Constraining tropospheric ozone column through data assimilation

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.

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.

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.

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.

<strong class="journal-contentHeaderColor">Abstract.</strong> This study evaluates the future evolution of atmospheric ozone between 2015 and 2099 simulated with the Earth System Model (ESM) SOCOLv4. Simulations have been performed based on two potential Shared Socioeconomic Pathways (SSP): the &ldquo;middle-of-the-road&rdquo; (SSP2-4.5) and &ldquo;fossil-fueled&rdquo; (SSP5-8.5) scenarios. In both scenarios, the model projects a decline in tropospheric ozone in the future that starts in the 2030s in SSP2-4.5 and after the 2060s in SSP5-8.5 due to a decrease in concentrations of ozone precursors like NO_x and CO. The results also suggest a very likely ozone increase in the mesosphere, upper and middle stratosphere, as well as at high latitudes of the lower stratosphere. Under SSP5-8.5, the ozone increase in the stratosphere is higher because of stronger cooling (&gt; 1 &deg;K/decade) induced by the greenhouse gases (GHG), which slows the catalytic ozone destruction cycles. In contrast, in the tropical lower stratosphere ozone concentrations decrease in both experiments and increase over the middle and high latitudes of both hemispheres due to the intensification of meridional transport, which is stronger in SSP5-8.5. No evidence was found of a decline in ozone levels in the lower stratosphere at mid-latitudes. In both future scenarios, the total column ozone is expected to be distinctly higher than present in mid-to-high latitudes and might be lower in the tropics, which causes a decrease/increase in the surface level of UV radiation. The results of SOCOLv4 suggest that the stratospheric ozone evolution throughout the 21^st century is strongly governed not only by a decline in halogen concentration, but also by future GHGs forcing. In addition, the tropospheric ozone column changes, mainly due to the changes in anthropogenic emissions of ozone precursors, also have a strong impact on the total column. Therefore, even though the anthropogenic halogen loading problem has been brought under control to date, the sign of future ozone column changes, globally and regionally, is still unclear and largely depends on diverse future human activities. The results of this work are, thus, relevant for developing future strategies for socioeconomic pathways.

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.

The GASCOD (Gas Analyzer Spectrometer Correlating Optical Differences) has been installed at the 'Mario Zucchelli' Antarctic station since 1996. It measures the zenith sky radiation in the 405-465 nm spectral range in unattended and automatic mode. The application to the spectral data of the DOAS (Differential Optical Absorption Spectroscopy) algorithms coupled with a Radiative Transfer Model (RTM) for the computation of the Air Mass Factor (AMF), allows for the retrieval of the total content of the main absorber in this spectral range, namely nitrogen dioxide (NO2). Moreover, the application of sophisticated inversion schemes to the output of the DOAS program, using the AMF matrix as the kernel of the inversion algorithm, permits the determination of the vertical distribution of the above mentioned compound. The full dataset of the spectral data obtained with GASCOD during the period 1996-2008, was re-analyzed with a modified version of the software tool previously utilized. Even if the spectral range examined with GASCOD is not the most favorable for the ozone total column and vertical profile retrieval, the re-processing of the spectral data allowed for the determination of the total ozone columns (TOC). The uncertainties range from 4% to 8% for ozone and 3% to 6% for NO2. The peculiar features of the seasonal variation of NO2 total columns (i.e. the normal decreasing during the austral fall and the irregular growing towards the summer month) are presented and discussed. The confirmations of the significant declining of the ozone total columns during the 'Ozone Hole' periods (mid-August to mid-October) are reported. The vertical distributions obtained for the preceding atmospheric compounds are shown and examined.

Ozone changes and associated climate impacts in the Coupled Model Intercomparison Project Phase 5 (CMIP5) simulations are analyzed over the historical (1960–2005) and future (2006–2100) period under four Representative Concentration Pathways (RCP). In contrast to CMIP3, where half of the models prescribed constant stratospheric ozone, CMIP5 models all consider past ozone depletion and future ozone recovery. Multimodel mean climatologies and long‐term changes in total and tropospheric column ozone calculated from CMIP5 models with either interactive or prescribed ozone are in reasonable agreement with observations. However, some large deviations from observations exist for individual models with interactive chemistry, and these models are excluded in the projections. Stratospheric ozone projections forced with a single halogen, but four greenhouse gas (GHG) scenarios show largest differences in the northern midlatitudes and in the Arctic in spring (~20 and 40 Dobson units (DU) by 2100, respectively). By 2050, these differences are much smaller and negligible over Antarctica in austral spring. Differences in future tropospheric column ozone are mainly caused by differences in methane concentrations and stratospheric input, leading to ~10 DU increases compared to 2000 in RCP 8.5. Large variations in stratospheric ozone particularly in CMIP5 models with interactive chemistry drive correspondingly large variations in lower stratospheric temperature trends. The results also illustrate that future Southern Hemisphere summertime circulation changes are controlled by both the ozone recovery rate and the rate of GHG increases, emphasizing the importance of simulating and taking into account ozone forcings when examining future climate projections.

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.

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.

The Madden-Julian Oscillation (MJO) is the leading mode of intra-seasonal variability in the tropical troposphere, characterized by an eastward moving ‘pulse’ of cloud and rainfall near the equator. In this study, total precipitable water (TPW) and total column ozone (TCO) datasets from ECMWF ERA-Interim reanalysis were used to analyse the impact of the MJO on the distribution of water vapor and column ozone in the tropics from 1979 to 2013. The results show that seasonal variations of TPW modulated by the MJO are maximized in the tropics of about 10°S-10°N during boreal winter, while the variation in TCO is maximized in the mid-latitudes of about 30°S - 40°N in the same season. The composite analysis shows that MJO modulates TPW and TCO anomalies eastward across the globe. The underlying mechanism of the MJO’s impact on TPW is mainly associated with variation of tropical convection modulated by the MJO, while the underlying mechanism of the MJO’s impact on TCO is mainly associated with an intra-seasonal variability of tropopause height modulated by the MJO activity. This knowledge helps to improve the prediction skill of the intra-seasonal variation of water vapor and column ozone in the tropics during boreal winter.

Abstract. We derived global tropospheric ozone (O3) columns from GOME-2A (Global Ozone Monitoring Experiment) and OMI (Ozone Monitoring Instrument) O3 profiles, which were simultaneously assimilated into the TM5 (Tracer Model, version 5) global chemistry transport model for the year 2008. The horizontal model resolution has been increased by a factor of 6 for more accurate results. To reduce computational cost, the number of model layers has been reduced from 44 to 31. The model ozone fields are used to derive tropospheric ozone, which is defined here as the partial column between mean sea level and 6 km altitude. Two methods for calculating the tropospheric columns from the free model run and assimilated O3 fields are compared. In the first method, we calculate the residual between assimilated total columns and the partial model column between 6 km and the top of atmosphere. In the second method, we perform a direct integration of the assimilated O3 fields between the surface and 6 km. The results are validated against tropospheric columns derived from ozone sonde measurements. Our results show that the residual method has too large a variation to be used reliably for the determination of tropospheric ozone, so the direct integration method has been used instead. The median global bias is smaller for the assimilated O3 fields than for the free model run, but the large variation makes it difficult to make definitive statements on a regional or local scale. The monthly mean ozone fields show significant improvements and more detail when comparing the assimilated O3 fields with the free model run, especially for features such as biomass-burning-enhanced O3 concentrations and outflow of O3 rich air from Asia over the Pacific.

Abstract. Observations of trace gases, such as O3, HCHO, and NO2, and their seasonal dependence can be made using satellite and ground-based data from the Ozone Monitoring Instrument (OMI) satellite and Pandora ground-based instruments. Both operate with spectrometers that have similar characteristics in wavelength range and spectral resolution that enable them to retrieve total column amounts of formaldehyde (TCHCHO) and nitrogen dioxide (TCNO2) and total column ozone (TCO). The polar orbiting OMI observes at 13:30 ± 0:25 LST (local solar time) plus an occasional second side-scan point 90 min later at mid-latitudes. The ground-based Pandora spectrometer system observes the direct sun all day, with a temporal resolution of 2 min. At most sites, the Pandora data show a strong seasonal dependence for TCO and TCHCHO and less seasonal dependence for TCNO2. Use of a low-pass filter LOWESS(3-month) can reveal the seasonal dependence of TCNO2 for both OMI and Pandora at mid-latitude sites usually correlated with seasonal heating using natural gas or oil. Compared to Pandora, OMI underestimates the amount of NO2 air pollution that occurs during most days, as the OMI TCNO2 retrieval occurs around 13:30 ± 0:25 LST, which tends to be near the frequent minimum of the daily TCNO2 time series. Even when the Pandora data are restricted to between 13:00 and 14:00 LST, OMI retrieves less TCNO2 than Pandora over urban sites because of OMI's large field of view. The seasonal behavior of TCHCHO is mostly caused by the release of HCHO precursors from plant growth and emissions from lakes that peak in the summer, as observed by Pandora and OMI. Long-term averages show that OMI TCHCHO usually has the same seasonal dependence but differs in magnitude from the amount measured by Pandora and is frequently larger. Comparisons of OMI total column NO2 and HCHO with Pandora daily time series show both agreement and disagreement at various sites and for different days, with the Pandora results frequently being larger. For ozone, daily time-dependent comparisons of OMI TCO with those retrieved by Pandora show good agreement in most cases. Additional diurnal comparisons are shown of Pandora TCO with hourly retrievals during a day from the EPIC (Earth Polychromatic Imaging Camera) spacecraft instrument orbiting the Earth–Sun Lagrange point L1.