Abstract. High-quality long-term observational records are essential to ensure appropriate and reliable trend detection of tropospheric ozone. However, the necessity of maintaining high sampling frequency, in addition to continuity, is often under-appreciated. A common assumption is that, so long as long-term records (e.g., a span of a few decades) are available, (1) the estimated trends are accurate and precise, and (2) the impact of small-scale variability (e.g., weather) can be eliminated. In this study, we show that the undercoverage bias (e.g., a type of sampling error resulting from statistical inference based on sparse or insufficient samples, such as once-per-week sampling frequency) can persistently reduce the trend accuracy of free tropospheric ozone, even if multi-decadal time series are considered. We use over 40 years of nighttime ozone observations measured at Mauna Loa, Hawaii (representative of the lower free troposphere), to make this demonstration and quantify the bias in monthly means and trends under different sampling strategies. We also show that short-term meteorological variability remains a cause of an inflated long-term trend uncertainty. To improve the trend precision and accuracy due to sampling bias, two remedies are proposed: (1) a data variability attribution of colocated meteorological influence can efficiently reduce estimation uncertainty and moderately reduce the impact of sparse sampling, and (2) an adaptive sampling strategy based on anomaly detection enables us to greatly reduce the sampling bias and produce more accurate trends using fewer samples compared to an intense regular sampling strategy.
Abstract. Free tropospheric ozone (O3) trends in the Central East China (CEC) and export regions are investigated for 2008–2017 using the IASI (Infrared Atmospheric Sounding Interferometer) O3 observations and the LMDZ-OR-INCA model simulations, including the most recent Chinese emission inventory. The observed and modelled trends in the CEC region are −0.07 ± 0.02 and −0.08 ± 0.02 DU yr−1, respectively, for the lower free troposphere (3–6 km column) and −0.05 ± 0.02 and −0.06 ± 0.02 DU yr−1, respectively, for the upper free troposphere (6–9 km column). The statistical p value is smaller to 0.01 for all the derived trends. A good agreement between the observations and the model is also observed in the region, including the Korean Peninsula and Japan and corresponding to the region of pollution export from China. Based on sensitivity studies conducted with the model, we evaluate, at 60 % and 52 %, the contribution of the Chinese anthropogenic emissions to the trend in the lower and upper free troposphere, respectively. The second main contribution to the trend is the meteorological variability (34 % and 50 %, respectively). These results suggest that the reduction in NOx anthropogenic emissions that has occurred since 2013 in China led to a decrease in ozone in the Chinese free troposphere, contrary to the increase in ozone at the surface. We designed some tests to compare the trends derived by the IASI observations and the model to independent measurements, such as the In-service Aircraft for a Global Observing System (IAGOS) or other satellite measurements (Ozone Monitoring Instrument (OMI)/Microwave Limb Sounder (MLS)). These comparisons do not confirm the O3 decrease and stress the difficulty in analysing short-term trends using multiple data sets with various sampling and the risk of overinterpreting the results.
Tropospheric ozone vertical profile measurements have been carried out at OHP (Observatoire de Haute Provence, 44°N, 6.7°E, 690 m) since 1991 using both UV DIAL (DIfferential Absorption Lidar) and ECC (Electrochemical Concentration Cell) ozonesondes. For the first time, ECC and lidar data measured at the same site, have been compared over a 24 year period. The comparison conducted reveals a bias between both measurement types (ECC - lidar) of the order of 0.6 ppbv. The measurements of both instruments have been however combined to decrease the impact of short-term atmospheric variability on the trend estimate. Air mass trajectories have been calculated for all the ozone observations available at OHP including ECMWF potential vorticity (PV) and humidity chnage along the trajectories. The interannual ozone variability shows a negligible trend in the mid troposphere, but a 0.36 ppbv/year significant positive ozone trend in the upper troposphere. The trends will be discussed using the variability of the meteorological parameters. Data clustering using PV and air mass trajectories is useful to identify the role of Stratosphere-Tropopshere Exchanges and long range transport of pollutants in the observed long term trends. In the lower troposphere, the interannual variability shows contrasted trends with an ozone decrease between 1998 and 2008, consistent with the NO x emission decrease, but a new period of ozone increase since 2008 which is not very well understood.
Tropospheric ozone is a greenhouse gas and pollutant detrimental to human health and crop and ecosystem productivity. Since 1990 a large portion of the anthropogenic emissions that react in the atmosphere to produce ozone have shifted from North America and Europe to Asia. This rapid shift, coupled with limited ozone monitoring in developing nations, has left scientists unable to answer the most basic questions: Is ozone continuing to decline in nations with strong emission controls? To what extent is ozone increasing in the developing world? IGAC’s Tropospheric Ozone Assessment Report (TOAR) has been designed to answer these questions and this presentation will show the results from the TOAR-Climate initiative, focusing on the present-day distribution and trends of global tropospheric ozone from satellite observations. Five satellite products based on OMI (2 products using two different retrieval methods) and IASI (also 2 products using two different retrieval methods) and the OMI/MLS combined product were intercompared. An important result is the close agreement among the five products regarding the quantification of the total mass of all tropospheric ozone, the so called tropospheric ozone burden (TOB). The mean estimate for TOB between 60° N and 60° S is 296 Tg, with all products agreeing within ± 4%. However, on a regional basis the five satellite products have notable differences and there is no agreement in terms of ozone trends over the past decade. Continuing work is exploring the causes of these differences.
As part of the Ozone and Precursors in the Tropics (OPT) working group of the Tropospheric Ozone Assessment Report Phase 2 (TOAR-II), we present the first results on the distribution of tropospheric ozone (O3) and its precursors (carbon monoxide, CO; formaldehyde, HCHO; nitrogen dioxide, NO2) in the tropics over the past 20-25 years. The goal is to give an overview of the seasonal, geographical and vertical variabilities of tropical tropospheric O3 and its precursors. To do so, we use in situ measurements of O3 and its precursors from surface sites, sounding balloons (SHADOZ) and instrumented aircraft (IAGOS and ATOM), as well as ground-based (FTIR) and spatial (IASI, OMI, GOME-2) remote-sensed observations. The observations are averaged monthly over the longest available time-period as well as over the first five years of the time period. The results for these two time periods give the context to interpret distributions and variabilities of O3 and its precursors over the most recent five years as we call it “Present-day”.  Special emphasis is given to the differences of O3 and its precursors’ distributions between remote and polluted regions and to the relationships between the gaseous species. Model output will be included to fill gaps in space and time when necessary to help the interpretation of the analysis based on observations.From IAGOS measurements, the highest O3 and CO maxima occur in the lower troposphere of Northern Hemisphere Africa, which remains the most influenced by biomass burning. CO maxima are attributed using SOFT-IO model to anthropogenic emissions by 60%. Second maxima are observed in the lower troposphere of Asia, mostly due to anthropogenic emissions. The highest amount of transported CO in the tropics originates from Africa.
Abstract. Ozone is a key constituent of the troposphere where it drives photochemical processes, impacts air quality, and acts as a climate forcer. Large-scale in situ observations of ozone commensurate with the grid resolution of current Earth system models are necessary to validate model outputs and satellite retrievals. In this paper, we examine measurements from the Atmospheric Tomography (ATom, 4 deployments in 2016–2018) and the HIAPER Pole-to-Pole Observations (HIPPO; 5 deployments in 2009–2011) experiments, two global-scale airborne campaigns covering the Pacific (HIPPO and ATom) and Atlantic (ATom) basins. ATom and HIPPO represent the first global-scale, vertically resolved measurements of O3 distributions throughout the troposphere, with HIPPO sampling the Pacific basin and ATom sampling both the Pacific and Atlantic basins. Given the relatively limited temporal resolution of these two campaigns, we first compare ATom and HIPPO ozone data to longer-term observational records to establish the representativeness of our dataset. We show that these two airborne campaigns captured on average 53, 54, and 38 % of the ozone variability in the marine boundary layer, free troposphere, and upper troposphere/lower stratosphere (UTLS), respectively, at nine well-established ozonesonde sites. Additionally, ATom captured the most frequent ozone concentrations measured by regular commercial aircraft flights in the northern Atlantic UTLS. We then use the repeated vertical profiles carried out during these two campaigns to provide a global-scale picture of tropospheric ozone spatial and vertical distributions throughout the remote troposphere. We highlight a clear hemispheric gradient, with greater ozone in the northern hemisphere consistent with greater precursor emissions. We also show that the ozone distribution below 8 km was similar in the extra-tropics of the Atlantic and Pacific basins due to zonal circulation patterns. However, twice as much ozone was found in the tropical Atlantic than in the tropical Pacific, due to well-documented dynamical patterns transporting continental air masses over the Atlantic. We finally show that the seasonal variability of tropospheric ozone over the Pacific and the Atlantic basins is driven by transported continental plumes and photochemistry, and the vertical distribution is driven by photochemistry and mixing with stratospheric air. This new dataset is essential for improving our understanding of both ozone production and loss processes in remote regions, as well as the influence of anthropogenic emissions on baseline ozone.
Abstract. Daily global analyses and 5 day forecasts are generated in the context of the European Monitoring Atmospheric Composition and Climate (MACC) project using an extended version of the Integrated Forecasting System (IFS) of the European Centre for Medium-Range Weather Forecasts (ECMWF). IFS now includes modules for chemistry, deposition and emission of reactive gases, aerosols, and greenhouse gases, and the 4-dimensional variational data assimilation scheme makes use of multiple satellite observations of atmospheric composition in addition to meteorological observations. This paper describes the data assimilation setup of the new Composition-IFS (C-IFS) with respect to reactive gases and validates analysis fields of ozone (O3), carbon monoxide (CO), and nitrogen dioxide (NO2) for the year 2008 against independent observations and a control run without data assimilation. The largest improvement in CO by assimilation of MOPITT CO columns is seen in the lower troposphere of the Northern Hemisphere (NH) Extratropics during winter, and during the South African biomass burning season. The assimilation of several O3 total column and stratospheric profile retrievals greatly improves the total column, stratospheric and upper tropospheric O3 analysis fields relative to the control run. The impact on lower tropospheric ozone, which comes from the residual of the total column and stratospheric profile O3 data, is smaller, but nevertheless there is some improvement particularly in the NH during winter and spring. The impact of the assimilation of OMI tropospheric NO2 columns is small because of the short lifetime of NO2, suggesting that NO2 observations would be better used to adjust emissions instead of initial conditions. The results further indicate that the quality of the tropospheric analyses and of the stratospheric ozone analysis obtained with the C-IFS system has improved compared to the previous "coupled" model system of MACC.
Abstract. Tropical tropospheric ozone (TTO) is important for the global radiation budget because the longwave radiative effect of tropospheric ozone is higher in the tropics than midlatitudes. In recent decades the TTO burden has increased, partly due to the ongoing shift of ozone precursor emissions from midlatitude regions toward the Equator. In this study, we assess the distribution and trends of TTO using ozone profiles measured by high-quality in situ instruments from the IAGOS (In-Service Aircraft for a Global Observing System) commercial aircraft, the SHADOZ (Southern Hemisphere ADditional OZonesondes) network, and the ATom (Atmospheric Tomographic Mission) aircraft campaign, as well as six satellite records reporting tropical tropospheric column ozone (TTCO): TROPOspheric Monitoring Instrument (TROPOMI), Ozone Monitoring Instrument (OMI), OMI/Microwave Limb Sounder (MLS), Ozone Mapping Profiler Suite (OMPS)/Modern-Era Retrospective analysis for Research and Applications version 2 (MERRA-2), Cross-track Infrared Sounder (CrIS), and Infrared Atmospheric Sounding Interferometer (IASI)/Global Ozone Monitoring Experiment 2 (GOME2). With greater availability of ozone profiles across the tropics we can now demonstrate that tropical India is among the most polluted regions (e.g., western Africa, tropical South Atlantic, Southeast Asia, Malaysia and Indonesia), with present-day 95th percentile ozone values reaching 80 nmol mol−1 in the lower free troposphere, comparable to midlatitude regions such as northeastern China and Korea. In situ observations show that TTO increased between 1994 and 2019, with the largest mid- and upper-tropospheric increases above India, Southeast Asia, and Malaysia and Indonesia (from 3.4 ± 0.8 to 6.8 ± 1.8 nmol mol−1 decade−1), reaching 11 ± 2.4 and 8 ± 0.8 nmol mol−1 decade−1 close to the surface (India and Malaysia–Indonesia, respectively). The longest continuous satellite records only span 2004–2019 but also show increasing ozone across the tropics when their full sampling is considered, with maximum trends over Southeast Asia of 2.31 ± 1.34 nmol mol−1 decade−1 (OMI) and 1.69 ± 0.89 nmol mol−1 decade−1 (OMI/MLS). In general, the sparsely sampled aircraft and ozonesonde records do not detect the 2004–2019 ozone increase, which could be due to the genuine trends on this timescale being masked by the additional uncertainty resulting from sparse sampling. The fact that the sign of the trends detected with satellite records changes above three IAGOS regions, when their sampling frequency is limited to that of the in situ observations, demonstrates the limitations of sparse in situ sampling strategies. This study exposes the need to maintain and develop high-frequency continuous observations (in situ and remote sensing) above the tropical Pacific Ocean, the Indian Ocean, western Africa, and South Asia in order to estimate accurate and precise ozone trends for these regions. In contrast, Southeast Asia and Malaysia–Indonesia are regions with such strong increases in ozone that the current in situ sampling frequency is adequate to detect the trends on a relatively short 15-year timescale.
