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.

The Infrared Atmospheric Sounding Interferometer (IASI) forms the main infrared sounding component of the European Organisation for the Exploitation of Meteorological Satellites's (EUMETSAT's) Meteorological Operation (MetOp)-A satellite (Klaes et al. 2007), which was launched in October 2006. This article presents the results of the first 4 yr of the operational IASI mission. The performance of the instrument is shown to be exceptional in terms of calibration and stability. The quality of the data has allowed the rapid use of the observations in operational numerical weather prediction (NWP) and the development of new products for atmospheric chemistry and climate studies, some of which were unexpected before launch. The assimilation of IASI observations in NWP models provides a significant forecast impact; in most cases the impact has been shown to be at least as large as for any previous instrument. In atmospheric chemistry, global distributions of gases, such as ozone and carbon monoxide, can be produced in near–real time, and short-lived species, such as ammonia or methanol, can be mapped, allowing the identification of new sources. The data have also shown the ability to track the location and chemistry of gaseous plumes and particles associated with volcanic eruptions and fires, providing valuable data for air quality monitoring and aircraft safety. IASI also contributes to the establishment of robust long-term data records of several essential climate variables. The suite of products being developed from IASI continues to expand as the data are investigated, and further impacts are expected from increased use of the data in NWP and climate studies in the coming years. The instrument has set a high standard for future operational hyperspectral infrared sounders and has demonstrated that such instruments have a vital role in the global observing system.

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.

[1] First partial tropospheric ozone columns (0 -6 km) derived from radiances observed by the IASI instrument aboard the MetOp-A platform over Europe during summer 2007 are presented. They were retrieved using an altitudedependent regularization method. Comparison with measurements from balloon sondes shows excellent agreement. Space-borne observations show large lower tropospheric ozone amounts over South-Eastern Europe during the heat wave period, which are also displayed by simulations with a regional chemistry-transport model CHIMERE.

Abstract. Three scientific ozone products from the Infrared Atmospheric Sounding Interferometer (IASI) aboard MetOp-A, retrieved in three different research teams (LA, LATMOS/ULB, LISA) with different retrieval schemes, are characterized and validated using ozonesondes measurements. The characteristics of the products are analyzed in terms of retrieval sensitivity, systematic and random errors, and ability to retrieve the natural variability of ozone and focus on different partial columns from the lower troposphere up to 30 km. The validation covers the midlatitudes and the tropics and the period from January to December 2008. The products present degrees of freedom (DOF) in the troposphere between 1 and 1.2 on average in the midlatitudes and between 1 and 1.4 in the tropics. The DOF are distributed differently on the vertical depending on the profiles and the season: summer leading to a better sensitivity to the lower troposphere, as expected. The error estimates range between 10 and 20 % from the lower tropospheric partial columns (0-6 km and 0-8 km for the midlatitudes and the tropics respectively) to the UTLS partial columns (8-16 km and 11-20 km for the midlatitudes and the tropics respectively) for all the products and are about 5 % in the stratosphere (16-30 km) and for the column up to 30 km. The main feature that arises from the comparison with the ozonesondes is a systematic overestimation of ozone in the UTLS (between 10 and 25 %) by the three products in the midlatitudes and the tropics, attributed to the moderate vertical resolution of IASI and possibly to spectroscopic inconsistencies. The ability of the products to reproduce natural variability of tropospheric ozone is fairly good and depends on the considered season and region.

IASI observations of tropospheric ozone over the Beijing, Shanghai and Hong Kong areas during one year (2008) have been analysed, demonstrating the capability of space-borne infrared nadir measurements to probe seasonal and even day-to-day variations of lower tropospheric ozone (0–6 km partial columns) on the regional scale of highly populated areas. The monthly variations of lower tropospheric ozone retrieved from IASI clearly show the influence of the Asian summer monsoon that brings clean air masses from the Pacific during summer. They exhibit indeed a sharp ozone maximum in late spring and early summer (May–June) followed by a summer minimum. The time periods and the intensities of the maxima and of the decreases are latitude-dependent: they are more pronounced in Hong Kong and Shanghai than in Beijing. Moreover, IASI provides the opportunity to follow the spatial variations of ozone over the surroundings of each megacity as well as its daily variability. We show here that the large lower tropospheric ozone amounts (0–6 km partial columns) observed with IASI are mainly downwind the highest populated areas in each region, thus possibly suggesting the anthropogenic origin of the large ozone amounts observed. Finally, an analysis of the mean ozone profiles over each region – for selected days with high ozone events – in association with the analysis of the meteorological situation shows that the high ozone amounts observed during winter are likely related to descents of ozone-rich air from the stratosphere, whereas in spring and summer the tropospheric ozone is likely enhanced by photochemical production in polluted areas and/or in air masses from fire plumes

Abstract. We present a new multispectral approach for observing lowermost tropospheric ozone from space by synergism of atmospheric radiances in the thermal infrared (TIR) observed by IASI (Infrared Atmospheric Sounding Interferometer) and earth reflectances in the ultraviolet (UV) measured by GOME-2 (Global Ozone Monitoring Experiment-2). Both instruments are onboard the series of MetOp satellites (in orbit since 2006 and expected until 2022) and their scanning capabilities offer global coverage every day, with a relatively fine ground pixel resolution (12 km-diameter pixels spaced by 25 km for IASI at nadir). Our technique uses altitude-dependent Tikhonov-Phillips-type constraints, which optimize sensitivity to lower tropospheric ozone. It integrates the VLIDORT (Vector Linearized Discrete Ordinate Radiative Transfer) and KOPRA (Karlsruhe Optimized and Precise Radiative transfer Algorithm) radiative transfer codes for simulating UV reflectance and TIR radiance, respectively. We have used our method to analyse real observations over Europe during an ozone pollution episode in the summer of 2009. The results show that the multispectral synergism of IASI (TIR) and GOME-2 (UV) enables the observation of the spatial distribution of ozone plumes in the lowermost troposphere (LMT, from the surface up to 3 km a.s.l., above sea level), in good agreement with the CHIMERE regional chemistry-transport model. In this case study, when high ozone concentrations extend vertically above 3 km a.s.l., they are similarly observed over land by both the multispectral and IASI retrievals. On the other hand, ozone plumes located below 3 km a.s.l. are only clearly depicted by the multispectral retrieval (both over land and over ocean). This is achieved by a clear enhancement of sensitivity to ozone in the lowest atmospheric layers. The multispectral sensitivity in the LMT peaks at 2 to 2.5 km a.s.l. over land, while sensitivity for IASI or GOME-2 only peaks at 3 to 4 km a.s.l. at lowest (above the LMT). The degrees of freedom for the multispectral retrieval increase by 0.1 (40 % in relative terms) with respect to IASI only retrievals for the LMT. Validations with ozonesondes (over Europe during summer 2009) show that our synergetic approach for combining IASI (TIR) and GOME-2 (UV) measurements retrieves lowermost tropospheric ozone with a mean bias of 1 % and a precision of 16 %, when smoothing by the retrieval vertical sensitivity (1 % mean bias and 21 % precision for direct comparisons).Published by Copernicus Publications on behalf of the European Geosciences Union. 9676

Simultaneous ACE (Atmospheric Chemistry Experiment) upper tropospheric CO, C2H6, HCN, CH3Cl, CH4, C2H2, CH3OH, HCOOH, and OCS measurements show plumes up to 185 ppbv (10−9 per unit volume) for CO, 1.36 ppbv for C2H6, 755 pptv (10−12 per unit volume) for HCN, 1.12 ppbv for CH3Cl, 1.82 ppmv (10−6 per unit volume) for CH4, 0.178 ppbv for C2H2, 3.89 ppbv for CH3OH, 0.843 ppbv for HCOOH, and 0.48 ppbv for OCS in western Canada and Alaska at 50°N–68°N latitude between 29 June and 23 July 2004. Enhancement ratios and emission factors for HCOOH, CH3OH, HCN, C2H6, and OCS relative to CO at 250–350 hPa are inferred from measurements of young plumes compared with lower mixing ratios assumed to represent background conditions based on a CO emission factor derived from boreal measurements. Results are generally consistent with the limited data reported for various vegetative types and emission phases measured in extratropical forests including boreal forests. The low correlation between fire product emission mixing ratios and the SF6 mixing ratio is consistent with no significant SF6 emissions from the biomass fires.