Decadal tropospheric ozone radiative forcing estimations with offline radiative modelling and IAGOS aircraft observations

Ozone is the third strongest anthropogenic greenhouse gas with highest radiative efficiency in the tropical upper troposphere. Variability driven by El Niño‐Southern Oscillation (ENSO) modulates tropospheric column ozone instantaneous radiative forcing (TCO‐IRF) through changes in atmospheric dynamics, natural emissions, and stratospheric‐tropospheric exchange in the tropics. Using the Geophysical Fluid Dynamics Laboratory Atmospheric Model v4.1, which includes detailed ozone chemistry, we analyze the impacts of drivers on the ozone profile associated with El Niño and La Niña events between 2004 and 2019. Findings show that alongside ENSO‐driven atmospheric circulation changes, lightning‐induced nitrogen oxide over Atlantic and Pacific oceans, subtropical stratospheric intrusions, and biomass burning in equatorial Asia significantly impact TCO‐IRF in the tropics. Additionally, radiative effects from tropical tropospheric ozone increase by up to 0.03 Wm−2 during La Niña seasons and weaken by 0.02 Wm−2 in El Niño seasons, highlighting the importance of assessing ENSO‐driven TCO‐IRF variability for understanding future climate.

A tropospheric ozone time series from 1995 until end 2022 has been generated within ESA’s Climate Change Initiative+ programme. The GOME-type Tropical Tropospheric Ozone Essential Climate Variable (GTTO-ECV) satellite data record combines data from GOME, SCIAMACHY, OMI and the three GOME-2 missions. The retrieval is based on the Convective Cloud Differential technique, which limits the coverage to the tropical belt (20°S to 20°N). We generated two monthly mean data sets at 1° x 1° resolution: one corresponds to a tropospheric column up to 200 hPa as in the previous CCI data release (Heue et al., 2016), while the other is limited to 270 hPa and includes the operational Sentinel-5P data as an additional sensor. An internal reprocessing of S5P CCD using 200 hPa is planned but might not be ready in time. Besides a consistent reprocessing of the CCD data for individual sensors, we also updated the harmonising scheme. The mean bias as well as the mean annual cycle relative to the reference instrument (OMI) are used to correct for the differences between the sensors.Heue et al (2016) claimed a mean tropospheric ozone trend of +0.7 DU/decade (1995-2015). How did the trend change with the extended data set? The GTTO-ECV data record will be used to investigate the tropical mean trend as well as temporal and local changes in the trends. Also, a comparison with modelled tropospheric ozone data and the respective trends might be given.As a second data product we provide the global S5P-BASCOE tropospheric ozone data. The complete time series of the S5P total ozone columns has been reprocessed recently. The reprocessing includes an update of the Level1 data as well as reprocessed cloud and O3 total columns. We use the reprocessed OFFL ozone data set in combination with BASCOE assimilation constrained stratospheric ozone profiles to calculate the tropospheric ozone columns. Relative to ground-based observations the total OFFL columns show a small positive bias. Before the retrieval of the tropospheric ozone column this bias is subtracted. The updated tropospheric ozone columns might also be compared to modelled tropospheric ozone columns.

The satellite measurements in nadir and limb viewing geometry provide a complementary view of the atmosphere. An effective combination of the limb and nadir measurements can provide a new information about atmospheric composition. In this work, we present tropospheric ozone column datasets that have been created using combination of total ozone column from OMI and TROPOMI with stratospheric ozone column dataset from several available limb-viewing instruments (MLS, OSIRIS, MIPAS, SCIAMACHY, OMPS-LP, GOMOS). We have developed further the methodological aspects of assessment of tropospheric ozone using the residual method using simulations with the chemistry-transport model SILAM. It has been shown that the accurate assessment of ozone in the upper troposphere and the lower stratosphere (UTLS) is of high importance for detecting the ground-level ozone patterns. The stratospheric ozone column is derived from a combination of ozone profiles from several satellite instruments in limb-viewing geometry. We developed a method for the data homogenization, which includes the removal of biases and a-posteriori estimation (validation) of random uncertainties, thus making the data from different instruments compatible with each other. The high horizontal and vertical resolution dataset of ozone profiles is created via interpolation of the limb profiles from each day to 1° × 1° horizonal grid. A new kriging-type interpolation method, which takes into account data uncertainties and the information about natural ozone variations from the SILAM-adjusted ozone field, has been developed. To mitigate the limited accuracy and coverage of the limb profile data in the UTLS, a smooth transition to the model data is applied below the tropopause. This allows estimation of stratospheric ozone column with full coverage of the UTLS. The derived ozone profiles are in very good agreement with collocated ozonesonde measurements. The residual method was successfully applied to OMI and TROPOMI clear-sky total ozone data in combination with the stratospheric ozone column from the high-resolution limb profile dataset. The resulting tropospheric ozone column is in very good agreement with other satellite data. The global distributions of tropospheric ozone exhibit enhancements associated with the regions of high tropospheric ozone production. The main created datasets are (i) monthly 1° × 1° global tropospheric ozone column dataset using OMI and limb instruments, (ii) monthly 1° × 1° global tropospheric ozone column dataset using TROPOMI and limb instruments and (iii) daily 1° × 1° interpolated stratospheric ozone column from limb instruments. Other datasets, which are created as an intermediate step of creating the tropospheric ozone column data, are: (i) daily 1° × 1° clear sky and total ozone column from OMI and TROPOMI (ii) Daily 1° × 1° homogenized and interpolated dataset of ozone profiles and (iii) daily 1° × 1° dataset of ozone profiles from SILAM simulations with adjustment to satellite data. These datasets can be used in various studies related to ozone distributions, variability and trends, both in the troposphere and the stratosphere.

This study uses the tropospheric ozone data derived from combined observations of Ozone Monitoring Instrument/Microwave Limb Sounder instruments by using the tropospheric ozone residual method. The main objective was to study the spatial distribution and temporal evolution in the troposphere ozone columns over Pakistan during the time period of 2004 to 2014. Results showed an overall increase of 3.2 ± 1.1DU in tropospheric ozone columns over Pakistan. Spatial distribution showed enhanced ozone columns in the Punjab and southern Sindh consistent to high population, urbanization, and extensive anthropogenic activities, and exhibited statistically significant temporal increase. Seasonal variations in tropospheric ozone columns are driven by various factors such as seasonality in UV-B fluxes, seasonality in ozone precursor gases such as NOx and volatile organic compounds (caused by temperature dependent biogenic emission) and agricultural fire activities in Pakistan. A strong correlation of 96% (r = 0.96) was found between fire events and tropospheric ozone columns in Pakistan.

This study analyzes tropospheric column ozone variability in the southern hemisphere as a function of ozone transport from the stratosphere to the troposphere and photochemical formation. Geographically, the study area was located in the mid-latitudes in South America (33 degrees S), to the west of the Andes mountain range, in an area highly susceptible to stratospheric intrusions. Monthly ozonesonde measurements were recorded in Colina to ascertain seasonal vertical ozone distribution from the surface to the stratosphere between September 2010 and May 2012. Vertical distribution of the tropospheric ozone was measured in Talagante for fronts crossing from west to east in central Chile, during two periods in September 2014 and March 2015. These periods were significantly different in terms of the stratospheric ozone annual cycle and height of the tropopause. Our results showed rapid increases of approximately 50% in the tropospheric column ozone at time intervals shorter than 1 week. At the surface level, unusually enhanced ozone levels up to 10 parts per billion volume (ppbv) were observed during nighttime. Additionally, stratosphere-troposphere exchange (STE) preferentially occurred in spring and winter, with higher contribution during spring when the tropospheric column ozone attained its maximum concentration. These results provide valuable information regarding tropospheric ozone, a major local and global climate pollutant, to decision makers. In addition, they provide the research community with experimental data from the southern hemisphere, which helps bridge knowledge gaps in a region that has been rarely studied by national and international scientific communities.

Abstract. We present a new tropospheric ozone dataset based on TROPOspheric Monitoring Instrument (TROPOMI)/Sentinel-5 Precursor (S5P) total ozone measurements combined with stratospheric ozone data from the Belgian Assimilation System for Chemical ObsErvations (BASCOE) constrained by assimilating ozone observations from the Microwave Limb Sounder (MLS). The BASCOE stratospheric data are interpolated to the S5P observations and subtracted from the TROPOMI total ozone data. The difference is equal to the tropospheric ozone residual column from the surface up to the tropopause. The tropospheric ozone columns are retrieved at the full spatial resolution of the TROPOMI sensor (5.5×3.5 km2) with daily global coverage. Compared to the Ozone Mapping and Profiler Suite Modern-Era Retrospective analysis for Research and Applications 2 (OMPS-MERRA-2) data, a global mean positive bias of 3.3 DU is found for the analysed period April 2018 to June 2020. A small negative bias of about −0.91 DU is observed in the tropics relative to the operational TROPOMI tropical tropospheric data based on the convective cloud differential (CCD) algorithm throughout the same period. The new tropospheric ozone data (S5P-BASCOE) are compared to a set of globally distributed ozonesonde data integrated up to the tropopause level. We found 2254 comparisons with cloud-free TROPOMI observations within 25 km of the stations. In the global mean, S5P-BASCOE deviates by 2.6 DU from the integrated ozonesondes. Depending on the latitude the S5P-BASCOE deviate from the sondes and between −4.8 and 7.9 DU, indicating a good agreement. However, some exceptional larger positive deviations up to 12 DU are found, especially in the northern polar regions (north of 70∘). The monthly mean tropospheric column and time series for selected areas showed the expected spatial and temporal pattern, such as the wave one structure in the tropics or the seasonal cycle, including a summer maximum, in the mid-latitudes.

Abstract. Stratosphere-to-troposphere transport (STT) provides an important natural source of ozone to the upper troposphere, but the characteristics of STT events in the Southern Hemisphere extratropics and their contribution to the regional tropospheric ozone budget remain poorly constrained. Here, we develop a quantitative method to identify STT events from ozonesonde profiles. Using this method we estimate the seasonality of STT events and quantify the ozone transported across the tropopause over Davis (69° S, 2006–2013), Macquarie Island (54° S, 2004–2013), and Melbourne (38° S, 2004–2013). STT seasonality is determined by two distinct methods: a Fourier bandpass filter of the vertical ozone profile and an analysis of the Brunt–Väisälä frequency. Using a bandpass filter on 7–9 years of ozone profiles from each site provides clear detection of STT events, with maximum occurrences during summer and minimum during winter for all three sites. The majority of tropospheric ozone enhancements owing to STT events occur within 2.5 and 3 km of the tropopause at Davis and Macquarie Island respectively. Events are more spread out at Melbourne, occurring frequently up to 6 km from the tropopause. The mean fraction of total tropospheric ozone attributed to STT during STT events is ∼ 1. 0–3. 5 % at each site; however, during individual events, over 10 % of tropospheric ozone may be directly transported from the stratosphere. The cause of STTs is determined to be largely due to synoptic low-pressure frontal systems, determined using coincident ERA-Interim reanalysis meteorological data. Ozone enhancements can also be caused by biomass burning plumes transported from Africa and South America, which are apparent during austral winter and spring and are determined using satellite measurements of CO. To provide regional context for the ozonesonde observations, we use the GEOS-Chem chemical transport model, which is too coarsely resolved to distinguish STT events but is able to accurately simulate the seasonal cycle of tropospheric ozone columns over the three southern hemispheric sites. Combining the ozonesonde-derived STT event characteristics with the simulated tropospheric ozone columns from GEOS-Chem, we estimate STT ozone flux near the three sites and see austral summer dominated yearly amounts of between 5. 7 and 8. 7 × 1017 molecules cm−2 a−1.

The Tropospheric Emission Spectrometer (TES) is an infrared, high‐resolution Fourier transform spectrometer which was launched onboard NASA's Aura satellite in 2004 and is providing global, vertically resolved measurements of ozone in the troposphere. TES version 2 (V002) data profiles have been validated in the troposphere and lower stratosphere by way of comparison to ozonesondes and aircraft measurements. TES measurements also have sensitivity throughout the stratosphere, and therefore TES ozone profiles can be integrated to determine the total and stratospheric column in addition to the tropospheric column ozone values. In this work we compare the ozone in the stratosphere measured by TES to observations from the Microwave Limb Sounder (MLS) instrument in order to show the quality of the TES measurements in the stratosphere. We also compare the determination of a total column value for ozone based on the TES profiles to the column measured by the Ozone Monitoring Instrument (OMI). The TES tropospheric ozone column value is also calculated from the TES profiles and compared with column values determined from ozonesonde data. Column measurements are useful because the errors are markedly reduced from errors at the profile levels and can be used to assess both biases and quality of the TES ozone retrievals. TES observations of total or partial column ozone compare well with the other instruments but tend toward higher values than the other measurements. Specifically, TES is higher than OMI by ∼10 Dobson units (DU) for the total ozone column. TES measures higher values in the stratosphere (above 100 hPa) by ∼3 DU and measures higher ozone column values (∼4 DU) in the troposphere than ozonesondes. While the strength of the TES nadir ozone product is the vertical resolution it provides in the troposphere, a tropospheric column value derived from TES have utility in analyses using or validating tropospheric ozone residual products.

Tropospheric ozone is known as surface ozone and caused several health impact. The objective of this study was to analysis spatial distribution of tropospheric ozone over Indonesia case study forest fire event in 2015. Monthly observation measured by Ozone Monitoring Instrument (OMI) have been analysed from January – December 2015 to study spatial distribution of tropospheric ozone related to forest fire event 2015. The study discovered high level of tropospheric column ozone (TCO) from October to November 2015. The result shows increasing average of TCO from September to October almost 6 DU. Meanwhile, monthly number of hotspot is higher in September 2015 with total number 257 hotspot which is acquired by Moderate Resolution Imaging Spectrometer (MODIS) Terra version 6.1 with confidence level same or more than 90%. The hotspot distribution compared with spatial TCO distribution and shows interesting time lag with respect to hotspot distribution, one month. Further study for daily comparison of TCO and forest fire event needed. This result suggested that the tropospheric ozone over the Indonesian region increases in 2015 were remarkable and corresponded to forest fire event.

Abstract. Non-methane volatile organic compounds (NMVOCs) influence air quality and global climate change through their effects on secondary air pollutants and climate forcers. Here we simulate the air quality and radiative forcing (RF) impacts of changes in ozone, methane, and sulfate from halving anthropogenic NMVOC emissions globally and from 10 regions individually, using a global chemical transport model and a standalone radiative transfer model. Halving global NMVOC emissions decreases global annual average tropospheric methane and ozone by 36.6 ppbv and 3.3 Tg, respectively, and surface ozone by 0.67 ppbv. All regional reductions slow the production of peroxyacetyl nitrate (PAN), resulting in regional to intercontinental PAN decreases and regional NOx increases. These NOx increases drive tropospheric ozone increases nearby or downwind of source regions in the Southern Hemisphere (South America, Southeast Asia, Africa, and Australia). Some regions' NMVOC emissions contribute importantly to air pollution in other regions, such as East Asia, the Middle East, and Europe, whose impact on US surface ozone is 43%, 34%, and 34% of North America's impact. Global and regional NMVOC reductions produce widespread negative net RFs (cooling) across both hemispheres from tropospheric ozone and methane decreases, and regional warming and cooling from changes in tropospheric ozone and sulfate (via several oxidation pathways). The 100 yr and 20 yr global warming potentials (GWP100, GWP20) are 2.36 and 5.83 for the global reduction, and 0.079 to 6.05 and −1.13 to 18.9 among the 10 regions. The NMVOC RF and GWP estimates are generally lower than previously modeled estimates, due to the greater NMVOC/NOx emissions ratios simulated, which result in less sensitivity to NMVOC emissions changes and smaller global O3 burden responses, in addition to differences in the representation of NMVOCs and oxidation chemistry among models. Accounting for a fuller set of RF contributions may change the relative magnitude of each region's impacts. The large variability in the RF and GWP of NMVOCs among regions suggest that regionally specific metrics may be necessary to include NMVOCs in multi-gas climate trading schemes.

Abstract. A global climatology of tropospheric and stratospheric column ozone is derived by combining six years of Aura Ozone Monitoring Instrument (OMI) and Microwave Limb Sounder (MLS) ozone measurements for the period October 2004 through December 2010. The OMI/MLS tropospheric ozone climatology exhibits large temporal and spatial variability which includes ozone accumulation zones in the tropical south Atlantic year-round and in the subtropical Mediterranean/Asia region in summer months. High levels of tropospheric ozone in the Northern Hemisphere also persist in mid-latitudes over the eastern part of the North American continent extending across the Atlantic Ocean and the eastern part of the Asian continent extending across the Pacific Ocean. For stratospheric ozone climatology from MLS, largest column abundance is in the Northern Hemisphere in the latitude range 70° N–80° N in February–April and in the Southern Hemisphere around 40° S–50° S during August–October. Largest stratospheric ozone lies in the Northern Hemisphere and extends from the eastern Asian continent eastward across the Pacific Ocean and North America. With the advent of many newly developing 3-D chemistry and transport models it is advantageous to have such a dataset for evaluating the performance of the models in relation to dynamical and photochemical processes controlling the ozone distributions in the troposphere and stratosphere. The OMI/MLS gridded ozone climatology data are made available to the science community via the NASA Goddard Space Flight Center ozone and air quality website http://ozoneaq.gsfc.nasa.gov/.

Global distributions of the tropospheric ozone column (TOC) and its error are estimated by assimilating satellite observations of total ozone column and stratospheric ozone profiles in a global chemistry‐transport model. A quantitative comparison of the calculated TOC with collocated ozonesondes observations shows good agreement over a wide range of latitudes for the period studied (July–September 1992), even at the daily timescale. In most cases, the difference with the ozonesonde‐based TOC is within the calculated error estimate. Comparison with the TOC distribution by Thompson and Hudson [1999] does not lead to any quantitative conclusion due to a mix of similarities and differences, even in the geographical distribution of the TOC. A positive TOC bias with respect to ozonesondes is found in this study over Hilo and Irene, probably due to a misrepresentation of the transport of ozone in a region of strong TOC gradients. In September 1992 the LIDAR observations from the TRACE‐A campaign are also assimilated. This is shown to provide a constraint on the TOC that significantly propagates across the Atlantic Ocean, indicating the importance of point measurements of ozone for constraining its large‐scale distribution.

Abstract. The Geostationary Environment Monitoring Spectrometer (GEMS) is scheduled to be launched in 2019–2020 on board the GEO-KOMPSAT (GEOstationary KOrea Multi-Purpose SATellite)-2B, contributing as the Asian partner of the global geostationary constellation of air quality monitoring. To support this air quality satellite mission, we perform a cross-evaluation of simulated GEMS ozone profile retrievals from OMI (Ozone Monitoring Instrument) data based on the optimal estimation and ozonesonde measurements within the GEMS domain, covering from 5∘ S (Indonesia) to 45∘ N (south of the Russian border) and from 75 to 145∘ E. The comparison between ozonesonde and GEMS shows a significant dependence on ozonesonde types. Ozonesonde data measured by modified Brewer–Mast (MBM) at Trivandrum and New Delhi show inconsistent seasonal variabilities in tropospheric ozone compared to carbon–iodine (CI) and electrochemical condensation cell (ECC) ozonesondes at other stations in a similar latitude regime. CI ozonesonde measurements are negatively biased relative to ECC measurements by 2–4 DU; better agreement is achieved when simulated GEMS ozone retrievals are compared to ECC measurements. ECC ozone data at Hanoi, Kuala Lumpur, and Singapore show abnormally worse agreements with simulated GEMS retrievals than other ECC measurements. Therefore, ECC ozonesonde measurements at Hong Kong, Pohang, Naha, Sapporo, and Tsukuba are finally identified as an optimal reference dataset. The accuracy of simulated GEMS retrievals is estimated to be ∼5.0 % for both tropospheric and stratospheric column ozone with the precision of 15 % and 5 %, which meets the GEMS ozone requirements.

Radiative forcing calculations of changes in tropospheric ozone in the period 1980 to 1996 are performed. The tropospheric ozone changes used in this study are from a chemistry transport model [Karlsdóttir et al., this issue]. For the radiative transfer calculations, schemes for thermal infrared radiation and shortwave radiation are used. Effects of reduced stratospheric ozone and emissions of tropospheric ozone precursors on the changes in tropospheric ozone are taken into account. Large positive radiative forcing is estimated over Southeast Asia, due to emissions of ozone precursors. Effects of decreased stratospheric ozone have reduced the radiative forcing due to change in tropospheric ozone from 1980 to 1996, particularly at high latitudes where the radiative forcing is negative.

Observational records of meteorological and chemical variables are imprinted by an unknown combination of anthropogenic activity, natural forcings, and internal variability. With a 15-member initial-condition ensemble generated from the CESM2-WACCM6 chemistry-climate model for 1950–2014, we extract signals of anthropogenic (‘forced’) change from the noise of internally arising climate variability on observed tropospheric ozone trends. Positive trends in free tropospheric ozone measured at long-term surface observatories, by commercial aircraft, and retrieved from satellite instruments generally fall within the ensemble range. CESM2-WACCM6 tropospheric ozone trends are also bracketed by those in a larger ensemble constructed from five additional chemistry-climate models. Comparison of the multi-model ensemble with observed tropospheric column ozone trends in the northern tropics implies an underestimate in regional precursor emission growth over recent decades. Positive tropospheric ozone trends clearly emerge from 1950 to 2014, exceeding 0.2 DU yr−1 at 20–40 N in all CESM2-WACCM6 ensemble members. Tropospheric ozone observations are often only available for recent decades, and we show that even a two-decade record length is insufficient to eliminate the role of internal variability, which can produce regional tropospheric ozone trends oppositely signed from ensemble mean (forced) changes. By identifying regions and seasons with strong anthropogenic change signals relative to internal variability, initial-condition ensembles can guide future observing systems seeking to detect anthropogenic change. For example, analysis of the CESM2-WACCM6 ensemble reveals year-round upper tropospheric ozone increases from 1995 to 2014, largest at 30 S–40 N during boreal summer. Lower tropospheric ozone increases most strongly in the winter hemisphere, and internal variability leads to trends of opposite sign (ensemble overlaps zero) north of 40 N during boreal summer. This decoupling of ozone trends in the upper and lower troposphere suggests a growing prominence for tropospheric ozone as a greenhouse gas despite regional efforts to abate warm season ground-level ozone.