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.

Ozone pollution in eastern China has become one of the top environmental issues. Quantifying the temporal trend of surface ozone helps to assess the impacts of the anthropogenic precursor reductions and the likely effects of emission control strategies implemented. In this paper, ozone data collected at the Shangdianzi (SDZ) regional atmospheric background station from 2003 to 2015 are presented and analyzed to obtain the variation in the trend of surface ozone in the most polluted region of China, north of eastern China or the North China Plain. A modified Kolmogorov–Zurbenko (KZ) filter method was performed on the maximum daily average 8 h (MDA8) concentrations of ozone to separate the contributions of different factors from the variation of surface ozone and remove the influence of meteorological fluctuations on surface ozone. Results reveal that the short-term, seasonal and long-term components of ozone account for 36.4, 57.6 and 2.2 % of the total variance, respectively. The long-term trend indicates that the MDA8 has undergone a significant increase in the period of 2003–2015, with an average rate of 1.13 ± 0.01 ppb year⁻¹ (R² = 0.92). It is found that meteorological factors did not significantly influence the long-term variation of ozone and the increase may be completely attributed to changes in emissions. Furthermore, there is no significant correlation between the long-term O₃ and NO₂ trends. This study suggests that emission changes in VOCs might have played a more important role in the observed increase of surface ozone at SDZ.

Regional ozone pollution has become one of the top environmental concerns in China, especially in those economically vibrant and densely populated regions, such as North China region including Beijing. To address this issue, surface ozone and ancillary data over the period 2004–2006 from the Shangdianzi Regional Background Station in north China were analyzed. Due to the suitable location and valley topography of the site, transport of pollutants from the North China Plain was easily observed and quantified according to surface wind directions. Regional (polluted) and background (clean) ozone concentrations were obtained by detailed statistic analysis. Contribution of pollutants from North China Plain to surface ozone at SDZ was estimated by comparing ozone concentrations observed under SW wind conditions and that under NE wind conditions. The average daily accumulated ozone contribution was estimated to be 240 ppb·hr. The average regional contributions to surface ozone at SDZ from the North China Plain were 21.8 ppb for the whole year, and 19.2, 28.9, 25.0, and 10.0 ppb for spring, summer, autumn, and winter, respectively. The strong ozone contribution in summer led to disappearance of the spring ozone maximum phenomenon at SDZ under winds other than from the NNW to E sectors. The emissions of nitrogen oxide in the North China plain cause a decrease in ozone concentrations in winter.

Tropospheric ozone is an important atmospheric oxidant, greenhouse gas and atmospheric pollutant at the same time. The oxidation capacity of the atmosphere, climate, human and vegetation health can be impacted by the increase of the ozone level. Therefore, long-term determination of trends of baseline ozone is highly needed information for environmental and climate change assessment. So far, studies on the long-term trends of ozone at representative sites are mainly available for European and North American sites. Similar studies are lacking for China and many other developing countries. Measurements of surface ozone were carried out at a baseline Global Atmospheric Watch (GAW) station in the north-eastern Tibetan Plateau region (Mt Waliguan, 36°17′ N, 100°54′ E, 3816 m a.s.l.) for the period of 1994 to 2013. To uncover the variation characteristics, long-term trends and influencing factors of surface ozone at this remote site in western China, a two-part study has been carried out, with this part focusing on the overall characteristics of diurnal, seasonal and long-term variations and the trends of surface ozone. To obtain reliable ozone trends, we performed the Mann–Kendall trend test and the Hilbert–Huang transform (HHT) analysis on the ozone data. Our results confirm that the mountain-valley breeze plays an important role in the diurnal cycle of surface ozone at Waliguan, resulting in higher ozone values during the night and lower ones during the day, as was previously reported. Systematic diurnal and seasonal variations were found in mountain-valley breezes at the site, which were used in defining season-dependent daytime and nighttime periods for trend calculations. Significant positive trends in surface ozone were detected for both daytime (0.24 ± 0.16 ppbv year⁻¹) and nighttime (0.28 ± 0.17 ppbv year⁻¹). The largest nighttime increasing rate occurred in autumn (0.29 ± 0.11 ppbv year⁻¹), followed by spring (0.24 ± 0.12 ppbv year⁻¹), summer (0.22 ± 0.20 ppbv year⁻¹) and winter (0.13 ± 0.10 ppbv year⁻¹), respectively. The HHT spectral analysis identified four different stages with different positive trends, with the largest increase occurring around May 2000 and October 2010. The HHT results suggest that there were 2–4a, 7a and 11a periodicities in the time series of surface ozone at Waliguan. The results of this study can be used for assessments of climate and environment change and in the validation of chemistry–climate models.

The real-time measurements of NH₃ and trace gases were conducted, in conjunction with semi-continuous measurements of water-soluble ions in PM_2.5 at a rural site in the North China Plain (NCP) from May to September 2013 in order to better understand chemical characteristics of ammonia and the impact of secondary ammonium aerosols on formation in the NCP. Extremely high NH₃ and NH₄⁺ concentrations were observed after a precipitation event within 7–10 days following urea application. Elevated NH₃ levels coincided with elevated NH₄⁺, indicating that NH₃ likely influenced particulate ammonium mass. For the sampling period, the average conversion ∕ oxidation ratios for NH₄⁺ (NHR), SO₄²⁻ (SOR), and NO₃⁻ (NOR) were estimated to be 0.30, 0.64, and 0.24, respectively. The increased NH₃ concentrations, mainly from agricultural activities and regional transport, coincided with the prevailing meteorological conditions. The high NH₃ level with NHR of about 0.30 indicates that the emission of NH₃ in the NCP is much higher than needed for aerosol acid neutralisation, and NH₃ plays an important role in the formation of secondary aerosols as a key neutraliser. The hourly data obtained were used to investigate gas–aerosol partitioning characteristics using the thermodynamic equilibrium model ISORROPIA-II. Modelled SO₄²⁻, NO₃⁻, and NH₃ values agree well with the measurements, while the modelled NH₄⁺ values largely underestimate the measurements. Our observation and modelling results indicate that strong acids in aerosol are completely neutralised. Additional NH₄⁺ exists in aerosol, probably a result of the presence of a substantial amount of oxalic and other diacids.

China is facing a severe ozone problem, but the origin of its ozone remains unclear. Here we use a GEOS-Chem based global–regional two-way coupled model system to quantify the individual contributions of eight emission source regions worldwide to springtime ozone in 2008 over China. The model reproduces the observed ozone from 31 ground sites and various aircraft and ozonesonde measurements in China and nearby countries, with a mean bias of 10 %–15 % both near the surface and in the troposphere. We then combine zero-out simulations, tagged ozone simulations, and a linear weighting approach to account for the effect of nonlinear chemistry on ozone source attribution. We find considerable contributions of total foreign anthropogenic emissions to surface ozone over China (2–11 ppb). For ozone of anthropogenic origin averaged over China, foreign regions together contribute 40 %–60 % below the height of 2 km and 85 % in the upper troposphere. For total ozone contributed by foreign anthropogenic emissions over China at various heights, the portion of transboundary ozone produced within foreign emission source regions is less than 50 %, with the rest produced by precursors transported out of those source regions. Japan and Korea contribute 0.6–2.1 ppb of surface ozone over the east coastal regions. Southeast Asia contributes 1–5 ppb over much of southern China and South Asia contributes up to 5–10 ppb of surface ozone over the border of southwestern China; and their contributions increase with height due to strong upwelling over the source regions. The European contribution reaches 2.1–3.0 ppb for surface ozone over the northern border of China and 1.5 ppb in the lower troposphere averaged over China. North America contributes 0.9–2.7 ppb of surface ozone over most of China (1.5–2.1 ppb over the North China Plain), with a China average at 1.5–2.5 ppb at different heights below 8 km, due to its large anthropogenic emissions and the transport-favorable midlatitude westerly wind. In addition to domestic emission control, global emission reduction is critical for China's ozone mitigation.