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This analysis provides an up‐to‐date assessment of long‐term (1990–2010) rural ozone trends using all available data in the western (12 sites) and eastern (41 sites) USA. Rather than focus solely on average ozone values or air quality standard violations, we consider the full range of ozone values, reporting trends for the 5th, 50th and 95th percentiles. Domestic ozone precursor emissions decreased strongly during 1990–2010. Accordingly 83%, 66% and 20% of summertime eastern U.S. sites experienced statistically significant ozone decreases in the 95th, 50th and 5th percentiles, respectively. During spring 43% of the eastern sites have statistically significant ozone decreases for the 95th percentile with no sites showing a significant increase. At the 50th percentile there is little overall change in the eastern U.S. In contrast, only 17% (2 sites) and 8% (1 site) of summertime western U.S. sites have statistically significant ozone decreases in the 95th and 50th percentiles, respectively. During spring no western site has a significant decrease, while 50% have a significant median increase. This dichotomy in U.S. ozone trends is discussed in terms of changing anthropogenic and biomass burning emissions. Consideration is given to the concept that increasing baseline ozone flowing into the western U.S. is counteracting ozone reductions due to domestic emission reductions. An update to the springtime free tropospheric ozone trend above western North America shows that ozone has increased significantly from 1995 to 2011 at the rate of 0.41 ± 0.27 ppbv yr−1. Finally, the ozone changes are examined in relation to regional temperature trends. Key Points Median ozone in the eastern US is decreasing in summer but unchanged in spring Half of the western US rural sites have increasing median ozone in spring Increasing western ozone is inconsistent with decreasing US precursor emissions

Quantification and attribution of long-term tropospheric ozone trends are critical for understanding the impact of human activity and climate change on atmospheric chemistry but are also challenged by the limited coverage of long-term ozone observations in the free troposphere where ozone has higher production efficiency and radiative potential compared to that at the surface. In this study, we examine observed tropospheric ozone trends, their attributions, and radiative impacts from 1995–2017 using aircraft observations from the In-service Aircraft for a Global Observing System database (IAGOS), ozonesondes, and a multi-decadal GEOS-Chem chemical model simulation. IAGOS observations above 11 regions in the Northern Hemisphere and 19 of 27 global ozonesonde sites have measured increases in tropospheric ozone (950–250 hPa) by 2.7 ± 1.7 and 1.9 ± 1.7 ppbv per decade on average, respectively, with particularly large increases in the lower troposphere (950–800 hPa) above East Asia, the Persian Gulf, India, northern South America, the Gulf of Guinea, and Malaysia/Indonesia by 2.8 to 10.6 ppbv per decade. The GEOS-Chem simulation driven by reanalysis meteorological fields and the most up-to-date year-specific anthropogenic emission inventory reproduces the overall pattern of observed tropospheric ozone trends, including the large ozone increases over the tropics of 2.1–2.9 ppbv per decade and above East Asia of 0.5–1.8 ppbv per decade and the weak tropospheric ozone trends above North America, Europe, and high latitudes in both hemispheres, but trends are underestimated compared to observations. GEOS-Chem estimates an increasing trend of 0.4 Tg yr−1 of the tropospheric ozone burden in 1995–2017. We suggest that uncertainties in the anthropogenic emission inventory in the early years of the simulation (e.g., 1995–1999) over developing regions may contribute to GEOS-Chem's underestimation of tropospheric ozone trends. GEOS-Chem sensitivity simulations show that changes in global anthropogenic emission patterns, including the equatorward redistribution of surface emissions and the rapid increases in aircraft emissions, are the dominant factors contributing to tropospheric ozone trends by 0.5 Tg yr−1. In particular, we highlight the disproportionately large, but previously underappreciated, contribution of aircraft emissions to tropospheric ozone trends by 0.3 Tg yr−1, mainly due to aircraft emitting NOx in the mid-troposphere and upper troposphere where ozone production efficiency is high. Decreases in lower-stratospheric ozone and the stratosphere–troposphere flux in 1995–2017 contribute to an ozone decrease at mid-latitudes and high latitudes. We estimate the change in tropospheric ozone radiative impacts from 1995–1999 to 2013–2017 is +18.5 mW m−2, with 43.5 mW m−2 contributed by anthropogenic emission changes (20.5 mW m−2 alone by aircraft emissions), highlighting that the equatorward redistribution of emissions to areas with strong convection and the increase in aircraft emissions are effective for increasing tropospheric ozone's greenhouse effect.

City-level estimates of ambient ozone concentrations and associated disease burdens are sparsely available, especially for low and middle-income countries. Recently available high-resolution gridded global ozone concentration estimates allow for estimating ozone concentrations and mortality at urban scales and for urban-rural catchment areas worldwide. We applied existing fine resolution global surface ozone estimates, developed by integrating observations (8834 sites globally) with nine atmospheric chemistry models, in an epidemiologically-derived health impact function to estimate chronic respiratory disease mortality worldwide in 2019. We compared ozone season daily maximum 8 h mixing ratio concentrations and ozone-attributable mortality for urban areas worldwide (including cities and densely-populated towns), and their surrounding peri-urban, peri-rural, and rural areas. In 2019, population-weighted mean ozone among all urban-rural catchment areas was greatest in peri-urban areas (52 ppb), followed by urban areas (cities and towns; 49 ppb). Of 423 100 estimated global ozone-attributable deaths, 37% (147 100) occurred in urban areas, where 40% of the world’s population resides, and 56% (254 000) occurred in peri-urban areas (<1 h from an urban area), where 47% of the world’s population resides. Across 12 946 cities (excluding towns), average population-weighted mean ozone was 51 ppb (sd = 13 ppb, range = 10–78 ppb). Three quarters of the ozone-attributable deaths worldwide (77%; 112 700) occurred in cities of South and East Asia. City-level ozone-attributable mortality rates varied by a factor of 10 across world regions. Ozone levels and attributable mortality were greatest in Asian and African cities; however, cities of higher-income regions, like high-income Asia Pacific and North America, continue to experience high ozone concentrations and attributable mortality rates, despite successful national air quality measures for reducing ozone precursor emissions. The disproportionate magnitude of ozone mortality compared with population size in peri-urban areas indicates that reducing ozone precursor emissions in places that influence peri-urban concentrations can yield substantial health benefits in these areas.

Source attribution science can help areas of the U.S. west At Earth's surface, ozone is an air pollutant that causes respiratory health effects in humans and impairs plant growth and productivity ( 1 ). The Clean Air Act (CAA) of 1970 mandates that the U.S. Environmental Protection Agency (EPA) assess the ozone standard every 5 years and revise when necessary to protect human health. With a decision expected in October 2015 as to whether the standard will be toughened, we discuss limitations of ozone and precursor observations that hinder the ability of state and local air pollution–control agencies to accurately attribute sources of ozone within their jurisdictions. Attaining a lower standard may be particularly challenging in high elevations of the western United States, which are more likely to be affected by ozone that has been transported long distances or that originated in the stratosphere.

The published literature debates the extent to which naturally occurring stratospheric ozone intrusions reach the surface and contribute to exceedances of the U.S. National Ambient Air Quality Standard (NAAQS) for ground‐level ozone (75 ppbv implemented in 2008). Analysis of ozonesondes, lidar, and surface measurements over the western U.S. from April to June 2010 show that a global high‐resolution (∼50 × 50 km2) chemistry‐climate model (GFDL AM3) captures the observed layered features and sharp ozone gradients of deep stratospheric intrusions, representing a major improvement over previous chemical transport models. Thirteen intrusions enhanced total daily maximum 8‐h average (MDA8) ozone to ∼70–86 ppbv at surface sites. With a stratospheric ozone tracer defined relative to a dynamically varying tropopause, we find that stratospheric intrusions can episodically increase surface MDA8 ozone by 20–40 ppbv (all model estimates are bias corrected), including on days when observed ozone exceeds the NAAQS threshold. These stratospheric intrusions elevated background ozone concentrations (estimated by turning off North American anthropogenic emissions in the model) to MDA8 values of 60–75 ppbv. At high‐elevation western U.S. sites, the 25th–75th percentile of the stratospheric contribution is 15–25 ppbv when observed MDA8 ozone is 60–70 ppbv, and increases to ∼17–40 ppbv for the 70–85 ppbv range. These estimates, up to 2–3 times greater than previously reported, indicate a major role for stratospheric intrusions in contributing to springtime high‐O3events over the high‐altitude western U.S., posing a challenge for staying below the ozone NAAQS threshold, particularly if a value in the 60–70 ppbv range were to be adopted. Key Points Stratospheric intrusions can episodically increase surface ozone by 20‐40 ppbv These intrusion events can push ground‐level ozone over the health‐based limit Global high‐res model, satellite and in situ observations yield process insights

Surface ozone is a greenhouse gas and pollutant detrimental to human health and crop and ecosystem productivity. The Tropospheric Ozone Assessment Report (TOAR) is designed to provide the research community with an up-to-date observation-based overview of tropospheric ozone’s global distribution and trends. The TOAR Surface Ozone Database contains ozone metrics at thousands of monitoring sites around the world, densely clustered across mid-latitude North America, western Europe and East Asia. Calculating regional ozone trends across these locations is challenging due to the uneven spacing of the monitoring sites across urban and rural areas. To meet this challenge we conducted a spatial and temporal trend analysis of several TOAR ozone metrics across these three regions for summertime (April–September) 2000–2014, using the generalized additive mixed model (GAMM). Our analysis indicates that East Asia has the greatest human and plant exposure to ozone pollution among investigating regions, with increasing ozone levels through 2014. The results also show that ozone mixing ratios continue to decline significantly over eastern North America and Europe, however, there is less evidence for decreases of daytime average ozone at urban sites. The present-day spatial coverage of ozone monitors in East Asia (South Korea and Japan) and eastern North America is adequate for estimating regional trends by simply taking the average of the individual trends at each site. However the European network is more sparsely populated across its northern and eastern regions and therefore a simple average of the individual trends at each site does not yield an accurate regional trend. This analysis demonstrates that the GAMM technique can be used to assess the regional representativeness of existing monitoring networks, indicating those networks for which a regional trend can be obtained by simply averaging the trends of all individual sites and those networks that require a more sophisticated statistical approach.

Tropospheric NO2 and ozone simulations have large uncertainties, but their biases, seasonality, and trends can be improved with NO2 assimilations. We perform global top-down estimates of monthly NOx emissions using two Ozone Monitoring Instrument (OMI) NO2 retrievals (NASAv3 and DOMINOv2) from 2005 to 2016 through a hybrid 4D-Var/mass balance inversion. Discrepancy inNO2 retrieval products is a major source of uncertainties in the top-down NOx emission estimates. The different vertical sensitivities in the two NO2 retrievals affect both magnitude and seasonal variations of top-down NOx emissions. The 12-year averages of regional NOx budgets from the NASA posterior emissions are 37 % to 53 % smaller than the DOMINO posterior emissions. Consequently, the DOMINO posterior surface NO2 simulations greatly reduced the negative biases in China (by 15 %) and the US (by 22 %) compared to surface NO2 measurements. Posterior NOx emissions show consistent trends over China, the US, India, and Mexico constrained by the two retrievals. Emission trends are less robust over South America, Australia, western Europe, and Africa, where the two retrievals show less consistency. NO2 trends have more consistent decreases (by 26 %) with the measurements (by 32 %) in the US from 2006 to 2016 when using the NASA posterior emissions. The performance of posterior ozone simulations has spatial heterogeneities from region to region. On a global scale, ozone simulations using NASA-based emissions alleviate the double peak in the prior simulation of global ozone seasonality. The higher abundances of NO2 from the DOMINO posterior simulations increase the global background ozone concentrations and therefore reduce the negative biases more than the NASA posterior simulations using GEOS-Chem v12 at remote sites. Compared to surface ozone measurements, posterior simulations have more consistent magnitude and interannual variations than the prior estimates, but the performance from the NASA-based and DOMINO-based emissions varies across ozone metrics. The limited availability of remote-sensing data and the use of prior NOx diurnal variations hinder improvement of ozone diurnal variations from the assimilation, and therefore have mixed performance on improving different ozone metrics. Additional improvements in posterior NO2 and ozone simulations require more precise and consistent NO2 retrieval products, more accurate diurnal variations of NOx and VOC emissions, and improved simulations of ozone chemistry and depositions.

Extracting globally representative trend information from lower tropospheric ozone observations is extremely difficult due to the highly variable distribution and interannual variability of ozone, and the ongoing shift of ozone precursor emissions from high latitudes to low latitudes. Here we report surface ozone trends at 27 globally distributed remote locations (20 in the Northern Hemisphere, 7 in the Southern Hemisphere), focusing on continuous time series that extend from the present back to at least 1995. While these sites are only representative of less than 25% of the global surface area, this analysis provides a range of regional long-term ozone trends for the evaluation of global chemistry-climate models. Trends are based on monthly mean ozone anomalies, and all sites have at least 20 years of data, which improves the likelihood that a robust trend value is due to changes in ozone precursor emissions and/or forced climate change rather than naturally occurring climate variability. Since 1995, the Northern Hemisphere sites are nearly evenly split between positive and negative ozone trends, while 5 of 7 Southern Hemisphere sites have positive trends. Positive trends are in the range of 0.5–2 ppbv decade–1, with ozone increasing at Mauna Loa by roughly 50% since the late 1950s. Two high elevation Alpine sites, discussed by previous assessments, exhibit decreasing ozone trends in contrast to the positive trend observed by IAGOS commercial aircraft in the European lower free-troposphere. The Alpine sites frequently sample polluted European boundary layer air, especially in summer, and can only be representative of lower free tropospheric ozone if the data are carefully filtered to avoid boundary layer air. The highly variable ozone trends at these 27 surface sites are not necessarily indicative of free tropospheric trends, which have been overwhelmingly positive since the mid-1990s, as shown by recent studies of ozonesonde and aircraft observations.

From the earliest observations of ozone in the lower atmosphere in the 19th century, both measurement methods and the portion of the globe observed have evolved and changed. These methods have different uncertainties and biases, and the data records differ with respect to coverage (space and time), information content, and representativeness. In this study, various ozone measurement methods and ozone datasets are reviewed and selected for inclusion in the historical record of background ozone levels, based on relationship of the measurement technique to the modern UV absorption standard, absence of interfering pollutants, representativeness of the well-mixed boundary layer and expert judgement of their credibility. There are significant uncertainties with the 19th and early 20th-century measurements related to interference of other gases. Spectroscopic methods applied before 1960 have likely underestimated ozone by as much as 11% at the surface and by about 24% in the free troposphere, due to the use of differing ozone absorption coefficients. There is no unambiguous evidence in the measurement record back to 1896 that typical mid-latitude background surface ozone values were below about 20 nmol mol–1, but there is robust evidence for increases in the temperate and polar regions of the northern hemisphere of 30–70%, with large uncertainty, between the period of historic observations, 1896–1975, and the modern period (1990–2014). Independent historical observations from balloons and aircraft indicate similar changes in the free troposphere. Changes in the southern hemisphere are much less. Regional representativeness of the available observations remains a potential source of large errors, which are difficult to quantify. The great majority of validation and intercomparison studies of free tropospheric ozone measurement methods use ECC ozonesondes as reference. Compared to UV-absorption measurements they show a modest (~1–5% ±5%) high bias in the troposphere, but no evidence of a change with time. Umkehr, lidar, and FTIR methods all show modest low biases relative to ECCs, and so, using ECC sondes as a transfer standard, all appear to agree to within one standard deviation with the modern UV-absorption standard. Other sonde types show an increase of 5–20% in sensitivity to tropospheric ozone from 1970–1995. Biases and standard deviations of satellite retrieval comparisons are often 2–3 times larger than those of other free tropospheric measurements. The lack of information on temporal changes of bias for satellite measurements of tropospheric ozone is an area of concern for long-term trend studies.

Long-term atmospheric ozone observations in Western North America (WNA) provide essential data for assessing tropospheric ozone trends. Backward atmospheric simulations based on these observations establish the source–receptor relationships (SRRs) to improve our understanding of the factors driving ozone trends across different regions, time periods, and atmospheric layers. In this study, we integrated 28 years of ozone observations (1994–2021) from ozonesondes, lidar, commercial aircraft, and aircraft campaigns across WNA, spanning the upper atmospheric boundary layer, free troposphere, and upper troposphere (i.e., 900 to 300 hPa). We integrated the multiplatform datasets using a data fusion framework to generate 553 608 gridded ozone receptors. For each receptor, we use the FLEXible PARTicle (FLEXPART) dispersion model, driven by ERA5 reanalysis data, to produce the SRRs calculations, providing global simulations at high temporal (hourly) and spatial (1°×1°) resolution from the surface up to 20 km a.g.l. (above ground level). This SRR database retains detailed information for each receptor, including the gridded ozone value product, which enables user to illustrate and identify source contributions to various subsets of ozone observations in the troposphere above WNA over nearly 3 decades at different vertical layers and temporal scales, such as diurnal, daily, seasonal, intra-annual, and decadal. More generally, the calculated SRRs are applicable to any study looking to evaluate origins of airmasses reaching WNA. As such, this database can support source contribution analyses for other atmospheric components observed over WNA, if other co-located observations have been made at the spatial and temporal scales defined for some or all of the gridded ozone receptors used here. The entire dataset is publicly available at https://doi.org/10.5067/ASDC/WNA-BackTraj (Cui et al., 2025).