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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.

MOZAIC-IAGOS data are used to assess the ability of the MACC reanalysis (REAN) to reproduce distributions of ozone (O3) and carbon monoxide (CO), along with vertical and inter-annual variability in the upper troposphere/lower stratosphere region (UTLS) over Europe for the period 2003–2010. A control run (CNTRL, without assimilation) is compared with the MACC reanalysis (REAN, with assimilation) to assess the impact of assimilation. On average over the period, REAN underestimates ozone by 60 ppbv in the lower stratosphere (LS), whilst CO is overestimated by 20 ppbv. In the upper troposphere (UT), ozone is overestimated by 50 ppbv, while CO is partly over or underestimated by up to 20 ppbv. As expected, assimilation generally improves model results but there are some exceptions. Assimilation leads to increased CO mixing ratios in the UT which reduce the biases of the model in this region but the difference in CO mixing ratios between LS and UT has not changed and remains underestimated after assimilation. Therefore, this leads to a significant positive bias of CO in the LS after assimilation. Assimilation improves estimates of the amplitude of the seasonal cycle for both species. Additionally, the observations clearly show a general negative trend of CO in the UT which is rather well reproduced by REAN. However, REAN misses the observed inter-annual variability in summer. The O3–CO correlation in the Ex-UTLS is rather well reproduced by the CNTRL and REAN, although REAN tends to miss the lowest CO mixing ratios for the four seasons and tends to oversample the extra-tropical transition layer (ExTL region) in spring. This evaluation stresses the importance of the model gradients for a good description of the mixing in the Ex-UTLS region, which is inherently difficult to observe from satellite instruments.

Utilising a fleet of commercial airliners, MOZAIC/IAGOS provides atmospheric composition data on a regular basis that are widely used for modelling applications. Due to the specific operational context of the platforms, such observations are collected close to international airports and hence in an environment characterised by high anthropogenic emissions. This provides opportunities for assessing emission inventories of major metropolitan areas around the world, but also challenges in representing the observations in typical chemical transport models. We assess here the contribution of different sources of error to overall model–data mismatch using the example of MOZAIC/IAGOS carbon monoxide (CO) profiles collected over the European regional domain in a time window of 5 yr (2006–2011). The different sources of error addressed in the present study are: 1) mismatch in modelled and observed mixed layer height; 2) bias in emission fluxes and 3) spatial representation error (related to unresolved spatial variations in emissions). The modelling framework combines a regional Lagrangian transport model (STILT) with EDGARv4.3 emission inventory and lateral boundary conditions from the MACC reanalysis. The representation error was derived by coupling STILT with emission fluxes aggregated to different spatial resolutions. We also use the MACC reanalysis to assess uncertainty related to uncertainty sources 2) and 3). We treat the random and the bias components of the uncertainty separately and found that 1) and 3) have a comparable impact on the random component for both models, while 2) is far less important. On the other hand, the bias component shows comparable impacts from each source of uncertainty, despite both models being affected by a low bias of a factor of 2–2.5 in the emission fluxes. In addition, we suggested methods to correct for biases in emission fluxes and in mixing heights. Lastly, the evaluation of the spatial representation error against model–data mismatch between MOZAIC/IAGOS observations and the MACC reanalysis revealed that the representation error accounts for roughly 15–20% of the model–data mismatch uncertainty.

In December 2000, a fully automatic NOy instrument was installed on one of the five Airbus A340 aircraft used in the MOZAIC project (Measurement of Ozone and Water Vapour by Airbus in-service Aircraft) for measurements of O3 and H2O since 1994. This long-range aircraft was operated by Lufthansa, mainly out of Frankfurt and Munich. After an initial testing period, regular data collection started in May 2001. Until May 2005, 1533 flights have been recorded, corresponding to 8500 flight hours of NOy measurements. Concurrent data of NOy and O3 are available from 1433 flights and concurrent data for CO, O3 and NOy exist from 1125 flights since 2002. The paper describes the data availability in terms of geographical, vertical and seasonal distribution and discusses the quality and limitations of the data, including interference by HCN. The vast majority of vertical profiles were measured over Frankfurt, followed by Munich and North American airports. While most of the data were collected in the upper troposphere and lower stratosphere over the North Atlantic, significant data sets exist also from flights to Far and Middle East, whereas data from the tropics and the Southern Hemisphere are relatively sparse.

We analysed ozone and carbon monoxide profiles measured by commercial aircrafts from the MOZAIC/IAGOS fleet, during ascending and descending flights over Caracas, in Venezuela, from August 1994 to December 2009, over Rio de Janeiro, from 1994 to 2004 and from July 2012 to June 2013, and over São Paulo, in Brazil, from August 1994 to 2005. For ozone, results showed a clean atmosphere over Caracas presenting the highest seasonal mean in March, April and May. Backward trajectory analyses with FLEXPART, of case studies for which the measured concentrations were high, showed that contributions from local, Central and North America, the Caribbean and Africa either from anthropogenic emissions, biomass burning or lightning were possible. Satellite products as fire counts from MODIS, lightning flash rates from LIS, and CO and O3 from Infrared Atmospheric Sounding Interferometer and wind maps at different levels helped corroborate previous findings. Sensitivity studies performed with the chemical transport model GEOS-Chem captured the effect of anthropogenic emissions but underestimated the influence of biomass burning, which could be due to an underestimation of GFEDv2 emission inventory. The model detected the contribution of lightning from Africa in JJA and SON and from South America in DJF, possibly from the northeast of Brazil. Over São Paulo and Rio de Janeiro, GEOS-Chem captured the seasonal variability of lightning produced in South America and attributed this source as the most important in this region, except in JJA, when anthropogenic emissions were addressed as the more impacting source of ozone precursors. However, comparison with the measurements indicated that the model overestimated ozone formation, which could be due to the convective parameterisation or the stratospheric influence. The highest ozone concentration was observed during September to November, but the model attributed only a small influence of biomass burning from South America, with no contribution of long-range transport from Africa.

A large quantity of tropospheric ozone observations are conducted all over the world using different platforms and techniques for different purposes and goals. These observations are commonly used to derive seasonal cycles, interannual variations and long-term trends of ozone in the troposphere. In addition, they are used for comparison with three-dimensional chemistry-transport models to evaluate their performance and hence to test our current understanding of the tropospheric ozone variability. It is still challenging to provide robust tropospheric ozone trends throughout the world because of the great variability of ozone, its complex photochemical reactions, the rarity of long-term records, the diversity of measurement techniques and platforms, and the issues with data quality. In this work, we evaluated, with emphasis on the lower troposphere, the consistency of tropospheric ozone observations made by means of multiple platforms, including surface sites, sondes and regular aircraft, that are publicly available in the global databases, but excluding space-borne platforms. Concomitant observations were examined on an hourly basis (except for ±3 hours for sonde versus aircraft) for pairs of locations at less than 100-km distance. Generally, we found good agreement between sonde and surface observations. We also found that there was no need to apply any correction factor to ozonesonde observations except for Brewer–Mast sondes at Hohenpeissenberg. Because of a larger distance between the site pairs, the correlations found between the aircraft and surface measurements were poorer than those between sonde and surface measurements. However, a relatively simple wind segregation improved the agreement between the aircraft versus surface measurements. We found also that due to diurnal cycles, the sonde launching at a fixed local time led to positive or negative biases against the surface observations, suggesting that great attention should be paid to local time and diurnal variations when using ozonesonde in the analysis of seasonal cycles, long-term trends and interannual variations of lower tropospheric ozone. The comparison of surface data at Mt. Happo to regular aircraft data over Tokyo/Narita showed a relatively reasonable agreement, ensuring regionally representative ozone data sets in this region for trend analysis.

The European Research Infrastructure IAGOS (In-service Aircraft for a Global Observing System) operates a global-scale monitoring system for atmospheric trace gases, aerosols and clouds utilising the existing global civil aircraft. This new monitoring infrastructure builds on the heritage of the former research projects MOZAIC (Measurement of Ozone and Water Vapour on Airbus In-service Aircraft) and CARIBIC (Civil Aircraft for the Regular Investigation of the Atmosphere Based on an Instrument Container). CARIBIC continues within IAGOS and acts as an important airborne measurement reference standard within the wider IAGOS fleet. IAGOS is a major contributor to the in-situ component of the Copernicus Atmosphere Monitoring Service (CAMS), the successor to the Global Monitoring for the Environment and Security – Atmospheric Service, and is providing data for users in science, weather services and atmospherically relevant policy. IAGOS is unique in collecting regular in-situ observations of reactive gases, greenhouse gases and aerosol concentrations in the upper troposphere and lowermost stratosphere (UTLS) at high spatial resolution. It also provides routine vertical profiles of these species in the troposphere over continental sites or regions, many of which are undersampled by other networks or sampling studies, particularly in Africa, Southeast Asia and South America. In combination with MOZAIC and CARIBIC, IAGOS has provided long-term observations of atmospheric chemical composition in the UTLS since 1994. The longest time series are 20 yr of temperature, H2O and O3, and 9–15 yr of aerosols, CO, NO y , CO2, CH4, N2O, SF6, Hg, acetone, ~30 HFCs and ~20 non-methane hydrocarbons. Among the scientific highlights which have emerged from these data sets are observations of extreme concentrations of O3 and CO over the Pacific basin that have never or rarely been recorded over the Atlantic region for the past 12 yr; detailed information on the temporal and regional distributions of O3, CO, H2O, NO y and aerosol particles in the UTLS, including the impacts of cross-tropopause transport, deep convection and lightning on the distribution of these species; characterisation of ice-supersaturated regions in the UTLS; and finally, improved understanding of the spatial distribution of upper tropospheric humidity including the finding that the UTLS is much more humid than previously assumed.

In continuation of previous research for evaluation of the high ozone levels observed during summer time over the eastern Mediterranean, MOZAIC profiles collected at the airport of Cairo from 1994 to 2008 are analysed. Average profiles corresponding, respectively, to the highest and the lowest ozone mixing ratios for the 0–1.5 km layer over Cairo in summer (JJA) (94 profiles) are examined along with their corresponding composite maps of geopotential height (and anomalies), vertical velocity (and anomalies), specific humidity anomalies, precipitable water anomalies, air temperature anomalies and wind speed at 850 hPa. In addition, backward trajectories arriving in the boundary layer over Cairo during the days with highest or lowest ozone mixing ratios are examined. During the 7% highest ozone days at the 0–1500 m layer over Cairo, very high ozone concentrations of about 80 ppb on average are observed from the surface up to 4–5 km altitude. The difference in ozone concentrations between the 7% highest and the 7% lowest ozone days reaches maximum values around 60 ppb close to the ground. During the highest ozone days for both 1.5–5 and 0–1.5 km layer, there are extended regions of strong subsidence in the eastern Mediterranean but also in eastern and northern Europe and over these regions the atmosphere is dryer than average. In addition, characteristic profiles with the highest ozone concentrations in the 0–1500 m layer are examined in order to assess the influence of atmospheric transport and photochemistry on the ozone concentrations over the area.

Abstract Long-term observations of reactive gases in the troposphere are important for understanding trace gas cycles and the oxidation capacity of the atmosphere, assessing impacts of emission changes, verifying numerical model simulations, and quantifying the interactions between short-lived compounds and climate change. The World Meteorological Organization’s (WMO) Global Atmosphere Watch (GAW) program coordinates a global network of surface stations some of which have measured reactive gases for more than 40 years. Gas species included under this umbrella are ozone, carbon monoxide, nitrogen oxides, and volatile organic compounds (VOCs). There are many challenges involved in setting-up and maintaining such a network over many decades and to ensure that data are of high quality, regularly updated and made easily accessible to users. This overview describes the GAW surface station network of reactive gases, its unique quality management framework, and discusses the data that are available from the central archive. Highlights of data use from the published literature are reviewed, and a brief outlook into the future of GAW is given. This manuscript constitutes the overview of a special feature on GAW reactive gases observations with individual papers reporting on research and data analysis of particular substances being covered by the program.

This article is based on the study of the seasonal and interannual variability of carbon monoxide (CO) and ozone (O3) at different altitudes of the troposphere over Hyderabad, India, during 2006–2010 using Measurement of OZone and water vapour by Airbus In-Service Aircraft (MOZAIC) and observation from Tropospheric Emission Spectrometer (TES) aboard NASA's Aura satellite. The MOZAIC observations show maximum seasonal variability in both CO and O3 during winter and pre-monsoon season, with CO in the range (100–200)±13 ppbv and O3 in the range (50–70)±9 ppbv. The time-series of MOZAIC data shows a significant increase of 4.2±1.3 % in the surface CO and 6.7±1.3 % in the surface O3 during 2006–2010 in Hyderabad. From MOZAIC observations, we identify CO and O3 profiles that are anomalous with respect to the monthly mean and compare those with Weather Research Forecast model coupled with Chemistry (WRF-Chem) and Model for OZone and Related Tracers, version 4 profiles for the same day. The anomalous profiles of WRF-Chem are simulated using three convection schemes. The goodness of comparison depends on the convection scheme and the altitude region of the troposphere.

We present the features seen in the first 2 months (July and August 2012) of data collected over the Pacific by IAGOS (In-service Aircraft for a Global Observing System)-equipped aircraft. IAGOS is the continuation and development of the well-known MOZAIC (Measurement of Ozone and Water Vapour on Airbus in-service Aircraft) project where scientific instruments were carried on commercially operated A340 aircraft to make measurements of chemical species in the atmosphere. Here, we show data from an aircraft operated by China Airlines on routes from Taipei to Vancouver, which provided the first trans-Pacific measurements by an IAGOS-equipped aircraft. We describe the chemical composition of the extratropical upper troposphere/lower stratosphere (Ex-UTLS) across the Pacific basin in the Northern Hemisphere. The observed concentrations of ozone span a range from 18 to 500 ppbv indicating sources in the marine boundary layer and lowermost stratosphere, respectively. Concentrations of carbon monoxide (CO) greater than 400 ppbv are observed in the Ex-UTLS suggesting that plumes of pollution have been exported from the continent. These low concentrations of ozone and high concentrations of CO were rarely recorded in 8 yr of MOZAIC observations over the Atlantic.

This article presents the In-service Aircraft of a Global Observing System (IAGOS) developed for operations on commercial long-range Airbus aircraft (A330/A340) for monitoring the atmospheric composition. IAGOS is the continuation of the former Measurement of OZone and water vapour on Airbus In-service airCraft (MOZAIC) programme (1994–2014) with five aircraft operated by European airlines over 20 yr. MOZAIC has provided unique scientific database used worldwide by the scientific community. In continuation of MOZAIC, IAGOS aims to equip a fleet up to 20 aircraft around the world and for operations over decades. IAGOS started in July 2011 with the first instruments installed aboard a Lufthansa A340-300, and a total of six aircraft are already in operation. We present the technical aircraft system concept, with basic instruments for O3, CO, water vapour and clouds; and optional instruments for measuring either NOy, NOx, aerosols or CO2/CH4. In this article, we focus on the O3 and CO instrumentation while other measurements are or will be described in specific papers. O3 and CO are measured by optimised but well-known methods such as UV absorption and IR correlation, respectively. We describe the data processing/validation and the data quality control for O3 and CO. Using the first two overlapping years of MOZAIC/IAGOS, we conclude that IAGOS can be considered as the continuation of MOZAIC with the same data quality of O3 and CO measurements.

This paper describes the NOy plumes originating from lightning emissions based on 4 yr (2001–2005) of MOZAIC measurements in the upper troposphere of the northern mid-latitudes, together with ground- and space-based observations of lightning flashes and clouds. This analysis is primarily for the North Atlantic region where the MOZAIC flights are the most frequent and for which the measurements are well representative in space and time. The study investigates the influence of lightning NOx (LNOx) emissions on large-scale (300–2000 km) plumes (LSPs) of NOy. One hundred and twenty seven LSPs (6% of the total MOZAIC NOy dataset) have been attributed to LNOx emissions. Most of these LSPs were recorded over North America and the Atlantic mainly in spring and summer during the maximum lightning activity occurrence. The majority of the LSPs (74%) is related to warm conveyor belts and extra-tropical cyclones originating from North America and entering the intercontinental transport pathway between North America and Europe, leading to a negative (positive) west to east NOy (O3) zonal gradient with −0.4 (+18) ppbv difference during spring and −0.6 (+14) ppbv difference in summer. The NOy zonal gradient can correspond to the mixing of the plume with the background air. On the other hand, the O3 gradient is associated with both mixing of background air and with photochemical production during transport. Such transatlantic LSPs may have a potential impact on the European pollution. The remaining sampled LSPs are related to mesoscale convection over Western Europe and the Mediterranean Sea (18%) and to tropical convection (8%).