Deriving tropospheric ozone from assimilated profiles

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.

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.

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.

Retrievals from the Microwave Limb Sounder (MLS) and the Ozone Monitoring Instrument (OMI) on EOS‐Aura were included in the Goddard Earth Observing System version 4 (GEOS‐4) ozone data assimilation system. The distribution and daily to seasonal evolution of ozone in the stratosphere and troposphere during 2005 are investigated. In the lower stratosphere, where dynamical processes dominate, comparisons with independent ozonesonde and Measurement of Ozone and Water Vapour by Airbus In‐Service Aircraft (MOZAIC) data indicate mean agreement within 10%. In the troposphere, OMI and MLS provide constraints on the ozone column, but the ozone profile shape results from the parameterized ozone chemistry and the resolved and parameterized transport. Assimilation of OMI and MLS data improves tropospheric column estimates in the Atlantic region but leads to an overestimation in the tropical Pacific and an underestimation in the northern high and middle latitudes in winter and spring. Transport and data biases are considered in order to understand these discrepancies. Comparisons of assimilated tropospheric ozone columns with ozonesonde data reveal root‐mean‐square (RMS) differences of 2.9–7.2 Dobson units (DU), which are smaller than the model‐sonde RMS differences of 3.2–8.7 DU. Four different definitions of the tropopause using temperature lapse rate, potential vorticity (PV), and isentropic surfaces or ozone isosurfaces are compared with respect to their global impact on the estimated tropospheric ozone column. The largest sensitivity in the tropospheric ozone column is found near the subtropical jet, where the ozone‐ or PV‐determined tropopause typically lies below the lapse rate tropopause.

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.

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. 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/.

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 assimilate stratospheric ozone profiles from MLS (Microwave Limb Sounder) into the MOCAGE Chemistry Transport Model (CTM) to study Stratosphere-Troposphere Exchange (STE). This study uses two horizontal grid resolutions of 2° and 0.2°. The combined impacts of MLS ozone assimilation and high horizontal resolution are illustrated in two case studies where STE events occurred (23 June 2009 and 17 July 2009). At high resolution the filamentary structures of stratospheric air which characterise STE events are captured by the model. To test the impact of the assimilation and the resolution, we compare model outputs from different experiments (high resolution and low resolution; MLS assimilation run and free run) with independent data (MOZAIC aircraft ozone data; WOUDC ozone sonde network data). MLS ozone analyses show a better description of the Upper Troposphere Lower Stratosphere (UTLS) region and the stratospheric intrusions than the free model run. In particular, at high horizontal resolution the MLS ozone analyses present realistic filamentary ozone structures in the UTLS and laminae structures in the ozone profile. Despite a low aspect ratio between horizontal resolution and vertical resolution in the UTLS at high horizontal resolution, MLS ozone analyses improve the vertical structures of the ozone fields. Results from backward trajectories and ozone forecasts show that assimilation at high horizontal resolution of MLS ozone profiles between 10 hPa and 215 hPa has an impact on tropospheric ozone.

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.

Abstract. We have assessed the sensitivity of the operational Ozone Monitoring Instrument (OMI) ozone profile retrieval algorithm to a number of a priori and radiative transfer assumptions. We studied the effect of stray light correction, surface albedo assumptions and a priori ozone profiles on the retrieved ozone profile. Then, we studied how to modify the algorithm to improve the retrieval of tropospheric ozone. We found that stray light corrections have a significant effect on the retrieved ozone profile but mainly at high altitudes. Surface albedo assumptions, on the other hand, have the largest impact at the lowest layers. Choice of an ozone profile climatology which is used as a priori information has small effects on the retrievals at all altitudes. However, the usage of climatological a priori covariance matrix has a significant effect. Based on these sensitivity tests, we made several modifications to the retrieval algorithm: the a priori ozone climatology was replaced with a new tropopause-dependent climatology, the a priori covariance matrix was calculated from the climatological ozone variability values, and the surface albedo was assumed to be linearly dependent on wavelength in the 311.5–330 nm channel. As expected, we found that the a priori covariance matrix basically defines the vertical distribution of degrees of freedom for a retrieval. Moreover, our case study over Europe showed that the modified version produced over 10% smaller ozone abundances in the troposphere which reduced the systematic overestimation of ozone in the retrieval algorithm and improved correspondence with Infrared Atmospheric Sounding Instrument (IASI) retrievals. The comparison with ozonesonde measurements over North America showed that the operational retrieval performed better in the upper troposphere/lower stratosphere (UTLS), whereas the modified version improved the retrievals in the lower troposphere and upper stratosphere. These comparisons showed that the systematic biases in the OMI ozone profile retrievals are not caused by the a priori information but by some still unidentified problem in the radiative transfer modelling. Instead, the a priori information pushes the systematically wrong ozone profiles towards the true values. The smaller weight of the a priori information in the modified retrieval leads to better visibility of tropospheric ozone structures, because it has a smaller tendency to damp the variability of the retrievals in the troposphere. In summary, the modified retrieval unmasks systematic problems in the radiative transfer/instrument model and is more sensitive to tropospheric ozone variation; that is, it is able to capture the tropospheric ozone morphology better.

Measurements from the Ozone Monitoring Instrument (OMI) and Microwave Limb Sounder (MLS), both on board the Aura spacecraft, have been used to produce daily global maps of column and profile ozone since August 2004. Here we compare and evaluate three strategies to obtain daily maps of tropospheric and stratospheric ozone from OMI and MLS measurements: trajectory mapping, direct profile retrieval, and data assimilation. Evaluation is based on an assessment that includes validation using ozonesondes and comparisons with the Global Modeling Initiative (GMI) chemical transport model. We investigate applications of the three ozone data products from near‐decadal and interannual time scales to day‐to‐day case studies. Interannual changes in zonal mean tropospheric ozone from all of the products in any latitude range are of the order 1–2 Dobson units while changes (increases) over the 8 year Aura record investigated vary by 2–4 Dobson units. It is demonstrated that all of the ozone products can measure and monitor exceptional tropospheric ozone events including major forest fire and pollution transport events. Stratospheric ozone during the Aura record has several anomalous interannual events including split stratospheric warmings in the Northern Hemisphere extratropics that are well captured using the data assimilation ozone profile product. Data assimilation with continuous daily global coverage and vertical ozone profile information is the best of the three strategies at generating a global tropospheric and stratospheric ozone product for science applications.

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.

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.

ABSTRACTThe seasonal and inter annual variability of Tropospheric Nitrogen dioxide (NO2), Ozone (O3) and lightning activity over Maharashtra and adjoining part of states (15.5°N-22.5°N, 72.5°E-81.5°E) of India, is analyzed to study the role of lightning activity in the seasonal variation of NO2 and O3. Satellite observations of Tropospheric NO2 and O3 from Aura- Ozone Monitoring Instrument (OMI)/Microwave Limb Sounder (MLS) for the period 2005–2016 and lightning data of 2014–2016 from lightning detection network over Maharashtra are used for analysis. Analyses show that the seasonal variations of all the three quantities are closely related to each other. The scatter plot between monthly NO2 concentration verses monthly lightning activity for years 2014–2016 also show good correlation between these two parameters (r = 0.71, significant at 99.9%). Our analysis demonstrates that the seasonal and inter-annual variations in NO2 and O3 are affecting by lightning activity over study region. However, biomass burning during April-May and increased air pollution during winter months (November-January) also play important role in the intra seasonal variations of NO2 and O3 over this region.