precursor, while measured O 3 changes increase more rapidly than these emission estimates.

In support of the first Tropospheric Ozone Assessment Report (TOAR) a relational database of global surface ozone observations has been developed and populated with hourly measurement data and enhanced metadata. A comprehensive suite of ozone data products including standard statistics, health and vegetation impact metrics, and trend information, are made available through a common data portal and a web interface. These data form the basis of the TOAR analyses focusing on human health, vegetation, and climate relevant ozone issues, which are part of this special feature.Cooperation among many data centers and individual researchers worldwide made it possible to build the world's largest collection of in-situ hourly surface ozone data covering the period from 1970 to 2015. By combining the data from almost 10,000 measurement sites around the world with global metadata information, new analyses of surface ozone have become possible, such as the first globally consistent characterisations of measurement sites as either urban or rural/remote. Exploitation of these global metadata allows for new insights into the global distribution, and seasonal and long-term changes of tropospheric ozone and they enable TOAR to perform the first, globally consistent analysis of present-day ozone concentrations and recent ozone changes with relevance to health, agriculture, and climate.Considerable effort was made to harmonize and synthesize data formats and metadata information from various networks and individual data submissions. Extensive quality control was applied to identify questionable and erroneous data, including changes in apparent instrument offsets or calibrations. Such data were excluded from TOAR data products. Limitations of a posteriori data quality assurance are discussed. As a result of the work presented here, global coverage of surface ozone data for scientific analysis has been significantly extended. Yet, large gaps remain in the surface observation network both in Schultz et al: Tropospheric Ozone Assessment Report Art. 58, page 2 of 26 terms of regions without monitoring, and in terms of regions that have monitoring programs but no public access to the data archive. Therefore future improvements to the database will require not only improved data harmonization, but also expanded data sharing and increased monitoring in data-sparse regions.

[1] This article introduces an international regional experiment, East Asian Regional Experiment 2005 (EAREX 2005), carried out in March-April 2005 in the east Asian region, as one of the first phase regional experiments under the UNEP Atmospheric Brown Cloud (ABC) project, and discusses some outstanding features of aerosol characteristics and its direct radiative forcing in the east Asian region, with some comparison with the results obtained in another ABC early phase regional experiment, ABC Maldives Monsoon Experiment (APMEX) conducted in the south Asian region. Time series of aerosol optical thickness (AOT), single scattering albedo (SSA), aerosol extinction cross section profile and CO concentration shows that air pollutants and mineral dust were transported every 5 to 7 days in the EAREX region to produce SSA values at wavelength of 700 nm from 0.86 to 0.96 and large clear-sky shortwave forcing efficiency at 500 nm from 60 W m À2 to 90 W m À2 , though there are some unexplained inconsistencies depending on the evaluation method. The simulated whole-sky total forcing in the EAREX region is À1 to À2 W m À2 at TOA and À2 to À10 W m À2 at surface in March 2005 which is smaller in magnitude than in the APMEX region, mainly because of large cloud fraction in this region (0.70 at Gosan versus 0.51 at Hanimadhoo in the ISCCP total cloud fraction). We suggest there may be an underestimation of the forcing due to overestimation of the simulated cloudiness and aerosol scale height. On the other hand, the possible error in the simulated surface albedo may cause an overestimation of the magnitude of the forcing over the land area. We also propose simple formulae for shortwave radiative forcing to understand the role of aerosol parameters and surface condition to determine the aerosol forcing. Such simple formulae are useful to check the consistency among the observed quantities.

Abstract. The Community Earth System Model (CESM1) CAM4-chem has been used to perform the Chemistry Climate Model Initiative (CCMI) reference and sensitivity simulations. In this model, the Community Atmospheric Model version 4 (CAM4) is fully coupled to tropospheric and stratospheric chemistry. Details and specifics of each configuration, including new developments and improvements are described. CESM1 CAM4-chem is a low-top model that reaches up to approximately 40 km and uses a horizontal resolution of 1.9 • latitude and 2.5 • longitude. For the specified dynamics experiments, the model is nudged to ModernEra Retrospective Analysis for Research and Applications (MERRA) reanalysis. We summarize the performance of the three reference simulations suggested by CCMI, with a focus on the last 15 years of the simulation when most observations are available. Comparisons with selected data sets are employed to demonstrate the general performance of the model. We highlight new data sets that are suited for multimodel evaluation studies. Most important improvements of the model are the treatment of stratospheric aerosols and the corresponding adjustments for radiation and optics, the updated chemistry scheme including improved polar chemistry and stratospheric dynamics and improved dry deposition rates. These updates lead to a very good representation of tropospheric ozone within 20 % of values from available observations for most regions. In particular, the trend and magnitude of surface ozone is much improved compared to earlier versions of the model. Furthermore, stratospheric column ozone of the Southern Hemisphere in winter and spring is reasonably well represented. All experiments still underestimate CO most significantly in Northern Hemisphere spring and show a significant underestimation of hydrocarbons based on surface observations.

The Chemical Weather Forecast System (CFORS) is designed to aid in the design of field experiments and in the interpretation/postanalysis of observed data. The system integrates a regional chemical transport model with a multitracer, online system built within the Regional Atmospheric Modeling System (RAMS) mesoscale model. CFORS was deployed in forecast and postanalysis modes during the NASA Global Tropospheric Experiment (GTE)‐Transport and Chemical Evolution over the Pacific (TRACE‐P), International Global Atmospheric Chemistry project (IGAC)‐International Geosphere‐Biosphere Programme (IGBP) Asian Pacific Regional Aerosol Characterization Experiment (ACE‐Asia), and National Oceanic and Atmospheric Administration Intercontinental Transport and Chemical Transformation of Anthropogenic Pollution 2002 (ITCT 2K2) field studies. A description of the CFORS model system is presented. The model is used to help interpret the Variability of Maritime Aerosol Properties (VMAP) surface observation data. The CFORS model results help to explain the time variation of both anthropogenic pollutants (sulfate, black carbon, and CO) and natural constituents including radon and mineral dust. Time series and time‐height cross‐section analysis of gases and aerosols are presented to help identify key processes. Synoptic‐scale weather changes are found to play an important role in the continental‐scale transport of pollution in the springtime in East Asia. The complex vertical and horizontal structure of pollutants in these outflow events is also presented and discussed.