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At least 361 records · Page 20

Estimation of Smoothing Error in SBUV Profile and Total Ozone Retrieval

Data from the Nimbus-4, Nimbus-7 Solar Backscatter Ultra Violet (SBUV) and seven of the NOAA series of SBUV/2 instruments spanning 41 years are being reprocessed using V8.6 algorithm. The data are scheduled to be released by the end of August 2011. An important focus of the new algorithm is to estimate various sources of errors in the SBUV profiles and total ozone retrievals. We discuss here the smoothing errors that describe the components of the profile variability that the SBUV observing system can not measure. The SBUV(/2) instruments have a vertical resolution of 5 km in the middle stratosphere, decreasing to 8 to 10 km below the ozone peak and above 0.5 hPa. To estimate the smoothing effect of the SBUV algorithm, the actual statistics of the fine vertical structure of ozone profiles must be known. The covariance matrix of the ensemble of measured ozone profiles with the high vertical resolution would be a formal representation of the actual ozone variability. We merged the MLS (version 3) and sonde ozone profiles to calculate the covariance matrix, which in general case, for single profile retrieval, might be a function of the latitude and month. Using the averaging kernels of the SBUV(/2) measurements and calculated total covariance matrix one can estimate the smoothing errors for the SBUV ozone profiles. A method to estimate the smoothing effect of the SBUV algorithm is described and the covariance matrixes and averaging kernels are provided along with the SBUV(/2) ozone profiles. The magnitude of the smoothing error varies with altitude, latitude, season and solar zenith angle. The analysis of the smoothing errors, based on the SBUV(/2) monthly zonal mean time series, shows that the largest smoothing errors were detected in the troposphere and might be as large as 15-20% and rapidly decrease with the altitude. In the stratosphere above 40 hPa the smoothing errors are less than 5% and between 10 and 1 hPa the smoothing errors are on the order of 1%. We validate our estimated smoothing errors by comparing the SBUV ozone profiles with other ozone profiling sensors.

Kramarova, N. A.↗

Multimodel Assessment of the Factors Driving Stratospheric Ozone Evolution over the 21st Century

The evolution of stratospheric ozone from 1960 to 2100 is examined in simulations from 14 chemistry-climate models, driven by prescribed levels of halogens and greenhouse gases. There is general agreement among the models that total column ozone reached a minimum around year 2000 at all latitudes, projected to be followed by an increase over the first half of the 21st century. In the second half of the 21st century, ozone is projected to continue increasing, level off, or even decrease depending on the latitude. Separation into partial columns above and below 20 hPa reveals that these latitudinal differences are almost completely caused by differences in the model projections of ozone in the lower stratosphere. At all latitudes, upper stratospheric ozone increases throughout the 21st century and is projected to return to 1960 levels well before the end of the century, although there is a spread among models in the dates that ozone returns to specific historical values. We find decreasing halogens and declining upper atmospheric temperatures, driven by increasing greenhouse gases, contribute almost equally to increases in upper stratospheric ozone. In the tropical lower stratosphere, an increase in upwelling causes a steady decrease in ozone through the 21st century, and total column ozone does not return to 1960 levels in most of the models. In contrast, lower stratospheric and total column ozone in middle and high latitudes increases during the 21st century, returning to 1960 levels well before the end of the century in most models.

Oman, L. D.↗

Quantifying TOLNet Ozone Lidar Accuracy During the 2014 DISCOVER-AQ and FRAPPE Campaigns

The Tropospheric Ozone Lidar Network (TOLNet) is a unique network of lidar systems that measure high-resolution atmospheric profiles of ozone. The accurate characterization of these lidars is necessary to determine the uniformity of the network calibration. From July to August 2014, three lidars, the TROPospheric OZone (TROPOZ) lidar, the Tunable Optical Profiler for Aerosol and oZone (TOPAZ) lidar, and the Langley Mobile Ozone Lidar (LMOL), of TOLNet participated in the Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) mission and the Front Range Air Pollution and Photochemistry Experiment (FRAPPA) to measure ozone variations from the boundary layer to the top of the troposphere. This study presents the analysis of the intercomparison between the TROPOZ, TOPAZ, and LMOL lidars, along with comparisons between the lidars and other in situ ozone instruments including ozonesondes and a P-3B airborne chemiluminescence sensor. The TOLNet lidars measured vertical ozone structures with an accuracy generally better than +/-15 % within the troposphere. Larger differences occur at some individual altitudes in both the near-field and far-field range of the lidar systems, largely as expected. In terms of column average, the TOLNet lidars measured ozone with an accuracy better than +/-5 % for both the intercomparison between the lidars and between the lidars and other instruments. These results indicate that these three TOLNet lidars are suitable for use in air quality, satellite validation, and ozone modeling efforts.

TOLNet↗

Atmospheric Ozone Response to the Disrupted 2015-2016 Quasi-Biennial Oscillation

The quasi-biennial oscillation (QBO) - a quasi-periodic alternation between easterly and westerly zonal winds in the tropical stratosphere - is a main driver of inter-annual ozone variability in the stratosphere. During the late-2015 through 2016 time period, the QBO experienced a major disruption unlike any observed since wind measurements began in 1953. We examined the ozone response to this QBO disruption using profile ozone measurements from the Aura Microwave Limb Sounder (MLS) and Ozone Mapping and Profiler Suite Limb Profiler and total column measurements from the Solar Backscatter Ultraviolet (SBUV) Merged Ozone Data Set (MOD). Positive anomalies in stratospheric equatorial O3 developed between 50 and 30 hPa in May-September of 2016, and negative ozone anomalies were observed in the subtropics of both hemispheres. As a consequence of this QBO disruption, extratropical total ozone values during the spring-summer 2016 were at or near seasonal record lows over the more than 40 years of the total ozone record, resulting in an increase of surface UV index during northern hemisphere summer. We found very consistent responses in all considered ozone observations in terms of time, amplitude and spatial patterns. We will show the ozone changes associated with this disrupted QBO throughout the winter and spring 2017.

Kramarova, N. A.↗

An Update on Ozone Profile Trends for the Period 2000 to 2016

Ozone profile trends over the period 2000 to 2016 from several merged satellite ozone data sets and from ground-based data measured by four techniques at stations of the Network for the Detection of Atmospheric Composition Change indicate significant ozone increases in the upper stratosphere, between 35 and 48 kilometers altitude (5 and 1 hectopascals). Near 2 hectopascals (42 kilometers), ozone has been increasing by about 1.5 percent per decade in the tropics (20 degrees S to 20 degrees N), and by 2 to 2.5 percent per decade in the 35 to 60 degree latitude bands of both hemispheres. At levels below 35 kilometers (5 hectopascals), 2000 to 2016 ozone trends are smaller and not statistically significant. The observed trend profiles are consistent with expectations from chemistry climate model simulations. This study confirms positive trends of upper stratospheric ozone already reported, e.g., in the WMO/UNEP (World Meteorological Organization/United Nations Environmental Programme) Ozone Assessment 2014 or by Harris et al. (2015). Compared to those studies, three to four additional years of observations, updated and improved data sets with reduced drift, and the fact that nearly all individual data sets indicate ozone increase in the upper stratosphere, all give enhanced confidence. Uncertainties have been reduced, for example for the trend near 2 hectopascals in the 35 to 60 degree latitude bands from about plus or minus 5 percent (2 sigma) in Harris et al. (2015) to less than plus or minus 2 percent (2 sigma). Nevertheless, a thorough analysis of possible drifts and differences between various data sources is still required, as is a detailed attribution of the observed increases to declining ozone-depleting substances and to stratospheric cooling. Ongoing quality observations from multiple independent platforms are key for verifying that recovery of the ozone layer continues as expected.

chemistry climate model simulations↗

Tropospheric Ozone in the NASA GEOS Model: Effects of Satellite NO2 Data Assimilation and Improvements in Background NOx Chemistry

Tropospheric ozone is a major atmospheric oxidant, the primary source of the hydroxyl radical, and a greenhouse gas. In the troposphere, it is produced from the oxidation of carbon monoxide and volatile organic compounds in the presence of nitrogen oxides (NOx=NO+NO2) or has its origins in the stratosphere. The tropospheric ozone burdens in global atmospheric chemistry models disagree by a factor of 1.5, indicating an incomplete understanding of ozone sources and sinks. Here we examine the tropospheric ozone simulation in NASA Global Modeling and Assimilation Office’s (GMAO’s) GEOS model with the GEOS-Chem chemistry mechanism (version 14.2), using observations from satellites, aircraft, ozonesondes, and surface sites. This modeling framework is used to produce GMAO’s GEOS Composition Forecasts (GEOS-CF), and it has been updated extensively with new emission inventories, improved model physics, satellite data assimilation capability, and an up-to-date chemical mechanism that includes tropospheric halogen chemistry and NOx recycling from particulate nitrate. Earlier versions of the model using GEOS-Chem version 12.0 showed an underestimate in tropospheric ozone in the northern hemisphere. We evaluate the ozone simulation in the updated model, focusing on the effects of assimilating satellite NO2 data from the Ozone Monitoring Instrument (OMI), constraining stratospheric ozone to satellite data, and updates to the NOx chemistry. We will examine changes in the vertical profiles of tropospheric ozone over the US in support of the Tropospheric Emissions: Monitoring of Pollution (TEMPO), and discuss implications for the tropospheric ozone budget.

V. Shah↗

Tropospheric Ozone in the NASA GEOS Model: Effects of Satellite Data Assimilation and Improvements in Background NO x Chemistry

Tropospheric ozone is a major atmospheric oxidant, the primary source of the hydroxyl radical, and a greenhouse gas. In the troposphere, it is produced from the oxidation of carbon monoxide and volatile organic compounds in the presence of nitrogen oxides (NO x =NO+NO 2 ) or has its origins in the stratosphere. The tropospheric ozone burdens in global atmospheric chemistry models disagree by a factor of 1.5, indicating an incomplete understanding of ozone sources and sinks. Here we examine the tropospheric ozone simulation in NASA Global Modeling and Assimilation Office’s (GMAO’s) GEOS model with the GEOS-Chem chemistry mechanism (version 14.2), using observations from satellites, aircraft, ozonesondes, and surface sites. This modeling framework is used to produce GMAO’s GEOS Composition Forecasts (GEOS-CF), and it has been updated extensively with new emission inventories, improved model physics, satellite data assimilation capability, and an up-to-date chemical mechanism that includes tropospheric halogen chemistry and NOx recycling from particulate nitrate. Earlier versions of the model using GEOS-Chem version 12.0 showed an underestimate in tropospheric ozone in the northern hemisphere. We evaluate the ozone simulation in the updated model, focusing on the effects of assimilating satellite NO 2 data from the Ozone Monitoring Instrument (OMI), constraining stratospheric ozone to satellite data, and updates to the NOx chemistry. We will examine changes in the vertical profiles of tropospheric ozone over the US in support of the Tropospheric Emissions: Monitoring of Pollution (TEMPO), and discuss implications for the tropospheric ozone budget.

Viral Shah↗

Estimating Wildfire-Generated Ozone Over North America Using Ozonesonde Profiles and a Differential Back Trajectory Technique

An objective method, employing HYSPLIT back-trajectories and Moderate Resolution Imaging Spectroradiometer (MODIS) fire observations, is developed to estimate ozone enhancement in air transported from regions of active forest fires at 18 ozone sounding sites located across North America. The Differential Back Trajectory (DBT) method compares mean differences between ozone concentrations associated with fire-affected and fire-unaffected parcels. It is applied to more than 1100 ozonesonde profiles collected from these sites during the summer months June to August, 2006, 2008, 2010 and 2011. Layers of high ozone associated with low humidity were first removed from the ozonesonde profiles to minimize the potential effects of stratospheric intrusions on the calculations. No significant influence on average ozone levels by North American fires was found for stations located at Arctic latitudes. The ozone enhancement for stations nearer large fires, such as Trinidad Head and Bratt’s Lake, was up to 324.8% of the TTOC (Total Tropospheric Ozone Column). Fire ozone accounted for up to 8.3% of TTOC at downwind sites such as Yarmouth, Sable Island, Narragansett, and Walsingham. The results are consistent with other studies that have reported an increase in ozone production with the age of the smoke plume.

Moderate Resolution Imaging Spectroradiometer (MOD↗

Ten Year Ozone Profile Record From Suomi NPP OMPS Limb Profiler

In this study, we evaluate a decadal ozone profile record derived from Suomi NPP Ozone Mapping and Profiler Suite (OMPS) Limb Profiler (LP). The data from OMPS LP were re-processed with the new retrieval algorithm from 2012 to present. The new reprocessing includes adjustments in both Level 1 and Level 2 algorithms. The sensor’s altitude registration, updates in radiometric calibrations, under-sampling and stray light corrections were addressed in Level 1 processing. The new retrieval algorithm (version 2.7) combines measurements from UV and VIS parts of the spectra to retrieve a single vertical ozone profile between 12.5 km (or cloud tops) and 57.5 km, unlike to previous version 2.5 where ozone profiles were retrieved independently from UV and VIS. To improve ozone retrievals in the Upper Troposphere Lower Stratosphere (UTLS) region, we implemented a new aerosol correction that assumes a gamma-function particle size distribution. In addition, ozone and nitrogen dioxide cross sections and climatologies were updated. We discuss sensitivity of the ozone retrievals to implemented changes in Level 1 and Level 2 algorithms. We focus our analysis on evaluation of the stability of the 10-year record from OMPS LP. We show results from the internal methods for characterizing the stability of the LP altitude registration and compare the LP reflectivity and ozone with the similar quantities measured by OMPS nadir sensors. Finally, we will show results from comparisons with independent satellite (MLS and SAGE III) and ozone sonde measurements.

Ozone↗

Surface Ozone Variability and Trends over the South African Highveld from 1990 to 2007

Surface ozone is a secondary air pollutant formed from reactions between nitrogen oxides (NOx = NO + NO2) and volatile organic compounds in the presence of sunlight. In this work we examine effects of the climate pattern known as the El Niño-Southern Oscillation (ENSO) and NOx variability on surface ozone from 1990 to 2007 over the South African Highveld, a heavily populated region in South Africa with numerous industrial facilities. Over summer and autumn (December-May) on the Highveld, El Niño, as signified by positive sea surface temperature (SST) anomalies over the central Pacific Ocean, is typically associated with drier and warmer than normal conditions favoring ozone formation. Conversely, La Niña, or negative SST anomalies over the central Pacific Ocean, is typically associated with cloudier and above normal rainfall conditions, hindering ozone production. We use a generalized regression model to identify any linear dependence that the Highveld ozone, measured at five air quality monitoring stations, may have on ENSO and NOx. Our results indicate that four out of the five stations exhibit a statistically significant sensitivity to ENSO at some point over the December-May period where El Niño amplifies ozone formation and La Niña reduces ozone formation. Three out of the five stations reveal statistically significant sensitivity to NOx variability, primarily in winter and spring. Accounting for ENSO and NOx effects throughout the study period of 18 years, two stations exhibit statistically significant negative ozone trends in spring, one station displays a statistically significant positive trend in August, and two stations show no statistically significant change in surface ozone.

NOx↗

The Global Structure of UTLS Ozone in GEOS-5: A Multi-Year Assimilation of EOS Aura Data

Eight years of ozone measurements retrieved from the Ozone Monitoring Instrument (OMI) and the Microwave Limb Sounder, both on the EOS Aura satellite, have been assimilated into the Goddard Earth Observing System version 5 (GEOS-5) data assimilation system. This study thoroughly evaluates this assimilated product, highlighting its potential for science. The impact of observations on the GEOS-5 system is explored by examining the spatial distribution of the observation-minus-forecast statistics. Independent data are used for product validation. The correlation coefficient of the lower-stratospheric ozone column with ozonesondes is 0.99 and the bias is 0.5%, indicating the success of the assimilation in reproducing the ozone variability in that layer. The upper-tropospheric assimilated ozone column is about 10% lower than the ozonesonde column but the correlation is still high (0.87). The assimilation is shown to realistically capture the sharp cross-tropopause gradient in ozone mixing ratio. Occurrence of transport-driven low ozone laminae in the assimilation system is similar to that obtained from the High Resolution Dynamics Limb Sounder (HIRDLS) above the 400 K potential temperature surface but the assimilation produces fewer laminae than seen by HIRDLS below that surface. Although the assimilation produces 5 - 8 fewer occurrences per day (up to approximately 20%) during the three years of HIRDLS data, the interannual variability is captured correctly. This data-driven assimilated product is complementary to ozone fields generated from chemistry and transport models. Applications include study of the radiative forcing by ozone and tracer transport near the tropopause.

GEOS-5↗

Global Distribution and Trends of Tropospheric Ozone: An Observation-Based Review

Tropospheric ozone plays a major role in Earth's atmospheric chemistry processes and also acts as an air pollutant and greenhouse gas. Due to its short lifetime, and dependence on sunlight and precursor emissions from natural and anthropogenic sources, tropospheric ozone's abundance is highly variable in space and time on seasonal, interannual and decadal time-scales. Recent, and sometimes rapid, changes in observed ozone mixing ratios and ozone precursor emissions inspired us to produce this up-to-date overview of tropospheric ozone's global distribution and trends. Much of the text is a synthesis of in situ and remotely sensed ozone observations reported in the peer-reviewed literature, but we also include some new and extended analyses using well-known and referenced datasets to draw connections between ozone trends and distributions in different regions of the world. In addition, we provide a brief evaluation of the accuracy of rural or remote surface ozone trends calculated by three state-of-the-science chemistry-climate models, the tools used by scientists to fill the gaps in our knowledge of global tropospheric ozone distribution and trends.

Mixing ratios↗

Understanding the Laminar Distribution of Tropospheric Ozone from Ground-Based, Airborne, Spaceborne, and Modeling Perspectives

Laminar ozone structure is a ubiquitous feature of tropospheric-ozone distributions resulting from dynamic and chemical atmospheric processes. Understanding the characteristics of these ozone laminae and the mechanisms responsible for producing them is important to outline the transport pathways of trace gases and to quantify the impact of different sources on tropospheric background ozone. In this study, we present a new method to detect ozone laminae to understand their climatological characteristics of occurrence frequency in terms of thickness and altitude. We employ both ground-based and airborne ozone lidar measurements and other synergistic observations and modeling to investigate the sources and mechanisms such as biomass burning transport, stratospheric intrusion, lightning-generated NOx, and nocturnal low-level jets that are responsible for depleted or enhanced tropospheric ozone layers. Spaceborne (e.g., OMI (Ozone Monitoring Instrument), TROPOMI (Tropospheric Monitoring Instrument), TEMPO (Tropospheric Emissions: Monitoring of Pollution)) measurements of these laminae will observe greater horizontal extent and lower vertical resolution than balloon-borne or lidar measurements will quantify. Using integrated ground-based, airborne, and spaceborne observations in a modeling framework affords insight into how to gain knowledge of both the vertical and horizontal evolution of these ubiquitous ozone laminae.

Tropospheric Ozone↗

Multidecadal Changes in the UTLS Ozone from the MERRA-2 Reanalysis and the GMI Chemistry Model

Long-term changes of ozone in the UTLS (Upper Troposphere / Lower Stratosphere) reflect the response to decreases in the stratospheric concentrations of ozone-depleting substances as well as changes in the stratospheric circulation induced by climate change. To date, studies of UTLS ozone changes and variability have relied mainly on satellite and in-situ observations as well as chemistry-climate model simulations. By comparison, the potential of reanalysis ozone data remains relatively untapped. This is despite evidence from recent studies, including detailed analyses conducted under SPARC (Scalable Processor Architecture) Reanalysis Intercomparison Project (S-RIP), that demonstrate that stratospheric ozone fields from modern atmospheric reanalyses exhibit good agreement with independent data while delineating issues related to inhomogeneities in the assimilated observations. In this presentation, we will explore the possibility of inferring long-term geographically and vertically resolved behavior of the lower stratospheric (LS) ozone from NASA's MERRA-2 (Modern-Era Retrospective Analysis for Research and Applications -2) reanalysis after accounting for the few known discontinuities and gaps in its assimilated input data. This work builds upon previous studies that have documented excellent agreement between MERRA-2 ozone and ozonesonde observations in the LS. Of particular importance is a relatively good vertical resolution of MERRA-2 allowing precise separation of tropospheric and stratospheric ozone contents. We also compare the MERRA-2 LS ozone results with the recently completed 37-year simulation produced using Goddard Earth Observing System in "replay" mode coupled with the GMI (Global Modeling Initiative) chemistry mechanism. Replay mode dynamically constrains the model with the MERRA-2 reanalysis winds, temperature, and pressure. We will emphasize the areas of agreement of the reanalysis and replay and interpret differences between them in the context of our increasing understanding of model transport driven by assimilated winds.

Ozone↗

Validation of Ozone Profile Retrievals Derived from the OMPS LP Version 2.5 Algorithm Against Correlative Satellite Measurements

The Limb Profiler (LP) is a part of the Ozone Mapping and Profiler Suite launched on board of the Suomi NPP satellite in October 2011. The LP measures solar radiation scattered from the atmospheric limb in ultraviolet and visible spectral ranges between the surface and 80 km. These measurements of scattered solar radiances allow for the retrieval of ozone profiles from cloud tops up to 55 km. The LP started operational observations in April 2012. In this study we evaluate more than 5.5 years of ozone profile measurements from the OMPS LP processed with the new NASA GSFC version 2.5 retrieval algorithm. We provide a brief description of the key changes that had been implemented in this new algorithm, including a pointing correction, new cloud height detection, explicit aerosol correction and a reduction of the number of wavelengths used in the retrievals. The OMPS LP ozone retrievals have been compared with independent satellite profile measurements obtained from the Aura Microwave Limb Sounder (MLS), Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) and Odin Optical Spectrograph and InfraRed Imaging System (OSIRIS). We document observed biases and seasonal differences and evaluate the stability of the version 2.5 ozone record over 5.5 years. Our analysis indicates that the mean differences between LP and correlative measurements are well within required +/- 10% between 18 and 42 km. In the upper stratosphere and lower mesosphere (>43 km) LP tends to have a negative bias. We find larger biases in the lower stratosphere and upper troposphere, but LP ozone retrievals have significantly improved in version 2.5 compared to version 2 due to the implemented aerosol correction. In the northern high latitudes we observe larger biases between 20 and 32 km due to the remaining thermal sensitivity issue. Our analysis shows that LP ozone retrievals agree well with the correlative satellite observations in characterizing vertical, spatial and temporal ozone distribution associated with natural processes, like the seasonal cycle and quasi-biennial oscillations. We found a small positive drift approx. 0.5%/yr in the LP ozone record against MLS and OSIRIS that is more pronounced at altitudes above 35 km. This pattern in the relative drift is consistent with a possible 100m drift in the LP sensor pointing detected by one of our altitude-resolving methods.

Ozone Mapping↗

Investigations on the Anthropogenic Reversal of the Natural Ozone Gradient Between Northern and Southern Midlatitudes

Our quantitative understanding of natural tropospheric ozone concentrations is limited by the paucity of reliable measurements before the 1980s. We utilize the existing measurements to compare the long-term ozone changes that occurred within the marine boundary layer at northern and southern midlatitudes. Since 1950 ozone concentrations have increased by a factor of 2.1 ± 0.2 in the Northern Hemisphere (NH) and are presently larger than in the Southern Hemisphere (SH), where only a much smaller increase has occurred. These changes are attributed to increased ozone production driven by anthropogenic emissions of photochemical ozone precursors that increased with industrial development. The greater ozone concentrations and increases in the NH are consistent with the predominant location of anthropogenic emission sources in that hemisphere. The available measurements indicate that this interhemispheric gradient was much smaller and was likely reversed in the pre-industrial troposphere with higher concentrations in the SH. Six Earth system model (ESM) simulations indicate similar total NH increases (1.9 with a standard deviation of 0.3), but they occurred more slowly over a longer time period, and the ESMs do not find higher pre-industrial ozone in the SH. Several uncertainties in the ESMs may cause these model–measurement disagreements: the assumed natural nitrogen oxide emissions may be too large, the relatively greater fraction of ozone injected by stratosphere–troposphere exchange to the NH may be overestimated, ozone surface deposition to ocean and land surfaces may not be accurately simulated, and model treatment of emissions of biogenic hydrocarbons and their photochemistry may not be adequate.

natural tropospheric ozone concentrations↗

Tropospheric Ozone Retrieval By A Combination of TROPOMI/S5P Measurements With BASCOE Assimilated Data

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 km 2 ) 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.

Satellite Retrieval↗

Changes in Anthropogenic Precursor Emissions Drive Shifts in the Ozone Seasonal Cycle Throughout the Northern Midlatitude Troposphere

Simulations by six Coupled Model Intercomparison Project Phase 6 (CMIP6) Earth system models indicate that the seasonal cycle of baseline tropospheric ozone at northern midlatitudes has been shifting since the mid-20th century. Beginning in ∼ 1940, the magnitude of the seasonal cycle increased by ∼10 ppb (measured from seasonal minimum to maximum), and the seasonal maximum shifted to later in the year by about 3 weeks. This shift maximized in the mid-1980s, followed by a reversal – the seasonal cycle decreased in amplitude and the maximum shifted back to earlier in the year. Similar changes are seen in measurements collected from the 1970s to the present. The timing of the seasonal cycle changes is generally concurrent with the rise and fall of anthropogenic emissions that followed industrialization and the subsequent implementation of air quality emission controls. A quantitative comparison of the temporal changes in the ozone seasonal cycle at sites in both Europe and North America with the temporal changes in ozone precursor emissions across the northern midlatitudes found a high degree of similarity between these two temporal patterns. We hypothesize that changing precursor emissions are responsible for the shift in the ozone seasonal cycle; this is supported by the absence of such seasonal shifts in southern midlatitudes where anthropogenic emissions are much smaller. We also suggest a mechanism by which changing emissions drive the changing seasonal cycle: increasing emissions of NOx allow summertime photochemical production of ozone to become more important than ozone transported from the stratosphere, and increasing volatile organic compounds (VOCs) lead to progressively greater photochemical ozone production in the summer months, thereby increasing the amplitude of the seasonal ozone cycle. Decreasing emissions of both precursor classes then reverse these changes. The quantitative parameter values that characterize the seasonal shifts provide useful benchmarks for evaluating model simulations, both against observations and between models.

Ozone↗